#### Sample records for aerosol particle sources

1. Sources and transformations of atmospheric aerosol particles

Science.gov (United States)

Cross, Eben Spencer

transported towards Europe. In this study, particles were highly processed prior to sampling, with residence times of a few days in the atmosphere. The MILAGRO campaign focused on the evolution of the Mexico City plume as it was transported north. During this study, regional and locally emitted particles were measured with residence times varying from minutes to days in the atmosphere. In both studies, the light scattering - AMS system provided detailed information about the density and composition of single particles, leading to important insights into how atmospheric processing transforms the particle properties. In Mexico City, the light scattering-AMS system was used for the first time as a true single particle mass spectrometer and revealed specific details about the atmospheric processing of primary particles from combustion sources. To quantify the radiative effects of the particles on climate, the processing and ultimate fate of primary emissions (often containing black carbon or soot) must be understood. To provide a solid basis for the interpretation of the data obtained during the field studies, experiments were conducted with a well characterized soot generation-sampling system developed by the Boston College research group. The laboratory soot source was combined with the light scattering - AMS system and a Cloud Condensation Nuclei Counter (CCNC) to measure the change in cloud-forming activity of soot particles as they are processed in the atmosphere. Because of the importance of black carbon in the atmosphere, several instruments have been developed to measure black carbon. In July of 2008, an intercomparison study of 18 instruments was conducted in the Boston College laboratory, with soot particles produced and processed to mimic a wide range of atmospherically-relevant conditions. Transformations in the physical, chemical, and optical properties of soot particles were monitored with the combined suite of aerosol instrumentation. Results from the

2. Sources and composition of urban aerosol particles

Science.gov (United States)

Vogt, M.; Johansson, C.; Mårtensson, M.; Struthers, H.; Ahlm, L.; Nilsson, D.

2011-09-01

From May 2008 to March 2009 aerosol emissions were measured using the eddy covariance method covering the size range 0.25 to 2.5 μm diameter (Dp) from a 105 m tower, in central Stockholm, Sweden. Supporting chemical aerosol data were collected at roof and street level. Results show that the inorganic fraction of sulfate, nitrate, ammonium and sea salt accounts for approximately 15% of the total aerosol mass traffic (as inferred from the ratio of the incremental concentrations of nitrogen oxides (NOx) and BC measured on a densely trafficked street) and the fluxes of non-volatile material at tower level are in close agreement, suggesting a traffic source of BC. We have estimated the emission factors (EFs) for non-volatile particles traffic activity data. Light (LDV) and heavy duty vehicle (HDV) EFs were estimated using multiple linear regression and reveal that for non-volatile particulate matter in the 0.25 to 0.6 μm Dp range, the EFHDV is approximately twice as high as the EFLDV, the difference not being statistically significant.

3. Sources and composition of urban aerosol particles

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M. Vogt

2011-09-01

Full Text Available From May 2008 to March 2009 aerosol emissions were measured using the eddy covariance method covering the size range 0.25 to 2.5 μm diameter (Dp from a 105 m tower, in central Stockholm, Sweden. Supporting chemical aerosol data were collected at roof and street level. Results show that the inorganic fraction of sulfate, nitrate, ammonium and sea salt accounts for approximately 15% of the total aerosol mass <1 μm Dp (PM1 with water soluble soil contributing 11% and water insoluble soil 47%. Carbonaceous compounds were at the most 27% of PM1 mass. It was found that heating the air from the tower to 200 °C resulted in the loss of approximately 60% of the aerosol volume at 0.25 μm Dp whereas only 40% of the aerosol volume was removed at 0.6 μm Dp. Further heating to 300 °C caused very little additional losses <0.6 μm Dp. The chemical analysis did not include carbonaceous compounds, but based on the difference between the total mass concentration and the sum of the analyzed non-carbonaceous materials, it can be assumed that the non-volatile particulate material (heated to 300 °C consists mainly of carbonaceous compounds, including elemental carbon. Furthermore, it was found that the non-volatile particle fraction <0.6 μm Dp correlated (r2 = 0.4 with the BC concentration at roof level in the city, supporting the assumption that the non-volatile material consists of carbonaceous compounds. The average diurnal cycles of the BC emissions from road traffic (as inferred from the ratio of the incremental concentrations of nitrogen oxides (NOx and BC measured on a densely trafficked street and the fluxes of non-volatile material at tower level are in close agreement, suggesting a traffic source of BC. We have estimated the emission factors (EFs for non

4. Sources of optically active aerosol particles over the Amazon forest

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Guyon, Pascal; Graham, Bim; Roberts, Gregory C.; Mayol-Bracero, Olga L.; Maenhaut, Willy; Artaxo, Paulo; Andreae, Meinrat O.

Size-fractionated ambient aerosol samples were collected at a pasture site and a primary rainforest site in the Brazilian Amazon Basin during two field campaigns (April-May and September-October 1999), as part of the European contribution to the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA-EUSTACH). The samples were analyzed for up to 19 trace elements by particle-induced X-ray emission analysis (PIXE), for equivalent black carbon (BC e) by a light reflectance technique and for mass concentration by gravimetric analysis. Additionally, we made continuous measurements of absorption and light scattering by aerosol particles. The vertical chemical composition gradients at the forest site have been discussed in a companion article (Journal of Geophysical Research-Atmospheres 108 (D18), 4591 (doi:4510.1029/2003JD003465)). In this article, we present the results of a source identification and quantitative apportionment study of the wet and dry season aerosols, including an apportionment of the measured scattering and absorption properties of the total aerosol in terms of the identified aerosol sources. Source apportionments (obtained from absolute principal component analysis) revealed that the wet and dry season aerosols contained the same three main components, but in different (absolute and relative) amounts: the wet season aerosol consisted mainly of a natural biogenic component, whereas pyrogenic aerosols dominated the dry season aerosol mass. The third component identified was soil dust, which was often internally mixed with the biomass-burning aerosol. All three components contributed significantly to light extinction during both seasons. At the pasture site, up to 47% of the light absorption was attributed to biogenic particles during the wet season, and up to 35% at the tower site during the wet-to-dry transition period. The results from the present study suggest that, in addition to pyrogenic particles, biogenic and soil dust aerosols must be

5. Source apportionment of single aerosol particles in the atmosphere of Shanghai city

Institute of Scientific and Technical Information of China (English)

2001-01-01

A nuclear microprobe with high spatial resolution and high analyti cal sensitivity was applied to analyze atmospheric aerosol at five monitoring sites in Shanghai city. Meantime, a new pattern recognition technique, which used the micro PIXE spectrum of a single aerosol particle as its fingerprint, was developed to identify the origin of the particle. The results showed that the major contributors to the at mosphere pollution were soil dust (31.6%), building dust (30.8%), and the next were vehicle exhaust (13.7%), metallurgic industry excrements (5.6%), oil combustion (5%) and coal combustion (2.3%). Besides these, about 10% of the particles could not be identified. Based on the cluster analysis of these particles, they could be divided into eight groups. By inference, they might belong to some sub-pollution sources from soil dust, building dust and metallurgic industry excrements. Moreover, some new pollution sources from tyres and chemical plants were also revealed.

6. The generation of diesel exhaust particle aerosols from a bulk source in an aerodynamic size range similar to atmospheric particles

Directory of Open Access Journals (Sweden)

Daniel J Cooney

2008-08-01

Full Text Available Daniel J Cooney1, Anthony J Hickey21Department of Biomedical Engineering; 2School of Pharmacy, University of North Carolina, Chapel Hill, NC, USAAbstract: The influence of diesel exhaust particles (DEP on the lungs and heart is currently a topic of great interest in inhalation toxicology. Epidemiological data and animal studies have implicated airborne particulate matter and DEP in increased morbidity and mortality due to a number of cardiopulmonary diseases including asthma, chronic obstructive pulmonary disorder, and lung cancer. The pathogeneses of these diseases are being studied using animal models and cell culture techniques. Real-time exposures to freshly combusted diesel fuel are complex and require significant infrastructure including engine operations, dilution air, and monitoring and control of gases. A method of generating DEP aerosols from a bulk source in an aerodynamic size range similar to atmospheric DEP would be a desirable and useful alternative. Metered dose inhaler technology was adopted to generate aerosols from suspensions of DEP in the propellant hydrofluoroalkane 134a. Inertial impaction data indicated that the particle size distributions of the generated aerosols were trimodal, with count median aerodynamic diameters less than 100 nm. Scanning electron microscopy of deposited particles showed tightly aggregated particles, as would be expected from an evaporative process. Chemical analysis indicated that there were no major changes in the mass proportion of 2 specific aromatic hydrocarbons (benzo[a]pyrene and benzo[k]fluoranthene in the particles resulting from the aerosolization process.Keywords: diesel exhaust particles, aerosol, inhalation toxicology

7. Isotope source apportionment of carbonaceous aerosol as a function of particle size and thermal refractiveness

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Masalaite, Agne; Holzinger, Rupert; Remeikis, Vidmantas; Röckmann, Thomas; Dusek, Ulrike

2016-04-01

The stable carbon isotopes can be used to get information about sources and processing of carbonaceous aerosol. We will present results from source apportionment of carbonaceous aerosol as a function of particle size thermal refractiveness. Separate source apportionment for particles smaller than 200 nm and for different carbon volatility classes are rarely reported and give new insights into aerosol sources in the urban environment. Stable carbon isotope ratios were measured for the organic carbon (OC) fraction and total carbon (TC) of MOUDI impactor samples that were collected on a coastal site (Lithuania) during the winter 2012 and in the city of Vilnius (Lithuania) during the winter of 2009. The 11 impactor stages spanned a size range from 0.056 to 18 μm, but only the 6 stages in the submicron range were analysed. The δ13C values of bulk total carbon (δ13CTC) were determined with an elemental analyser (Flash EA 1112) coupled with an isotope ratio mass spectrometer (Thermo Finnigan Delta Plus Advantage) (EA - IRMS). Meanwhile δ13COC was measured using thermal-desorption isotope ratio mass spectrometry (IRMS) system. This allows a rough separation of the more volatile OC fraction (desorbed in the oven of IRMS up to 250 0C) from the more refractory fraction (desorbed up to 400 0C). In this study we investigated the composition of organic aerosol desorbed from filter samples at different temperatures using the thermal-desorption proton-transfer-reaction mass spectrometry (TD-PTR-MS) technique. During winter-time in Lithuania we expect photochemistry and biogenic emissions to be of minor importance. The main sources of aerosol carbon should be fossil fuel and biomass combustion. In both sites, the coastal and the urban site, δ13C measurements give a clear indication that the source contributions differ for small and large particles. Small particles grants Nr. 820.01.001, and 834.08.002).

8. Sources and characteristics of fine particles over the Yellow Sea and Bohai Sea using online single particle aerosol mass spectrometer.

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Fu, Huaiyu; Zheng, Mei; Yan, Caiqing; Li, Xiaoying; Gao, Huiwang; Yao, Xiaohong; Guo, Zhigang; Zhang, Yuanhang

2015-03-01

Marine aerosols over the East China Seas are heavily polluted by continental sources. During the Chinese Comprehensive Ocean Experiment in November 2012, size and mass spectra of individual atmospheric particles in the size range from 0.2 to 2.0 μm were measured on board by a single particle aerosol mass spectrometer (SPAMS). The average hourly particle number (PN) was around 4560±3240 in the South Yellow Sea (SYS), 2900±3970 in the North Yellow Sea (NYS), and 1700±2220 in the Bohai Sea (BS). PN in NYS and BS varied greatly over 3 orders of magnitude, while that in SYS varied slightly. The size distributions were fitted with two log-normal modes. Accumulation mode dominated in NYS and BS, especially during episodic periods. Coarse mode particles played an important role in SYS. Particles were classified using an adaptive resonance theory based neural network algorithm (ART-2a). Six particle types were identified with secondary-containing, aged sea-salt, soot-like, biomass burning, fresh sea-salt, and lead-containing particles accounting for 32%, 21%, 18%, 16%, 4%, and 3% of total PN, respectively. Aerosols in BS were relatively enriched in particles from anthropogenic sources compared to SYS, probably due to emissions from more developed upwind regions and indicating stronger influence of continental outflow on marine environment. Variation of source types depended mainly on origins of transported air masses. This study examined rapid changes in PN, size distribution and source types of fine particles in marine atmospheres. It also demonstrated the effectiveness of high-time-resolution source apportionment by ART-2a.

9. Impact of interannual variations in aerosol particle sources on orographic precipitation over California's Central Sierra Nevada

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Creamean, J. M.; Ault, A. P.; White, A. B.; Neiman, P. J.; Ralph, F. M.; Minnis, P.; Prather, K. A.

2015-01-01

Aerosols that serve as cloud condensation nuclei (CCN) and ice nuclei (IN) have the potential to profoundly influence precipitation processes. Furthermore, changes in orographic precipitation have broad implications for reservoir storage and flood risks. As part of the CalWater field campaign (2009-2011), the variability and associated impacts of different aerosol sources on precipitation were investigated in the California Sierra Nevada using an aerosol time-of-flight mass spectrometer for precipitation chemistry, S-band profiling radar for precipitation classification, remote sensing measurements of cloud properties, and surface meteorological measurements. The composition of insoluble residues in precipitation samples collected at a surface site contained mostly local biomass burning and long-range transported dust and biological particles (2009), local sources of biomass burning and pollution (2010), and long-range transport from distant sources (2011). Although differences in the sources were observed from year-to-year, the most consistent source of dust and biological residues were associated with storms consisting of deep convective cloud systems with significant quantities of precipitation initiated in the ice phase. Further, biological residues were dominant (up to 40%) during storms with relatively warm cloud temperatures (up to -15 °C), supporting the important role bioparticles can play as ice nucleating particles. On the other hand, lower percentages of residues from local biomass burning and pollution were observed over the three winter seasons (on average 31 and 9%, respectively). When precipitation quantities were relatively low, these residues most likely served as CCN, forming smaller more numerous cloud droplets at the base of shallow cloud systems, and resulting in less efficient riming processes. The correlation between the source of aerosols within clouds and precipitation type and quantity will be further probed in models to understand the

10. Chemical composition and sources of coastal marine aerosol particles during the 2008 VOCALS-REx campaign

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Y.-N. Lee

2013-10-01

Full Text Available The chemical composition of aerosol particles (Dp ≤ 1.5 μm was measured over the southeast Pacific ocean during the VOCALS-REx experiment between 16~October and 15 November 2008 using the US DOE G-1 aircraft. The objective of these flights was to gain an understanding of the sources and evolution of these aerosols, and how they interacted with the marine stratus cloud layer that prevails in this region of the globe. Our measurements showed that the marine boundary layer (MBL aerosol mass was dominated by non-sea-salt SO42−, followed by Na+, Cl−, Org, NH4+, and NO3−, in decreasing order of importance; CH3SO3−1 (MSA, Ca2+, and K+ rarely exceeded their limits of detection of ~0.05 and ~0.15 μg m−3 for anions and cations, respectively. The aerosols were strongly acidic as the NH4+ to SO42− equivalence ratio was typically − deficits caused by both HNO3 and H2SO4, and were externally mixed with SO42− particles as the AMS detected no NO3− whilst uptake of HNO3 occurred only on SSA particles. The SSA loading as a function of wind speed agreed with that calculated from published relationships, and contributed only a small fraction of the total accumulation mode particle number. Vertical distribution of MBL SSA particles (Dp ≤ ~1.5 μm was uniform, suggesting a very limited dilution from entrainment of free tropospheric (FT air. It was inferred that because all of the aerosol species (except SSA exhibited a strong land-to-sea gradient, they were of continental origin. Comparison of relative changes in median values using LOWESS fits as proxies suggests that (1 an oceanic source of NH3 is present between 72° W and 76° W, and (2 additional organic aerosols from biomass burns or biogenic precursors were emitted from coastal regions south of 31° S, with possible cloud processing, and (3 FT contributions to MBL gas and aerosols were negligible. Positive Matrix Factorization analysis of organic aerosol mass spectra obtained with

11. Online laser desorption-multiphoton postionization mass spectrometry of individual aerosol particles: molecular source indicators for particles emitted from different traffic-related and wood combustion sources.

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Bente, Matthias; Sklorz, Martin; Streibel, Thorsten; Zimmermann, Ralf

2008-12-01

Direct inlet aerosol mass spectrometry plays an increasingly important role in applied and fundamental aerosol and nanoparticle research. Laser desorption/ionization (LDI) based techniques for single particle time-of-flight mass spectrometry (LDI-SP-TOFMS) are a promising approach in the chemical analysis of single aerosol particles, especially for the detection of inorganic species and distinction of particle classes. However, until now the detection of molecular organic compounds on a single particle basis has been difficult due to the high laser power densities which are required for the LDI process as well as due to the inherent matrix effects associated with this ionization technique. By the application of a two-step approach, where an IR desorption laser pulse is applied to perform a gentle desorption of organic material from the single particle surface and a second UV-laser performs the soft ionization of the desorbed species, this drawback of laser based single particles mass spectrometry can be overcome. The postionization of the desorbed molecules has been accomplished in this work by resonance enhanced multiphoton ionization (REMPI) using a KrF excimer laser (248 nm). REMPI allows an almost fragmentation free trace analysis of polycyclic aromatic hydrocarbons (PAHs) and their derivatives from individual single particles (laser desorption-REMPI postionization-single particle-time-of-flight mass spectrometry or LD-REMPI-SP-TOFMS). Crucial system parameters of the home-built aerosol mass spectrometer such as the power densities and the relative timing of both lasers were optimized with respect to the detectability of particle source specific organic signatures using well characterized standard particles. In a second step, the LD-REMPI-SP-TOFMS system was applied to analyze different real world aerosols (spruce wood combustion, gasoline car exhaust, beech wood combustion, and diesel car exhaust). It was possible to distinguish the particles from different

12. Physical properties of the arctic summer aerosol particles in relation to sources at Ny-Alesund, Svalbard

C G Deshpande; A K Kamra

2014-02-01

Measurements of the number concentration and size distribution of aerosol particles in the size range of 0.5–20 m diameter were made with an aerodynamic particle sizer at an Arctic site at Ny-Alesund, Svalbard in August–September 2007 during the International Polar Year 2007–2008. Data are analyzed to study the aerosol number concentration–wind speed relationships. The sea-salt particles of marine origin generated within the Arctic circle are identified as the main source of the Arctic summer aerosols. Total number concentration of aerosol particles increases with increase in wind speed, the increase being more when winds from open leads over the oceanic sector are reaching the station as compared to when winds from pack ice in other directions are reaching the station. The larger increase with winds from the oceanic sector is attributed to the enhanced bubble-breaking activity and increased entrainment of dimethyl sulphide particles at the sea surface. Although, the increase in total aerosol number concentration associated with the winds from the oceanic sector is spread over the whole range of particle sizes, the increase in coarse mode particles is more prominent than that in the accumulation mode particles. The age of airmass over pack ice is also an important factor to determine the aerosol concentration over the Arctic region. The process of rainout/washout of the aerosol particles due to drizzle/snowfall is an effective sink mechanism in the Arctic environment. The aerosol particle concentration starts decreasing within a few minutes from the start of these events but requires a few hours to restore to the normal background aerosol level after the end of event.

13. Primary and secondary organic aerosol origin by combined gas-particle phase source apportionment

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M. Crippa

2013-08-01

Full Text Available Secondary organic aerosol (SOA, a prominent fraction of particulate organic mass (OA, remains poorly constrained. Its formation involves several unknown precursors, formation and evolution pathways and multiple natural and anthropogenic sources. Here a combined gas-particle phase source apportionment is applied to wintertime and summertime data collected in the megacity of Paris in order to investigate SOA origin during both seasons. This was possible by combining the information provided by an aerosol mass spectrometer (AMS and a proton transfer reaction mass spectrometer (PTR-MS. A better constrained apportionment of primary OA (POA sources is also achieved using this methodology, making use of gas-phase tracers. These tracers made possible the discrimination between biogenic and continental/anthropogenic sources of SOA. We found that continental SOA was dominant during both seasons (24–50% of total OA, while contributions from photochemistry-driven SOA (9% of total OA and marine emissions (13% of total OA were also observed during summertime. A semi-volatile nighttime component was also identified (up to 18% of total OA during wintertime. This approach was successfully applied here and implemented in a new source apportionment toolkit.

14. Physical properties, chemical composition, sources, spatial distribution and sinks of indoor aerosol particles in a university lecture hall

Science.gov (United States)

Salma, I.; Dosztály, K.; Borsós, T.; Söveges, B.; Weidinger, T.; Kristóf, G.; Péter, N.; Kertész, Zs.

2013-01-01

PM10 mass, particle number (N) and CO2 concentrations, particle number size distributions and meteorological parameters were determined with high time resolution, and daily aerosol samples were collected in the PM10-2.0 and PM2.0 size fractions for chemical analysis in the middle of a university lecture hall for one week. Median concentrations for the PM10 mass and N of 15.3 μg m-3 and 3.7 × 103 cm-3, respectively were derived. The data are substantially smaller than the related outdoor levels or typical values for residences. There were considerable concentration differences for workdays, weekends and various lectures. Main sources of PM10 mass include the usage of chalk sticks for writing, wiping the blackboard, ordinary movements and actions of students and cleaning. High PM10 mass concentration levels up to 100 μg m-3 were realised for short time intervals after wiping the blackboard. The mass concentrations decreased rapidly after the emission source ceased to be active. Two classes of coarse particles were identified. General indoor dust particles exhibited a residence time of approximately 35 min, while the residence time for the chalk dust particles was approximately 20 min as lower estimates. Emission source rate for wiping the blackboard was estimated to be between 8 and 14 mg min-1. This represents a substantial emission rate but the source is active only up to 1 min. Suspension of the chalk (made mainly of gypsum) dust particles was confirmed by enrichment of Ca and S in the hall with respect to ambient urban aerosol. Contribution of ambient aerosol via the heating, ventilation and air conditioning (HVAC) facility was considerable for time intervals when the indoor sources of PM10 mass were not intensive. The HVAC facility introduces, however, the major amount of aerosol particles from the outdoors as far as their number concentration is regarded. Mean contribution of ultrafine particles to the total particle number was (69 ± 7)%, which is smaller

15. Long-term aerosol measurements in Gran Canaria, Canary Islands: Particle concentration, sources and elemental composition

Science.gov (United States)

Gelado-Caballero, MaríA. D.; López-GarcíA, Patricia; Prieto, Sandra; Patey, Matthew D.; Collado, Cayetano; HéRnáNdez-Brito, José J.

2012-02-01

There are very few sets of long-term measurements of aerosol concentrations over the North Atlantic Ocean, yet such data is invaluable in quantifying atmospheric dust inputs to this ocean region. We present an 8-year record of total suspended particles (TSP) collected at three stations on Gran Canaria Island, Spain (Taliarte at sea level, Tafira 269 m above sea level (a.s.l.) and Pico de la Gorra 1930 m a.s.l.). Using wet and dry deposition measurements, the mean dust flux was calculated at 42.3 mg m-2 d-1. Air mass back trajectories (HYSPLIT, NOAA) suggested that the Sahara desert is the major source of African dust (dominant during 32-50% of days), while the Sahel desert was the major source only 2-10% of the time (maximum in summer). Elemental composition ratios of African samples indicate that, despite the homogeneity of the dust in collected samples, some signatures of the bedrocks can still be detected. Differences were found for the Sahel, Central Sahara and North of Sahara regions in Ti/Al, Mg/Al and Ca/Al ratios, respectively. Elements often associated with pollution (Pb, Cd, Ni, Zn) appeared to share a common origin, while Cu may have a predominantly local source, as suggested by a decrease in the enrichment factor (EF) of Cu during dust events. The inter-annual variability of dust concentrations is investigated in this work. During winter, African dust concentration measurements at the Pico de la Gorra station were found to correlate with the North Atlantic Oscillation (NAO) index.

16. Identification of aerosol particle sources in semi-rural area of Kwabenya, near Accra, Ghana, by EDXRF techniques

DEFF Research Database (Denmark)

Aboh, Innocent Joy Kwame; Henrikson, Dag; Laursen, Jens

2009-01-01

is frequently exposed to Harmattan dust from the Sahara-Sahel region. In total 171 filters each of PM2.5 and PM(2.5-10) were collected during 1 year. Levels of elements, black carbon (BC) and mass, were determined for both particle sizes. Principal component analysis (PCA) was performed on the datasets from...... for different sources were identified from correlation coefficients and regression analysis of the data. Sahara sand aerosol was the major source in both study periods, but influence from biomass burning, sea-spray and metal industries was also observed....

17. Aerosol properties, source identification, and cloud processing in orographic clouds measured by single particle mass spectrometry on a central European mountain site during HCCT-2010

Science.gov (United States)

Roth, A.; Schneider, J.; Klimach, T.; Mertes, S.; van Pinxteren, D.; Herrmann, H.; Borrmann, S.

2016-01-01

Cloud residues and out-of-cloud aerosol particles with diameters between 150 and 900 nm were analysed by online single particle aerosol mass spectrometry during the 6-week study Hill Cap Cloud Thuringia (HCCT)-2010 in September-October 2010. The measurement location was the mountain Schmücke (937 m a.s.l.) in central Germany. More than 160 000 bipolar mass spectra from out-of-cloud aerosol particles and more than 13 000 bipolar mass spectra from cloud residual particles were obtained and were classified using a fuzzy c-means clustering algorithm. Analysis of the uncertainty of the sorting algorithm was conducted on a subset of the data by comparing the clustering output with particle-by-particle inspection and classification by the operator. This analysis yielded a false classification probability between 13 and 48 %. Additionally, particle types were identified by specific marker ions. The results from the ambient aerosol analysis show that 63 % of the analysed particles belong to clusters having a diurnal variation, suggesting that local or regional sources dominate the aerosol, especially for particles containing soot and biomass burning particles. In the cloud residues, the relative percentage of large soot-containing particles and particles containing amines was found to be increased compared to the out-of-cloud aerosol, while, in general, organic particles were less abundant in the cloud residues. In the case of amines, this can be explained by the high solubility of the amines, while the large soot-containing particles were found to be internally mixed with inorganics, which explains their activation as cloud condensation nuclei. Furthermore, the results show that during cloud processing, both sulfate and nitrate are added to the residual particles, thereby changing the mixing state and increasing the fraction of particles with nitrate and/or sulfate. This is expected to lead to higher hygroscopicity after cloud evaporation, and therefore to an increase of

18. Wind reduction by aerosol particles

Science.gov (United States)

Jacobson, Mark Z.; Kaufman, Yoram J.

2006-12-01

Aerosol particles are known to affect radiation, temperatures, stability, clouds, and precipitation, but their effects on spatially-distributed wind speed have not been examined to date. Here, it is found that aerosol particles, directly and through their enhancement of clouds, may reduce near-surface wind speeds below them by up to 8% locally. This reduction may explain a portion of observed disappearing winds'' in China, and it decreases the energy available for wind-turbine electricity. In California, slower winds reduce emissions of wind-driven soil dust and sea spray. Slower winds and cooler surface temperatures also reduce moisture advection and evaporation. These factors, along with the second indirect aerosol effect, may reduce California precipitation by 2-5%, contributing to a strain on water supply.

19. Vapor scavenging by atmospheric aerosol particles

Energy Technology Data Exchange (ETDEWEB)

Andrews, E.

1996-05-01

Particle growth due to vapor scavenging was studied using both experimental and computational techniques. Vapor scavenging by particles is an important physical process in the atmosphere because it can result in changes to particle properties (e.g., size, shape, composition, and activity) and, thus, influence atmospheric phenomena in which particles play a role, such as cloud formation and long range transport. The influence of organic vapor on the evolution of a particle mass size distribution was investigated using a modified version of MAEROS (a multicomponent aerosol dynamics code). The modeling study attempted to identify the sources of organic aerosol observed by Novakov and Penner (1993) in a field study in Puerto Rico. Experimentally, vapor scavenging and particle growth were investigated using two techniques. The influence of the presence of organic vapor on the particles hydroscopicity was investigated using an electrodynamic balance. The charge on a particle was investigated theoretically and experimentally. A prototype apparatus--the refractive index thermal diffusion chamber (RITDC)--was developed to study multiple particles in the same environment at the same time.

20. AEROSOL PARTICLE COLLECTOR DESIGN STUDY

Energy Technology Data Exchange (ETDEWEB)

Lee, S; Richard Dimenna, R

2007-09-27

A computational evaluation of a particle collector design was performed to evaluate the behavior of aerosol particles in a fast flowing gas stream. The objective of the work was to improve the collection efficiency of the device while maintaining a minimum specified air throughput, nominal collector size, and minimal power requirements. The impact of a range of parameters was considered subject to constraints on gas flow rate, overall collector dimensions, and power limitations. Potential improvements were identified, some of which have already been implemented. Other more complex changes were identified and are described here for further consideration. In addition, fruitful areas for further study are proposed.

1. On-line matrix addition for detecting aerosol particles

Institute of Scientific and Technical Information of China (English)

ZHOU; Liuzhu; ZHU; Yuan; GUO; Xiaoyong; ZHAO; Wenwu; ZHENG; Haiyang; Gu; Xuejun; FANG; Li; ZHANG; Weijun

2006-01-01

Single aerosol particles were measured by matrix-assisted laser desorption/ionization (MALDI) with an aerosol time-of-flight mass spectrometer (ATOFMS). The inlet to the ATOFMS was coupled with an evaporation/condensation flow cell that allowed matrix addition by condensation onto the particles. The coated particles entered the ion source through three-stage differentially pumped capillary inlet and were then ionized by a focused 266 nm Nd:YAG laser. The mass spectra and aerodynamic size of the single particles can be obtained simultaneously. The on-line matrix addition technique makes it possible to identify biological aerosols in real-time.

2. Long-term real-time measurements of aerosol particle composition in Beijing, China: seasonal variations, meteorological effects, and source analysis

Directory of Open Access Journals (Sweden)

Y. L. Sun

2015-05-01

Full Text Available High concentrations of fine particles (PM2.5 are frequently observed during all seasons in Beijing, China, leading to severe air pollution and human health problems in this megacity. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1 species (sulfate, nitrate, ammonium, chloride, and organics in Beijing using an Aerodyne Aerosol Chemical Speciation Monitor for 1 year, from July 2011 to June 2012. This is the first long-term, highly time-resolved (~ 15 min measurement of fine particle composition in China. The seasonal average (± 1σ mass concentration of NR-PM1 ranged from 52 (± 49 μg m−3 in the spring season to 62 (± 49 μg m−3 in the summer season, with organics being the major fraction (40–51%, followed by nitrate (17–25% and sulfate (12–17%. Organics and chloride showed pronounced seasonal variations, with much higher concentrations in winter than in the other seasons, due to enhanced coal combustion emissions. Although the seasonal variations of secondary inorganic aerosol (SIA = sulfate + nitrate + ammonium concentrations were not significant, higher contributions of SIA were observed in summer (57–61% than in winter (43–46%, indicating that secondary aerosol production is a more important process than primary emissions in summer. Organics presented pronounced diurnal cycles that were similar among all seasons, whereas the diurnal variations of nitrate were mainly due to the competition between photochemical production and gas–particle partitioning. Our data also indicate that high concentrations of NR-PM1 (> 60 μg m−3 are usually associated with high ambient relative humidity (RH (> 50% and that severe particulate pollution is characterized by different aerosol composition in different seasons. All NR-PM1 species showed evident concentration gradients as a function of wind direction, generally with higher values associated with wind from the south, southeast or east. This

3. Regional air quality in Leipzig, Germany: detailed source apportionment of size-resolved aerosol particles and comparison with the year 2000.

Science.gov (United States)

van Pinxteren, D; Fomba, K W; Spindler, G; Müller, K; Poulain, L; Iinuma, Y; Löschau, G; Hausmann, A; Herrmann, H

2016-07-18

A detailed source apportionment of size-resolved aerosol particles in the area of Leipzig, Germany, was performed. Sampling took place at four sites (traffic, traffic/residential, urban background, regional background) in parallel during summer 2013 and the winters 2013/14/15. Twenty-one samples were taken per season with a 5-stage Berner impactor and analysed for particulate mass, inorganic ions, organic and elemental carbon, water-soluble organic carbon, trace metals, and a wide range of organic species. The compositional data were used to estimate source contributions to particulate matter (PM) in quasi-ultrafine (up to 140 nm), accumulation mode, and coarse size ranges using Positive Matrix Factorisation (PMF) receptor modelling. Traffic (exhaust and general traffic emissions), coal combustion, biomass combustion, photochemistry, general secondary formation, cooking, fungal spores, urban dust, fresh sea/road salt, and aged sea salt were all found to contribute to different extents to observed PM concentrations. PMF derived estimates agreed reasonably with estimates from established macrotracer approaches. Quasi-ultrafine PM originated mainly from traffic (20-50%) and photochemistry (30-50%) in summer, while it was dominated by solid fuel (mainly biomass) combustion in winter (50-70%). Tentatively identified cooking aerosol contributed up to 36% on average at the residential site. For accumulation mode particles, two secondary sources typically contributed 40-90% to particle mass. In winter, biomass and coal combustion contributions were up to ca. 25% and 45%, respectively. Main sources of coarse particles were diverse and included nearly all PMF-resolved ones depending on season and air mass origin. For PM10, traffic (typically 20-40% at kerbside sites), secondary formation (30-60%), biomass combustion (10-15% in winter), and coal combustion (30-40% in winter with eastern air mass inflow) were the main quantified sources. At the residential site, contributions

4. Size distribution and source apportionment of polycyclic aromatic hydrocarbons (PAHs) in aerosol particle samples from the atmospheric environment of Delhi, India.

Science.gov (United States)

Gupta, Sandeep; Kumar, Krishan; Srivastava, Arun; Srivastava, Alok; Jain, V K

2011-10-15

Ambient aerosol particles were collected using a five-stage impactor at six different sites in Delhi. The impactor segregates the TSPM into five different sizes (viz. >10.9, 10.9-5.4, 5.4-1.6, 1.6-0.7, and 10.9+10.9 to 5.4+5.4 to 1.6μm) and fine (1.6 to 0.7+<0.7μm). It was observed that the dominant PAHs found were pyrene, benzo(a)pyrene, benzo(ghi)perylene and benzo(b)fluoranthene for both the coarse and fine fractions. Source apportionment of polycyclic aromatic hydrocarbons (PAHs) has been carried out using principal component analysis method (PCA) in both coarse and fine size modes. The major sources identified in this study, responsible for the elevated concentration of PAHs in Delhi, are vehicular emission and coal combustion. Some contribution from biomass burning was also observed.

5. Laboratory Experiments and Instrument Intercomparison Studies of Carbonaceous Aerosol Particles

Energy Technology Data Exchange (ETDEWEB)

Davidovits, Paul [Boston College, Chestnut Hill, MA (United States)

2015-10-20

Aerosols containing black carbon (and some specific types of organic particulate matter) directly absorb incoming light, heating the atmosphere. In addition, all aerosol particles backscatter solar light, leading to a net-cooling effect. Indirect effects involve hydrophilic aerosols, which serve as cloud condensation nuclei (CCN) that affect cloud cover and cloud stability, impacting both atmospheric radiation balance and precipitation patterns. At night, all clouds produce local warming, but overall clouds exert a net-cooling effect on the Earth. The effect of aerosol radiative forcing on climate may be as large as that of the greenhouse gases, but predominantly opposite in sign and much more uncertain. The uncertainties in the representation of aerosol interactions in climate models makes it problematic to use model projections to guide energy policy. The objective of our program is to reduce the uncertainties in the aerosol radiative forcing in the two areas highlighted in the ASR Science and Program Plan. That is, (1) addressing the direct effect by correlating particle chemistry and morphology with particle optical properties (i.e. absorption, scattering, extinction), and (2) addressing the indirect effect by correlating particle hygroscopicity and CCN activity with particle size, chemistry, and morphology. In this connection we are systematically studying particle formation, oxidation, and the effects of particle coating. The work is specifically focused on carbonaceous particles where the uncertainties in the climate relevant properties are the highest. The ongoing work consists of laboratory experiments and related instrument inter-comparison studies both coordinated with field and modeling studies, with the aim of providing reliable data to represent aerosol processes in climate models. The work is performed in the aerosol laboratory at Boston College. At the center of our laboratory setup are two main sources for the production of aerosol particles: (a

6. A conceptual framework for mixing structures in individual aerosol particles

Science.gov (United States)

Li, Weijun; Sun, Jiaxing; Xu, Liang; Shi, Zongbo; Riemer, Nicole; Sun, Yele; Fu, Pingqing; Zhang, Jianchao; Lin, Yangting; Wang, Xinfeng; Shao, Longyi; Chen, Jianmin; Zhang, Xiaoye; Wang, Zifa; Wang, Wenxing

2016-11-01

This study investigated the particle size- and age-dependent mixing structures of individual particles in clean and polluted air. Aerosols were classified into eight components: sea salt, mineral dust, fly ash, metal, soot, sulfates, nitrates, and organic matter (OM). Based on our aerosol classification, a particle that consists of two or more aerosol components can be defined as an internally mixed particle. Otherwise, it is considered to be an externally mixed particle. Within the internally mixed particle class, we identified four heterogeneous mixing structures: core-shell, dumbbell, OM coating, and dispersed OM, as well as one homogeneous-like mixing structure. Homogeneous-like mixing mainly occurred in fine particles (<1 µm), while the frequency of heterogeneously mixed particles increased with particle size. Our study demonstrated that particle mixing structures depend on particle size and location and evolve with time. OM-coating and core-shell structures are important indicators for particle aging in air as long as they are distant from specific emission sources. Long-range transported particles tended to have core-shell and OM-coating structures. We found that secondary aerosol components (e.g., sulfates, nitrates, and organics) determined particle mixing structures, because their phases change following particle hydration and dehydration under different relative humidities. Once externally mixed particles are transformed into internally mixed particles, they cannot revert to their former state, except when semivolatile aerosol components are involved. Categorizing mixing structures of individual particles is essential for studying their optical and hygroscopic properties and for tracing the development of their physical or chemical properties over time.

7. Characterizing gas flow from aerosol particle injectors

CERN Document Server

Horke, Daniel; Worbs, Lena; Küpper, Jochen

2016-01-01

A novel methodology for measuring gas flow from small orifices or nozzles into vacuum is presented. It utilizes a high-intensity femtosecond laser pulse to create a plasma within the gas plume produced by the nozzle, which is imaged by a microscope. Calibration of the imaging system at known chamber pressures allows for the extraction of absolute number densities, and we show detection down to helium densities of $4\\times10^{16}$~cm$^{-3}$ with a spatial resolution of a few micrometer. The technique is used to characterize the gas flow from a convergent-nozzle aerosol injector as used in single-particle diffractive imaging experiments at free-electron laser sources. Based on the measured gas-density profile we estimate the scattering background signal under typical operating conditions of single-particle imaging experiments and estimate that fewer than 50 photons per shot can be expected on the typical detector of such an experiment.

8. An overview of aerosol particle sensors for size distribution measurement

Directory of Open Access Journals (Sweden)

Panich Intra

2007-08-01

Full Text Available Fine aerosols are generally referred to airborne particles of diameter in submicron or nanometer size range. Measurement capabilities are required to gain understanding of these particle dynamics. One of the most important physical and chemical parameters is the particle size distribution. The aim of this article is to give an overview of recent development of already existing sensors for particle size distribution measurement based on electrical mobility determination. Available instruments for particle size measurement include a scanning mobility particle sizer (SMPS, an electrical aerosol spectrometer (EAS, an engine exhaust particle sizer (EEPS, a bipolar charge aerosol classifier (BCAC, a fast aerosol spectrometer (FAS a differential mobility spectrometer (DMS, and a CMU electrical mobility spectrometer (EMS. The operating principles, as well as detailed physical characteristics of these instruments and their main components consisting of a particle charger, a mobility classifier, and a signal detector, are described. Typical measurements of aerosol from various sources by these instruments compared with an electrical low pressure impactor (ELPI are also presented.

9. Coagulation in the presence of stochastic nano-particle sources

Science.gov (United States)

Vrtala, A.; Wagner, P. E.

2000-08-01

The behavior of atmospheric aerosols undergoing coagulation processes in the presence of aerosol particle sources with randomly distributed source strength is reported. Numerical calculations were performed for a set of different initial conditions and random source. It is shown that the interplay of aerosol formation and aging can lead to trimodal aerosols with modal radii corresponding to nucleation, the so called Aitken' and accumulation mode.

10. Carbonaceous aerosol particles from common vegetation in the Grand Canyon

Energy Technology Data Exchange (ETDEWEB)

Hallock, K.A.; Mazurek, M.A. (Brookhaven National Lab., Upton, NY (United States)); Cass, G.R. (California Inst. of Tech., Pasadena, CA (United States). Dept. of Environmental Engineering Science)

1992-05-01

The problem of visibility reduction in the Grand Canyon due to fine organic aerosol particles in the atmosphere has become an area of increased environmental concern. Aerosol particles can be derived from many emission sources. In this report, we focus on identifying organic aerosols derived from common vegetation in the Grand Canyon. These aerosols are expected to be significant contributors to the total atmospheric organic aerosol content. Aerosol samples from living vegetation were collected by resuspension of surface wax and resin components liberated from the leaves of vegetation common to areas of the Grand Canyon. The samples were analyzed using high-resolution gas chromatography/mass spectrometry (GC/MS). Probable identification of compounds was made by comparison of sample spectra with National Institute of Standards and Technology (NIST) mass spectral references and positive identification of compounds was made when possible by comparison with authentic standards as well as NIST references. Using these references, we have been able to positively identify the presence of n-alkane and n-alkanoic acid homolog series in the surface waxes of the vegetation sampled. Several monoterpenes, sesquiterpenes, and diterpenes were identified also as possible biogenic aerosols which may contribute to the total organic aerosol abundance leading to visibility reduction in the Grand Canyon.

11. Dynamics of neutral and charged aerosol particles

Energy Technology Data Exchange (ETDEWEB)

Leppae, J.

2012-07-01

Atmospheric aerosol particles have various climate effects and adverse health effects, which both depend on the size and number concentration of the particles. Freshly-formed particles are not large enough to impact neither health nor climate and they are most susceptible to removal by collisions with larger pre-existing particles. Consequently, the knowledge of both the formation and the growth rate of particles are crucially important when assessing the health and climate effects of atmospheric new particle formation. The purpose of this thesis is to increase our knowledge of the dynamics of neutral and charged aerosol particles with a specific interest towards the particle growth rate and processes affecting the aerosol charging state. A new model, Ion-UHMA, which simulates the dynamics of neutral and charged particles, was developed for this purpose. Simple analytical formulae that can be used to estimate the growth rate due to various processes were derived and used to study the effects of charged particles on the growth rate. It was found that the growth rate of a freshly-formed particle population due to condensation and coagulation could be significantly increased when a considerable fraction of the particles are charged. Finally, recent data-analysis methods that have been applied to the aerosol charging states obtained from the measurements were modified for a charge asymmetric framework. The methods were then tested on data obtained from aerosol dynamics simulations. The methods were found to be able to provide reasonable estimates on the growth rate and proportion of particles formed via ion-induced nucleation, provided that the growth rate is high enough and that the charged particles do not grow much more rapidly than the neutral ones. A simple procedure for estimating whether the methods are suitable for analysing data obtained in specific conditions was provided. In this thesis, the dynamics of neutral and charged aerosol particles were studied in

12. Single-particle characterization of the High Arctic summertime aerosol

Directory of Open Access Journals (Sweden)

B. Sierau

2014-01-01

Full Text Available Single-particle mass spectrometric measurements were carried out in the High Arctic north of 80° during summer 2008. The campaign took place onboard the icebreaker \\textit{Oden} and was part of the Arctic Summer Cloud Ocean Study (ASCOS. The instrument deployed was an Aerosol Time-of-Flight Mass Spectrometer (ATOFMS that provides information on the chemical composition of individual particles and their mixing state in real-time. Aerosols were sampled in the marine boundary layer at stations in the open ocean, in the marginal ice zone, and in the pack ice region. The largest fraction of particles detected for subsequent analysis in the size range of the ATOFMS between approximately 200 nm to 3000 nm in diameter showed mass spectrometric patterns indicating an internal mixing state and a biomass burning and/or biofuel source. The majority of these particles were connected to an air mass layer of elevated particle concentration mixed into the surface mixed layer from the upper part of the marine boundary layer. The second largest fraction was represented by sea salt particles. The chemical analysis of the over-ice sea salt aerosol revealed tracer compounds that reflect chemical aging of the particles during their long-range advection from the marginal ice zone, or open waters south thereof prior to detection at the ship. From our findings we conclude that long-range transport of particles is one source of aerosols in the High Arctic. To assess the importance of long-range particle sources for aerosol–cloud interactions over the inner Arctic in comparison to local and regional biogenic primary aerosol sources, the chemical composition of the detected particles was analyzed for indicators of marine biological origin. Only a~minor fraction showed chemical signatures of potentially ocean-derived primary particles of that kind. However, a chemical bias in the ATOFMS's detection capabilities observed during ASCOS might suggest a presence of a

13. Aerosol characteristics and sources for the Amazon Basin during the wet season

Science.gov (United States)

Artaxo, Paulo; Maenhaut, Willy; Stroms, Hedwig; van Grieken, Rene

1990-09-01

An attempt is made to obtain the main chemical and morphological characteristics of particles released to the atmosphere by the tropical rain forest during the wet season. Fine and coarse aerosol fractions were collected and analyzed for elemental composition by bulk and individual particle analysis techniques. Elemental concentrations were measured by the particle-induced X-ray emission technique. Absolute principal factor analysis was applied to the elemental concentrations in order to derive source profiles for the identified sources of aerosols. Total mass source apportionment was used to obtain a quantitative assessment of the biogenic aerosol component and of the other aerosol sources. Total aerosol mass source apportionment showed that biogenic particles account for 55-95 percent of the airborne concentrations, indicating that biogenic particles can play an important role in the global aerosol budget and in the global biogeochemical cycles of various elements.

14. Synthesis of nanosized metal particles from an aerosol

Directory of Open Access Journals (Sweden)

Srećko R. Stopić

2013-10-01

Full Text Available The synthesis of metallic nanoparticles from the precursor solution of salts using the ultrasonic spray pyrolysis method was considered in this work. During the control of process parameters (surface tension and density, the concentration of solution, residence time of aerosol in the reactor, presence of additives, gas flow rate, decomposition temperature of aerosol, type of precursor and working atmosphere it is possible to guide the process in order to obtain powders with such a morphology which satisfies more complex requirements for the desired properties of advanced engineering materials.  Significant advance in the improvement of powder characteristics (lower particles sizes, better spheroidity, higher surface area was obtained by the application of the ultrasonic generator for the preparation of aerosols. Ultrasonic spray pyrolysis is performed by the action of a powerful source of ultrasound on the corresponding precursor solution forming the aerosol with a constant droplet size, which depends on the characteristics of liquid and the frequency of ultrasound. The produced aerosols were transported into the hot reactor, which enables the reaction to occur in a very small volume of a particle and formation of  nanosized powder. Spherical, nanosized particles of metals (Cu, Ag, Au, Co were produced with new and improved physical and chemical characteristics at the IME, RWTH Aachen University. The high costs associated with small quantities of produced nanosized particles represent a limitation of the USP-method. Therefore, scale up of the ultrasonic spray pyrolysis was performed as a final target in the synthesis of nanosized powder.

15. Particle size dependent response of aerosol counters

Science.gov (United States)

Ankilov, A.; Baklanov, A.; Colhoun, M.; Enderle, K.-H.; Gras, J.; Julanov, Yu.; Kaller, D.; Lindner, A.; Lushnikov, A. A.; Mavliev, R.; McGovern, F.; O'Connor, T. C.; Podzimek, J.; Preining, O.; Reischl, G. P.; Rudolf, R.; Sem, G. J.; Szymanski, W. W.; Vrtala, A. E.; Wagner, P. E.; Winklmayr, W.; Zagaynov, V.

During an international workshop at the Institute for Experimental Physics of the University of Vienna, Austria, which was coordinated within the Committee on Nucleation and Atmospheric Aerosols (IAMAS-IUGG), 10 instruments for aerosol number concentration measurement were studied, covering a wide range of methods based on various different measuring principles. In order to investigate the detection limits of the instruments considered with respect to particle size, simultaneous number concentration measurements were performed for monodispersed aerosols with particle sizes ranging from 1.5 to 50 nm diameter and various compositions. The instruments considered show quite different response characteristics, apparently related to the different vapors used in the various counters to enlarge the particles to an optically detectable size. A strong dependence of the 50% cutoff diameter on the particle composition in correlation with the type of vapor used in the specific instrument was found. An enhanced detection efficiency for ultrafine hygroscopic sodium chloride aerosols was observed with water operated systems, an analogous trend was found for n-butanol operated systems with nonhygroscopic silver and tungsten oxide particles.

16. Organic aerosol processing in tropical deep convective clouds: Development of a new model (CRM-ORG) and implications for sources of particle number

Science.gov (United States)

Murphy, B. N.; Julin, J.; Riipinen, I.; Ekman, A. M. L.

2015-10-01

The difficulty in assessing interactions between atmospheric particles and clouds is due in part to the chemical complexity of the particles and to the wide range of length and timescales of processes occurring simultaneously during a cloud event. The new Cloud-Resolving Model with Organics (CRM-ORG) addresses these interactions by explicitly predicting the formation, transport, uptake, and re-release of surrogate organic compounds consistent with the volatility basis set framework within a nonhydrostatic, three-dimensional cloud-resolving model. CRM-ORG incorporates photochemical production, explicit condensation/evaporation of organic and inorganic vapors, and a comprehensive set of four different mechanisms describing particle formation from organic vapors and sulfuric acid. We simulate two deep convective cloud events over the Amazon rain forest in March 1998 and compare modeled particle size distributions with airborne observations made during the time period. The model predictions agree well with the observations for Aitken mode particles in the convective outflow (10-14 km) but underpredict nucleation mode particles by a factor of 20. A strong in-cloud particle formation process from organic vapors alone is necessary to reproduce even relatively low ultrafine particle number concentrations (~1500 cm-3). Sensitivity tests with variable initial aerosol loading and initial vertical aerosol profile demonstrate the complexity of particle redistribution and net gain or loss in the cloud. In-cloud particle number concentrations could be enhanced by as much as a factor of 3 over the base case simulation in the cloud outflow but were never reduced by more than a factor of 2 lower than the base. Additional sensitivity cases emphasize the need for constrained estimates of surface tension and affinity of organic vapors to ice surfaces. When temperature-dependent organic surface tension is introduced to the new particle formation mechanisms, the number concentration of

17. Giant dendritic carbonaceous particles in Soweto aerosols

Energy Technology Data Exchange (ETDEWEB)

Wentzel, M.; Annegarn, H.J.; Helas, G.; Weinbruch, S.; Balogh, A.G.; Sithole, J.S. [Max Planck Institute of Chemistry, Mainz (Germany). Biogeochemistry Dept.

1999-03-01

Gravimetric analyses of aerosol filter samples from Soweto, southwest of Johannesburg, have revealed an anomalous mass-size distribution. Instead of the coal fire generated aerosol forming sub-micron aerosols as expected, most of the mass of the winter smoke is in particles greater than 3{mu}m aerodynamic diameter. A high-resolution scanning electron microscope was used to examine coarse and fine-mode aerosol fractions from two contrasting sites in the conurbation. Unanticipated giant carbonaceous conglomerates (10-100 {mu}m diameter), which comprise the bulk of the aerosol mass on the filters examined, were found. The outer shape of the conglomerates tends towards spherical, rather than the branched, chain-like structures of high-temperature soot. Internal structure varies from highly dendritic with 20-nm-wide branches, through a coarser sponge-like structure to an almost solid melted toffee irregular surface. Possible modes of formation of these conglomerates are discussed in terms of condensation aerosols conglomeration, and subsequent partial melting or solvent condensation. The occurrence of the giant carbonaceous conglomerates as a general feature of the Soweto winter atmosphere explains the anomalous size-mass distribution results from bulk filter analyses.

18. A large source of low-volatility secondary organic aerosol.

Science.gov (United States)

Ehn, Mikael; Thornton, Joel A; Kleist, Einhard; Sipilä, Mikko; Junninen, Heikki; Pullinen, Iida; Springer, Monika; Rubach, Florian; Tillmann, Ralf; Lee, Ben; Lopez-Hilfiker, Felipe; Andres, Stefanie; Acir, Ismail-Hakki; Rissanen, Matti; Jokinen, Tuija; Schobesberger, Siegfried; Kangasluoma, Juha; Kontkanen, Jenni; Nieminen, Tuomo; Kurtén, Theo; Nielsen, Lasse B; Jørgensen, Solvejg; Kjaergaard, Henrik G; Canagaratna, Manjula; Maso, Miikka Dal; Berndt, Torsten; Petäjä, Tuukka; Wahner, Andreas; Kerminen, Veli-Matti; Kulmala, Markku; Worsnop, Douglas R; Wildt, Jürgen; Mentel, Thomas F

2014-02-27

Forests emit large quantities of volatile organic compounds (VOCs) to the atmosphere. Their condensable oxidation products can form secondary organic aerosol, a significant and ubiquitous component of atmospheric aerosol, which is known to affect the Earth's radiation balance by scattering solar radiation and by acting as cloud condensation nuclei. The quantitative assessment of such climate effects remains hampered by a number of factors, including an incomplete understanding of how biogenic VOCs contribute to the formation of atmospheric secondary organic aerosol. The growth of newly formed particles from sizes of less than three nanometres up to the sizes of cloud condensation nuclei (about one hundred nanometres) in many continental ecosystems requires abundant, essentially non-volatile organic vapours, but the sources and compositions of such vapours remain unknown. Here we investigate the oxidation of VOCs, in particular the terpene α-pinene, under atmospherically relevant conditions in chamber experiments. We find that a direct pathway leads from several biogenic VOCs, such as monoterpenes, to the formation of large amounts of extremely low-volatility vapours. These vapours form at significant mass yield in the gas phase and condense irreversibly onto aerosol surfaces to produce secondary organic aerosol, helping to explain the discrepancy between the observed atmospheric burden of secondary organic aerosol and that reported by many model studies. We further demonstrate how these low-volatility vapours can enhance, or even dominate, the formation and growth of aerosol particles over forested regions, providing a missing link between biogenic VOCs and their conversion to aerosol particles. Our findings could help to improve assessments of biosphere-aerosol-climate feedback mechanisms, and the air quality and climate effects of biogenic emissions generally.

19. Single particle multichannel bio-aerosol fluorescence sensor

Science.gov (United States)

Kaye, P. H.; Stanley, W. R.; Hirst, E.; Foot, E. V.; Baxter, K. L.; Barrington, S. J.

2005-05-01

We describe a prototype low-cost multi-channel aerosol fluorescence sensor designed for unattended deployment in medium to large area bio-aerosol detection networks. Individual airborne particles down to ~1μm in size are detected and sized by measurement of light scattered from a continuous-wave diode laser (660nm). This scatter signal is then used to trigger the sequential firing of two xenon sources which irradiate the particle with UV pulses at ~280 nm and ~370 nm, optimal for excitation of bio-fluorophores tryptophan and NADH (nicotinamide adenine dinucleotide) respectively. For each excitation wavelength, fluorescence is detected across two bands embracing the peak emissions of the same bio-fluorophores. Current measurement rates are up to ~125 particles/s, corresponding to all particles for concentrations up to 1.3 x 104 particles/l. Developments to increase this to ~500 particles/s are in hand. Device sensitivity is illustrated in preliminary data recorded from aerosols of E.coli, BG spores, and a variety of non-biological materials.

20. Nuclear track radiography of 'hot' aerosol particles

CERN Document Server

Boulyga, S F; Kievets, M K; Lomonosova, E M; Zhuk, I V; Yaroshevich, O I; Perelygin, V P; Petrova, R I; Brandt, R; Vater, P

1999-01-01

Nuclear track radiography was applied to identify aerosol 'hot' particles which contain elements of nuclear fuel and fallout after Chernobyl NPP accident. For the determination of the content of transuranium elements in radioactive aerosols the measurement of the alpha-activity of 'hot' particles by SSNTD was used in this work, as well as radiography of fission fragments formed as a result of the reactions (n,f) and (gamma,f) in the irradiation of aerosol filters by thermal neutrons and high energy gamma quanta. The technique allowed the sizes and alpha-activity of 'hot' particles to be determined without extracting them from the filter, as well as the determination of the uranium content and its enrichment by sup 2 sup 3 sup 5 U, sup 2 sup 3 sup 9 Pu and sup 2 sup 4 sup 1 Pu isotopes. Sensitivity of determination of alpha activity by fission method is 5x10 sup - sup 6 Bq per particle. The software for the system of image analysis was created. It ensured the identification of track clusters on an optical imag...

1. Aerosol nucleation induced by a high energy particle beam

DEFF Research Database (Denmark)

Enghoff, Martin Andreas Bødker; Pedersen, Jens Olaf Pepke; Uggerhøj, Ulrik I.

2011-01-01

We have studied sulfuric acid aerosol nucleation in an atmospheric pressure reaction chamber using a 580 MeV electron beam to ionize the volume of the reaction chamber. We find a clear contribution from ion-induced nucleation and consider this to be the first unambiguous observation of the ion......-effect on aerosol nucleation using a particle beam under conditions that resemble the Earth's atmosphere. By comparison with ionization using a gamma source we further show that the nature of the ionizing particles is not important for the ion-induced component of the nucleation. This implies that inexpensive...... ionization sources - as opposed to expensive accelerator beams - can be used for investigations of ion-induced nucleation....

2. Ice Nucleation Activity of Various Agricultural Soil Dust Aerosol Particles

Science.gov (United States)

Schiebel, Thea; Höhler, Kristina; Funk, Roger; Hill, Thomas C. J.; Levin, Ezra J. T.; Nadolny, Jens; Steinke, Isabelle; Suski, Kaitlyn J.; Ullrich, Romy; Wagner, Robert; Weber, Ines; DeMott, Paul J.; Möhler, Ottmar

2016-04-01

Recent investigations at the cloud simulation chamber AIDA (Aerosol Interactions and Dynamics in the Atmosphere) suggest that agricultural soil dust has an ice nucleation ability that is enhanced up to a factor of 10 compared to desert dust, especially at temperatures above -26 °C (Steinke et al., in preparation for submission). This enhancement might be caused by the contribution of very ice-active biological particles. In addition, soil dust aerosol particles often contain a considerably higher amount of organic matter compared to desert dust particles. To test agricultural soil dust as a source of ice nucleating particles, especially for ice formation in warm clouds, we conducted a series of laboratory measurements with different soil dust samples to extend the existing AIDA dataset. The AIDA has a volume of 84 m3 and operates under atmospherically relevant conditions over wide ranges of temperature, pressure and humidity. By controlled adiabatic expansions, the ascent of an air parcel in the troposphere can be simulated. As a supplement to the AIDA facility, we use the INKA (Ice Nucleation Instrument of the KArlsruhe Institute of Technology) continuous flow diffusion chamber based on the design by Rogers (1988) to expose the sampled aerosol particles to a continuously increasing saturation ratio by keeping the aerosol temperature constant. For our experiments, soil dust was dry dispersed into the AIDA vessel. First, fast saturation ratio scans at different temperatures were performed with INKA, sampling soil dust aerosol particles directly from the AIDA vessel. Then, we conducted the AIDA expansion experiment starting at a preset temperature. The combination of these two different methods provides a robust data set on the temperature-dependent ice activity of various agriculture soil dust aerosol particles with a special focus on relatively high temperatures. In addition, to extend the data set, we investigated the role of biological and organic matter in more

3. Aerosol nucleation induced by a high energy particle beam

DEFF Research Database (Denmark)

Enghoff, Martin Andreas Bødker; Pedersen, Jens Olaf Pepke; Uggerhøj, Ulrik I.

atmospheric conditions using a 580 MeV electron beam to ionize the volume of the reaction chamber. We find a clear and significant contribution from ion induced nucleation and consider this to be an unambiguous observation of the ion-effect on aerosol nucleation using a particle beam under conditions not far......The effect of ions in aerosol nucleation is a subject where much remains to be discovered. That ions can enhance nucleation has been shown by theory, observations, and experiments. However, the exact mechanism still remains to be determined. One question is if the nature of the ionization affects...... the nucleation. This is an essential question since many experiments have been performed using radioactive sources that ionize differently than the cosmic rays which are responsible for the majority of atmospheric ionization. Here we report on an experimental study of sulphuric acid aerosol nucleation under near...

4. Aerosol composition and sources during the Chinese Spring Festival: fireworks, secondary aerosol, and holiday effects

Science.gov (United States)

Jiang, Q.; Sun, Y. L.; Wang, Z.; Yin, Y.

2015-06-01

Aerosol particles were characterized by an Aerodyne aerosol chemical speciation monitor along with various collocated instruments in Beijing, China, to investigate the role of fireworks (FW) and secondary aerosol in particulate pollution during the Chinese Spring Festival of 2013. Three FW events, exerting significant and short-term impacts on fine particles (PM2.5), were observed on the days of Lunar New Year, Lunar Fifth Day, and Lantern Festival. The FW were shown to have a large impact on non-refractory potassium, chloride, sulfate, and organics in submicron aerosol (PM1), of which FW organics appeared to be emitted mainly in secondary, with its mass spectrum resembling that of secondary organic aerosol (SOA). Pollution events (PEs) and clean periods (CPs) alternated routinely throughout the study. Secondary particulate matter (SPM = SOA + sulfate + nitrate + ammonium) dominated the total PM1 mass on average, accounting for 63-82% during nine PEs in this study. The elevated contributions of secondary species during PEs resulted in a higher mass extinction efficiency of PM1 (6.4 m2 g-1) than during CPs (4.4 m2 g-1). The Chinese Spring Festival also provides a unique opportunity to study the impact of reduced anthropogenic emissions on aerosol chemistry in the city. Primary species showed ubiquitous reductions during the holiday period with the largest reduction being in cooking organic aerosol (OA; 69%), in nitrogen monoxide (54%), and in coal combustion OA (28%). Secondary sulfate, however, remained only slightly changed, and the SOA and the total PM2.5 even slightly increased. Our results have significant implications for controlling local primary source emissions during PEs, e.g., cooking and traffic activities. Controlling these factors might have a limited effect on improving air quality in the megacity of Beijing, due to the dominance of SPM from regional transport in aerosol particle composition.

5. Identification of origin of single aerosol particles using polycapillary X-ray lens

Energy Technology Data Exchange (ETDEWEB)

Sun Tianxi [Key Laboratory of Beam Technology and Materials Modification of Ministry of Education, Beijing Normal University, Beijing 100875 (China) and Institute of Low Energy Nuclear Physics, Beijing Normal University, Beijing 100875 (China) and Beijing Radiation Center, Beijing 100875 (China)], E-mail: stxbeijing@163.com; Liu Zhiguo; Zhu Guanghua; Liu Hui [Key Laboratory of Beam Technology and Materials Modification of Ministry of Education, Beijing Normal University, Beijing 100875 (China); Institute of Low Energy Nuclear Physics, Beijing Normal University, Beijing 100875 (China); Beijing Radiation Center, Beijing 100875 (China); Xu Qing [Institute of High Energy Physics, Chinese Academy of Science, Beijing 100039 (China); Li Yude; Wang Guangpu; Sun Hongbo; Luo Ping; Pan Qiuli; Ding Xunliang [The Key Laboratory of Beam Technology and Materials Modification of Ministry of Education, Beijing Normal University, Beijing 100875 (China); Institute of Low Energy Nuclear Physics, Beijing Normal University, Beijing 100875 (China); Beijing Radiation Center, Beijing 100875 (China)

2009-01-15

A micro X-ray fluorescence (Micro-XRF) spectrometer based on a polycapillary focusing X-ray lens (PFXRL) and a laboratory X-ray source was designed to carry out the XRF analysis of single aerosol particles. The minimum detection limit (MDL) of this Micro-XRF spectrometer was 9 ppm for the Fe-K{alpha}. The percentage of the particles of vehicle exhaust among aerosol particles was studied in Beijing, Chinese capital, during the test of odd-even driving restrictions for Beijing 2008 Olympics Games. This Micro-XRF spectrometer had potential applications in the analysis of single aerosol particles.

6. On the composition of ammonia–sulfuric-acid ion clusters during aerosol particle formation

OpenAIRE

S. Schobesberger; Franchin, A.; Bianchi, F.(University of Turin, Turin, I-10125, Italy); L. Rondo; Duplissy, J.; Kürten, A.; Ortega, I. K.; Metzger, A.; R. Schnitzhofer; Almeida, J; Amorim, A.; Dommen, J.; Dunne, E.M.; Ehn, M.; S. Gagné

2015-01-01

The formation of particles from precursor vapors is an important source of atmospheric aerosol. Research at the Cosmics Leaving OUtdoor Droplets (CLOUD) facility at CERN tries to elucidate which vapors are responsible for this new-particle formation, and how in detail it proceeds. Initial measurement campaigns at the CLOUD stainless-steel aerosol chamber focused on investigating particle formation from ammonia (NH3) and sulfuric acid (H2SO4). Experiments were conducted in th...

7. On the composition of ammonia-sulfuric acid clusters during aerosol particle formation

OpenAIRE

S. Schobesberger; Franchin, A.; Bianchi, F.(University of Turin, Turin, I-10125, Italy); L. Rondo; Duplissy, J.; Kürten, A.; Ortega, I. K.; Metzger, A.; R. Schnitzhofer; Almeida, J; Amorim, A.; Dommen, J.; Dunne, E.M.; Ehn, M.; S. Gagné

2014-01-01

The formation of particles from precursor vapors is an important source of atmospheric aerosol. Research at the Cosmics Leaving OUtdoor Droplets (CLOUD) facility at CERN tries to elucidate which vapors are responsible for this new particle formation, and how in detail it proceeds. Initial measurement campaigns at the CLOUD stainless-steel aerosol chamber focused on investigating particle formation from ammonia (NH3) and sulfuric acid (H2SO4). Experiments wer...

8. Methods of analyzing composition of aerosol particles

Science.gov (United States)

Reilly, Peter T.A.

2013-02-12

An aerosol particle analyzer includes a laser ablation chamber, a gas-filled conduit, and a mass spectrometer. The laser ablation chamber can be operated at a low pressure, which can be from 0.1 mTorr to 30 mTorr. The ablated ions are transferred into a gas-filled conduit. The gas-filled conduit reduces the electrical charge and the speed of ablated ions as they collide and mix with buffer gases in the gas-filled conduit. Preferably, the gas filled-conduit includes an electromagnetic multipole structure that collimates the nascent ions into a beam, which is guided into the mass spectrometer. Because the gas-filled conduit allows storage of vast quantities of the ions from the ablated particles, the ions from a single ablated particle can be analyzed multiple times and by a variety of techniques to supply statistically meaningful analysis of composition and isotope ratios.

9. Connecting Chemistry and Climate through Aerosol Particles : Laboratory and Field Studies of Cloud Condensation Nuclei /

OpenAIRE

2014-01-01

The influence of aerosol particles on the Earth's climate is a major driver of scientific uncertainty in assessing future conditions. The importance of aerosols in their role as cloud condensation nuclei (CCN) and ice nuclei (IN), known as the Aerosol Indirect Effect, is most poorly understood. The number concentration of CCN available to nucleate droplets can have important influences on cloud albedo, lifetime, and propensity to form precipitation. Natural sources are of particular importanc...

10. Glyoxal and Methylglyoxal in Atlantic Seawater and marine Aerosol Particles

Science.gov (United States)

van Pinxteren, Manuela; Herrmann, Hartmut

2014-05-01

The two α-dicarbonyls glyoxal (CHOCHO; GLY) and methylglyoxal (CH3COCHO; MGLY) have attracted increasing attention over the past years because of their potential role in secondary organic aerosol formation. Recently Sinreich et al. (2010) suggested the open ocean as an important (so far unknown) source for GLY in the atmosphere. To date, there are few available field data of these compounds in the marine area. In this study we present measurements of GLY and MGLY in seawater and marine aerosol particles sampled during a transatlantic Polarstern cruise in spring 2011. In seawater we especially investigated the sea surface microlayer (sampled with the glass plate technique) as it is the direct interface between ocean and atmosphere. Analytical measurements were based on derivatisation with o-(2,3,4,5,6-Pentafluorobenzyl)-hydroxylamine reagent, solvent extraction and GC-MS (SIM) analysis. The results show that GLY and MGLY are present in the sea surface microlayer of the ocean and corresponding bulkwater with average concentrations of 228 ng L-1 (GLY) and 196 ng L-1 (MGLY). Significant enrichment (factor of 4) of GLY and MGLY in the sea surface microlayer was found implying photochemical production of the two carbonyls though a clear connection to global radiation was not observed. On aerosol particles, both carbonyls were detected (average concentration 0.2 ng m-3) and are strongly connected to each other, suggesting similar formation mechanisms. Both carbonyls show a very good correlation with particulate oxalate, supporting the idea of a secondary formation of oxalic acid via GLY and MGLY. A slight correlation of the two carbonyls in the sea surface microlayer and in the aerosol particles was found at co-located sampling areas. In summary, the results of GLY and MGLY in marine aerosol particles and in the oceanic water give first insights towards interaction processes of these alpha dicarbonyls between ocean and atmosphere (van Pinxteren and Herrmann (2013

11. Single-particle Analyses of Compositions, Morphology, and Viscosity of Aerosol Particles Collected During GoAmazon2014

Science.gov (United States)

Adachi, K.; Gong, Z.; Bateman, A. P.; Martin, S. T.; Cirino, G. G.; Artaxo, P.; Sedlacek, A. J., III; Buseck, P. R.

2014-12-01

Single-particle analysis using transmission electron microscopy (TEM) shows composition and morphology of individual aerosol particles collected during the GoAmazon2014 campaign. These TEM results indicate aerosol types and mixing states, both of which are important for evaluating particle optical properties and cloud condensation nuclei activity. The samples were collected at the T3 site, which is located in the Amazon forest with influences from the urban pollution plume from Manaus. Samples were also collected from the T0 site, which is in the middle of the jungle with minimal to no influences of anthropogenic sources. The aerosol particles mainly originated from 1) anthropogenic pollution (e.g., nanosphere soot, sulfate), 2) biogenic emissions (e.g., primary biogenic particles, organic aerosols), and 3) long-range transport (e.g., sea salts). We found that the biogenic organic aerosol particles contain homogeneously distributed potassium. Particle viscosity is important for evaluating gas-particle interactions and atmospheric chemistry for the particles. Viscosity can be estimated from the rebounding behavior at controlled relative humidities, i.e., highly viscous particles display less rebound on a plate than low-viscosity particles. We collected 1) aerosol particles from a plate (non-rebounded), 2) those that had rebounded from the plate and were then captured onto an adjacent sampling plate, and 3) particles from ambient air using a separate impactor sampler. Preliminary results show that more than 90% of non-rebounded particles consisted of nanosphere soot with or without coatings. The coatings mostly consisted of organic matter. Although rebounded particles also contain nanosphere soot (number fraction 64-69%), they were mostly internally mixed with sulfate, organic matter, or their mixtures. TEM tilted images suggested that the rebounded particles were less deformed on the substrate, whereas the non-rebounded particles were more deformed, which could

12. A missing source of aerosols in Antarctica - beyond long-range transport, phytoplankton, and photochemistry

Science.gov (United States)

Giordano, Michael R.; Kalnajs, Lars E.; Avery, Anita; Goetz, J. Douglas; Davis, Sean M.; DeCarlo, Peter F.

2017-01-01

Understanding the sources and evolution of aerosols is crucial for constraining the impacts that aerosols have on a global scale. An unanswered question in atmospheric science is the source and evolution of the Antarctic aerosol population. Previous work over the continent has primarily utilized low temporal resolution aerosol filters to answer questions about the chemical composition of Antarctic aerosols. Bulk aerosol sampling has been useful in identifying seasonal cycles in the aerosol populations, especially in populations that have been attributed to Southern Ocean phytoplankton emissions. However, real-time, high-resolution chemical composition data are necessary to identify the mechanisms and exact timing of changes in the Antarctic aerosol. The recent 2ODIAC (2-Season Ozone Depletion and Interaction with Aerosols Campaign) field campaign saw the first ever deployment of a real-time, high-resolution aerosol mass spectrometer (SP-AMS - soot particle aerosol mass spectrometer - or AMS) to the continent. Data obtained from the AMS, and a suite of other aerosol, gas-phase, and meteorological instruments, are presented here. In particular, this paper focuses on the aerosol population over coastal Antarctica and the evolution of that population in austral spring. Results indicate that there exists a sulfate mode in Antarctica that is externally mixed with a mass mode vacuum aerodynamic diameter of 250 nm. Springtime increases in sulfate aerosol are observed and attributed to biogenic sources, in agreement with previous research identifying phytoplankton activity as the source of the aerosol. Furthermore, the total Antarctic aerosol population is shown to undergo three distinct phases during the winter to summer transition. The first phase is dominated by highly aged sulfate particles comprising the majority of the aerosol mass at low wind speed. The second phase, previously unidentified, is the generation of a sub-250 nm aerosol population of unknown composition

13. A large source of low-volatility secondary organic aerosol

DEFF Research Database (Denmark)

Ehn, Mikael; Thornton, Joel A.; Kleist, Einhard;

2014-01-01

particles from sizes of less than three nanometres up to the sizes of cloud condensation nuclei (about one hundred nanometres) in many continental ecosystems requires abundant, essentially non-volatile organic vapours, but the sources and compositions of such vapours remain unknown. Here we investigate......Forests emit large quantities of volatile organic compounds (VOCs) to the atmosphere. Their condensable oxidation products can form secondary organic aerosol, a significant and ubiquitous component of atmospheric aerosol, which is known to affect the Earth's radiation balance by scattering solar...... radiation and by acting as cloud condensation nuclei. The quantitative assessment of such climate effects remains hampered by a number of factors, including an incomplete understanding of how biogenic VOCs contribute to the formation of atmospheric secondary organic aerosol. The growth of newly formed...

14. Secondary organic aerosol formation from fossil fuel sources contribute majority of summertime organic mass at Bakersfield

Science.gov (United States)

Secondary organic aerosols (SOA), known to form in the atmosphere from oxidation of volatile organic compounds (VOCs) emitted by anthropogenic and biogenic sources, are a poorly understood but substantial component of atmospheric particles. In this study, we examined the chemic...

15. Comprehensive airborne characterization of aerosol from a major bovine source

Directory of Open Access Journals (Sweden)

A. Sorooshian

2008-06-01

Full Text Available We report an extensive airborne characterization of aerosol downwind of a massive bovine source in the San Joaquin Valley (California on two flights during July 2007. The Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS Twin Otter probed chemical composition, particle size distribution, mixing state, sub- and supersaturated water uptake behavior, light scattering properties, and the interrelationship between these parameters and meteorology. Total PM1.0 levels and concentrations of organics, nitrate, and ammonium were enhanced in the plume from the source as compared to the background aerosol. Organics dominated the plume aerosol mass (~56–64%, followed either by sulfate or nitrate, and then ammonium. Particulate amines were detected in the plume aerosol by a particle-into-liquid sampler (PILS and via mass spectral markers in the Aerodyne cToF-AMS. Amines were found to be a significant atmospheric base even in the presence of ammonia; particulate amine concentrations are estimated as at least 14–23% of that of ammonium in the plume. Enhanced sub- and supersaturated water uptake and reduced refractive indices were coincident with lower organic mass fractions, higher nitrate mass fractions, and the detection of amines. Kinetic limitations due to hydrophobic organic material are shown to have likely suppressed droplet growth. After removing effects associated with size distribution and mixing state, the normalized activated fraction of cloud condensation nuclei (CCN increased as a function of the subsaturated hygroscopic growth factor, with the highest activated fractions being consistent with relatively lower organic mass fractions and higher nitrate mass fractions. Subsaturated hygroscopic growth factors for the organic fraction of the aerosol are estimated based on employing the Zdanovskii-Stokes Robinson (ZSR mixing rule. Representative values for a parameterization treating particle water uptake in both the

16. Comprehensive airborne characterization of aerosol from a major bovine source

Directory of Open Access Journals (Sweden)

H. Jonsson

2008-09-01

Full Text Available We report an extensive airborne characterization of aerosol downwind of a massive bovine source in the San Joaquin Valley (California on two flights during July 2007. The Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS Twin Otter probed chemical composition, particle size distribution, mixing state, sub- and supersaturated water uptake behavior, light scattering properties, and the interrelationship between these parameters and meteorology. Total PM1.0 levels and concentrations of organics, nitrate, and ammonium were enhanced in the plume from the source as compared to the background aerosol. Organics dominated the plume aerosol mass (~56–64%, followed either by sulfate or nitrate, and then ammonium. Particulate amines were detected in the plume aerosol by a particle-into-liquid sampler (PILS and via mass spectral markers in the Aerodyne C-ToF-AMS. Amines were found to be a significant atmospheric base even in the presence of ammonia; particulate amine concentrations are estimated as at least 14–23% of that of ammonium in the plume. Enhanced sub- and supersaturated water uptake and reduced refractive indices were coincident with lower organic mass fractions, higher nitrate mass fractions, and the detection of amines. The likelihood of suppressed droplet growth owing to kinetic limitations from hydrophobic organic material is explored. After removing effects associated with size distribution and mixing state, the normalized activated fraction of cloud condensation nuclei (CCN increased as a function of the subsaturated hygroscopic growth factor, with the highest activated fractions being consistent with relatively lower organic mass fractions and higher nitrate mass fractions. Subsaturated hygroscopic growth factors for the organic fraction of the aerosol are estimated based on employing the Zdanovskii-Stokes Robinson (ZSR mixing rule. Representative values for a parameterization treating particle water

17. Sulfur isotope analyses of individual aerosol particles in the urban aerosol at a central European site (Mainz, Germany

Directory of Open Access Journals (Sweden)

B. Winterholler

2008-05-01

Full Text Available Sulfur isotope analysis of atmospheric aerosols is a well established tool for identifying sources of sulfur in the atmosphere, estimating emission factors, and tracing the spread of sulfur from anthropogenic sources through ecosystems. Conventional gas mass spectrometry averages the isotopic compositions of several different types of sulfur aerosol particles, and therefore masks the individual isotopic signatures. In contrast, the new single particle technique presented here determines the isotopic signature of the individual particles.

Primary aerosol particles retain the original isotopic signature of their source. The isotopic composition of secondary sulfates depends on the isotopic composition of precursor SO2 and the oxidation process. The fractionation with respect to the source SO2 is −9‰ for homogeneous and +16.5‰ for heterogeneous oxidation. The sulfur isotope ratio of secondary sulfate particles can therefore be used to identify the oxidation pathway by which this sulfate was formed. With the new single particle technique, different types of primary and secondary sulfates were first identified based on their chemical composition, and then their individual isotopic signature was measured separately. Our samples were collected in Mainz, Germany, in an urban environment. Secondary sulfates (ammonium sulfate, gypsum, mixed sulfates and coatings on silicates or organic aerosol dominated sulfate loadings in our samples. Comparison of the chemical and isotopic composition of secondary sulfates showed that the isotopic composition was homogeneous, independent of the chemical composition. This is typical for particles that derive from in-cloud processing. The isotopic composition of the source SO2 of secondary sulfates was calculated based on the isotopic composition of particles with known oxidation pathway and showed a strong dependence on wind direction. The contribution of heterogeneous

18. Microphysical processing of aerosol particles in orographic clouds

Directory of Open Access Journals (Sweden)

S. Pousse-Nottelmann

2015-01-01

Full Text Available An explicit and detailed treatment of cloud-borne particles allowing for the consideration of aerosol cycling in clouds has been implemented in the regional weather forecast and climate model COSMO. The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener-Bergeron-Findeisen process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snow flakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snow flakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. However, the processes not only impact the total aerosol number and mass, but also the shape of the aerosol size distributions by enhancing the internally mixed/soluble accumulation mode and generating coarse mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases the cloud droplet number concentration with possible

19. Hygroscopicity and chemical composition of Antarctic sub-micrometre aerosol particles and observations of new particle formation

Directory of Open Access Journals (Sweden)

E. Asmi

2009-12-01

Full Text Available The Antarctic near-coastal sub-micrometre aerosol particle features in summer were characterised based on measured data on aerosol hygroscopicity, size distributions, volatility and chemical ion and organic carbon mass concentrations. Hysplit model was used to calculate the history of the air masses to predict the particle origin. Additional measurements of meteorological parameters were utilised. The hygroscopic properties of particles mostly resembled those of marine aerosols. The measurements took place at 130 km from the Southern Ocean, which was the most significant factor affecting the particle properties. This is explained by the lack of additional sources on the continent of Antarctica. The Southern Ocean was thus a likely source of the particles and nucleating and condensing vapours. The particles were very hygroscopic (HGF 1.75 at 90 nm and very volatile. Most of the sub-100 nm particle volume volatilised below 100 °C. Based on chemical data, particle hygroscopic and volatile properties were explained by a large fraction of non-neutralised sulphuric acid together with organic material. The hygroscopic growth factors assessed from chemical data were similar to measured. Hygroscopicity was higher in dry continental air masses compared with the moist marine air masses. This was explained by the aging of the marine organic species and lower methanesulphonic acid volume fraction together with the changes in the inorganic aerosol chemistry as the aerosol had travelled long time over the continental Antarctica. Special focus was directed in detailed examination of the observed new particle formation events. Indications of the preference of negative over positive ions in nucleation could be detected. However, in a detailed case study, the neutral particles dominated the particle formation process. Freshly nucleated particles had the smallest hygroscopic growth factors, which increased subsequent to particle aging.

20. Hygroscopicity and chemical composition of Antarctic sub-micrometre aerosol particles and observations of new particle formation

Directory of Open Access Journals (Sweden)

E. Asmi

2010-05-01

Full Text Available The Antarctic near-coastal sub-micrometre aerosol particle features in summer were characterised based on measured data on aerosol hygroscopicity, size distributions, volatility and chemical ion and organic carbon mass concentrations. Hysplit model was used to calculate the history of the air masses to predict the particle origin. Additional measurements of meteorological parameters were utilised. The hygroscopic properties of particles mostly resembled those of marine aerosols. The measurements took place at 130 km from the Southern Ocean, which was the most significant factor affecting the particle properties. This is explained by the lack of additional sources on the continent of Antarctica. The Southern Ocean was thus a likely source of the particles and nucleating and condensing vapours. The particles were very hygroscopic (HGF 1.75 at 90 nm and very volatile. Most of the sub-100 nm particle volume volatilised below 100 °C. Based on chemical data, particle hygroscopic and volatile properties were explained by a large fraction of non-neutralised sulphuric acid together with organic material. The hygroscopic growth factors assessed from chemical data were similar to measured. Hygroscopicity was higher in dry continental air masses compared with the moist marine air masses. This was explained by the aging of the marine organic species and lower methanesulphonic acid volume fraction together with the changes in the inorganic aerosol chemistry as the aerosol had travelled long time over the continental Antarctica. Special focus was directed in detailed examination of the observed new particle formation events. Indications of the preference of negative over positive ions in nucleation could be detected. However, in a detailed case study, the neutral particles dominated the particle formation process. Freshly nucleated particles had the smallest hygroscopic growth factors, which increased subsequent to particle aging.

1. Fluorescence spectra and elastic scattering characteristics of atmospheric aerosol in Las Cruces, New Mexico, USA: Variability of concentrations and possible constituents and sources of particles in various spectral clusters

Science.gov (United States)

Pinnick, R. G.; Fernandez, E.; Rosen, J. M.; Hill, S. C.; Wang, Y.; Pan, Y. L.

2013-02-01

The UV-excited laser-induced-fluorescence (UV-LIF) spectra of single atmospheric particles and the three-band integrating-nephelometer elastic scattering of atmospheric aerosol were measured during four approximately 24-h periods on May 2007 in Las Cruces, New Mexico, USA. Aerosol scattering measurements in the nephelometer red channel (50-nm band centered at 700-nm) ranged from around 3-10 times the molecular (Rayleigh) scattering background. On average 22.8% of particles with size greater than about 1 μm diameter have fluorescence above a preset fluorescence threshold. A hierarchical cluster analysis indicates that most of the single-particle UV-LIF spectra fall into about 10 categories (spectral clusters) as found previously at other geographic sites (Pinnick et al., 2004; Pan et al., 2007). The clusters include spectra characteristic of various humic/fulvic acids, humic-like-substances (HULIS), chemically aged terpenes, fungal spores, polycyclic aromatic hydrocarbons, bacteria, cellulose/pollens, and mixtures of various organic carbon compounds. By far the most populated cluster category is similar to those of chemically aged terpenes/humic-materials; on average this population comprises about 62% of fluorescent particles. Clusters with spectra similar to that of some HULIS aerosol contain on average 10.0% of particles; those characteristic of some fungal spores (or perhaps mixtures of aromatic organic compounds) 8.4% of particles; bacteria-like spectra 1.6% of particles; and cellulose/pollen-like spectra 0.8% of particles. Measurements of fluorescent particles over relatively short (24 min) periods reveal that the concentrations of particles in the most populated clusters are highly correlated, suggesting that the particles populating them derive from the same region; these particles might be composed of crustal material coated with secondary organic carbon. On the other hand, concentrations of particles having cellulose-like spectra are generally

2. Particle size distribution of the stratospheric aerosol from SCIAMACHY limb measurements

Science.gov (United States)

Rozanov, Alexei; Malinina, Elizaveta; Rozanov, Vladimir; Hommel, Rene; Burrows, John

2016-04-01

Stratospheric aerosols are of a great scientific interest because of their crucial role in the Earth's radiative budget as well as their contribution to chemical processes resulting in ozone depletion. While the permanent aerosol background in the stratosphere is determined by the tropical injection of SO2, COS and sulphate particles from the troposphere, major perturbations of the stratospheric aerosol layer result form an uplift of SO2 after strong volcanic eruptions. Satellite measurements in the visible spectral range represent one of the most important sources of information about the vertical distribution of the stratospheric aerosol on the global scale. This study employs measurements of the scattered solar light performed in the limb viewing geometry from the space borne spectrometer SCIAMACHY, which operated onboard the ENVISAT satellite, from August 2002 to April 2012. A retrieval approach to obtain parameters of the stratospheric aerosol particle size distribution will be reported along with the sensitivity studies and first results.

3. Characterization of aerosol composition, concentrations, and sources at Baengnyeong Island, Korea using an aerosol mass spectrometer

Science.gov (United States)

Lee, Taehyoung; Choi, Jinsoo; Lee, Gangwoong; Ahn, Junyoung; Park, Jin Soo; Atwood, Samuel A.; Schurman, Misha; Choi, Yongjoo; Chung, Yoomi; Collett, Jeffrey L.

2015-11-01

To improve understanding of the sources and chemical properties of particulate pollutants on the western side of the Korean Peninsula, an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) measured non-refractory fine (PM1) particles from May to November, 2011 at Baengnyeong Island, South Korea. Organic matter and sulfate were generally the most abundant species and exhibited maximum concentrations of 36 μg/m3 and 39 μg/m3, respectively. Nitrate concentrations peaked at 32 μg/m3 but were typically much lower than sulfate and organic matter concentrations. May, September, October, and November featured the highest monthly average concentrations, with lower concentrations typically observed from June through August. Potential source contribution function (PSCF) analysis and individual case studies revealed that transport from eastern China, an area with high SO2 emissions, was associated with high particulate sulfate concentrations at the measurement site. Observed sulfate aerosol sometimes was fully neutralized by ammonium but often was acidic; the average ammonium to sulfate molar ratio was 1.49. Measured species size distributions revealed a range of sulfate particle size distributions with modes between 100 and 600 nm. Organic aerosol source regions were widespread, including contributions from eastern China and South Korea. Positive matrix factorization (PMF) analysis indicated three "factors," or types of organic aerosol, comprising one primary, hydrocarbon-like organic aerosol (HOA) and two oxidized organic aerosol (OOA) components, including a more oxidized (MO-OOA) and a less oxidized (LO-OOA) oxidized organic aerosol. On average, HOA and OOA contributed 21% and 79% of the organic mass (OM), respectively, with the MO-OOA fraction nearly three times as abundant as the LO-OOA fraction. Biomass burning contributions to observed OM were low during the late spring/early summer agricultural burning season in eastern China, since

4. Microphysical processing of aerosol particles in orographic clouds

Directory of Open Access Journals (Sweden)

S. Pousse-Nottelmann

2015-08-01

aerosol cycling in clouds has been implemented into COSMO-Model, the regional weather forecast and climate model of the Consortium for Small-scale Modeling (COSMO. The effects of aerosol scavenging, cloud microphysical processing and regeneration upon cloud evaporation on the aerosol population and on subsequent cloud formation are investigated. For this, two-dimensional idealized simulations of moist flow over two bell-shaped mountains were carried out varying the treatment of aerosol scavenging and regeneration processes for a warm-phase and a mixed-phase orographic cloud. The results allowed us to identify different aerosol cycling mechanisms. In the simulated non-precipitating warm-phase cloud, aerosol mass is incorporated into cloud droplets by activation scavenging and released back to the atmosphere upon cloud droplet evaporation. In the mixed-phase cloud, a first cycle comprises cloud droplet activation and evaporation via the Wegener–Bergeron–Findeisen (WBF process. A second cycle includes below-cloud scavenging by precipitating snow particles and snow sublimation and is connected to the first cycle via the riming process which transfers aerosol mass from cloud droplets to snowflakes. In the simulated mixed-phase cloud, only a negligible part of the total aerosol mass is incorporated into ice crystals. Sedimenting snowflakes reaching the surface remove aerosol mass from the atmosphere. The results show that aerosol processing and regeneration lead to a vertical redistribution of aerosol mass and number. Thereby, the processes impact the total aerosol number and mass and additionally alter the shape of the aerosol size distributions by enhancing the internally mixed/soluble Aitken and accumulation mode and generating coarse-mode particles. Concerning subsequent cloud formation at the second mountain, accounting for aerosol processing and regeneration increases the cloud droplet number concentration with possible implications for the ice crystal number

5. Optimized sparse-particle aerosol representations for modeling cloud-aerosol interactions

Science.gov (United States)

Fierce, Laura; McGraw, Robert

2016-04-01

Sparse representations of atmospheric aerosols are needed for efficient regional- and global-scale chemical transport models. Here we introduce a new framework for representing aerosol distributions, based on the method of moments. Given a set of moment constraints, we show how linear programming can be used to identify collections of sparse particles that approximately maximize distributional entropy. The collections of sparse particles derived from this approach reproduce CCN activity of the exact model aerosol distributions with high accuracy. Additionally, the linear programming techniques described in this study can be used to bound key aerosol properties, such as the number concentration of CCN. Unlike the commonly used sparse representations, such as modal and sectional schemes, the maximum-entropy moment-based approach is not constrained to pre-determined size bins or assumed distribution shapes. This study is a first step toward a new aerosol simulation scheme that will track multivariate aerosol distributions with sufficient computational efficiency for large-scale simulations.

6. Quantitative ED-EPMA of Individual Particles and its Application for Characterization of Atmospheric Aerosol Particles

Science.gov (United States)

Ro, C.

2008-12-01

correlated with longer residence times over the continent (interaction with anthropogenic emissions) and in marine atmosphere (coagulation with deliquesced sea-salts). (2) Six urban aerosol samples collected in a megacity of Korea, namely Incheon, during a period of March 9-15, 2006 were characterized. Many different particle types, such as "soil-derived particles", "reacted sea-salts", "reacted CaCO3-containing particles", "genuine sea-salts", "reacted sea-salts + others", "Fe-containing particles", "anthropogenic organics", (NH4)2SO4, "K-containing particles", and "fly ashes", can be identified and their emission source, transport, and reactivity in the air can be elucidated. Also, different characteristics of the samples were clearly revealed. (3) When the technique was applied for the characterization of indoor subway station aerosols, it was observed that iron-containing particles are predominant. Agglomerated iron-containing particles, nano-size particles adsorbed on the other particles, and partially oxidized iron particles were frequently encountered, which implies that Iron-containing particles are generated mainly by the friction between break pad, wheel, and rails.

7. Particle Acceleration in Astrophysical Sources

CERN Document Server

Amato, Elena

2015-01-01

Astrophysical sources are extremely efficient accelerators. Some sources emit photons up to multi-TeV energies, a signature of the presence, within them, of particles with energies much higher than those achievable with the largest accelerators on Earth. Even more compelling evidence comes from the study of Cosmic Rays, charged relativistic particles that reach the Earth with incredibly high energies: at the highest energy end of their spectrum, these subatomic particles are carrying a macroscopic energy, up to a few Joules. Here I will address the best candidate sources and mechanisms as cosmic particle accelerators. I will mainly focus on Galactic sources such as Supernova Remnants and Pulsar Wind Nebulae, which being close and bright, are the best studied among astrophysical accelerators. These sources are held responsible for most of the energy that is put in relativistic particles in the Universe, but they are not thought to accelerate particles up to the highest individual energies, $\\approx 10^{20}$ eV...

8. Marine submicron aerosol gradients, sources and sinks

Science.gov (United States)

Ceburnis, Darius; Rinaldi, Matteo; Ovadnevaite, Jurgita; Martucci, Giovanni; Giulianelli, Lara; O'Dowd, Colin D.

2016-10-01

Aerosol principal sources and sinks over eastern North Atlantic waters were studied through the deployment of an aerosol chemistry gradient sampling system. The chemical gradients of primary and secondary aerosol components - specifically, sea salt (SS), water-insoluble organic matter (WIOM), water-soluble organic matter (WSOM), nitrate, ammonium, oxalate, amines, methanesulfonic acid (MSA) and water-soluble organic nitrogen (WSON) - were examined in great detail. Sea salt fluxes were estimated by the boundary layer box model and ranged from 0.3 to 3.5 ng m-2 s-1 over the wind speed range of 5-12 m s-1 and compared well with the derived fluxes from existing sea salt source parameterisations. The observed seasonal pattern of sea salt gradients was mainly driven by wind stress in addition to the yet unquantified effect of marine OM modifying fractional contributions of SS and OM in sea spray. WIOM gradients were a complex combination of rising and waning biological activity, especially in the flux footprint area, and wind-driven primary sea spray production supporting the coupling of recently developed sea spray and marine OM parameterisations.

9. Effect of source location on particle dispersion in displacement ventilation rooms

Institute of Scientific and Technical Information of China (English)

Ke Zhong; Yanming Kang; Youjun Wang

2008-01-01

A proposed computer model for predicting aerosol particle dispersion in indoor spaces was validated with experimental data found in the literature,and is then used to study the effect of the area and point source locations on particle dispersion in displacement ventilation (DV) rooms.The results show that aerosol source location has a strong impact on the spatial distribution and removal rate of indoor particles.Particle removal performance depends strongly on ventilation efficiency and particle deposition rate on indoor surfaces.Important consideration for both relative ventilation efficiency and deposition rate consists of the position of the aerosol source relative to the main airflow pattern and the occupied zone.

10. Identification of characteristic mass spectrometric markers for primary biological aerosol particles and comparison with field data from submicron pristine aerosol particles

Science.gov (United States)

Freutel, F.; Schneider, J.; Zorn, S. R.; Drewnick, F.; Borrmann, S.; Hoffmann, T.; Martin, S. T.

2009-04-01

The contribution of primary biological aerosol (PBA) to the total aerosol particle concentration is estimated to range between 25 and 80%, depending on location and season. Especially in the tropical rain forest it is expected that PBA is a major source of particles in the supermicron range, and is also an important fraction of the submicron aerosol. PBA particles like plant fragments, pollen, spores, fungi, viruses etc. contain chemical compounds as proteins, sugars, amino acids, chlorophyll, and cellular material as cellulose. For this reason we have performed mass spectrometric laboratory measurements (Aerodyne C-ToF and W-ToF AMS, single particle laser ablation instrument SPLAT) on pure submicron aerosol particles containing typical PBA compounds in order to identify typical mass spectral patterns of these compounds and to explain the observed fragmentation patterns on the basis of molecular structures. These laboratory data were compared to submicron particle mass spectra obtained during AMAZE-08 (Amazonian Aerosol CharacteriZation Experiment, Brazil, February/March 2008). The results indicate that characteristic m/z ratios for carbohydrates (e.g., glucose, saccharose, levoglucosan, mannitol) can be identified, for example m/z = 60(C2H4O2+) or m/z = 61(C2H5O2+). Certain characteristic peaks for amino acids were also identified in the laboratory experiments. In the field data from AMAZE-08, these characteristic peaks for carbohydrates and amino acids were found, and their contribution to the total organic mass was estimated to about 5%. Fragment ions from peptides and small proteins were also identified in laboratory experiments. Larger proteins, however, seem to become oxidized to CO2+ to a large extend in the vaporizing process of the AMS. Thus, detection of proteins in atmospheric aerosol particles with the AMS appears to be difficult.

11. Accommodation coefficient of HOBr on deliquescent sodium bromide aerosol particles

Directory of Open Access Journals (Sweden)

M. Wachsmuth

2002-01-01

Full Text Available Uptake of HOBr on sea salt aerosol, sea salt brine or ice is believed to be a key process providing a source of photolabile bromine (Br2 and sustaining ozone depletion cycles in the Arctic troposphere. In the present study, uptake of HOBr on sodium bromide (NaBr aerosol particles was investigated at an extremely low HOBr concentration of 300 cm-3 using the short-lived radioactive isotopes 83-86Br. Under these conditions, at maximum one HOBr molecule was taken up per particle. The rate of uptake was clearly limited by the mass accommodation coefficient, which was calculated to be 0.6 ± 0.2. This value is a factor of 10 larger than estimates used in earlier models. The atmospheric implications are discussed using the box model "MOCCA'', showing that the increase of the accommodation coefficient of HOBr by a factor of 10 only slightly affects net ozone loss, but significantly increases chlorine release.

12. DUSTER lidar: transatlantic transport of aerosol particles from the Sahara and other sources: first results from the recently installed lidar and sunphotometer in Natal/Brazil

Science.gov (United States)

Landulfo, Eduardo; Lopes, Fábio J. S.; Montilla, Elena; Guedes, Anderson G.; Hoelzemann, Judith J.; Fernandez, José H.; Alados-Arboledas, Lucas; Guerrero-Rascado, Juan L.

2016-10-01

The lidar confederative network for monitoring optical properties of aerosol on Latin America, LALINET, faces an important challenger to cover a large area of Latin America with so few lidar systems. Currently in Brazil there are only three operative lidar systems, two operating on Southeastern region and other on North region of Brazil. Taking into accounting the large dimension of Brazilian territory there is a lack of lidar system monitoring in several regions. In 2014 Laser Environmental Application Laboratory (LEAL) at Nuclear and Energy Research Institute (IPEN) together with Federal University of Rio Grande do Norte (UFRN), have started the first efforts to install a depolarization lidar system at the city of Natal-RN (5°50'29'' S ,35°11'57'' W, 0 m asl), in the Northeast region of Brazil. This new lidar station intends to be in the future integrated to the LALINET network, and has as a first aim to detect and to identify aerosol layers from Saharan dust and biomass burning type arriving from African continent. To examine these transports it is paramount to have a temporally and spatially well resolved observational platforms, which will be able to describe with accuracy the transport patterns followed by these aerosol layers over the Atlantic. To yield a good coverage based on the previously mentioned requirements satellite-based platforms are very well suited, but unless a geostationary system is provided a reasonable temporal representativeness may not be achieved. Our current study is devoted to the first results aiming to detect and identify aerosol layers arriving over the Northeastern region of the South American continent, with a lidar and a sun-photometer recently installed in the city of Natal. Here we present the first aerosol observation results with the lidar system and the sunphotometer carried out from January through May 2016 with the indication of potential dust and other-type aerosol layers through some backscatter profiles.

13. Basic phenomena utilised in aerosol particle measurement techniques; Hiukkasmittaustekniikoiden perusilmioet

Energy Technology Data Exchange (ETDEWEB)

Janka, K. [Dekati Oy, Tampere (Finland)

2006-10-15

The project deals with development of basic phenomena and mechanism utilised in aerosol particle measurement techniques. The areas under development are: particle-charging techniques, photoelectric charging, particle concentrating using virtual-impactor technique, and optical characterising techniques of particles. Results will be applied on detection techniques of bioaerosol attract, particle emission sensors for diesel exhaust gases, and widening the application areas of existing measurement techniques. (orig.)

14. Transmission electron microscopy study of aerosol particles from the brown hazes in northern China

Science.gov (United States)

Li, Weijun; Shao, Longyi

2009-05-01

Airborne aerosol collections were performed in urban areas of Beijing that were affected by regional brown haze episodes over northern China from 31 May to 12 June 2007. Morphologies, elemental compositions, and mixing states of 810 individual aerosol particles of different sizes were obtained by transmission electron microscopy coupled with energy-dispersive X-ray spectrometry. The phases of some particles were verified using selected-area electron diffraction. Aerosol particle types less than 10 μm in diameter include mineral, complex secondary (Ca-S, K-, and S-rich), organic, soot, fly ash, and metal (Fe-rich and Zn-bearing). Most soot, fly ash, and organic particles are less than 2 μm in diameter. Approximately 84% of the analyzed mineral particles have diameters between 2 and 10 μm, while 81% of the analyzed complex secondary and metal particles are much smaller, from 0.1 to 2 μm. Trajectory analysis with fire maps show that southerly air masses arriving at Beijing have been transported through many agricultural biomass burning sites and heavy industrial areas. Spherical fly ash and Fe-rich particles were from industrial emissions, and abundant K-rich and organic particles likely originated from field burning of crop residues. Abundant Zn-bearing particles are associated with industrial activities and local waste incinerators. On the basis of the detailed analysis of 443 analyzed aerosol particles, about 70% of these particles are internally mixed with two or more aerosol components from different sources. Most mineral particles are covered with visible coatings that contain N, O, Ca (or Mg), minor S, and Cl. K- and S-rich particles tend to be coagulated with fly ash, soot, metal, and fine-grained mineral particles. Organic materials internally mixed with K- and S-rich particles can be their inclusions and coatings.

15. Aerosolization, Chemical Characterization, Hygroscopicity and Ice Formation of Marine Biogenic Particles

Science.gov (United States)

Alpert, P. A.; Radway, J.; Kilthau, W.; Bothe, D.; Knopf, D. A.; Aller, J. Y.

2013-12-01

The oceans cover the majority of the earth's surface, host nearly half the total global primary productivity and are a major source of atmospheric aerosol particles. However, effects of biological activity on sea spray generation and composition, and subsequent cloud formation are not well understood. Our goal is to elucidate these effects which will be particularly important over nutrient rich seas, where microorganisms can reach concentrations of 10^9 per mL and along with transparent exopolymer particles (TEP) can become aerosolized. Here we report the results of mesocosm experiments in which bubbles were generated by two methods, either recirculating impinging water jets or glass frits, in natural or artificial seawater containing bacteria and unialgal cultures of three representative phytoplankton species, Thalassiosira pseudonana, Emiliania huxleyi, and Nannochloris atomus. Over time we followed the size distribution of aerosolized particles as well as their hygroscopicity, heterogeneous ice nucleation potential, and individual physical-chemical characteristics. Numbers of cells and the mass of dissolved and particulate organic carbon (DOC, POC), TEP (which includes polysaccharide-containing microgels and nanogels >0.4 μm in diameter) were determined in the bulk water, the surface microlayer, and aerosolized material. Aerosolized particles were also impacted onto substrates for ice nucleation and water uptake experiments, elemental analysis using computer controlled scanning electron microscopy and energy dispersive analysis of X-rays (CCSEM/EDX), and determination of carbon bonding with scanning transmission X-ray microscopy and near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Regardless of bubble generation method, the overall concentration of aerosol particles, TEP, POC and DOC increased as concentrations of bacterial and phytoplankton cells increased, stabilized, and subsequently declined. Particles air. Our results provide improved

16. Airborne observations of aerosol microphysical properties and particle ageing processes in the troposphere above Europe

Directory of Open Access Journals (Sweden)

T. Hamburger

2012-12-01

Full Text Available In-situ measurements of aerosol microphysical properties were performed in May 2008 during the EUCAARI-LONGREX campaign. Two aircraft, the FAAM BAe-146 and DLR Falcon 20, operated from Oberpfaffenhofen, Germany. A comprehensive data set was obtained comprising the wider region of Europe north of the Alps throughout the whole tropospheric column. Prevailing stable synoptic conditions enabled measurements of accumulating emissions inside the continental boundary layer reaching a maximum total number concentration of 19 000 particles cm−3 stp. Ultra-fine particles as indicators for nucleation events were observed within the boundary layer during high pressure conditions and after updraft of emissions induced by frontal passages above 8 km altitude in the upper free troposphere. Aerosol ageing processes during air mass transport are analysed using trajectory analysis. The ratio of particles containing a non-volatile core (250 °C to the total aerosol number concentration was observed to increase within the first 12 to 48 h from the particle source from 50 to 85% due to coagulation. Aged aerosol also features an increased fraction of accumulation mode particles of approximately 40% of the total number concentration. The presented analysis provides an extensive data set of tropospheric aerosol microphysical properties on a continental scale which can be used for atmospheric aerosol models and comparisons of satellite retrievals.

17. Airborne observations of aerosol microphysical properties and particle ageing processes in the troposphere above Europe

Science.gov (United States)

Hamburger, T.; McMeeking, G.; Minikin, A.; Petzold, A.; Coe, H.; Krejci, R.

2012-12-01

In-situ measurements of aerosol microphysical properties were performed in May 2008 during the EUCAARI-LONGREX campaign. Two aircraft, the FAAM BAe-146 and DLR Falcon 20, operated from Oberpfaffenhofen, Germany. A comprehensive data set was obtained comprising the wider region of Europe north of the Alps throughout the whole tropospheric column. Prevailing stable synoptic conditions enabled measurements of accumulating emissions inside the continental boundary layer reaching a maximum total number concentration of 19 000 particles cm-3 stp. Ultra-fine particles as indicators for nucleation events were observed within the boundary layer during high pressure conditions and after updraft of emissions induced by frontal passages above 8 km altitude in the upper free troposphere. Aerosol ageing processes during air mass transport are analysed using trajectory analysis. The ratio of particles containing a non-volatile core (250 °C) to the total aerosol number concentration was observed to increase within the first 12 to 48 h from the particle source from 50 to 85% due to coagulation. Aged aerosol also features an increased fraction of accumulation mode particles of approximately 40% of the total number concentration. The presented analysis provides an extensive data set of tropospheric aerosol microphysical properties on a continental scale which can be used for atmospheric aerosol models and comparisons of satellite retrievals.

18. Aerosol particle properties in a South American megacity

Science.gov (United States)

Ulke, Ana; Torres-Brizuela, Marcela; Raga, Graciela; Baumgardner, Darrel; Cancelada, Marcela

2015-04-01

The subtropical city of Buenos Aires is located on the western shore of Río de la Plata, on the southeastern coast of Argentina. It is the second largest metropolitan area in South America, with a population density of around 14 thousand people per km2. When all 24 counties of the Great Buenos Aires Metropolitan Area are included it is the third-largest conurbation in Latin America, with a population of around fifteen million inhabitants. The generalized worldwide trend to concentrate human activities in urban regions that continue to expand in area, threatens the local and regional environment. Air pollution in the Buenos Aires airshed is due to local sources (mainly the mobile sources, followed by the electric power plants and some industries) and to distant sources (like biomass burning, dust, marine aerosols and occasionally volcanic ash) whose products arrive in the city area due to the regional transport patterns. Previous research suggests that ambient aerosol particle concentrations should be considered an air quality problem. A field campaign was conducted in Buenos Aires in 2011 in order to characterize some aerosol particles properties measured for the first time in the city. Measurements began in mid- April and continued until December. The field observations were done in a collaborative effort between the Universities of Mexico (UNAM) and Buenos Aires (UBA). A suite of instruments was installed on the roof of an UBA laboratory and classroom buildings (34.54° S, 58.44° W) at an altitude of approximately 30 m above sea level. The measurements included the number concentration of condensation nuclei (CN) larger than approximately 50 nm, the mass concentration of particle-bound polycyclic aromatic hydrocarbons (PPAH), the scattering (Bscat) and absorption (Babs) coefficients at 550 nm and the vertical profiles of backscattered light from aerosols at a wavelength of 910 nm using a ceilometer. In addition, a weather station recorded the meteorological

19. Sources of anions in aerosols in northeast Greenland during late winter

DEFF Research Database (Denmark)

Lauridsen, Marlene Fenger; Sørensen, Lise Lotte; Kristensen, Kasper

2013-01-01

affecting the composition of aerosols in the high Arctic. Therefore size-segregated aerosols were sampled at a high Arctic site, Station Nord (Northeast Greenland), in March 2009 using a Micro Orifice Uniform Deposit Impactor. The aerosol samples were extracted in order to analyse three water-soluble anions......−4 is by far the dominating anion accounting for 50–85% of the analyzed mass. The analysis suggests that Cl− and NO−3 in coarser particles (> 1.5 μm) originate from local/regional sources. Under conditions where the air mass is transported over sea ice at high wind speeds, very coarse particles (> 18 μm...

20. Mass Spectrometric Analysis of Pristine Aerosol Particles During the wet Season of Amazonia - Detection of Primary Biological Particles?

Science.gov (United States)

Schneider, J.; Zorn, S. R.; Freutel, F.; Borrmann, S.; Chen, Q.; Farmer, D. K.; Jimenez, J. L.; Flores, M.; Roldin, P.; Artaxo, P.; Martin, S. T.

2008-12-01

The contribution of primary biological aerosol (POA) particles to the natural organic aerosol is a subject of current research. Estimations of the POA contribution to the total aerosol particle concentration range between 25 and 80%, depending on location and season. Especially in the tropical rain forest it is expected that POA is a major source of supermicron, possibly also of submicron particles. During AMAZE (Amazonian Aerosol CharacteriZation Experiment), a field project near Manaus, Brazil, in February/March 2008, an Aerodyne ToF-AMS was equipped with a high pressure aerodynamic lens. This high pressure lens (operating pressure 14.6 torr) is designed with the objective to extend the detectable size range of the AMS into the supermicron size range where primary biological particles are expected. Size distribution measured by the AMS were compared with size distribution from an optical particle counter and indicate that the high pressure lens has a 50% cut-off at a vacuum aerodynamic diameter of about 1 μm, but still has significant transmission up to a vacuum aerodynamic diameter of about 2 μm, thus extending the detectable size range of the AMS into the coarse mode. The measuring instruments were situated in a container at ground level. The aerosol was sampled through a 40 m vertical, laminar inlet, which was heated and dried to maintain a relative humidity between 30 and 40%. The inlet was equipped with a 7 μm cut-off cyclone. Size distributions recorded with an optical particle counter parallel to the AMS show that the inlet transmitted aerosol particles up to an optically detected diameter of 10 μm. POA particles like plant fragments, pollen, spores, fungi, viruses etc. contain chemical compounds as proteins, sugars, amino acids, chlorophyll, and cellular material as cellulose. Laboratory experiments have been performed in order to identify typical mass spectral patterns of these compounds. These laboratory data were compared to size resolved particle

1. Single-particle characterization of the high-Arctic summertime aerosol

Directory of Open Access Journals (Sweden)

B. Sierau

2014-07-01

Full Text Available Single-particle mass-spectrometric measurements were carried out in the high Arctic north of 80° during summer 2008. The campaign took place onboard the icebreaker Oden and was part of the Arctic Summer Cloud Ocean Study (ASCOS. The instrument deployed was an aerosol time-of-flight mass spectrometer (ATOFMS that provides information on the chemical composition of individual particles and their mixing state in real time. Aerosols were sampled in the marine boundary layer at stations in the open ocean, in the marginal ice zone, and in the pack ice region. The largest fraction of particles detected for subsequent analysis in the size range of the ATOFMS between approximately 200 and 3000 nm in diameter showed mass-spectrometric patterns, indicating an internal mixing state and a biomass burning and/or biofuel source. The majority of these particles were connected to an air mass layer of elevated particle concentration mixed into the surface mixed layer from the upper part of the marine boundary layer. The second largest fraction was represented by sea salt particles. The chemical analysis of the over-ice sea salt aerosol revealed tracer compounds that reflect chemical aging of the particles during their long-range advection from the marginal ice zone, or open waters south thereof prior to detection at the ship. From our findings we conclude that long-range transport of particles is one source of aerosols in the high Arctic. To assess the importance of long-range particle sources for aerosol–cloud interactions over the inner Arctic in comparison to local and regional biogenic primary aerosol sources, the chemical composition of the detected particles was analyzed for indicators of marine biological origin. Only a minor fraction showed chemical signatures of potentially ocean-derived primary particles of that kind. However, a chemical bias in the ATOFMS's detection capabilities observed during ASCOS might suggest the presence of a particle type of

2. On the potential contribution of open lead particle emissions to the central Arctic aerosol concentration

Directory of Open Access Journals (Sweden)

A. Held

2010-10-01

Full Text Available During the ice-breaker borne ASCOS expedition (Arctic Summer Cloud Ocean Study direct eddy covariance measurements of aerosol number fluxes were carried out in August 2008 on the edge of an ice floe drifting in the central Arctic Ocean between 2°–10° W longitude and 87°–87.5° N latitude. The median aerosol transfer velocities over different surface types (open water leads, ice ridges, snow and ice surfaces ranged from 0.27 to 0.68 mm s−1 during deposition-dominated episodes. Emission periods were observed more frequently over the open lead, while the snow behaved primarily as a deposition surface. Directly measured aerosol fluxes were compared with particle deposition parameterizations in order to estimate the emission flux from the observed net aerosol flux. Finally, the contribution of the open lead particle source to atmospheric variations in particle number concentration was evaluated and compared with the observed temporal evolution of particle number. The direct emission of aerosol particles from the open lead can only explain 5–10% of the observed particle number variation in the mixing layer close to the surface.

3. Airborne observations of aerosol microphysical properties and particle ageing processes in the troposphere above Europe

Directory of Open Access Journals (Sweden)

T. Hamburger

2012-08-01

Full Text Available In-situ measurements of aerosol microphysical properties were performed in May 2008 during the EUCAARI-LONGREX campaign. Two aircraft, the FAAM BAe-146 and DLR Falcon 20, operated from Oberpfaffenhofen, Germany. A comprehensive data set was obtained comprising the wider region of Europe north of the Alps throughout the whole tropospheric column. Prevailing stable synoptic conditions enabled measurements of accumulating emissions inside the continental boundary layer reaching a maximum total number concentration of 19 000 particles cm−3 stp. Nucleation events were observed within the boundary layer during high pressure conditions and after updraft of emissions induced by frontal passages above 8 km altitude in the upper free troposphere. Aerosol ageing processes during air mass transport are analysed using trajectory analysis. The ratio of particles containing a non-volatile core (250 °C to the total aerosol number concentration was observed to increase within the first 12 to 48 h from the particle source from 50 to 85% due to coagulation. Aged aerosol also features an increased fraction of accumulation mode particles of approximately 40% of the total number concentration. The presented analysis provides an extensive data set of tropospheric aerosol microphysical properties on a continental scale which can be used for atmospheric aerosol models and comparisons of satellite retrievals.

4. The on-line analysis of aerosol-delivered pharmaceuticals via single particle aerosol mass spectrometry.

Science.gov (United States)

Morrical, Bradley D; Balaxi, Maria; Fergenson, David

2015-07-15

The use of single particle aerosol mass spectrometry (SPAMS) was evaluated for the analysis of inhaled pharmaceuticals to determine the mass distribution of the individual active pharmaceutical ingredients (API) in both single ingredient and combination drug products. SPAMS is an analytical technique where the individual aerodynamic diameters and chemical compositions of many aerosol particles are determined in real-time. The analysis was performed using a Livermore Instruments SPAMS 3.0, which allowed the efficient analysis of aerosol particles with broad size distributions and can acquire data even under a very large particle load. Data similar to what would normally require roughly three days of experimentation and analysis was collected in a five minute period and analyzed automatically. The results were computed to be comparable to those returned by a typical Next Generation Impactor (NGI) particle size distribution experiment.

5. New apparatus of single particle trap system for aerosol visualization

Science.gov (United States)

Higashi, Hidenori; Fujioka, Tomomi; Endo, Tetsuo; Kitayama, Chiho; Seto, Takafumi; Otani, Yoshio

2014-08-01

Control of transport and deposition of charged aerosol particles is important in various manufacturing processes. Aerosol visualization is an effective method to directly observe light scattering signal from laser-irradiated single aerosol particle trapped in a visualization cell. New single particle trap system triggered by light scattering pulse signal was developed in this study. The performance of the device was evaluated experimentally. Experimental setup consisted of an aerosol generator, a differential mobility analyzer (DMA), an optical particle counter (OPC) and the single particle trap system. Polystylene latex standard (PSL) particles (0.5, 1.0 and 2.0 μm) were generated and classified according to the charge by the DMA. Singly charged 0.5 and 1.0 μm particles and doubly charged 2.0 μm particles were used as test particles. The single particle trap system was composed of a light scattering signal detector and a visualization cell. When the particle passed through the detector, trigger signal with a given delay time sent to the solenoid valves upstream and downstream of the visualization cell for trapping the particle in the visualization cell. The motion of particle in the visualization cell was monitored by CCD camera and the gravitational settling velocity and the electrostatic migration velocity were measured from the video image. The aerodynamic diameter obtained from the settling velocity was in good agreement with Stokes diameter calculated from the electrostatic migration velocity for individual particles. It was also found that the aerodynamic diameter obtained from the settling velocity was a one-to-one function of the scattered light intensity of individual particles. The applicability of this system will be discussed.

6. NUMBER CONCENTRATION, SIZE DISTRIBUTION AND FINE PARTICLE FRACTION OF TROPOSPHERIC AND STRATOSPHERIC AEROSOLS

Institute of Scientific and Technical Information of China (English)

Li Xu; Guangyu Shi; Li Zhang; Jun Zhou; Yasunobu Iwasaka

2003-01-01

Aerosol observations were carried out at Xianghe Scientific Balloon Base (39.45°N, 117°E) using a stratospheric balloon. The particle number concentrations of the tropospheric and stratospheric aerosols were directly explored.The vertical distributions of the number concentration, number-size (that is, particle number versus particle size)distribution, and the fraction of fine particles (0.5 μm＞r＞0.15 μm/r＞0.15 μm) are reported in this paper. The profiles of particle concentration present multi-peak phenomenon. The pattern of size distribution for atmospheric aerosol indicates a tri-modal (r=～0.2 μm, ～0.88 μm and ～7.0 μm) and a bi-modal (r=～0.13 μm and 2.0 μm). The number-size distribution almost fits the Junge distribution for particles with r＜0.5 μm in the stratosphere of 1993 and the troposphere of 1994. But the distributions of coarse particles (r＞0.5 μm) are not uniform. The number-size distribution exhibits also a wide size range in the troposphere of 1993. The results demonstrate that fine particles represent the major portion in the troposphere during the measurement period, reaching as high as 95% in 1994. Certain coarse particle peaks in the troposphere were attributed to clouds and other causes, and in the stratosphere to volcanic eruption. The stratospheric aerosol layer consists of unique fractions of fine or coarse particles depending on their sources. In summary, the process of gas-to-particles conversion was active and the coarse particles were rich over the Xianghe area. The measurements also demonstrate that the spatial and temporal atmospheric aerosol distributions are nonuniform and changeful.

7. Phosphorus-bearing Aerosol Particles From Volcanic Plumes

Science.gov (United States)

Obenholzner, J. H.; Schroettner, H.; Poelt, P.; Delgado, H.; Caltabiano, T.

2003-12-01

Particles rich in P or bulk geochemical data of volcanic aerosol particles showing high P contents are known from many volcanic plumes (Stanton, 1994; Obenholzner et al., 2003). FESEM/EDS analysis of individual particles obtained from the passively degassing plume of Popocatepetl volcano, Mx. (1997) and from the plume of Stromboli (May 2003) show P frequently. Even at the high resolution of the FESEM, euhedral apatite crystals could not be observed. At Popocatepetl (1997) spherical Ca-P-O particles are common. Fluffy, fractal or botryoidal particles also can contain EDS-detectable amounts of P. The EDS spectrum of such particles can comprise various elements. However most particles show P, S and Cl. P-S and P-S-metal species are known in chemistry but do they occur in volcanic plumes? Stoichiometric considerations had been made in the past suggesting the existence of P-S species in plumes (Stanton 1994), gas sampling and remote gas monitoring systems have not detected yet such molecules in plumes. The particle spectrum of the reawakened Popocateptel volcano might be related to accumulation of volatiles at the top of a magma chamber during the phase of dormancy. P-Fe rich, Ca-free aggregates are also known from the eruption of El Chichon 1982 (SEM/EDS by M. Sheridan, per. comm. 08-24-2003). Persistently active volcanoes (i.e. Stromboli) represent a different category according to continuous degassing and aerosol particle formation. A particle collector ( ca. 90 ml/min) accompanied a COSPEC helicopter flight at Stromboli (May 15, 2003) after one of the rare types of sub-plinian events on April 5 2003. P-bearing particles are very common. For instance, an Fe oxide grain (diam. = 2 æm) is partially covered by fluffy and euhedral P-bearing matter. The elements detected are P, Cl, Na, Mg, Al, Si, K, Ca, Ti and (Fe). The fluffy and the euhedral (rhombohedral?) matter show in SE-BSE-mix image almost identical grey colors. At Stromboli and Popocatepetl particles on which

8. TEM Study of Aerosol Particles in Brown Haze Episodes over Northern China in Spring 2007

Science.gov (United States)

Li, W.; Shao, L.; Buseck, P. R.

2008-12-01

Airborne aerosol collections were performed in eight brown haze episodes from 31 May to 21 June 2007 in Beijing, China. Morphologies, compositions, and mixing states of individual aerosol particles having different sizes were obtained using transmission electron microscopy (TEM). Aerosol particle types less than 2 μ m in diameter include mineral dust, fly ash, soot, organic material, and K-rich, S-rich, and metal particles (Fe- and Zn-rich). Mineral dust particles dominate in the range of 2 to 10 μ m. In addition to finding contributions from vehicle emissions and soil dust in Beijing, TEM results from the study provide new insights into sources such as agricultural biomass burning, industrial activities, and waste incineration. These sources can contribute not only great amounts of K-rich and metal particles but also reactive gases such as NH3, NOx, SO2, and VOCs to the haze. More than 80% of the analyzed aerosol particles are internally mixed. K- and S-rich particles tend to be coagulated with fly ash, soot, metal, and fine-grained mineral dust particles. Organic materials can act as inclusions in the K- and S-rich particles and their coatings. Over 90% of the analyzed internally mixed mineral particles are covered with Ca-, Mg-, or Na-rich coatings, and only 8% are associated with K- or S-rich coatings. The compositions of Ca-, Mg-, and Na-rich coatings suggest that they are possibly nitrates mixed with minor sulfates and chlorides. Calcium sulfate particles with diameters from 10 to 500 nm were also detected within Ca(NO3)2 and Mg(NO3)2 coatings. These results indicate that mineral dust particles in the brown haze episodes participated in heterogeneous reactions in the atmosphere with one or more of SO2, NO2, HCl, and HNO3. The development of coatings altered some mineral dust particles from hydrophobic to hydrophilic.

9. Natural Radionuclides and Isotopic Signatures for Determining Carbonaceous Aerosol Sources, Aerosol Lifetimes, and Washout Processes

Energy Technology Data Exchange (ETDEWEB)

Gaffney, Jeffrey [Univ. of Arkansas, Little Rock, AR (United States)

2012-12-12

This is the final technical report. The project description is as follows: to determine the role of aerosol radiative forcing on climate, the processes that control their atmospheric concentrations must be understood, and aerosol sources need to be determined for mitigation. Measurements of naturally occurring radionuclides and stable isotopic signatures allow the sources, removal and transport processes, as well as atmospheric lifetimes of fine carbonaceous aerosols, to be evaluated.

10. Intercomparison of number concentration measurements by various aerosol particle counters

Science.gov (United States)

Ankilov, A.; Baklanov, A.; Colhoun, M.; Enderle, K.-H.; Gras, J.; Julanov, Yu.; Kaller, D.; Lindner, A.; Lushnikov, A. A.; Mavliev, R.; McGovern, F.; Mirme, A.; O'Connor, T. C.; Podzimek, J.; Preining, O.; Reischl, G. P.; Rudolf, R.; Sem, G. J.; Szymanski, W. W.; Tamm, E.; Vrtala, A. E.; Wagner, P. E.; Winklmayr, W.; Zagaynov, V.

Total aerosol particle number concentrations, as measured by means of 16 different measurement systems, have been quantitatively compared during an international workshop at the Institute for Experimental Physics of the University of Vienna, Austria, which was coordinated within the Committee on Nucleation and Atmospheric Aerosols (ICCP-IUGG). The range of measuring instruments includes Pollak counters (PCO) in use already for several decades, presently available commercial particle counters, as well as laboratory prototypes. The operation of the instruments considered was based on different measurement principles: (1) adiabatic expansion condensation particle counter, (2) flow diffusion condensation particle counter, (3) turbulent mixing condensation particle counter, (4) laser optical particle counter, and (5) electrostatic particle measurement system. Well-defined test aerosols with various chemical compositions were considered: DEHS, sodium chloride, silver, hydrocarbons, and tungsten oxide. The test aerosols were nearly monodispersed with mean particle diameters between 4 and 520 nm, the particle number concentrations were varied over a range from about 4×10 1 to 7×10 6 cm -3. A few measurements were performed with two-component aerosol mixtures. For simultaneous concentration measurements, the various instruments considered were operated under steady state conditions in a linear flow system. A series of at least 10 single concentration measurements was performed by each individual instrument at each set of test aerosol parameters. The average of the concentration data measured by the various instruments was defined as a common reference. The number concentrations obtained from the various instruments typically agreed within a factor of about two over the entire concentration range considered. The agreement of the measured concentrations is notable considering the various different measurement principles applied in this study, and particularly in view of the

11. Aerosol optical depths and their contributing sources in Taiwan

Science.gov (United States)

Chan, K. L.; Chan, K. L.

2017-01-01

In this paper, we present a quantitative investigation of the contributions of different aerosols to the aerosol optical depths (AODs) in Taiwan using a global chemical transport model (GEOS-Chem) and remote sensing measurements. The study focus is on the period from June 2012 to October 2013. Five different types of aerosols are investigated: sea salt, dust, sulfate, organic carbon and black carbon. Three of these aerosols, namely sulfate, organic carbon and black carbon, have significant anthropogenic sources. Model simulation results were compared with both ground based sun photometer measurements and MODerate resolution Imaging Spectroradiometer (MODIS) satellite observations. The model data shows good agreement with satellite observations (R = 0.72) and moderate correlation with sun photometer measurements (R = 0.52). Simulation results show the anthropogenic aerosols contribute ∼65% to the total AOD in Taipei, while natural originated aerosols only show a minor impact (∼35%). Among all the aerosols, sulfate is the dominating species, contributing 62.4% to the annual average total AOD. Organic carbon and black carbons respectively contribute 7.3% and 1.5% to the annual averaged total AOD. The annual average contributions of sea salt and dust aerosols to the total AOD are 26.4% and 2.4%, respectively. A sensitivity study was performed to identify the contributions of anthropogenic aerosol sources in each region to the AODs in Taipei. North-East Asia was identified as the major contributing source region of anthropogenic aerosols to Taipei, accounting for more than 50% of total sulfate, 32% of total organic carbon and 51% of total black carbon aerosols. South-East Asia is the second largest contributing source region, contributing 35%, 24% and 34% of total sulfate, organic carbon and black carbon aerosols, respectively. The aerosols from continents other than Asia only show minor impacts to the aerosol load in Taipei. In addition, a case study of a biomass

12. Sub-Antarctic marine aerosol: significant contributions from biogenic sources

Directory of Open Access Journals (Sweden)

J. Schmale

2013-03-01

Full Text Available Biogenic influences on the composition and characteristics of aerosol were investigated on Bird Island (54°00' S, 38°03' W in the South Atlantic during November and December 2010. This remote marine environment is characterised by large seabird and seal colonies. The chemical composition of the submicron particles, measured by an aerosol mass spectrometer (AMS, was 21% non-sea salt sulfate 2% nitrate, 7% ammonium, 22% organics and 47% sea salt including sea salt sulfate. A new method to isolate the sea salt signature from the high-resolution AMS data was applied. Generally, the aerosol was found to be less acidic than in other marine environments due to the high availability of ammonia, from local fauna emissions. By positive matrix factorisation five different organic aerosol (OA profiles could be isolated: an amino acids/amine factor (AA-OA, 18% of OA mass, a methanesulfonic acid OA factor (MSA-OA, 25%, a marine oxygenated OA factor (M-OOA, 40%, a sea salt OA fraction (SS-OA, 7% and locally produced hydrocarbon-like OA (HOA, 9%. The AA-OA was dominant during the first two weeks of November and found to be related with the hatching of penguins in a nearby colony. This factor, rich in nitrogen (C : N ratio = 0.13, has implications for the biogeochemical cycling of nitrogen in the area as particulate matter is often transported over longer distances than gaseous N-rich compounds. The MSA-OA was mainly transported from more southerly latitudes where phytoplankton bloomed. The bloom was identified as one of three sources for particulate sulfate on Bird Island, next to sea salt sulfate and sulfate transported from South America. M-OOA was the dominant organic factor and found to be similar to marine OA observed at Mace Head, Ireland. An additional OA factor highly correlated with sea salt aerosol was identified (SS-OA. However, based on the available data the type of mixture, internal or external, could not be determined. Potassium was not

13. Sub-Antarctic marine aerosol: dominant contributions from biogenic sources

Directory of Open Access Journals (Sweden)

J. Schmale

2013-09-01

Full Text Available Biogenic influences on the composition and characteristics of aerosol were investigated on Bird Island (54°00' S, 38°03' W in the South Atlantic during November and December 2010. This remote marine environment is characterised by large seabird and seal colonies. The chemical composition of the submicron particles, measured by an aerosol mass spectrometer (AMS, was 21% non-sea-salt sulfate, 2% nitrate, 8% ammonium, 22% organics and 47% sea salt including sea salt sulfate. A new method to isolate the sea spray signature from the high-resolution AMS data was applied. Generally, the aerosol was found to be less acidic than in other marine environments due to the high availability of ammonia, from local fauna emissions. By positive matrix factorisation five different organic aerosol (OA profiles could be isolated: an amino acid/amine factor (AA-OA, 18% of OA mass, a methanesulfonic acid OA factor (MSA-OA, 25%, a marine oxygenated OA factor (M-OOA, 41%, a sea spray OA fraction (SS-OA, 7% and locally produced hydrocarbon-like OA (HOA, 9%. The AA-OA was dominant during the first two weeks of November and found to be related with the hatching of penguins in a nearby colony. This factor, rich in nitrogen (N : C ratio = 0.13, has implications for the biogeochemical cycling of nitrogen in the area as particulate matter is often transported over longer distances than gaseous N-rich compounds. The MSA-OA was mainly transported from more southerly latitudes where phytoplankton bloomed. The bloom was identified as one of three sources for particulate sulfate on Bird Island, next to sea salt sulfate and sulfate transported from South America. M-OOA was the dominant organic factor and found to be similar to marine OA observed at Mace Head, Ireland. An additional OA factor highly correlated with sea spray aerosol was identified (SS-OA. However, based on the available data the type of mixture, internal or external, could not be determined. Potassium was not

14. Characteristics and sources of carbonaceous aerosols from Shanghai, China

Directory of Open Access Journals (Sweden)

J.-J. Cao

2013-01-01

Full Text Available An intensive investigation of carbonaceous PM2.5 and TSP (total suspended particles from Pudong (China was conducted as part of the MIRAGE-Shanghai (Megacities Impact on Regional and Global Environment experiment in 2009. Data for organic and elemental carbon (OC and EC, organic species, including C17 to C40 n-alkanes and 17 polycyclic aromatic hydrocarbons (PAHs, and stable carbon isotopes OC (δ13COC and EC (δ13CEC were used to evaluate the aerosols' temporal variations and identify presumptive sources. High OC/EC ratios indicated a large fraction of secondary organic aerosol (SOA; high char/soot ratios indicated stronger contributions to EC from motor vehicles and coal combustion than biomass burning. Diagnostic ratios of PAHs indicated that much of the SOA was produced via coal combustion. Isotope abundances (δ13COC = −24.5 ± 0.8‰ and δ13CEC = −25.1 ± 0.6‰ indicated that fossil fuels were the most important source for carbonaceous PM2.5 (particulate matter less than 2.5 micrometers in diameter, with lesser impacts from biomass burning and natural sources. An EC tracer system and isotope mass balance calculations showed that the relative contributions to total carbon from coal combustion, motor vehicle exhaust, and SOA were 41%, 21%, and 31%; other primary sources such as marine, soil and biogenic emissions contributed 7%. Combined analyses of OC and EC, n-alkanes and PAHs, and stable carbon isotopes provide a new way to apportion the sources of carbonaceous particles.

15. Comparison of the DiSCmini aerosol monitor to a handheld condensation particle counter and a scanning mobility particle sizer for submicrometer sodium chloride and metal aerosols

OpenAIRE

Mills, Jessica B.; Park, Jae Hong; Peters, Thomas M.

2013-01-01

We evaluated the robust, lightweight DiSCmini (DM) aerosol monitor for its ability to measure the concentration and mean diameter of submicrometer aerosols. Tests were conducted with monodispersed and polydispersed aerosols composed of two particle types (sodium chloride, NaCl, and spark generated metal particles, which simulate particles found in welding fume) at three different steady-state concentration ranges (Low, 104 particles/cm3). Particle number concentration, lung deposited surface ...

16. Single-particle characterization of summertime arctic aerosols collected at Ny-Alesund, Svalbard.

Science.gov (United States)

Geng, Hong; Ryu, Jiyeon; Jung, Hae-Jin; Chung, Hyeok; Ahn, Kang-Ho; Ro, Chul-Un

2010-04-01

Single-particle characterization of summertime Arctic aerosols is useful to understand the impact of air pollutants on the polar atmosphere. In the present study, a quantitative single particle analytical technique, low-Z particle electron probe X-ray microanalysis, was used to characterize 8100 individual particles overall in 16 sets of aerosol samples collected at Ny-Alesund, Svalbard, Norway on 25-31 July, 2007. Based on their X-ray spectral and secondary electron image data of individual particles, 13 particle types were identified, in which particles of marine origin were the most abundant, followed by carbonaceous and mineral dust particles. A number of aged (reacted) sea salt (and mixture) particles produced by the atmospheric reaction of genuine sea-salts, especially with NO(x) or HNO(3), were significantly encountered in almost all the aerosol samples. They greatly outnumbered genuine sea salt particles, implying that the summertime Arctic atmosphere, generally regarded as a clean background environment, is disturbed by anthropogenic air pollutants. The main sources of airborne NO(x) (or HNO(3)) are probably ship emissions around the Arctic Ocean, industry emission from northern Europe and northwestern Siberia, and renoxification of NO(3)(-) within or on the melting snow/ice surface.

17. Molecular Characterization of Brown Carbon in Biomass Burning Aerosol Particles

Energy Technology Data Exchange (ETDEWEB)

Lin, Peng; Aiona, Paige K.; Li, Ying; Shiraiwa, Manabu; Laskin, Julia; Nizkorodov, Sergey A.; Laskin, Alexander

2016-11-01

Emissions from biomass burning are a significant source of brown carbon (BrC) in the atmosphere. In this study, we investigate the molecular composition of freshly-emitted biomass burning organic aerosol (BBOA) samples collected during test burns of selected biomass fuels: sawgrass, peat, ponderosa pine, and black spruce. We characterize individual BrC chromophores present in these samples using high performance liquid chromatography coupled to a photodiode array detector and a high-resolution mass spectrometer. We demonstrate that both the overall BrC absorption and the chemical composition of light-absorbing compounds depend significantly on the type of biomass fuels and burning conditions. Common BrC chromophores in the selected BBOA samples include nitro-aromatics, polycyclic aromatic hydrocarbon derivatives, and polyphenols spanning a wide range of molecular weights, structures, and light absorption properties. A number of biofuel-specific BrC chromophores are observed, indicating that some of them may be used as potential markers of BrC originating from different biomass burning sources. On average, ~50% of the light absorption above 300 nm can be attributed to a limited number of strong BrC chromophores, which may serve as representative light-absorbing species for studying atmospheric processing of BrC aerosol. The absorption coefficients of BBOA are affected by solar photolysis. Specifically, under typical atmospheric conditions, the 300 nm absorbance decays with a half-life of 16 hours. A “molecular corridors” analysis of the BBOA volatility distribution suggests that many BrC compounds in the fresh BBOA have low volatility (<1 g m-1) and will be retained in the particle phase under atmospherically relevant conditions.

18. Accelerated simulation of stochastic particle removal processes in particle-resolved aerosol models

Science.gov (United States)

Curtis, J. H.; Michelotti, M. D.; Riemer, N.; Heath, M. T.; West, M.

2016-10-01

Stochastic particle-resolved methods have proven useful for simulating multi-dimensional systems such as composition-resolved aerosol size distributions. While particle-resolved methods have substantial benefits for highly detailed simulations, these techniques suffer from high computational cost, motivating efforts to improve their algorithmic efficiency. Here we formulate an algorithm for accelerating particle removal processes by aggregating particles of similar size into bins. We present the Binned Algorithm for particle removal processes and analyze its performance with application to the atmospherically relevant process of aerosol dry deposition. We show that the Binned Algorithm can dramatically improve the efficiency of particle removals, particularly for low removal rates, and that computational cost is reduced without introducing additional error. In simulations of aerosol particle removal by dry deposition in atmospherically relevant conditions, we demonstrate about 50-times increase in algorithm efficiency.

19. Selection of quasi-monodisperse super-micron aerosol particles

Science.gov (United States)

Rösch, Michael; Pfeifer, Sascha; Wiedensohler, Alfred; Stratmann, Frank

2014-05-01

Size-segregated quasi monodisperse particles are essential for e.g. fundamental research concerning cloud microphysical processes. Commonly a DMA (Differential Mobility Analyzer) is used to produce quasi-monodisperse submicron particles. Thereto first, polydisperse aerosol particles are bipolarly charged by a neutralizer, and then selected according to their electrical mobility with the DMA [Knutson et al. 1975]. Selecting a certain electrical mobility with a DMA results in a particle size distribution, which contains singly charged particles as well as undesired multiply charged larger particles. Often these larger particles need to either be removed from the generated aerosol or their signals have to be corrected for in the data inversion and interpretation process. This problem becomes even more serious when considering super-micron particles. Here we will present two different techniques for generating quasi-monodisperse super-micron aerosol particles with no or only an insignificant number of larger sized particles being present. First, we use a combination of a cyclone with adjustable aerodynamic cut-off diameter and our custom-built Maxi-DMA [Raddatz et al. 2013]. The cyclone removes particles larger than the desired ones prior to mobility selection with the DMA. This results in a reduction of the number of multiply charged particles of up to 99.8%. Second, we utilize a new combination of cyclone and PCVI (Pumped Counterflow Virtual Impactor), which is based on purely inertial separation and avoids particle charging. The PCVI instrument was previously described by Boulter et al. (2006) and Kulkarni et al. (2011). With our two setups we are able to produce quasi-monodisperse aerosol particles in the diameter range from 0.5 to 4.4 µm without a significant number of larger undesired particles being present. Acknowledgements: This work was done within the framework of the DFG funded Ice Nucleation research UnIT (INUIT, FOR 1525) under WE 4722/1-1. References

20. Time Resolved Measurements of Primary Biogenic Aerosol Particles in Amazonia

Science.gov (United States)

Wollny, A. G.; Garland, R.; Pöschl, U.

2009-04-01

Biogenic aerosols are ubiquitous in the Earth's atmosphere and they influence atmospheric chemistry and physics, the biosphere, climate, and public health. They play an important role in the spread of biological organisms and reproductive materials, and they can cause or enhance human, animal, and plant diseases. Moreover, they influence the Earth's energy budget by scattering and absorbing radiation, and they can initiate the formation of clouds and precipitation as cloud condensation and ice nuclei. The composition, abundance, and origin of biogenic aerosol particles and components are, however, still not well understood and poorly quantified. Prominent examples of primary biogenic aerosol particles, which are directly emitted from the biosphere to the atmosphere, are pollen, bacteria, fungal spores, viruses, and fragments of animals and plants. During the Amazonian Aerosol Characterization Experiment (AMAZE-08) a large number of aerosol and gas-phase measurements were taken on a remote site close to Manaus, Brazil, during a period of five weeks in February and March 2008. This presented study is focused on data from an ultraviolet aerodynamic particle sizer (UVAPS, TSI inc.) that has been deployed for the first time in Amazonia. In this instrument, particle counting and aerodynamic sizing over the range of 0.5-20 µm are complemented by the measurement of UV fluorescence at 355 nm (excitation) and 420-575 nm (emission), respectively. Fluorescence at these wavelengths is characteristic for reduced pyridine nucleotides (e.g., NAD(P)H) and for riboflavin, which are specific for living cells. Thus particles exhibiting fluorescence signals can be regarded as "viable aerosols" or "fluorescent bioparticles" (FBAP), and their concentration can be considered as lower limit for the actual abundance of primary biogenic aerosol particles. Data from the UVAPS were averaged over 5 minute time intervals. The presence of bioparticles in the observed size range has been

1. AERONET-based microphysical and optical properties of smoke-dominated aerosol near source regions and transported over oceans, and implications for satellite retrievals of aerosol optical depth

Science.gov (United States)

Sayer, A. M.; Hsu, N. C.; Eck, T. F.; Smirnov, A.; Holben, B. N.

2013-09-01

Smoke aerosols from biomass burning are an important component of the global aerosol cycle. Analysis of Aerosol Robotic Network (AERONET) retrievals of size distribution and refractive index reveals variety between biomass burning aerosols in different global source regions, in terms of aerosol particle size and single scatter albedo (SSA). Case studies of smoke transported to coastal/island AERONET sites also mostly lie within the range of variability at near-source sites. Two broad ''families'' of aerosol properties are found, corresponding to sites dominated by boreal forest burning (larger, broader fine mode, with midvisible SSA ∼0.95), and those influenced by grass, shrub, or crop burning with additional forest contributions (smaller, narrower particles with SSA ∼0.88-0.9 in the midvisible). The strongest absorption is seen in southern African savannah at Mongu (Zambia), with average SSA ∼0.85 in the midvisible. These can serve as candidate sets of aerosol microphysical/optical properties for use in satellite aerosol optical depth (AOD) retrieval algorithms. The models presently adopted by these algorithms over ocean are often insufficiently absorbing to represent these biomass burning aerosols. A corollary of this is an underestimate of AOD in smoke outflow regions, which has important consequences for applications of these satellite datasets.

2. Aerosol and Cloud-Nucleating Particle Observations during an Atmospheric River Event

Science.gov (United States)

DeMott, P. J.; McCluskey, C. S.; Petters, M.; Suski, K. J.; Levin, E. J.; Hill, T. C. J.; Atwood, S. A.; Schill, G. P.; Rocci, K.; Boose, Y.; Martin, A.; Cornwell, G.; Al-Mashat, H.; Moore, K.; Prather, K. A.; Rothfuss, N.; Taylor, H.; Leung, L. R.; Tomlinson, J. M.; Mei, F.; Hubbe, J. M.; Rosenfeld, D.; Spackman, J. R.; Fairall, C. W.; Creamean, J.; White, A. B.; Kreidenweis, S. M.

2015-12-01

The multi-agency CalWater 2015 project occurred over North Central CA and the Eastern Pacific during January to March 2015 (Spackman et al., this session). The goals of the campaign were to document the structure of atmospheric rivers (ARs) that deliver much of the water vapor associated with major winter storms along the U.S. West Coast and to investigate the modulating effect of aerosols on precipitation. Aerosol sources that may influence orographic cloud properties for air lifted over the mountains in California in winter include pollution, biomass burning, soil dusts and marine aerosols, but their roles will also be influenced by transport, vertical stratification, and scavenging processes. We present results from a comprehensive study of aerosol distributions, compositions, and cloud nucleating properties during an intense winter storm during February 2015, including data from an NSF-supported measurement site at Bodega Bay, from the DOE-ARM Cloud Aerosol Precipitation Experiment that included sampling on the NOAA RV Ron Brown offshore and the G-1 aircraft over ocean and land, and with context provided by other NOAA aircraft and remote sensing facilities. With a special focus on the coastal site, we discuss changes in aerosol distributions, aerosol hygroscopicity, and number concentrations of fluorescent particles, cloud condensation nuclei (CCN), and ice nucleating particles (INPs) during the AR event. We compare with periods preceding and following the event. For example, total aerosol number and surface area concentrations at below 0.5 μm diameter decreased from typical values of a few thousand cm-3 and 100 μm2 cm-3, respectively, to a few hundred cm-3 and 10 μm2cm-3 at Bodega Bay during the AR event. CCN concentrations were similarly lower, but hygroscopicity parameter (kappa) increased from typical values of 0.2 to values > 0.5 during the AR.INP and fluorescent particle number concentrations were generally lower during the AR event than at any other

3. Mixing properties of individual submicrometer aerosol particles in Vienna

Science.gov (United States)

Individual aerosol particles were collected on 5 days with different meteorological conditions in March, April and June 1991 in the urban atmosphere of Vienna in Austria. The samples collected with an impactor were examined by electron microscopy. The mixing properties of submicrometer aerosol particles with radii between 0.1 and 1 μm were studied by using the dialysis (extraction) of water-soluble material. The averaged results showed that more than 85% of particles with radii between 0.1 and 0.7 μm were hygroscopic. However, more than 50% of particles with radii larger than 0.2 μm were mixed particles (hygroscopic particles with water-insoluble inclusions), and they were dominant (80%) in the size range 0.5-0.7 μm radius. The results also showed that the number proportion of mixed particles increased with increasing radius and the abundance increased with increasing particle loading in the atmosphere. The volume fraction of water-soluble material ( ɛ) in mixed particles tended to decrease with increasing radius, implying the formation of mixed particles by heterogeneous processes such as condensation and/or surface reaction. Some results of elemental composition in individual particles analyzed with an energy-dispersive X-ray (EDX) analyzer equipped with an electron microscope are also presented in this paper.

4. Improved identification of primary biological aerosol particles using single particle mass spectrometry

OpenAIRE

Zawadowicz, Maria A.; Froyd, Karl D.; Murphy, Daniel M.; Cziczo, Daniel J.

2016-01-01

Measurements of primary biological aerosol particles, especially at altitudes relevant to cloud formation, are scarce. Single particle mass spectrometry (SPMS) has been used to probe aerosol chemical composition from ground and aircraft for over 20 years. Here we develop a method for identifying bioaerosols using SPMS. We show that identification of bioaerosol using SPMS is complicated because phosphorus-bearing mineral dust and phosphorus-rich combustion by-products such as fly ash produce m...

5. Organic aerosol mixing observed by single-particle mass spectrometry.

Science.gov (United States)

Robinson, Ellis Shipley; Saleh, Rawad; Donahue, Neil M

2013-12-27

We present direct measurements of mixing between separately prepared organic aerosol populations in a smog chamber using single-particle mass spectra from the high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Docosane and docosane-d46 (22 carbon linear solid alkane) did not show any signs of mixing, but squalane and squalane-d62 (30 carbon branched liquid alkane) mixed on the time scale expected from a condensational-mixing model. Docosane and docosane-d46 were driven to mix when the chamber temperature was elevated above the melting point for docosane. Docosane vapors were shown to mix into squalane-d62, but not the other way around. These results are consistent with low diffusivity in the solid phase of docosane particles. We performed mixing experiments on secondary organic aerosol (SOA) surrogate systems finding that SOA derived from toluene-d8 (a surrogate for anthropogenic SOA (aSOA)) does not mix into squalane (a surrogate for hydrophobic primary organic aerosol (POA)) but does mix into SOA derived from α-pinene (biogenic SOA (bSOA) surrogate). For the aSOA/POA, the volatility of either aerosol does not limit gas-phase diffusion, indicating that the two particle populations do not mix simply because they are immiscible. In the aSOA/bSOA system, the presence of toluene-d8-derived SOA molecules in the α-pinene-derived SOA provides evidence that the diffusion coefficient in α-pinene-derived SOA is high enough for mixing on the time scale of 1 min. The observations from all of these mixing experiments are generally invisible to bulk aerosol composition measurements but are made possible with single-particle composition data.

6. Characteristics and sources of carbonaceous aerosols from Shanghai, China

Directory of Open Access Journals (Sweden)

J.-J. Cao

2012-07-01

Full Text Available An intensive investigation of carbonaceous PM2.5 and TSP from Pudong (China was conducted as part of the MIRAGE-Shanghai Experiment in 2009. Data for organic and elemental carbon (OC and EC, organic species, including C17 to C40 n-alkanes and 17 polycyclic aromatic hydrocarbons (PAHs, and stable C isotopes OC (δ13COC and EC (δ13CEC were used to evaluate the aerosols' temporal variations and identify presumptive sources. High OC/EC ratios indicated a large fraction of secondary organic aerosol (SOA; high char/soot ratios indicated stronger contributions to EC from motor vehicles and coal combustion than biomass burning. Diagnostic ratios of PAHs indicated that much of the SOA was produced via coal combustion. Isotope abundances (δ13COC = −24.5 ± 0.8‰ and δ13CEC = −25.1 ± 0.6‰ indicated that fossil fuels were the most important source for carbonaceous PM2.5, with lesser impacts from biomass burning and natural sources. An EC tracer system and isotope mass balance calculations showed that the relative contributions to total carbon from coal combustion, motor vehicle exhaust, and SOA were 41%, 21%, and 31%: other primary sources such as marine, soil and biogenic emissions contributed 7%. Combined analyses of OC and EC, n-alkanes and PAHs, and stable carbon isotopes provide a new way to apportion the sources of carbonaceous particles.

7. Chemical composition, main sources and temporal variability of PM1 aerosols in southern African grassland

Science.gov (United States)

Tiitta, P.; Vakkari, V.; Josipovic, M.; Croteau, P.; Beukes, J. P.; van Zyl, P. G.; Venter, A. D.; Jaars, K.; Pienaar, J. J.; Ng, N. L.; Canagaratna, M. R.; Jayne, J. T.; Kerminen, V.-M.; Kulmala, M.; Laaksonen, A.; Worsnop, D. R.; Laakso, L.

2013-06-01

Southern Africa is a significant source region of atmospheric pollution, yet long-term data on pollutant concentrations and properties from this region are rather limited. A recently established atmospheric measurement station in South Africa, Welgegund, is strategically situated to capture regional background emissions, as well as emissions from the major source regions in the interior of South Africa. We measured non-refractive submicron aerosols (NR-PM1) and black carbon over a one year period in Welgegund, and investigated the seasonal and diurnal patterns of aerosol concentration levels, chemical composition, acidity and oxidation level. Based on air mass back trajectories, four distinct source regions were determined for NR-PM1. Supporting data utilized in our analysis included particle number size distributions, aerosol absorption, trace gas concentrations, meteorological variables and the flux of carbon dioxide. The dominant submicron aerosol constituent during the dry season was organic aerosol, reflecting high contribution from savannah fires and other combustion sources. Organic aerosol concentrations were lower during the wet season, presumably due to wet deposition as well as reduced emissions from combustion sources. Sulfate concentrations were usually high and exceeded organic aerosol concentrations when air-masses were transported over regions containing major point sources. Sulfate and nitrate concentrations peaked when air masses passed over the industrial Highveld (iHV) area. In contrast, concentrations were much lower when air masses passed over the cleaner background (BG) areas. Air masses associated with the anti-cyclonic recirculation (ACBIC) source region contained largely aged OA. Positive Matrix Factorization (PMF) analysis of aerosol mass spectra was used to characterize the organic aerosol (OA) properties. The factors identified were oxidized organic aerosols (OOA) and biomass burning organic aerosols (BBOA) in the dry season and low

8. Sea-spray aerosol particles generated in the surf zone

NARCIS (Netherlands)

Eijk, A.M.J. van; Kusmierczyk‐Michulec, J.T.; Francius, M.J.; Tedeschi, G.; Piazzola,J.; Merritt, D.L.; Fontana, J.D.

2011-01-01

To assess the properties of aerosol particles generated over the surf zone, two experiments were held at the pier of Scripps Institution of Oceanography (SIO), La Jolla CA, and at the pier of the U.S. Army Corps of Engineers Field Research Facility (FRF) in Duck NC. On both sites concentrations of s

9. Impact of aerosols and atmospheric particles on plant leaf proteins

Science.gov (United States)

Yan, Xing; Shi, Wen Z.; Zhao, Wen J.; Luo, Na N.

2014-05-01

Aerosols and atmospheric particles can diffuse and absorb solar radiation, and directly affect plant photosynthesis and related protein expression. In this study, for the first time, we performed an extensive investigation of the effects of aerosols and atmospheric particles on plant leaf proteins by combining Geographic Information System and proteomic approaches. Data on particles with diameters of 0.1-1.0 μm (PM1) from different locations across the city of Beijing and the aerosol optical depth (AOD) over the past 6 years (2007-2012) were collected. In order to make the study more reliable, we segregated the influence of soil pollution by measuring the heavy metal content. On the basis of AOD and PM1, two regions corresponding to strong and weak diffuse solar radiations were selected for analyzing the changes in the expression of plant proteins. Our results demonstrated that in areas with strong diffuse solar radiations, plant ribulose bisphosphate carboxylase was expressed at higher levels, but oxygen evolved in enhancer protein and light-harvesting complex II protein were expressed at lower levels. The expression of ATP synthase subunit beta and chlorophyll a-b binding protein were similar in both regions. By analyzing the changes in the expression of these leaf proteins and their functions, we conclude that aerosols and atmospheric particles stimulate plant photosynthesis facilitated by diffuse solar radiations.

10. Light Absorption of Biogenic Aerosol Particles in Amazonia

Science.gov (United States)

Holanda, B. A.; Artaxo, P.; Ferreira De Brito, J.; Barbosa, H. M.; Andreae, M. O.; Saturno, J.; Pöhlker, C.; Holben, B. N.; Schafer, J.

2014-12-01

Aerosol absorption is a key issue in proper calculation of aerosol radiative forcing. Especially in the tropics with the dominance of natural biogenic aerosol and brown carbon, the so called anomalous absorption is of particular interest. A special experiment was designed to study the wavelength dependence of aerosol absorption for PM2.5 as well as for PM10 particles in the wet season in Central Amazonia. Aerosol analysis occurred from May to August 2014, in the ZF2 ecological reservation, situated at about 55 km North of Manaus in very pristine conditions Two 7 wavelengths AE33 Aethalometers were deployed measuring in parallel, but with a PM2.5 and PM10 inlets. Two MAAP (Multiangle Aerosol Absorption Photometer) were operated in parallel with the AE33 exactly at the same PM2.5 and PM10 inlets. Organic and elemental carbon was analyzed using collection with quartz filters and analysis using a Sunset OC/EC analyzer. Aerosol light scattering for 3 wavelengths was measured using Air Photon and TSI Nephelometers. Aerosol size distribution was measured with one TSI SMPS and a GRIMM OPC to have the size range from 10 nm to 10 micrometers. Particles were measured under dry conditions using diffusion dryers. Aerosol optical depth and absorption was also measured with an AERONET sunphotometer operated close to the site. As the experiment was run in the wet season, very low equivalent black carbon (EBC) were measured, with average concentrations around 50 ng/m³ during May, increasing to 130 ng/m³ in June and July. The measurements adjusted for similar wavelengths shows excellent agreement between the MAAP and AE33 for both inlets (PM2.5 and PM10). It was not possible statistically infer absorption from the coarse mode biogenic particles, since the absorption was completely dominated by fine mode particles. AERONET measurements shows very low values of AOD, at 0.17 at 500 nm and 0.13 at 870 nm, with very low absorption AOD values at 0.00086 at 676 nm and 0.0068 at 872 nm

11. Ultrasensitive detection of inhaled organic aerosol particles by accelerator mass spectrometry.

Science.gov (United States)

Parkhomchuk, E V; Gulevich, D G; Taratayko, A I; Baklanov, A M; Selivanova, A V; Trubitsyna, T A; Voronova, I V; Kalinkin, P N; Okunev, A G; Rastigeev, S A; Reznikov, V A; Semeykina, V S; Sashkina, K A; Parkhomchuk, V V

2016-09-01

Accelerator mass spectrometry (AMS) was shown to be applicable for studying the penetration of organic aerosols, inhaled by laboratory mice at ultra-low concentration ca. 10(3) cm(-3). We synthesized polystyrene (PS) beads, composed of radiocarbon-labeled styrene, for testing them as model organic aerosols. As a source of radiocarbon we used methyl alcohol with radioactivity. Radiolabeled polystyrene beads were obtained by emulsifier-free emulsion polymerization of synthesized (14)C-styrene initiated by K2S2O8 in aqueous media. Aerosol particles were produced by pneumatic spraying of diluted (14)C-PS latex. Mice inhaled (14)C-PS aerosol consisting of the mix of 10(3) 225-nm particles per 1 cm(3) and 5·10(3) 25-nm particles per 1 cm(3) for 30 min every day during five days. Several millions of 225-nm particles deposited in the lungs and slowly excreted from them during two weeks of postexposure. Penetration of particles matter was also observed for liver, kidneys and brain, but not for a heart.

12. Aerosol vertical distribution, new particle formation, and jet aircraft particle emissions in the free troposhere and tropopause region; Vertikalverteilung und Neubildungsprozesse des Aerosols und partikelfoermige Flugzeugemissionen in der freien Troposphaere und Tropopausenregion

Energy Technology Data Exchange (ETDEWEB)

Schroeder, F.P.

2000-07-01

A contribution to the understanding of natural and anthropogenously induced particle formation as well as aerosol physical transformation processes within the free troposphere (FT) is introduced. Documentation and interpretation of empirical data relevant with respect to possible climatologic impact of anthropogenous aerosol emissions into the atmosphere is presented. The first section describes new technique for high spatial resolution measurements of ultrafine aerosol particles by condensation nucleus counters (CNCs), a necessary prerequisite for the observation of natural particle formation and jet aircraft emissions. The second section illustrates vertical distribution and variability ranges of the aerosol in the FT and the tropopause region (TP). Typical microphysical states of the atmospheric aerosol within the Northern Hemisphere are documented by means of systematic measurements during more than 60 flight missions. Simple mathematical parameterizations of the aerosol vertical distribution and aerosol size distributions are developed. Important aerosol sources within the FT are localized and possible aerosol formation processes are discussed. The third section is focussed on jet-engine particle emissions within the FT and TP. A unique inflight experiment for detection of extremely high concentrations (>10{sup 6} cm{sup -3}) of extremely small (donw to <3 nm) aerosols inside the exhaust plumes of several jet aircraft is described. Particle emission indices and emission-controlling parameters are deduced. Most important topic is the impact of fuel sulfur content of kerosine on number, size and chemical composition of jet particle emissions. Generalized results are parameterized in form of lognormal aerosol particle size distributions. (orig.) [German] Ein Beitrag zum Verstaendnis natuerlicher und anthropogen induzierter Aerosolneubildung sowie physikalischer Aerosolumwandlung in der freien Troposphaere wird vorgestellt. Empirisch gewonnenes Datenmaterial wird

13. Individual particle morphology, coatings, and impurities of black carbon aerosols in Antarctic ice and tropical rainfall

Science.gov (United States)

Ellis, Aja; Edwards, Ross; Saunders, Martin; Chakrabarty, Rajan K.; Subramanian, R.; Timms, Nicholas E.; Riessen, Arie; Smith, Andrew M.; Lambrinidis, Dionisia; Nunes, Laurie J.; Vallelonga, Paul; Goodwin, Ian D.; Moy, Andrew D.; Curran, Mark A. J.; Ommen, Tas D.

2016-11-01

Black carbon (BC) aerosols are a large source of climate warming, impact atmospheric chemistry, and are implicated in large-scale changes in atmospheric circulation. Inventories of BC emissions suggest significant changes in the global BC aerosol distribution due to human activity. However, little is known regarding BC's atmospheric distribution or aged particle characteristics before the twentieth century. Here we investigate the prevalence and structural properties of BC particles in Antarctic ice cores from 1759, 1838, and 1930 Common Era (C.E.) using transmission electron microscopy and energy-dispersive X-ray spectroscopy. The study revealed an unexpected diversity in particle morphology, insoluble coatings, and association with metals. In addition to conventionally occurring BC aggregates, we observed single BC monomers, complex aggregates with internally, and externally mixed metal and mineral impurities, tar balls, and organonitrogen coatings. The results of the study show BC particles in the remote Antarctic atmosphere exhibit complexity that is unaccounted for in atmospheric models of BC.

14. Aerosol composition, sources and processes during wintertime in Beijing, China

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Y. L. Sun

2013-01-01

Full Text Available Air pollution is a major environmental concern among all seasons in megacity Beijing, China. Here we present the results from a winter study that was conducted from 21 November 2011 to 20 January 2012 with an Aerodyne Aerosol Chemical Speciation Monitor (ACSM and various collocated instruments. The non-refractory submicron aerosol (NR-PM1 species vary dramatically with clean periods and pollution episodes alternating frequently. Compared to summer, wintertime submicron aerosols show much enhanced organics and chloride, which on average account for 52% and 5%, respectively of the total NR-PM1 mass. All NR-PM1 species show quite different diurnal behaviors between summer and winter. For example, the wintertime nitrate presents a gradual increase during daytime and correlates well with secondary organic aerosol (OA, indicating a dominant role of photochemical production over gas-particle partitioning. Positive matrix factorization was performed on ACSM OA mass spectra, and identified three primary OA (POA factors, i.e. hydrocarbon-like OA (HOA, cooking OA (COA, and coal combustion OA (CCOA, and one secondary factor, i.e. oxygenated OA (OOA. The POA dominates OA during wintertime, contributing 69% with the rest of 31% being SOA. Further, all POA components show pronounced diurnal cycles with the highest concentrations occurring at nighttime. CCOA is the largest primary source during the heating season, on average accounting for 33% of OA and 17% of NR-PM1. CCOA also plays a significant role in chemically-resolved particulate matter (PM pollution as its mass contribution increases linearly as a function of NR-PM1 mass loadings. The SOA however presents a reversed trend, which might indicate the limited SOA formation during high PM pollution episodes in winter. The effects of meteorology on PM pollution and aerosol processing were also explored. In particular, the sulfate mass is largely enhanced

15. Apportionment of urban aerosol sources in Cork (Ireland) by synergistic measurement techniques.

Science.gov (United States)

Dall'Osto, Manuel; Hellebust, Stig; Healy, Robert M; O'Connor, Ian P; Kourtchev, Ivan; Sodeau, John R; Ovadnevaite, Jurgita; Ceburnis, Darius; O'Dowd, Colin D; Wenger, John C

2014-09-15

The sources of ambient fine particulate matter (PM2.5) during wintertime at a background urban location in Cork city (Ireland) have been determined. Aerosol chemical analyses were performed by multiple techniques including on-line high resolution aerosol time-of-flight mass spectrometry (Aerodyne HR-ToF-AMS), on-line single particle aerosol time-of-flight mass spectrometry (TSI ATOFMS), on-line elemental carbon-organic carbon analysis (Sunset_EC-OC), and off-line gas chromatography/mass spectrometry and ion chromatography analysis of filter samples collected at 6-h resolution. Positive matrix factorization (PMF) has been carried out to better elucidate aerosol sources not clearly identified when analyzing results from individual aerosol techniques on their own. Two datasets have been considered: on-line measurements averaged over 2-h periods, and both on-line and off-line measurements averaged over 6-h periods. Five aerosol sources were identified by PMF in both datasets, with excellent agreement between the two solutions: (1) regional domestic solid fuel burning--"DSF_Regional," 24-27%; (2) local urban domestic solid fuel burning--"DSF_Urban," 22-23%; (3) road vehicle emissions--"Traffic," 15-20%; (4) secondary aerosols from regional anthropogenic sources--"SA_Regional" 9-13%; and (5) secondary aged/processed aerosols related to urban anthropogenic sources--"SA_Urban," 21-26%. The results indicate that, despite regulations for restricting the use of smoky fuels, solid fuel burning is the major source (46-50%) of PM2.5 in wintertime in Cork, and also likely other areas of Ireland. Whilst wood combustion is strongly associated with OC and EC, it was found that peat and coal combustion is linked mainly with OC and the aerosol from these latter sources appears to be more volatile than that produced by wood combustion. Ship emissions from the nearby port were found to be mixed with the SA_Regional factor. The PMF analysis allowed us to link the AMS cooking organic

16. Internally mixed soot, sulfates, and organic matter in aerosol particles from Mexico City

Directory of Open Access Journals (Sweden)

2008-05-01

Full Text Available Soot particles are major aerosol constituents that result from emissions of burning of fossil fuel and biomass. Because they both absorb sunlight and contribute to cloud formation, they are an influence on climate on local, regional, and global scales. It is therefore important to evaluate their optical and hygroscopic properties and those effects on the radiation budget. Those properties commonly change through reaction with other particles or gases, resulting in complex internal mixtures. Using transmission electron microscopy, we measured ~8000 particles (25 samples with aerodynamic diameters from 0.05 to 0.3 μm that were collected in March 2006 from aircraft over Mexico City (MC and adjacent areas. More than 50% of the particles consist of internally mixed soot, organic matter, and sulfate. Imaging combined with chemical analysis of individual particles show that many are coated, consist of aggregates, or both. Coatings on soot particles can amplify their light absorption, and coagulation with sulfates changes their hygroscopic properties, resulting in shorter lifetime. Our results suggest that a mixture of materials from multiple sources such as vehicles, power plants, and biomass burning occurs in individual particles, thereby increasing their complexity. Through changes in their optical and hygroscopic properties, internally mixed soot particles have a greater effect on the regional climate than uncoated soot particles. Moreover, soot occurs in more than 60% of all particles in the MC plumes, suggesting its important role in the formation of secondary aerosol particles.

17. Visualizing aerosol-particle injection for diffractive-imaging experiments

CERN Document Server

Awel, Salah; Eckerskorn, Niko; Wiedorn, Max; Horke, Daniel A; Rode, Andrei V; Küpper, Jochen; Chapman, Henry N

2015-01-01

Delivering sub-micrometer particles to an intense x-ray focus is a crucial aspect of single-particle diffractive-imaging experiments at x-ray free-electron lasers. Enabling direct visualization of sub-micrometer aerosol particle streams without interfering with the operation of the particle injector can greatly improve the overall efficiency of single-particle imaging experiments by reducing the amount of time and sample consumed during measurements. We have developed in-situ non-destructive imaging diagnostics to aid real-time particle injector optimization and x-ray/particle-beam alignment, based on laser illumination schemes and fast imaging detectors. Our diagnostics are constructed to provide a non-invasive rapid feedback on injector performance during measurements, and have been demonstrated during diffraction measurements at the FLASH free-electron laser.

18. Mode resolved density of atmospheric aerosol particles

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P. Aalto

2008-09-01

Full Text Available In this study, we investigate the mode resolved density of ultrafine atmospheric particles measured in boreal forest environment. The method used here enables us to find the distinct density information for each mode in atmospheric fine particle population: the density values for nucleation, Aitken, and accumulation mode particles are presented. The experimental data was gained during 2 May 2005–19 May 2005 at the boreal forest measurement station "SMEAR II" in Hyytiälä, Southern Finland. The density values for accumulation mode varied from 1.1 to 2 g/cm3 (average 1.5 g/cm3 and for Aitken mode from 0.4 to 2 g/cm3 (average 0.97 g/cm3. As an overall trend during the two weeks campaign, the density value of Aitken mode was seen to gradually increase. With the present method, the time dependent behaviour of the particle density can be investigated in the time scale of 10 min. This allows us to follow the density evolution of the nucleation mode particles during the particle growth process following the nucleation burst. The density of nucleation mode particles decreased during the growth process. The density values for 15 nm particles were 1.2–1.5 g/cm3 and for grown 30 nm particles 0.5–1 g/cm3. These values are consistent with the present knowledge that the condensing species are semi-volatile organics, emitted from the boreal forest.

19. Functional group composition of ambient and source organic aerosols determined by tandem mass spectrometry

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J. Dron

2010-04-01

Full Text Available The functional group composition of various organic aerosols (OA is being investigated using a recently developed analytical approach based on atmospheric pressure chemical ionisation-tandem mass spectrometry (APCI-MS/MS. The determinations of the three functional groups' contents are performed quantitatively by neutral loss (carboxylic and carbonyl groups and precursor ion (nitro groups scanning modes of a tandem mass spectrometer. Major organic aerosol sources are studied: vehicular emission and wood combustion for primary aerosol sources; and a secondary organic aerosol (SOA produced through photo-oxidation of o-xylene. The results reveal significant differences in the functional group contents of these source aerosols. The laboratory generated SOA is dominated by carbonyls while carboxylics are preponderate in the wood combustion particles. On the other hand, vehicular emissions are characterised by a strong nitro content. The total amount of the three functional groups accounted for 1.7% (vehicular to 13.5% (o-xylene photo-oxidation of the organic carbon. The diagnostic functional group ratios are then used to tentatively differentiate sources of particles collected in an urban background environment located in an Alpine valley (Chamonix, France during a strong winter pollution event. The three functional groups under study account for a total functionalisation rate of 2.2 to 3.8% of the organic carbon in this ambient aerosol, which is also dominated by carboxylic moieties. In this particular case study of a deep alpine valley during winter, we show that the nitro- and carbonyl-to-carboxylic diagnostic ratios can be a useful tool to distinguish the sources. In these conditions, the total OA concentrations are highly dominated by wood combustion OA. This result is confirmed by an organic markers source apportionment approach which assesses a wood burning organic carbon contribution of about 60%. Finally, examples of functional group mass

20. Glyoxal processing by aerosol multiphase chemistry: towards a kinetic modeling framework of secondary organic aerosol formation in aqueous particles

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B. Ervens

2010-09-01

on aerosol loading or water content, which indicates a possibly catalytic role of aerosol water in SOA formation. However, the reversible nature of uptake under dark conditions is not captured by keffupt, and can be parameterized by an effective Henry's law constant including an equilibrium constant Kolig = 1000 (in ammonium sulfate solution. Such reversible glyoxal oligomerization contributes <1% to total predicted SOA masses at any time.

Sensitivity tests reveal five parameters that strongly affect the predicted SOA mass from glyoxal: (1 time scales to reach equilibrium states (as opposed to assuming instantaneous equilibrium, (2 particle pH, (3 chemical composition of the bulk aerosol, (4 particle surface composition, and (5 particle liquid water content that is mostly determined by the amount and hygroscopicity of aerosol mass and to a lesser extent by the ambient relative humidity.

Glyoxal serves as an example molecule, and the conclusions about SOA formation in aqueous particles can serve for comparative studies of other molecules that form SOA as the result of multiphase chemical processing in aerosol water. This SOA source is currently underrepresented in atmospheric models; if included it is likely to bring SOA predictions (mass and O/C ratio into better agreement with field observations.

1. Seasonal variations in aerosol particle composition at the puy-de-Dôme research station

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E. J. Freney

2011-10-01

Full Text Available Detailed investigations of the chemical and microphysical properties of atmospheric aerosol particles were performed at the puy-de-Dôme (pdD research station (1465 m in autumn (September and October 2008, winter (February and March 2009, and summer (June 2010 using a Time-of-Flight Aerosol Mass Spectrometer. Over the three campaigns, the average mass concentrations of the non-refractory submicron particles ranged from 10 μg m−3 up to 27 μg m−3. Highest nitrate and ammonium mass concentrations were measured during the winter and during periods when marine modified airmasses were arriving at the site, whereas highest concentrations of organic particles were measured during the summer and during periods when continental airmasses arrived at the site. The measurements reported in this paper show that atmospheric particle composition is strongly influenced by both the season and the origin of the airmass. The total organic mass spectra were analysed using positive matrix factorisation to separate individual organic components contributing to the overall organic particle mass concentrations. These organic components include a low volatility oxygenated organic aerosol particle (LV-OOA and a semi-volatile organic aerosol particle (SV-OOA. Correlations of the LV-OOA components with fragments of m/z 60 and m/z 73 (mass spectral markers of wood burning during the winter campaign suggest that wintertime LV-OOA are related to aged biomass burning emissions, whereas organic aerosol particles measured during the summer are likely linked to biogenic sources. Equivalent potential temperature calculations, gas-phase, and LIDAR measurements define whether the research site is in the planetary boundary layer (PBL or in the free troposphere (FT/residual layer (RL. We observe that SV-OOA and nitrate particles are associated with air masses arriving from the PBL where as particle composition measured from RL/FT airmasses

2. Source regions for atmospheric aerosol measured at Barrow, Alaska.

Science.gov (United States)

Polissar, A V; Hopke, P K; Harris, J M

2001-11-01

Aerosol data consisting of condensation nuclei (CN) counts, black carbon (BC) mass concentration, and aerosol light scattering coefficient at the wavelength of 450 nm (SC) measured at Barrow, AK, from 1986 to 1997 have been analyzed. BC and SC show an annual cycle with the Arctic haze maxima in the winter and spring and the minima in the summer. The CN time series shows two maxima in March and August. Potential source contribution function (PSCF) that combines the aerosol data with air parcel backward trajectories was applied to identify potential source areas and the preferred pathways that give rise to the observed high aerosol concentrations at Barrow. Ten-day isentropic back trajectories arriving twice daily at 500 and 1500 m above sea level were calculated for the period from 1986 to 1997. The PSCF analyses were performed based on the 80th percentile criterion values for the 2- and 24-h averages of the measured aerosol parameters. There was a good correspondence between PSCF maps for the 2- and 24-h averages, indicating that 1-day aerosol sampling in the Arctic adequately represents the aerosol source areas. In winter, the high PSCF values for BC and SC are related to industrial source areas in Eurasia. The trajectory domain in winter and spring is larger than in summer, reflecting weaker transport in summer. No high PSCF areas for BC and SC can be observed in summer. The result is related to the poor transport into the Arctic plus the strong removal of aerosol by precipitation in summer. In contrast to the BC and SC maps, the CN plot for summer shows high PSCF areas in the North Pacific Ocean. High CN values appearto be mostly connected with the long-range transport from Eurasia in winter and spring and with the reduced sulfur compound emission from biogenic activities in the ocean in the summer. PSCF analysis was found to be effective in identifying potential aerosol source areas.

3. Measurement of ambient aerosols in northern Mexico City by single particle mass spectrometry

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R. C. Moffet

2007-05-01

Full Text Available Continuous ambient measurements with aerosol time-of-flight mass spectrometry (ATOFMS were carried out in an industrial/residential section in the northern part of Mexico City as part of the Mexico City Metropolitan Area – 2006 campaign (MCMA-2006 between 7–27 March, 2006. Biomass and organic carbon (OC particle types were found to dominate the accumulation mode both day and night. The concentrations of both organic carbon and biomass particles were roughly equal early in the morning, but biomass became the largest contributor to the accumulation mode mass from the late morning until early evening. The diurnal pattern can be attributed to aging and/or a change in meteorology. Fresh elemental carbon (EC particles were observed during rush hour. The majority of the EC particles were mixed with nitrate, sulfate, organic carbon and potassium. Submicron particles from industrial sources in the northeast were composed of an internal mixture of Pb, Zn, EC and Cl and peaked early in the morning. A unique nitrogen-containing organic (NOC particle type was observed, and is hypothesized to be from industrial emissions based on the temporal profile and back trajectory analysis. This study provides unique insights into the real-time changes in single particle mixing state as a function of size and time for aerosols in Mexico City. These new findings indicate that biomass burning and industrial operations make significant contributions to particles in Mexico City. These sources have received relatively little attention in previous intensive field campaigns.

4. Evaluation of coarse and fine particulate sources using a portable aerosol monitor in a desert community.

Science.gov (United States)

Phalen, Robert N; Coleman, Ted

2012-08-01

The purpose of this study was to use a portable aerosol monitor as a preliminary screening tool to identify local sources of coarse (PM(10-2.5)) and fine (PM(2.5)) particulate matter within the Coachella Valley, a low-elevation desert community. The portable aerosol monitor proved to be useful in identifying particle sources unique to the region, namely, sand dunes with sparse ground cover (vegetation), a river wash, and diesel truck and freight train traffic. The general limitations relate to discrepancies in the fraction of PM(10-2.5) when compared to regional air quality data and a lack of accurate mass-based data.

5. Particle Characterization and Ice Nucleation Efficiency of Field-Collected Aerosol Particles

Science.gov (United States)

Wang, B.; Gilles, M. K.; Laskin, A.; Moffet, R.; Nizkorodov, S.; Roedel, T.; Sterckx, L.; Tivanski, A.; Knopf, D. A.

2011-12-01

Atmospheric ice formation by heterogeneous nucleation is one of the least understood processes resulting in cirrus and mixed-phase clouds which affect the global radiation budget, the hydrological cycle, and water vapor distribution. In particular, how organic aerosol affect ice nucleation is not well understood. Here we report on heterogeneous ice nucleation from particles collected during the CalNex campaign at the Caltech campus site, Pasadena, on May 19, 2010 at 6am-12pm (A2) and 12pm-6pm (A3) and May 23 at 6am-12pm (B2) and 6pm-12am (B4). The ice nucleation onsets and water uptake were determined as a function of temperature (200-273 K) and relative humidity with respect to ice (RHice). The ice nucleation efficiency was related to the particle chemical composition. Single particle characterization was provided by using computer controlled scanning electron microscopy with energy dispersive analysis of X-rays (CCSEM/EDX) and scanning transmission X-ray microscopy with near edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). The STXM/NEXAFS analysis indicates that the morning sample (A2) constitutes organic particles and organic particles with soot and inorganic inclusions. The afternoon sample (A3) is dominated by organic particles with a potentially higher degree of oxidation associated with soot. The B2 sample shows a higher number fraction of magnesium-containing particle indicative of a marine source and ~93% of the particles contained sulfur besides oxygen and carbon as derived from CCSEM/EDX analysis. The B4 sample lacks the strong marine influence and shows higher organic content. Above 230 K, we observed water uptake followed by condensation freezing at mean RH of 93-100% and 89-95% for A2 and A3, respectively. This indicates that the aged A3 particles are efficient ice nuclei (IN) for condensation freezing. Below 230 K A2 and A3 induced deposition ice nucleation between 125-155% RHice (at mean values of 134-150% RHice). The B2 and B4

6. ISS Ambient Air Quality: Updated Inventory of Known Aerosol Sources

Science.gov (United States)

Meyer, Marit

2014-01-01

Spacecraft cabin air quality is of fundamental importance to crew health, with concerns encompassing both gaseous contaminants and particulate matter. Little opportunity exists for direct measurement of aerosol concentrations on the International Space Station (ISS), however, an aerosol source model was developed for the purpose of filtration and ventilation systems design. This model has successfully been applied, however, since the initial effort, an increase in the number of crewmembers from 3 to 6 and new processes on board the ISS necessitate an updated aerosol inventory to accurately reflect the current ambient aerosol conditions. Results from recent analyses of dust samples from ISS, combined with a literature review provide new predicted aerosol emission rates in terms of size-segregated mass and number concentration. Some new aerosol sources have been considered and added to the existing array of materials. The goal of this work is to provide updated filtration model inputs which can verify that the current ISS filtration system is adequate and filter lifetime targets are met. This inventory of aerosol sources is applicable to other spacecraft, and becomes more important as NASA considers future long term exploration missions, which will preclude the opportunity for resupply of filtration products.

7. Impacts of aerosol particles on the microphysical and radiative properties of stratocumulus clouds over the southeast Pacific Ocean

Science.gov (United States)

Twohy, C. H.; Anderson, J. R.; Toohey, D. W.; Andrejczuk, M.; Adams, A.; Lytle, M.; George, R. C.; Wood, R.; Saide, P.; Spak, S.; Zuidema, P.; Leon, D.

2013-03-01

The southeast Pacific Ocean is covered by the world's largest stratocumulus cloud layer, which has a strong impact on ocean temperatures and climate in the region. The effect of anthropogenic sources of aerosol particles on the stratocumulus deck was investigated during the VOCALS field experiment. Aerosol measurements below and above cloud were made with a ultra-high sensitivity aerosol spectrometer and analytical electron microscopy. In addition to more standard in-cloud measurements, droplets were collected and evaporated using a counterflow virtual impactor (CVI), and the non-volatile residual particles were analyzed. Many flights focused on the gradient in cloud properties on an E-W track along 20° S from near the Chilean coast to remote areas offshore. Mean statistics, including their significance, from eight flights and many individual legs were compiled. Consistent with a continental source of cloud condensation nuclei, below-cloud accumulation-mode aerosol and droplet number concentration generally decreased from near shore to offshore. Single particle analysis was used to reveal types and sources of the enhanced particle number that influence droplet concentration. While a variety of particle types were found throughout the region, the dominant particles near shore were partially neutralized sulfates. Modeling and chemical analysis indicated that the predominant source of these particles in the marine boundary layer along 20° S was anthropogenic pollution from central Chilean sources, with copper smelters a relatively small contribution. Cloud droplets were smaller in regions of enhanced particles near shore. However, physically thinner clouds, and not just higher droplet number concentrations from pollution, both contributed to the smaller droplets. Satellite measurements were used to show that cloud albedo was highest 500-1000 km offshore, and actually slightly lower closer to shore due to the generally thinner clouds and lower liquid water paths

8. Neural networks for aerosol particles characterization

Science.gov (United States)

Berdnik, V. V.; Loiko, V. A.

2016-11-01

Multilayer perceptron neural networks with one, two and three inputs are built to retrieve parameters of spherical homogeneous nonabsorbing particle. The refractive index ranges from 1.3 to 1.7; particle radius ranges from 0.251 μm to 56.234 μm. The logarithms of the scattered radiation intensity are used as input signals. The problem of the most informative scattering angles selection is elucidated. It is shown that polychromatic illumination helps one to increase significantly the retrieval accuracy. In the absence of measurement errors relative error of radius retrieval by the neural network with three inputs is 0.54%, relative error of the refractive index retrieval is 0.84%. The effect of measurement errors on the result of retrieval is simulated.

9. Aerosol and CCN properties at Princess Elisabeth station, East Antarctica: seasonality, new particle formation events and properties around precipitation events

Science.gov (United States)

Mangold, Alexander; Laffineur, Quentin; De Backer, Hugo; Herenz, Paul; Wex, Heike; Gossart, Alexandra; Souverijns, Niels; Gorodetskaya, Irina; Van Lipzig, Nicole

2016-04-01

Since 2010, several complementary ground-based instruments for measuring the aerosol composition of the Antarctic atmosphere have been operated at the Belgian Antarctic research station Princess Elisabeth, in Dronning Maud Land, East Antarctica (71.95° S, 23.35° E, 1390 m asl.). In addition, three ground-based remote sensing instruments for cloud and precipitation observations have been installed for continuous operation, including a ceilometer (cloud base height, type, vertical extent), a 24 Ghz micro-rain radar (vertical profiles of radar effective reflectivity and Doppler velocity), and a pyrometer (cloud base temperature). The station is inhabited from November to end of February and operates under remote control during the other months. In this contribution, the general aerosol and cloud condensation nuclei (CCN) properties will be described with a special focus on new particle formation events and around precipitation events. New particle formation events are important for the atmospheric aerosol budget and they also show that aerosols are not only transported to Antarctica but are also produced there, also inland. Aerosols are essential for cloud formation and therefore also for precipitation, which is the only source for mass gain of the Antarctic ice sheet. Measured aerosol properties comprise size distribution, total number, total mass concentration, mass concentration of light-absorbing aerosol and absorption coefficient and total scattering coefficient. In addition, a CCN counter has been operated during austral summers 2013/14, 2014/15 and 2015/16. The baseline total number concentration N-total was around some hundreds of particles/cm3. During new particle formation events N-total increased to some thousands of particles/cm3. Simultaneous measurements of N-total, size distribution and CCN number revealed that mostly the number of particles smaller than 100 nm increased and that the concentration of cloud condensation nuclei increased only very

10. Chemical and statistical interpretation of sized aerosol particles collected at an urban site in Thessaloniki, Greece.

Science.gov (United States)

Tsitouridou, Roxani; Papazova, Petia; Simeonova, Pavlina; Simeonov, Vasil

2013-01-01

The size distribution of aerosol particles (PM0.015-PM18) in relation to their soluble inorganic species and total water soluble organic compounds (WSOC) was investigated at an urban site of Thessaloniki, Northern Greece. The sampling period was from February to July 2007. The determined compounds were compared with mass concentrations of the PM fractions for nano (N: 0.015 pollution were identified and an attempt is made to find patterns of similarity between the different sized aerosols and the seasons of monitoring. It was proven that several major latent factors are responsible for the data structure despite the size of the aerosols - mineral (soil) dust, sea sprays, secondary emissions, combustion sources and industrial impact. The seasonal separation proved to be not very specific.

11. Virtual Impactor for Sub-micron Aerosol Particles

Science.gov (United States)

Bolshakov, A. A.; Strawa, A. W.; Hallar, A. G.

2005-12-01

The objective of a virtual impactor is to separate out the larger particles in a flow from the smaller particles in such a way that both sizes of particles are available for sampling. A jet of particle-laden air is accelerated toward a collection probe so that a small gap exists between the acceleration nozzle and the probe. A vacuum is applied to deflect a major portion of the airstream away form the collection probe. Particles larger than a certain size have sufficient momentum so that they cross the deflected streamlines and enter the collection probe, whereas smaller particles follow the deflected streamlines. The result is that the collection probe will contain a higher concentration of larger particles than is in the initial airstream. Typically, virtual impactors are high-flow devices used to separate out particles greater than several microns in diameter. We have developed a special virtual impactor to concentrate aerosol particles of diameters between 0.5 to 1 micron for the purpose of calibrating the optical cavity ring-down instrument [1]. No similar virtual impactors are commercially available. In our design, we have exploited considerations described earlier [2-4]. Performance of our virtual impactor was evaluated in an experimental set-up using TSI 3076 nebulizer and TSI 3936 scanning mobility particle size spectrometer. Under experimental conditions optimized for the best performance of the virtual impactor, we were able to concentrate the 700-nm polystyrene particles no less than 15-fold. However, under experimental conditions optimized for calibrating our cavity ring-down instrument, a concentration factor attainable was from 4 to 5. During calibration experiments, maximum realized particle number densities were 190, 300 and 1600 cm-3 for the 900-nm, 700-nm and 500-nm spheres, respectively. This paper discusses the design of the impactor and laboratory studies verifying its performance. References: 1. A.W. Strawa, R. Castaneda, T. Owano, D.S. Baer

12. Composition and Particle Size Retrievals for Homogeneous Binary Aerosols

Science.gov (United States)

Niedziela, R. F.; Argon, P.; Bejcek, L.

2014-12-01

Tropospheric aerosols have widely varying compositions, shapes, and sizes. The ability to measure these physical characteristics, coupled with knowledge about their optical properties, can provide insight as to how these particles might participate in atmospheric processes, including their interaction with light. Over the past several years, our laboratory has been involved in developing methods to determine basic physical properties of laboratory-generated particles based on the analysis of infrared extinction spectra of multi-component aerosols. Here we report the results of a complete study on the applicability of well-known refractive index mixing rules to homogeneous binary liquid organic aerosols in an effort to yield in situ measurements of particle size and composition. In particular, we present results for terpenoid (carvone/nopinone) and long-chain hydrocarbon (squalane/squalene) mixtures. The included image shows model carvone/nopinone extinction spectra that were computed using the Lorentz-Lorenz mixing rule on complex refractive index data for the pure components.

13. Particle size distribution and behavior of sulfate aerosols in a coastal region

Energy Technology Data Exchange (ETDEWEB)

Fujimura, M.; Hashimoto, Y.

1979-01-01

To obtain fundamental knowledge about sulfate aerosols, a field research was conducted in a coastal region distant from industrial pollution sources. The aerosol samples were analyzed for some elements, sulfate and ammonium ions. Sulfate was determined by the turbidimetry with 2-aminoperimidine, and ammonium was by the colorimetry of indophenol method. Trace elements with short-lived nuclides were analyzed by instrumental neutron activation analysis. The mass-size distribution curve of total aerosols was the general bimodal pattern, although the concentration level was very low. Most of sulfate and ammonium salts were distributed in the fine particle range less than 2 microns in aerodynamic diameter, but sulfate had another peak, thought to be of maritime origin, in the coarse particle range. Nevertheless, many fine sulfate particles that had been produced secondarily in the atmosphere were found in such a less polluted coastal region. The change of the sulfate concentrations obtained by the two-stage Andersen type sampler showed a correlation with the humidity. This may suggest that the formation of sulfate aerosols from sulfur dioxide could be related to a catalytic oxidation process in water drops.

14. Source apportionment of ambient aerosol applying PMF on AMS mobile and stationary data

Science.gov (United States)

Mohr, C.; Weimer, S.; Richter, R.; Decarlo, P. F.; Chirico, R.; Heringa, M. F.; Prévôt, A. S. H.; Baltensperger, U.

2009-04-01

Ambient aerosols are divided into the categories "primary" and "secondary", referring to particles directly emitted into the air, or formed out of precursor species such as volatile organic compounds, respectively. Main sources for primary urban aerosol and precursor species are traffic emissions, but also wood burning for domestic heating purposes especially in winter time (Alfarra et al., 2007). The quantification of various types of aerosol components is important for source identification which in turn is the basis of all mitigation activities. Positive Matrix Factorization (PMF) is a statistical based source apportionment tool that uses constrained, weighted least squares estimation to determine source profiles and strengths. PMF has been applied recently for the first time on highly time resolved organic mass spectra (Lanz et al., 2007) measured by an Aerodyne aerosol mass spectrometer (AMS) (Canagaratna et al., 2007). For the data presented here, two AMS were deployed together with additional instrumentation in the metropolitan area of Zurich in winter 2007/2008. The high-resolution time-of-flight AMS was stationed at an urban background site in the center, 30 meters from and shielded against direct traffic emissions. The quadrupole-based AMS was deployed in a mobile van allowing for on-road submicron aerosol composition measurements, and investigations into the spatial variability of aerosol concentration and composition. Results indicate that traffic emissions are the main contributor to submicron aerosol concentrations measured on-road. Hydrocarbon-like organic aerosol (HOA), a marker for traffic emissions (Lanz et al. 2007), dominates the primary aerosol mass, together with black carbon (BC). BC was monitored with the MAAP (multi angle absorption photometer). Another significant contributor to primary organic aerosol mass in downtown Zurich is domestic wood burning for heating purposes. Traffic and wood burning emissions make up roughly 50% of the total

15. An Analysis of AERONET Aerosol Absorption Properties and Classifications Representative of Aerosol Source Regions

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Giles, David M.; Holben, Brent N.; Eck, Thomas F.; Sinyuk, Aliaksandr; Smirnov, Alexander; Slutsker, Ilya; Dickerson, R. R.; Thompson, A. M.; Schafer, J. S.

2012-01-01

Partitioning of mineral dust, pollution, smoke, and mixtures using remote sensing techniques can help improve accuracy of satellite retrievals and assessments of the aerosol radiative impact on climate. Spectral aerosol optical depth (tau) and single scattering albedo (omega (sub 0) ) from Aerosol Robotic Network (AERONET) measurements are used to form absorption [i.e., omega (sub 0) and absorption Angstrom exponent (alpha(sub abs))] and size [i.e., extinction Angstrom exponent (alpha(sub ext)) and fine mode fraction of tau] relationships to infer dominant aerosol types. Using the long-term AERONET data set (1999-2010), 19 sites are grouped by aerosol type based on known source regions to: (1) determine the average omega (sub 0) and alpha(sub abs) at each site (expanding upon previous work); (2) perform a sensitivity study on alpha(sub abs) by varying the spectral omega (sub 0); and (3) test the ability of each absorption and size relationship to distinguish aerosol types. The spectral omega (sub 0) averages indicate slightly more aerosol absorption (i.e., a 0.0 pollution and smoke with dust show stronger absorption than dust alone. Frequency distributions of alpha(sub abs) show significant overlap among aerosol type categories and at least 10% of the alpha(sub abs) retrievals in each category are below 1.0. Perturbing the spectral omega (sub 0) by +/- 0.03 induces significant alpha(sub abs) changes from the unperturbed value by at least approx. +/- 0.6 for Dust, approx. +/-0.2 for Mixed, and approx. +/-0.1 for Urban/Industrial and Biomass Burning. The omega (sub 0)440nm and alpha(sub ext) 440-870nm relationship shows the best separation among aerosol type clusters, providing a simple technique for determining aerosol type from surface- and future space-based instrumentation.

16. Receptor modeling application framework for particle source apportionment.

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Watson, John G; Zhu, Tan; Chow, Judith C; Engelbrecht, Johann; Fujita, Eric M; Wilson, William E

2002-12-01

Receptor models infer contributions from particulate matter (PM) source types using multivariate measurements of particle chemical and physical properties. Receptor models complement source models that estimate concentrations from emissions inventories and transport meteorology. Enrichment factor, chemical mass balance, multiple linear regression, eigenvector. edge detection, neural network, aerosol evolution, and aerosol equilibrium models have all been used to solve particulate air quality problems, and more than 500 citations of their theory and application document these uses. While elements, ions, and carbons were often used to apportion TSP, PM10, and PM2.5 among many source types, many of these components have been reduced in source emissions such that more complex measurements of carbon fractions, specific organic compounds, single particle characteristics, and isotopic abundances now need to be measured in source and receptor samples. Compliance monitoring networks are not usually designed to obtain data for the observables, locations, and time periods that allow receptor models to be applied. Measurements from existing networks can be used to form conceptual models that allow the needed monitoring network to be optimized. The framework for using receptor models to solve air quality problems consists of: (1) formulating a conceptual model; (2) identifying potential sources; (3) characterizing source emissions; (4) obtaining and analyzing ambient PM samples for major components and source markers; (5) confirming source types with multivariate receptor models; (6) quantifying source contributions with the chemical mass balance; (7) estimating profile changes and the limiting precursor gases for secondary aerosols; and (8) reconciling receptor modeling results with source models, emissions inventories, and receptor data analyses.

17. Quantifying the sources of atmospheric ice nuclei from carbonaceous combustion aerosol

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Schill, G. P.; Jathar, S.; Galang, A.; Farmer, D.; Friedman, B.; Levin, E. J.; DeMott, P. J.; Kreidenweis, S. M.

2015-12-01

Ice nucleation on particles is a fundamental atmospheric process, which governs precipitation, cloud lifetimes, and climate. Despite being a basic atmospheric process, our current understanding of ice nucleation in the atmosphere is low. One reason for this low understanding is that ice nuclei concentrations are low (only ~1 in 105 particles in the free troposphere nucleate ice), making it challenging to identify both the composition and sources of ambient ice nuclei. Carbonaceous combustion aerosol produced from biomass and fossil fuel combustion are one potential source of these ice nuclei, as they contribute to over one-third of all aerosol in the North American free troposphere. Unfortunately, previous results from field measurements in-cloud, aircraft measurements, and laboratory studies are in conflict, with estimates of the impact of combustion aerosol ranging from no effect to rivaling the well-known atmospheric ice nuclei mineral dust. It is, however, becoming clear that aerosols from combustion processes are more complex than model particles, and their ice activity depends greatly on both fuel type and combustion conditions. Given these dependencies, we propose that sampling from real-world biomass burning and fossil fuel sources would provide the most useful new information on the contribution of carbonaceous combustion aerosols to atmospheric ice nuclei particles. To determine the specific contribution of refractory black carbon (rBC) to ice nuclei concentrations, we have coupled the Single Particle Soot Photometer (SP2) to the Colorado State University Continuous Flow Diffusion Chamber (CFDC). The SP2 utilizes laser-induced incandescence to quantify rBC mass on a particle-by-particle basis; in doing so, it also selectively destroys rBC particles by heating them to their vaporization temperature. Thus, the SP2 can be used as a selective pre-filter for rBC into the CFDC. In this work, we will present recent results looking at contribution of diesel

18. Linking Aerosol Source Activities to Present and Future Climate Effects

Science.gov (United States)

Koch, D.; Bond, T. C.; Streets, D.; Menon, S.; Unger, N.

2007-05-01

Aerosol source sectors (transport, power, industry, residential, biomass burning) generate distinct mixtures of aerosol species. These mixtures in turn have different effects on climate. As sectoral emissions change in coming decades, whether by regulation or not, it is helpful to link pollution from source types to climate consequences. We do so, using our global (GISS GCM) aerosol model for present and future IPCC SRES scenarios. According to our model, residential and transport sectors have net positive 1995 aerosol forcings (0.04 and 0.03 W m-2) due to their large black carbon contents. However, the sulfate-dominated power and industry sectors have net negative 1995 forcings (-0.10 and -0.09 W m-2). Due to the near-balance of absorbing and scattering components, biomass burning forcing is small. For the 2050 SRES A1B scenario, the net (negative) aerosol forcing is double 1995 due primarily to increased sulfur emissions in the industry and power sectors. For 2050 B1 the net (negative) forcing decreases relative to 1995, as sulfur emissions are reduced. Both future scenarios project decreasing residential emissions. Yet transport emissions are expected to remain significant and thus become the dominant source of warming aerosols in the future. Aerosol pollution is projected to shift southward relative to the present, as the current industrialized regions generally reduce emissions and tropical and southern hemispheric regions continue to develop. Similar to these SRES scenarios, IIASA scenarios project a decline in residential emissions; however IIASA is more optimistic about transport sector emissions reductions. We will conduct present-day climate experiments, including aerosol direct and indirect effects, to study impacts of power and transport sectors on climate features such as air temperature and hydrologic cycle.

19. Oxalate metal complexes in aerosol particles: implications for the hygroscopicity of oxalate-containing particles

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T. Furukawa

2011-05-01

Full Text Available Atmospheric aerosols have both a direct and an indirect cooling effect that influences the radiative balance at the Earth's surface. It has been estimated that the degree of cooling is large enough to weaken the warming effect of carbon dioxide. Among the cooling factors, secondary organic aerosols (SOA play an important role in the solar radiation balance in the troposphere as SOA can act as cloud condensation nuclei (CCN and extend the lifespan of clouds because of their high hygroscopic and water soluble nature. Oxalic acid is an important component of SOA, and is produced via several formation pathways in the atmosphere. However, it is not certain whether oxalic acid exists as free oxalic acid or as metal oxalate complexes in aerosols, although there is a marked difference in their solubility in water and their hygroscopicity. We employed X-ray absorption fine structure spectroscopy to characterize the calcium (Ca and zinc (Zn in aerosols collected at Tsukuba in Japan. Size-fractionated aerosol samples were collected for this purpose using an impactor aerosol sampler. It was shown that 10–60% and 20–100% of the total Ca and Zn in the finer particles (<2.1 μm were present as Ca and Zn oxalate complexes, respectively. Oxalic acid is hygroscopic and can thus increase the CCN activity of aerosol particles, while complexes with various polyvalent metal ions such as Ca and Zn are not hygroscopic, which cannot contribute to the increase of the CCN activity of aerosols. Based on the concentrations of noncomplexed and metal-complexed oxalate species, we found that most of the oxalic acid is present as metal oxalate complexes in the aerosols, suggesting that oxalic acid does not always increase the hygroscopicity of aerosols in the atmosphere. Similar results are expected for other dicarboxylic acids, such as malonic and succinic acids. Thus, it is advisable that the cooling effect of organic aerosols should be estimated by including the

20. Measurements of Primary Biogenic Aerosol Particles with an Ultraviolet Aerodynamic Particle Sizer (UVAPS) During AMAZE-08

Science.gov (United States)

Wollny, A. G.; Garland, R.; Pöschl, U.

2008-12-01

Biogenic aerosols are ubiquitous in the Earth's atmosphere and they influence atmospheric chemistry and physics, the biosphere, climate, and public health. They play an important role in the spread of biological organisms and reproductive materials, and they can cause or enhance human, animal, and plant diseases. Moreover, they influence the Earth's energy budget by scattering and absorbing radiation, and they can initiate the formation of clouds and precipitation as cloud condensation and ice nuclei. The composition, abundance, and origin of biogenic aerosol particles and components are, however, still not well understood and poorly quantified. Prominent examples of primary biogenic aerosol particles, which are directly emitted from the biosphere to the atmosphere, are pollen, bacteria, fungal spores, viruses, and fragments of animals and plants. During the AMazonian Aerosol CharacteriZation Experiment (AMAZE-08) a large number of aerosol and gas-phase measurements were taken on a remote site close to Manaus, Brazil, during a period of five weeks in February and March 2008. The presented study is focused on data from an ultraviolet aerodynamic particle sizer (UVAPS, TSI inc.) that has been deployed for the first time in Amazonia. In this instrument, particle counting and aerodynamic sizing over the range of 0.5-20 μm are complemented by the measurement of UV fluorescence at 355 nm (excitation) and 420-575 nm (emission), respectively. Fluorescence at these wavelengths is characteristic for reduced pyridine nucleotides (e.g., NAD(P)H) and for riboflavin, which are specific for living cells. Thus particles exhibiting fluorescence signals can be regarded as 'viable aerosols' or 'fluorescent bioparticles' (FBAP), and their concentration can be considered as lower limit for the actual abundance of primary biogenic aerosol particles. First data analyses show a pronounced peak of FBAP at diameters around 2-3 μm. In this size range the biogenic particle fraction was

1. Size measurement of radioactive aerosol particles in intense radiation fields using wire screens and imaging plates

Energy Technology Data Exchange (ETDEWEB)

Oki, Yuichi; Tanaka, Toru; Takamiya, Koichi; Ishi, Yoshihiro; UesugI, Tomonori; Kuriyama, Yasutoshi; Sakamoto, Masaaki; Ohtsuki, Tsutomu [Kyoto University Research Reactor Institute, Osaka (Japan); Nitta, Shinnosuke [Graduate School of Engineering, Kyoto University, Kyoto (Japan); Osada, Naoyuki [Advanced Science Research Center, Okayama University, Okayama (Japan)

2016-09-15

2. Do anthropogenic or coastal aerosol sources impact on a clean marine aerosol signature at Mace Head?

Directory of Open Access Journals (Sweden)

C. O'Dowd

2013-03-01

Full Text Available Atmospheric aerosols have been sampled and characterised at the Mace Head North East (N.E. Atlantic atmospheric research station since 1958, with many interesting phenomena being discovered. However, with the range of new discoveries and scientific advances, there has been a range of concomitant criticisms challenging the representativeness of aerosol sampled at the station to that of aerosol over the open ocean. Two recurring criticisms relate to the lack of representativeness due to enhanced coastal sources, thereby leading to artificially high values to aerosol parameters, and to the influence of long-range transport of anthropogenic aerosol and its potential dominance over, or drowning-out of, a natural marine aerosol signal. Here we review the results of previous experimental studies into marine aerosols over the N.E. Atlantic and at Mace Head with the aim of evaluating their representativeness relative to that of an open ocean aerosol with negligible anthropogenic influence. Particular focus is given to organic matter (OM aerosol. In summary, no correlation was found between OM and black carbon (BC either at BC levels of 0–15 or 15–50 ng m−3, suggesting that OM concentrations up to peak values of 3.8 μg m−3 are predominantly natural in origin. Sophisticated carbon isotope analysis and aerosol mass spectral finger printing corroborate the natural source of OM with 80% biogenic source apportionment being observed for general clean air conditions, rising to 98% during specific primary marine organic plumes when peak concentrations >3 μg m−3 are observed. A range of other experiments are discussed which corroborate the dominance of a marine signal under Mace Head clean air criteria along. Further, analysis of a series of experiments conducted at Mace Head conclude that negligible coastal, surf zone, or tidal effects are discernible in the submicron size range for sampling heights of 7 m and above. The Mace Head clean air criteria

3. Measurement of aerosol-particle trajectories using a structured laser beam.

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Herzog, William D; Tysk, Shane M; Tardiff, David W; Cappiello, Gregory G; Jong, Jason M; Jeys, Thomas H; Hoffeld, Ronald H; Sanchez, Antonio; Daneu, Vincenzo

2007-06-01

What is believed to be a new concept for the measurement of micrometer-sized particle trajectories in an inlet air stream is introduced. The technique uses a light source and a mask to generate a spatial pattern of light within a volume in space. Particles traverse the illumination volume and elastically scatter light to a photodetector where the signal is recorded in time. The detected scattering waveform is decoded to find the particle trajectory. A design is presented for the structured laser beam, and the accuracy of the technique in determining particle position is demonstrated. It is also demonstrated that the structured laser beam can be used to measure and then correct for the spatially dependent instrument-response function of an optical-scattering-based particle-sizing system for aerosols.

4. Quantification and radiocarbon source apportionment of black carbon in atmospheric aerosols using the CTO-375 method

Science.gov (United States)

Zencak, Zdenek; Elmquist, Marie; Gustafsson, Örjan

To make progress towards linking the atmosphere and biogeosphere parts of the black carbon (BC) cycle, a chemothermal oxidation method (CTO-375), commonly applied for isolating BC from complex geomatrices such as soils, sediments and aquatic particles, was applied to investigate the BC also in atmospheric particles. Concentrations and 14C-based source apportionment of CTO-375 based BC was established for a reference aerosol (NIST RM-8785) and for wintertime aerosols collected in Stockholm and in a Swedish background area. The results were compared with thermal-optical (OC/EC) measurements. For NIST RM-8785, a good agreement was found between the BC CTO-375 concentration and the reported elemental carbon (EC) concentration measured by the "Speciation Trends Network—National Institute of Occupational Safety and Health" method (EC NIOSH) with BC CTO-375 of 0.054±0.002 g g -1 and EC NIOSH of 0.067±0.008 g g -1. In contrast, there was an average factor of ca. 20 difference between BC CTO-375 and EC NIOSH for the ambient Scandinavian wintertime aerosols, presumably reflecting a combination of BC CTO-375 isolating only the recalcitrant soot-BC portion of the BC continuum and the EC NIOSH metric inadvertently including some intrinsically non-pyrogenic organic matter. Isolation of BC CTO-375 with subsequent off-line radiocarbon analysis yielded fraction modern values (fM) for total organic carbon (TOC) of 0.93 (aerosols from a Swedish background area), and 0.58 (aerosols collected in Stockholm); whereas the fM for BC CTO-375 isolates were 1.08 (aerosols from a Swedish background area), and 0.87 (aerosols collected in Stockholm). This radiocarbon-based source apportionment suggests that contribution from biomass combustion to cold-season atmospheric BC CTO-375 in Stockholm was 70% and in the background area 88%.

5. Primary and secondary aerosols in Beijing in winter: sources, variations and processes

Science.gov (United States)

Sun, Yele; Du, Wei; Fu, Pingqing; Wang, Qingqing; Li, Jie; Ge, Xinlei; Zhang, Qi; Zhu, Chunmao; Ren, Lujie; Xu, Weiqi; Zhao, Jian; Han, Tingting; Worsnop, Douglas R.; Wang, Zifa

2016-07-01

Winter has the worst air pollution of the year in the megacity of Beijing. Despite extensive winter studies in recent years, our knowledge of the sources, formation mechanisms and evolution of aerosol particles is not complete. Here we have a comprehensive characterization of the sources, variations and processes of submicron aerosols that were measured by an Aerodyne high-resolution aerosol mass spectrometer from 17 December 2013 to 17 January 2014 along with offline filter analysis by gas chromatography/mass spectrometry. Our results suggest that submicron aerosols composition was generally similar across the winter of different years and was mainly composed of organics (60 %), sulfate (15 %) and nitrate (11 %). Positive matrix factorization of high- and unit-mass resolution spectra identified four primary organic aerosol (POA) factors from traffic, cooking, biomass burning (BBOA) and coal combustion (CCOA) emissions as well as two secondary OA (SOA) factors. POA dominated OA, on average accounting for 56 %, with CCOA being the largest contributor (20 %). Both CCOA and BBOA showed distinct polycyclic aromatic hydrocarbons (PAHs) spectral signatures, indicating that PAHs in winter were mainly from coal combustion (66 %) and biomass burning emissions (18 %). BBOA was highly correlated with levoglucosan, a tracer compound for biomass burning (r2 = 0.93), and made a considerable contribution to OA in winter (9 %). An aqueous-phase-processed SOA (aq-OOA) that was strongly correlated with particle liquid water content, sulfate and S-containing ions (e.g. CH2SO2+) was identified. On average aq-OOA contributed 12 % to the total OA and played a dominant role in increasing oxidation degrees of OA at high RH levels (> 50 %). Our results illustrate that aqueous-phase processing can enhance SOA production and oxidation states of OA as well in winter. Further episode analyses highlighted the significant impacts of meteorological parameters on aerosol composition, size

6. Potential sea salt aerosol sources from frost flowers in the pan-Arctic region

Energy Technology Data Exchange (ETDEWEB)

Xu, Li [Scripps Institution of Oceanography, University of California, San Diego, La Jolla California USA; Now at Department of Earth System Science, University of California, Irvine California USA; Russell, Lynn M. [Scripps Institution of Oceanography, University of California, San Diego, La Jolla California USA; Burrows, Susannah M. [Atmospheric Science and Global Change Division, Pacific Northwest National Laboratory, Richland Washington USA

2016-09-23

In order to better represent observed wintertime aerosol concentrations at Barrow, Alaska, we implemented an observationally-based parameterization for estimating sea salt production from frost flowers in the Community Earth System Model (CESM). In this work, we evaluate the potential influence of this sea salt source on the pan-Arctic (60ºN-90ºN) climate. Results show that frost flower salt emissions substantially increase the modeled surface sea salt aerosol concentration in the winter months when new sea ice and frost flowers are present. The parameterization reproduces both the magnitude and seasonal variation of the observed submicron sea salt aerosol concentration at surface in Barrow during winter much better than the standard CESM simulation without a frost-flower salt particle source. Adding these frost flower salt particle emissions increases aerosol optical depth by 10% and results in a small cooling at surface. The increase in salt particle mass concentrations of a factor of 8 provides nearly two times the cloud condensation nuclei concentration, as well as 10% increases in cloud droplet number and 40% increases in liquid water content near coastal regions adjacent to continents. These cloud changes reduce longwave cloud forcing by 3% and cause a small surface warming, increasing the downward longwave flux at the surface by 2 W m-2 in the pan-Arctic under the present-day climate.

7. A role of aerosol particles in forming urban skyglow and skyglow from distant cities

Science.gov (United States)

2016-05-01

Aerosol particles may represent the largest uncertainty about skyglow change in many locations under clear-sky conditions. This is because aerosols are ubiquitous in the atmosphere and influence the ground-reaching radiation in different ways depending on their concentrations, origins, shapes, sizes, and compositions. Large particles tend to scatter in Fraunhofer diffraction regime, while small particles can be treated in terms of Rayleigh formalism. However, the role of particle microphysics in forming the skyglow still remains poorly quantified. We have shown in this paper that the chemistry is somehow important for backscattering from large particles that otherwise work as efficient attenuators of light pollution if composed of absorbing materials. The contribution of large particles to the urban skyglow diminishes as they become more spherical in shape. The intensity of backscattering from non-absorbing particles is more-or-less linearly decreasing function of particle radius even if number size distribution is inversely proportional to the fourth power of particle radius. This is due to single particle backscattering that generally increases steeply as the particle radius approaches large values. Forward scattering depends on the particle shape but is independent of the material composition, thus allowing for a simplistic analytical model of skyglow from distant cities. The model we have developed is based on mean value theorem for integrals and incorporates the parametrizable Garstang's emission pattern, intensity decay along optical beam path, and near-forward scattering in an atmospheric environment. Such model can be used by modellers and experimentalists for rapid estimation of skyglow from distant light sources.

8. Possible effect of extreme solar energetic particle events of September–October 1989 on polar stratospheric aerosols: a case study

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I. A. Mironova

2013-09-01

Full Text Available The main ionization source of the middle and low Earth's atmosphere is related to energetic particles coming from outer space. Usually it is ionization from cosmic rays that is always present in the atmosphere. But in a case of a very strong solar eruption, some solar energetic particles (SEPs can reach middle/low atmosphere increasing the ionization rate up to some orders of magnitude at polar latitudes. We continue investigating such a special class of solar events and their possible applications for natural variations of the aerosol content. After the case study of the extreme SEP event of January 2005 and its possible effect upon polar stratospheric aerosols, here we analyze atmospheric applications of the sequence of several events that took place over autumn 1989. Using aerosol data obtained over polar regions from two satellites with space-borne optical instruments SAGE II and SAM II that were operating during September–October 1989, we found that an extreme major SEP event might have led to formation of new particles and/or growth of preexisting ultrafine particles in the polar stratospheric region. However, the effect of the additional ambient air ionization on the aerosol formation is minor, in comparison with temperature effect, and can take place only in the cold polar atmospheric conditions. The extra aerosol mass formed under the temperature effect allows attributing most of the changes to the "ion–aerosol clear sky mechanism".

9. Real time analysis of lead-containing atmospheric particles in Beijing during springtime by single particle aerosol mass spectrometry.

Science.gov (United States)

Ma, Li; Li, Mei; Huang, Zhengxu; Li, Lei; Gao, Wei; Nian, Huiqing; Zou, Lilin; Fu, Zhong; Gao, Jian; Chai, Fahe; Zhou, Zhen

2016-07-01

Using a single particle aerosol mass spectrometer (SPAMS), the chemical composition and size distributions of lead (Pb)-containing particles with diameter from 0.1 μm to 2.0 μm in Beijing were analyzed in the spring of 2011 during clear, hazy, and dusty days. Based on mass spectral features of particles, cluster analysis was applied to Pb-containing particles, and six major classes were acquired consisting of K-rich, carboneous, Fe-rich, dust, Pb-rich, and Cl-rich particles. Pb-containing particles accounted for 4.2-5.3%, 21.8-22.7%, and 3.2% of total particle number during clear, hazy and dusty days, respectively. K-rich particles are a major contribution to Pb-containing particles, varying from 30.8% to 82.1% of total number of Pb-containing particles, lowest during dusty days and highest during hazy days. The results reflect that the chemical composition and amount of Pb-containing particles has been affected by meteorological conditions as well as the emissions of natural and anthropogenic sources. K-rich particles and carbonaceous particles could be mainly assigned to the emissions of coal combustion. Other classes of Pb-containing particles may be associated with metallurgical processes, coal combustion, dust, and waste incineration etc. In addition, Pb-containing particles during dusty days were first time studied by SPAMS. This method could provide a powerful tool for monitoring and controlling of Pb pollution in real time.

10. Use of stable carbon and nitrogen isotope ratios in size segregated aerosol particles for the O/I penetration evaluation

Science.gov (United States)

Garbaras, Andrius; Garbariene, Inga; Masalaite, Agne; Ceburnis, Darius; Krugly, Edvinas; Kvietkus, Kestutis; Remeikis, Vidmantas; Martuzevicius, Dainius

2015-04-01

Stable carbon and nitrogen isotope ratio are successfully used in the atmospheric aerosol particle source identification [1, 2], transformation, pollution [3] research. The main purpose of this study was to evaluate the penetration of atmospheric aerosol particles from outdoor to indoor using stable carbon and nitrogen isotope ratios. Six houses in Kaunas (Lithuania) were investigated during February and March 2013. Electrical low pressure impactor was used to measure in real time concentration and size distribution of outdoor aerosol particles. ELPI+ includes 15 channels covering the size range from 0.017 to 10.0 µm. The 25 mm diameter aluminium foils were used to collect aerosol particles. Gravimetric analysis of samples was made using microbalance. In parallel, indoor aerosol samples were collected with a micro-orifice uniform deposition impactor (MOUDI model 110), where the aerosol particles were separated with the nominal D50 cut-off sizes of 0.056, 0.1, 0.18,0.32,0.56, 1.0, 1.8, 3.2, 5.6, 10, 18 μm for impactor stages 1-11, respectively. The impactor was run at a flow rate of 30 L/min. Air quality meters were used to record meteorological conditions (temperature, relative humidity) during the investigated period. All aerosol samples were analyzed for total carbon (TC) and total nitrogen (TN) contents and their isotopic compositions using elemental analyzer (EA) connected to the stable isotope ratio mass spectrometer (IRMS). TC concentration in indoors ranged from 1.5 to 247.5 µg/m3. During the sampling period outdoors TN levels ranged from 0.1 to 10.9 µg/m3. The obtained outdoor δ13C(PM2.5) values varied from -24.21 to -26.3‰, while the δ15N values varied from 2.4 to 11.1 ‰ (average 7.2±2.5 ‰). Indoors carbonaceous aerosol particles were depleted in 13C compared to outdoors in all sampling sites. This depletion in δ13C varied from 0.1 to 3.2 ‰. We think that this depletion occurs due ongoing chemical reactions (oxidation) when aerosol

11. Modelled radiative effects of sea spray aerosol using a source function encapsulating wave state

Science.gov (United States)

Partanen, Antti-Ilari; Dunne, Eimear M.; Bergman, Tommi; Laakso, Anton; Kokkola, Harri; Ovadnevaite, Jurgita; Sogacheva, Larisa; Baisnée, Dominique; Sciare, Jean; Manders, Astrid; O'Dowd, Colin; de Leeuw, Gerrit; Korhonen, Hannele

2014-05-01

Sea spray aerosol particles have significant effects on global climate by scattering solar radiation (direct effect) and modifying cloud properties (indirect effect). Sea spray consists mainly of sea salt, but in biologically active regions, major fraction of sea spray may come in the form of primary marine organic matter (PMOM). Traditionally, sea spray flux has been parameterized in global models in terms of wind speed, and organic fraction of sea spray in terms of chlorophyll-a concentration. In this study, we have incorporated recently developed parameterizations for the sea spray aerosol source flux into the global aerosol-climate model ECHAM-HAMMOZ. The parameterizations encapsulate the wave state via Reynolds number, and predict the organic fraction of the sea spray aerosol source flux. The model was then used to investigate the direct and indirect effects of sea spray aerosol particles. We compared simulated sea spray concentrations with in-situ measurements from Mace Head (North Atlantic), Point Reyes (North Pacific), and Amsterdam Island (Southern Indian Ocean). Aerosol optical depth (AOD) was compared with satellite measurements from PARASOL. Modelled annual mean global emissions of sea salt and PMOM were 805 Tg yr-1 (uncertainty range of 378-1233 Tg yr-1) and 1.1 Tg yr-1 (0.5-1.8 Tg yr-1), respectively. Sea salt emissions were considerably lower than the majority of previous estimates, but PMOM was in the range of previous studies. The model captured sea salt concentrations fairly well in the smaller size ranges at Mace Head (annual normalized mean bias of -13% for particles with vacuum aerodynamic diameter Dva

12. Aerosol Particles From Tropical Cirrus Clouds in the Lower Stratosphere

Science.gov (United States)

Kojima, T.; Buseck, P. R.; Wilson, J. C.; Reeves, J. M.

2002-12-01

Aerosol samples were collected from convective systems and cirrus layers over Florida during the July 2002 CRYSTAL-FACE Mission. Particles between 0.02 and 700 \\micron were deposited directly onto TEM grids. Here we report preliminary results of the TEM study of particles collected near and above the tropopause. Most particles are sulfate droplets that range from 0.8 to 5 \\micron in diameter on the TEM grids. All have a characteristic appearance that consists of a main central particle (0.3 -1 \\micron) surrounded by many smaller satellite droplets. Their appearance suggests that the droplets were sulfuric acid partially neutralized with ammonium at the time of collection, with ammonium sulfate and bisulfate constituting the central particles (Bigg, 1975, 1980). The degree of ammoniation in individual droplets, which is indicated by the size of central particles relative to satellite ring diameter, is fairly uniform. The ratio of central particle diameter to satellite ring diameter is generally around 0.3. Such ammoniated droplets with solid cores may be more efficient in nucleating cirrus than pure sulfuric acid droplets (Tabazadeh and Toon, 1998). Ammonium sulfate particles without satellites commonly coexist with the acid droplets. Minor particles consist of C-rich amorphous material, silicates, Na- and K-chlorides and sulfates, and Cr- and Ti-oxides. Some were coated with sulfate. Many of the C-rich particles contain significant amount of K, S, and O with lesser N. All silicate particles are flakes of clay minerals that have pseudohexagonal structures. They would work as effective ice nuclei (Pruppacher and Klett, 1997).

13. Impacts of aerosol particles on the microphysical and radiative properties of stratocumulus clouds over the Southeast Pacific ocean

Directory of Open Access Journals (Sweden)

C. H. Twohy

2012-08-01

Full Text Available The Southeast Pacific Ocean is covered by the world's largest stratocumulus cloud layer, which has a strong impact on ocean temperatures and climate in the region. The effect of anthropogenic sources of aerosol particles such as power plants, urban pollution and smelters on the stratocumulus deck was investigated during the VOCALS field experiment. Aerosol measurements below and above cloud were made with a ultra-high sensitivity aerosol spectrometer and analytical electron microscopy. In addition to more standard in-cloud measurements, droplets were collected and evaporated using a counterflow virtual impactor (CVI, and the non-volatile residual particles were analyzed.

Many flights focused on the gradient in cloud properties on an E-W track along 20° S from near the Chilean coast to remote areas offshore. Mean statistics from seven flights and many individual legs were compiled. Consistent with a continental source of cloud condensation nuclei, below-cloud accumulation-mode aerosol and droplet number concentration generally decreased from near shore to offshore. Single particle analysis was used to reveal types and sources of the enhanced particle number. While a variety of particle types were found throughout the region, the dominant particles near shore were partially neutralized sulfates. Modeling and chemical analysis indicated that the predominant source of these particles in the marine boundary layer along 20° S was anthropogenic pollution from central Chilean sources, with copper smelters a relatively small contribution.

Cloud droplets were more numerous and smaller near shore, and there was less drizzle. Higher droplet number concentration and physically thinner clouds both contributed to the smaller droplets near shore. Satellite measurements were used to show that cloud albedo was highest 500–1000 km offshore, and actually lower closer to shore due to the generally thinner clouds and lower liquid water paths

14. Physical and chemical properties of pollution aerosol particles transported from North America to Greenland as measured during the POLARCAT summer campaign

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B. Quennehen

2011-04-01

Full Text Available Within the framework of the POLARCAT-France campaign, aerosol physical, chemical and optical properties over Greenland were measured onboard the French ATR-42 research aircraft. The Lagrangian particle dispersion model FLEXPART was used to determine air mass origins. The study focuses particularly on the characterization of air masses transported from the North American continent. Air masses that picked up emissions from Canadian and Alaskan boreal forest fires as well as from the cities on the American east coast were identified and selected for a detailed study. Measurements of CO concentrations, aerosol chemical composition, aerosol size distributions, aerosol volatile fractions and aerosol light absorption (mainly from black carbon are used in order to study the relationship between CO enhancement, ageing of the air masses, aerosol particle concentrations and size distributions. Aerosol size distributions are in good agreement with previous studies, even though, wet scavenging potentially occurred along the pathway between the emission sources and Greenland leading to lower concentrations in the aerosol accumulation mode. The measured aerosol size distributions show a significant enhancement of Aitken mode particles. It is demonstrated that the Aitken mode is largely composed of black carbon, while the accumulation mode is more dominated by organics, as deduced from aerosol mass spectrometric AMS and aerosol volatility measurements. Overall, during the campaign rather small amounts of black carbon from the North American continent were transported towards Greenland. An important finding given the potential climate impacts of black carbon in the Arctic.

15. Urban increments of gaseous and aerosol pollutants and their sources using mobile aerosol mass spectrometry measurements

Science.gov (United States)

Elser, Miriam; Bozzetti, Carlo; El-Haddad, Imad; Maasikmets, Marek; Teinemaa, Erik; Richter, Rene; Wolf, Robert; Slowik, Jay G.; Baltensperger, Urs; Prévôt, André S. H.

2016-06-01

Air pollution is one of the main environmental concerns in urban areas, where anthropogenic emissions strongly affect air quality. This work presents the first spatially resolved detailed characterization of PM2.5 (particulate matter with aerodynamic equivalent diameter daero ≤ 2.5 µm) in two major Estonian cities, Tallinn and Tartu. The measurements were performed in March 2014 using a mobile platform. In both cities, the non-refractory (NR)-PM2.5 was characterized by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) using a recently developed lens which increases the transmission of super-micron particles. Equivalent black carbon (eBC) and several trace gases including carbon monoxide (CO), carbon dioxide (CO2), and methane (CH4) were also measured. The chemical composition of PM2.5 was found to be very similar in the two cities. Organic aerosol (OA) constituted the largest fraction, explaining on average about 52 to 60 % of the PM2.5 mass. Four sources of OA were identified using positive matrix factorization (PMF): hydrocarbon-like OA (HOA, from traffic emissions), biomass burning OA (BBOA, from biomass combustion), residential influenced OA (RIOA, probably mostly from cooking processes with possible contributions from waste and coal burning), and oxygenated OA (OOA, related to secondary aerosol formation). OOA was the major OA source during nighttime, explaining on average half of the OA mass, while during daytime mobile measurements the OA was affected by point sources and dominated by the primary fraction. A strong increase in the secondary organic and inorganic components was observed during periods with transport of air masses from northern Germany, while the primary local emissions accumulated during periods with temperature inversions. Mobile measurements offered the identification of different source regions within the urban areas and the assessment of the extent to which pollutants concentrations exceeded regional background

16. AERONET-based models of smoke-dominated aerosol near source regions and transported over oceans, and implications for satellite retrievals of aerosol optical depth

Science.gov (United States)

Sayer, A. M.; Hsu, N. C.; Eck, T. F.; Smirnov, A.; Holben, B. N.

2014-10-01

Smoke aerosols from biomass burning are an important component of the global aerosol system. Analysis of Aerosol Robotic Network (AERONET) retrievals of aerosol microphysical/optical parameters at 10 sites reveals variety between biomass burning aerosols in different global source regions, in terms of aerosol particle size and single scatter albedo (SSA). Case studies of smoke observed at coastal/island AERONET sites also mostly lie within the range of variability at the near-source sites. Differences between sites tend to be larger than variability at an individual site, although optical properties for some sites in different regions can be quite similar. Across the sites, typical midvisible SSA ranges from ~ 0.95-0.97 (sites dominated by boreal forest or peat burning, typically with larger fine-mode particle radius and spread) to ~ 0.88-0.9 (sites most influenced by grass, shrub, or crop burning, typically smaller fine-mode particle radius and spread). The tropical forest site Alta Floresta (Brazil) is closer to this second category, although with intermediate SSA ~ 0.92. The strongest absorption is seen in southern African savannah at Mongu (Zambia), with average midvisible SSA ~ 0.85. Sites with stronger absorption also tend to have stronger spectral gradients in SSA, becoming more absorbing at longer wavelengths. Microphysical/optical models are presented in detail so as to facilitate their use in radiative transfer calculations, including extension to UV (ultraviolet) wavelengths, and lidar ratios. One intended application is to serve as candidate optical models for use in satellite aerosol optical depth (AOD) retrieval algorithms. The models presently adopted by these algorithms over ocean often have insufficient absorption (i.e. too high SSA) to represent these biomass burning aerosols. The underestimates in satellite-retrieved AOD in smoke outflow regions, which have important consequences for applications of these satellite data sets, are consistent with

17. Source apportionment of carbonaceous aerosol in southern Sweden

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J. Genberg

2011-05-01

Full Text Available A one-year study was performed at the Vavihill background station in southern Sweden to estimate the anthropogenic contribution to the carbonaceous aerosol. Weekly samples of the particulate matter PM10 were collected on quartz filters, and the amounts of organic carbon, elemental carbon, radiocarbon (14C and levoglucosan were measured. This approach enabled source apportionment of the total carbon in the PM10 fraction using the concentration ratios of the sources. The sources considered in this study were emissions from the combustion of fossil fuels and biomass, as well as biogenic sources. During the summer, the carbonaceous aerosol mass was dominated by compounds of biogenic origin (82 %, which are associated with biogenic primary and secondary organic aerosols. During the winter months, biomass combustion (38 % and fossil fuel combustion (33 % were the main contributors to the carbonaceous aerosol. Elemental carbon concentrations in winter were about twice as large as during summer, and can be attributed to biomass combustion, probably from domestic wood burning. The contribution of fossil fuels to elemental carbon was stable throughout the year, although the fossil contribution to organic carbon increased during the winter. Thus, the organic aerosol originated mainly from natural sources during the summer and from anthropogenic sources during the winter. The result of this source apportionment was compared with results from the EMEP model. The model and measurements were generally consistent for total atmospheric organic carbon, however, the contribution of the sources varied substantially. E.g. the biomass burning contributions of OC were underestimated by the model by a factor of 8.2 compared to the measurements.

18. Comparison of the DiSCmini aerosol monitor to a handheld condensation particle counter and a scanning mobility particle sizer for submicrometer sodium chloride and metal aerosols.

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Mills, Jessica B; Park, Jae Hong; Peters, Thomas M

2013-01-01

We evaluated the robust, lightweight DiSCmini (DM) aerosol monitor for its ability to measure the concentration and mean diameter of submicrometer aerosols. Tests were conducted with monodispersed and polydispersed aerosols composed of two particle types (sodium chloride [NaCl] and spark-generated metal particles, which simulate particles found in welding fume) at three different steady-state concentration ranges (Low, 10(4) particles/cm(3)). Particle number concentration, lung deposited surface area (LDSA) concentration, and mean size measured with the DM were compared with those measured with reference instruments, a scanning mobility particle sizer (SMPS), and a handheld condensation particle counter (CPC). Particle number concentrations measured with the DM were within 16% of those measured by the CPC for polydispersed aerosols. Poorer agreement was observed for monodispersed aerosols (±35% for most tests and +101% for 300-nm NaCl). LDSA concentrations measured by the DM were 96% to 155% of those estimated with the SMPS. The geometric mean diameters measured with the DM were within 30% of those measured with the SMPS for monodispersed aerosols and within 25% for polydispersed aerosols (except for the case when the aerosol contained a substantial number of particles larger than 300 nm). The accuracy of the DM is reasonable for particles smaller than 300 nm, but caution should be exercised when particles larger than 300 nm are present. [Supplementary materials are available for this article. Go to the publisher's online edition of the Journal of Occupational and Environmental Hygiene for the following free supplemental resources: manufacturer-reported capabilities of instruments used, and information from the SMPS measurements for polydispersed test particles.].

19. Possible effect of extreme solar energetic particle event of 20 January 2005 on polar stratospheric aerosols: direct observational evidence

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I. A. Mironova

2012-01-01

Full Text Available Energetic cosmic rays are the main source of ionization of the low-middle atmosphere, leading to associated changes in atmospheric properties. Via the hypothetical influence of ionization on aerosol growth and facilitated formation of clouds, this may be an important indirect link relating solar variability to climate. This effect is highly debated, however, since the proposed theoretical mechanisms still remain illusive and qualitative, and observational evidence is inconclusive and controversial. Therefore, important questions regarding the existence and magnitude of the effect, and particularly the fraction of aerosol particles that can form and grow, are still open. Here we present empirical evidence of the possible effect caused by cosmic rays upon polar stratospheric aerosols, based on a case study of an extreme solar energetic particle (SEP event of 20 January 2005. Using aerosol data obtained over polar regions from different satellites with optical instruments that were operating during January 2005, such as the Stratospheric Aerosol and Gas Experiment III (SAGE III, and Optical Spectrograph and Infrared Imaging System (OSIRIS, we found a significant simultaneous change in aerosol properties in both the Southern and Northern Polar regions in temporal association with the SEP event. We speculate that ionization of the atmosphere, which was abnormally high in the lower stratosphere during the extreme SEP event, might have led to formation of new particles and/or growth of preexisting ultrafine particles in the polar stratospheric region. However, a detailed interpretation of the effect is left for subsequent studies. This is the first time high vertical resolution measurements have been used to discuss possible production of stratospheric aerosols under the influence of cosmic ray induced ionization. The observed effect is marginally detectable for the analyzed severe SEP event and can be undetectable for the majority of weak

20. Morphology and Optical Properties of Mixed Aerosol Particles

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Fard, Mehrnoush M.; Krieger, Ulrich; Rudich, Yinon; Marcolli, Claudia; Peter, Thomas

2016-04-01

Experiments and modeling studies have shown that deliquesced aerosols can exist not only as one-phase system containing organics, inorganic salts and water, but often as two-phase systems consisting of a predominantly organic and a predominantly inorganic aqueous phase (1,2). Recent laboratory studies conducted with model mixtures representing tropospheric aerosols (1,2,3), secondary organic aerosol (SOA) from smog chamber experiments (4), and field measurements (5) suggest that liquid-liquid phase separations (LLPS) is indeed a common phenomenon in mixed organic/ inorganic particles. During LLPS, particles may adopt different morphologies mainly core-shell and partially engulfed. A core-shell configuration will have consequences for heterogeneous chemistry and hygroscopicity and as a result will alter the optical properties of the particles in particular for organic phases containing absorbing molecules, e.g. brown carbon. The primary objective of this project is to establish a method for investigating the morphology of mixed inorganic and absorbing organic compounds of atmospheric relevance and study their radiative properties before, during, and after phase transitions mainly during LLPS. This will be the first study looking into the radiative effect of LLPS in detail. Our ternary model system consist of ammonium sulfate (AS)/ Polyethylene Glycol (PEG)/ and water (H2O). Carminic acid (CA) was added as a proxy for an absorbing organic compound to the system. The behavior of single droplets of above ternary mixture was monitored during relative humidity (RH) cycles using optical microscopy. The same ternary mixture particle was levitated in an electrodynamic balance (EDB) and the change in its absorption properties was measured at varying RH. In addition, Mie-code modeling is used to predict the absorption efficiency of the same ternary system and the result will be compared with the data obtained from EDB experiment. We also intend to determine the occurrence of

1. Aerosol composition, chemistry, and source characterization during the 2008 VOCALS Experiment

Energy Technology Data Exchange (ETDEWEB)

Lee, Y.; Springston, S.; Jayne, J.; Wang, J.; Senum, G.; Hubbe, J.; Alexander, L.; Brioude, J.; Spak, S.; Mena-Carrasco, M.; Kleinman, L.; Daum, P.

2010-03-15

Chemical composition of fine aerosol particles over the northern Chilean coastal waters was determined onboard the U.S. DOE G-1 aircraft during the VOCALS (VAMOS Ocean-Cloud-Atmosphere-Land Study) field campaign between October 16 and November 15, 2008. SO42-, NO3-, NH4+, and total organics (Org) were determined using an Aerodyne Aerosol Mass Spectrometer, and SO42-, NO3-, NH4+, Na+, Cl-, CH3SO3-, Mg2+, Ca2+, and K+ were determined using a particle-into-liquid sampler-ion chromatography technique. The results show the marine boundary layer (MBL) aerosol mass was dominated by non- sea-salt SO42- followed by Na+, Cl-, Org, NO3-, and NH4+, in decreasing importance; CH3SO3-, Ca2+, and K+ rarely exceeded their respective limits of detection. The SO42- aerosols were strongly acidic as the equivalent NH4+ to SO42- ratio was only {approx}0.25 on average. NaCl particles, presumably of sea-salt origin, showed chloride deficits but retained Cl- typically more than half the equivalency of Na+, and are externally mixed with the acidic sulfate aerosols. Nitrate was observed only on sea-salt particles, consistent with adsorption of HNO3 on sea-salt aerosols, responsible for the Cl- deficit. Dust particles appeared to play a minor role, judging from the small volume differences between that derived from the observed mass concentrations and that calculated based on particle size distributions. Because SO42- concentrations were substantial ({approx}0.5 - {approx}3 {micro}g/m3) with a strong gradient (highest near the shore), and the ocean-emitted dimethylsulfide and its unique oxidation product, CH3SO3-, were very low (i.e., {le} 40 parts per trillion and <0.05 {micro}g/m3, respectively), the observed SO42- aerosols are believed to be primarily of terrestrial origin. Back trajectory calculations indicate sulfur emissions from smelters and power plants along coastal regions of Peru and Chile are the main sources of these SO4- aerosols. However, compared to observations, model

2. Development of Laser-Based Handheld Aerosol Particle Counter

Institute of Scientific and Technical Information of China (English)

CHEN Chang; LI Hui

2005-01-01

The JC-CA300 handheld Aerosol particle counter is designed and developed based on light scattering principle. The JC-CA300 counter is composed of optical sensor, DSP component and microprocessor unit. The hardware architecture is designed in compact style by SMT IC chips. The whole counter weight is less than 2 pounds. With 32K RAM space, the JC-CA300 can store 500 sampling records and support standard printer and communicate with a computer through RS232 interface. Based on experimental results, the main performance of JC-CA300 is better than that of the ARTI'S HHPC-6 instrument.

3. Source appointment of fine particle number and volume concentration during severe haze pollution in Beijing in January 2013.

Science.gov (United States)

Liu, Zirui; Wang, Yuesi; Hu, Bo; Ji, Dongsheng; Zhang, Junke; Wu, Fangkun; Wan, Xin; Wang, Yonghong

2016-04-01

Extreme haze episodes repeatedly shrouded Beijing during the winter of 2012-2013, causing major environmental and health problems. To better understand these extreme events, particle number size distribution (PNSD) and particle chemical composition (PCC) data collected in an intensive winter campaign in an urban site of Beijing were used to investigate the sources of ambient fine particles. Positive matrix factorization (PMF) analysis resolved a total of eight factors: two traffic factors, combustion factors, secondary aerosol, two accumulation mode aerosol factors, road dust, and long-range transported (LRT) dust. Traffic emissions (54%) and combustion aerosol (27%) were found to be the most important sources for particle number concentration, whereas combustion aerosol (33%) and accumulation mode aerosol (37%) dominated particle volume concentrations. Chemical compositions and sources of fine particles changed dynamically in the haze episodes. An enhanced role of secondary inorganic species was observed in the formation of haze pollution. Regional transport played an important role for high particles, contribution of which was on average up to 24-49% during the haze episodes. Secondary aerosols from urban background presented the largest contributions (45%) for the rapid increase of fine particles in the severest haze episode. In addition, the invasion of LRT dust aerosols further elevated the fine particles during the extreme haze episode. Our results showed a clear impact of regional transport on the local air pollution, suggesting the importance of regional-scale emission control measures in the local air quality management of Beijing.

4. EVALUATION OF ACOUSTIC FORCES ON A PARTICLE IN AEROSOL MEDIUM

Energy Technology Data Exchange (ETDEWEB)

Lee, S; Richard Dimenna, R

2007-09-27

The acoustic force exerted on a solid particle was evaluated to develop a fundamental understanding of the critical physical parameters or constraints affecting particle motion and capture in a collecting device. The application of an acoustic force to the collection of a range of submicron-to-micron particles in a highly turbulent airflow stream laden with solid particles was evaluated in the presence of other assisting and competing forces. This scoping estimate was based on the primary acoustic force acting directly on particles in a dilute aerosol system, neglecting secondary interparticle effects such as agglomeration of the sub-micron particles. A simplified analysis assuming a stable acoustic equilibrium with an infinite sound speed in the solid shows that for a solid-laden air flow in the presence of a standing wave, particles will move toward the nearest node. The results also show that the turbulent drag force on a 1-{micro}m particle resulting from eddy motion is dominant when compared with the electrostatic force or the ultrasonic acoustic force. At least 180 dB acoustic pressure level at 1 MHz is required for the acoustic force to be comparable to the electrostatic or turbulent drag forces in a high-speed air stream. It is noted that particle size and pressure amplitude are dominant parameters for the acoustic force. When acoustic pressure level becomes very large, the acoustic energy will heat up the surrounding air medium, which may cause air to expand. With an acoustic power of about 600 watts applied to a 2000-lpm air flow, the air temperature can increase by as much as 15 C at the exit of the collector.

5. Ice nucleating particles at a coastal marine boundary layer site: correlations with aerosol type and meteorological conditions

Science.gov (United States)

Mason, R. H.; Si, M.; Li, J.; Chou, C.; Dickie, R.; Toom-Sauntry, D.; Pöhlker, C.; Yakobi-Hancock, J. D.; Ladino, L. A.; Jones, K.; Leaitch, W. R.; Schiller, C. L.; Abbatt, J. P. D.; Huffman, J. A.; Bertram, A. K.

2015-11-01

Information on what aerosol particle types are the major sources of ice nucleating particles (INPs) in the atmosphere is needed for climate predictions. To determine which aerosol particles are the major sources of immersion-mode INPs at a coastal site in Western Canada, we investigated correlations between INP number concentrations and both concentrations of different atmospheric particles and meteorological conditions. We show that INP number concentrations are strongly correlated with the number concentrations of fluorescent bioparticles between -15 and -25 °C, and that the size distribution of INPs is most consistent with the size distribution of fluorescent bioparticles. We conclude that biological particles were likely the major source of ice nuclei at freezing temperatures between -15 and -25 °C at this site for the time period studied. At -30 °C, INP number concentrations are also well correlated with number concentrations of the total aerosol particles ≥ 0.5 μm, suggesting that non-biological particles may have an important contribution to the population of INPs active at this temperature. As we found that black carbon particles were unlikely to be a major source of ice nuclei during this study, these non-biological INPs may include mineral dust. Furthermore, correlations involving chemical tracers of marine aerosols and marine biological activity, sodium and methanesulfonic acid, indicate that the majority of INPs measured at the coastal site likely originated from terrestrial rather than marine sources. Finally, six existing empirical parameterizations of ice nucleation were tested to determine if they accurately predict the measured INP number concentrations. We found that none of the parameterizations selected are capable of predicting INP number concentrations with high accuracy over the entire temperature range investigated. This finding illustrates that additional measurements are needed to improve parameterizations of INPs and their

6. Characterization of aerosol particle episodes in Finland caused by wildfires in Eastern Europe

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J. V. Niemi

2005-01-01

Full Text Available We studied the sources, compositions and size distributions of aerosol particles during long-range transport (LRT PM2.5 episodes which occurred on 12–15 August, 26–28 August and 5–6 September 2002 in Finland. Backward air mass trajectories, satellite detections of fire areas and dispersion modelling results indicate that emissions from wildfires in Russia and other Eastern European countries arrived in Finland during these episodes. Elemental analyses using scanning electron microscopy (SEM coupled with energy dispersive X-ray microanalyses (EDX showed that the proportions of S-rich particles and agglomerates (agglomeration was caused partly by the sampling method used increased during the episodes, and they contained elevated fractions of K, indicating emissions from biomass burning. These aerosols were mixed with S-rich emissions from fossil fuel burning during transport since air masses came through polluted areas of Europe. Minor amounts of coarse Ca-rich particles were also brought by LRT during the episodes, and they probably originated from wildfires and/or from Estonian and Russian oil-shale-burning industrial areas. Ion chromatography analysis showed that concentrations of sulphate (SO42-, total nitrate (NO3-+HNO3(g and total ammonium (NH4++NH3(g increased during the episodes, but the ratio of the total amount of these ions to PM10 concentration decreased, indicating unusually high fractions of other chemical components. Particle number size distribution measurements with differential mobility particle sizer (DMPS revealed that concentrations of particles 90–500 nm increased during the episodes, while concentrations of particles smaller than 90 nm decreased. The reduction of the smallest particles was caused by suppressed new particle formation due to vapour and molecular cluster uptake of LRT particles. Our results show that emissions from wildfires in Russian and other Eastern European countries deteriorated air quality of

7. Characteristics of trace metals in marine aerosols and their source identiifcation over the Southern Ocean

Institute of Scientific and Technical Information of China (English)

ZHAO Shuhui; CHEN Liqi; LIN Hongmei

2015-01-01

Atmospheric trace metals (Cu, Zn, Cd, Pb, Fe, V, and Cr), As, Al and Na in marine aerosols were studied over the Southern Ocean during the 28th Chinese National Antarctic Research Expedition. Fe was the most abundant of the analyzed trace metals, with an average concentration of 28.824 ng∙m-3. V and Zn concentrations were also high, and their average concentrations were 5.541 ng∙m-3 and 2.584 ng∙m-3, respectively. Although sea spray significantly influenced the marine aerosol particles measured (Na had the highest concentrations of the analyzed elements, with an average concentration of 2.65 μg∙m-3), multivariate analyses (enrichment factor and principal components analysis) indicated that most of the elements were not associated with oceanic sources. Over the Southern Ocean, Fe, Cd, As, Al and Cr in the aerosols mainly originated from crustal sources, while Cu, Pb, V and Zn originated from crustal sources and anthropogenic emissions. The enrichment factors (EFcrust) for most elements (Fe, Al, As, Cr, Cd, Cu and V) were much lower in the northern latitudes, indicating that when the sampling occurred closer to land the concentrations of these elements in aerosols were strongly affected by terrestrial crustal sources.

8. Technical Note: In-situ quantification of aerosol sources and sinks over regional geographical scales

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G. Buzorius

2009-01-01

Full Text Available In order to obtain the source/sink functions for atmospheric particulates located on the planetary surface or elevated in the atmosphere; direct aerosol emission measurements are required. For this purpose, the performance of an airborne aerosol flux measurement system with an improved 3-km spatial resolution is evaluated in this study. Eddy covariance method was used in flux calculations. A footprint for airborne flux sampling with the increased resolution becomes comparable in area to the footprint for tower sampling (with the footprint length being 2 to 10 km. The improvement in spatial resolution allows quantification of emission rates from individual sources located several kilometers apart. Locally measured aerosol flux provides useful information about aerosol sources and sinks located below or aloft of measurement altitude. The advantage is a moving platform that allows scanning of aerosol emissions or depositions over practically unlimited geographic scales. The technique delivers effective emission rates of atmospheric particulates from specific sources such as highway segments, city blocks, and remote and industrial areas. The improved spatial resolution airborne flux measurements were conducted in ambient conditions with low (<500 m mixed boundary layer heights. Measurement results are reported from clean and partly polluted marine environments, and heavily polluted continental environments. The upward and downward fluxes from the clean marine environment were smaller than 0.5×106 particles m−2 s−1 in absolute value. The effective emissions measured from a ship plume ranged from 2×108 to 3×108 m−2 s−1, and effective fluxes measured crossing cities plumes with populations of 10 000 to 12 000 inhabitants were in the range of 2×108 to 3×108 m−2 s−1. Correlations between heat and aerosol fluxes are

9. Aerosol source apportionment from 1-year measurements at the CESAR tower in Cabauw, the Netherlands

Science.gov (United States)

Schlag, Patrick; Kiendler-Scharr, Astrid; Blom, Marcus Johannes; Canonaco, Francesco; Sebastiaan Henzing, Jeroen; Moerman, Marcel; Prévôt, André Stephan Henry; Holzinger, Rupert

2016-07-01

Intensive measurements of submicron aerosol particles and their chemical composition were performed with an Aerosol Chemical Speciation Monitor (ACSM) at the Cabauw Experimental Site for Atmospheric Research (CESAR) in Cabauw, the Netherlands, sampling at 5 m height above ground. The campaign lasted nearly 1 year from July 2012 to June 2013 as part of the EU-FP7-ACTRIS project (Q-ACSM Network). Including equivalent black carbon an average particulate mass concentration of 9.50 µg m-3 was obtained during the whole campaign with dominant contributions from ammonium nitrate (45 %), organic aerosol (OA, 29 %), and ammonium sulfate (19 %). There were 12 exceedances of the World Health Organization (WHO) PM2.5 daily mean limit (25 µg m-3) observed at this rural site using PM1 instrumentation only. Ammonium nitrate and OA represented the largest contributors to total particulate matter during periods of exceedance. Source apportionment of OA was performed season-wise by positive matrix factorization (PMF) using the multilinear engine 2 (ME-2) controlled via the source finder (SoFi). Primary organic aerosols were attributed mainly to traffic (8-16 % contribution to total OA, averaged season-wise) and biomass burning (0-23 %). Secondary organic aerosols (SOAs, 61-84 %) dominated the organic fraction during the whole campaign, particularly on days with high mass loadings. A SOA factor which is attributed to humic-like substances (HULIS) was identified as a highly oxidized background aerosol in Cabauw. This shows the importance of atmospheric aging processes for aerosol concentration at this rural site. Due to the large secondary fraction, the reduction of particulate mass at this rural site is challenging on a local scale.

10. Formation of Secondary Particulate Matter by Reactions of Gas Phase Hexanal with Sulfate Aerosol Particles

Science.gov (United States)

Zhang, J.

2003-12-01

The formation of secondary particulate matter from the atmospheric oxidation of organic compounds can significantly contribute to the particulate burden, but the formation of organic secondary particulate matter is poorly understood. One way of producing organic secondary particulate matter is the oxidation of hydrocarbons with seven or more carbon atoms to get products with low vapor pressure. However, several recent reports suggest that relatively low molecular weight carbonyls can enter the particle phase by undergoing heterogeneous reactions. This may be a very important mechanism for the formation of organic secondary particulate matter. Atmospheric aldehydes are important carbonyls in the gas phase, which form via the oxidation of hydrocarbons emitted from anthropogenic and biogenic sources. In this poster, we report the results on particle growth by the heterogeneous reactions of hexanal. A 5 L Continuous Stirred Tank Reactor (CSTR) is set up to conduct the reactions in the presence of seed aerosol particles of deliquesced ammonia bisulfate. Hexanal is added into CSTR by syringe pump, meanwhile the concentrations of hexanal are monitored with High Pressure Liquid Chromatograph (HPLC 1050). A differential Mobility Analyzer (TSI 3071) set to an appropriate voltage is employed to obtain monodisperse aerosols, and another DMA associated with a Condensation Nuclear Counter (TSI 7610) is used to measure the secondary particle size distribution by the reaction in CSTR. This permits the sensitive determination of particle growth due to the heterogeneous reaction, very little growth occurs when hexanal added alone. Results for the simultaneous addition of hexanal and alcohols will also be presented.

11. Functional group composition of ambient and source organic aerosols determined by tandem mass spectrometry

Energy Technology Data Exchange (ETDEWEB)

Dron, J.; El Haddad, I.; Temime-Roussel, B.; Wortham, H.; Marchand, N. [Univ Aix Marseille, CNRS, Lab Chim Provence, Equipe Instrumentat and React Atmospher, UMR 6264, F-13331 Marseille 3 (France); Jaffrezo, J.L. [Univ Grenoble 1, CNRS, UMR 5183, Lab Glaciol and Geophys Environm, F-38402 St Martin Dheres (France)

2010-07-01

The functional group composition of various organic aerosols (OA) is investigated using a recently developed analytical approach based on atmospheric pressure chemical ionisation-tandem mass spectrometry (APCIMS/MS). The determinations of three functional groups contents are performed quantitatively by neutral loss (carboxylic and carbonyl groups, R-COOH and R-CO-R' respectively) and precursor ion (nitro groups, R-NO{sub 2}) scanning modes of a tandem mass spectrometer. Major organic aerosol sources are studied: vehicular emission and wood combustion for primary aerosol sources; and a secondary organic aerosol (SOA) produced through photooxidation of o-xylene. The results reveal significant differences in the functional group contents of these source aerosols. The laboratory generated SOA is dominated by carbonyls while carboxylics are preponderate in the wood combustion particles. On the other hand, vehicular emissions are characterised by a strong nitro content. The total amount of the three functional groups accounts for 1.7% (vehicular) to 13.5% (o-xylene photooxidation) of the organic carbon. Diagnostic functional group ratios are then used to tentatively discriminate sources of particles collected in an urban background environment located in an Alpine valley (Chamonix, France) during a strong winter pollution event. The three functional groups under study account for a total functionalization rate of 2.2 to 3.8% of the organic carbon in this ambient aerosol, which is also dominated by carboxylic moieties. In this particular case study of a deep alpine valley during winter, we show that the nitro- and carbonyl-to-carboxylic diagnostic ratios can be a useful tool to discriminate sources. In these conditions, the total OA concentrations are highly dominated by wood combustion OA. This result is confirmed by an organic markers source apportionment approach which assess a wood burning organic carbon contribution of about 60%. Finally, examples of functional

12. Functional group composition of ambient and source organic aerosols determined by tandem mass spectrometry

Directory of Open Access Journals (Sweden)

J. Dron

2010-08-01

Full Text Available The functional group composition of various organic aerosols (OA is investigated using a recently developed analytical approach based on atmospheric pressure chemical ionisation-tandem mass spectrometry (APCI-MS/MS. The determinations of three functional groups contents are performed quantitatively by neutral loss (carboxylic and carbonyl groups, R-COOH and R-CO-R´ respectively and precursor ion (nitro groups, R-NO2 scanning modes of a tandem mass spectrometer. Major organic aerosol sources are studied: vehicular emission and wood combustion for primary aerosol sources; and a secondary organic aerosol (SOA produced through photooxidation of o-xylene. The results reveal significant differences in the functional group contents of these source aerosols. The laboratory generated SOA is dominated by carbonyls while carboxylics are preponderate in the wood combustion particles. On the other hand, vehicular emissions are characterised by a strong nitro content. The total amount of the three functional groups accounts for 1.7% (vehicular to 13.5% (o-xylene photooxidation of the organic carbon. Diagnostic functional group ratios are then used to tentatively discriminate sources of particles collected in an urban background environment located in an Alpine valley (Chamonix, France during a strong winter pollution event. The three functional groups under study account for a total functionalisation rate of 2.2 to 3.8% of the organic carbon in this ambient aerosol, which is also dominated by carboxylic moieties. In this particular case study of a deep alpine valley during winter, we show that the nitro- and carbonyl-to-carboxylic diagnostic ratios can be a useful tool to discriminate sources. In these conditions, the total OA concentrations are highly dominated by wood combustion OA. This result is confirmed by an organic markers source apportionment approach which assess a wood burning organic carbon contribution of about 60

13. Deliquescence and Efflorescence Processes of Aerosol Particles Studied by in situ FTIR and Raman Spectroscopy

Institute of Scientific and Technical Information of China (English)

Li-jun Zhao; Feng Wang; Kun Zhang; Qing-xuan Zeng; Yun-hong Zhang

2008-01-01

Deliquescence and efflorescence are the two most important physicochemical processes of aerosol particles.In deliquescence and efflorescence cycles of aerosol particles,many fundamental problems need to be investigated in detail on the molecular level,including ion and molecule interactions in supersaturated aerosols,metastable solid phases that may be formed,and microscopic structures and deliquescence mechanisms of aerosol particles.This paper presents a summary of the progress made in recent investigations of deliquescence and efflorescence processes of aerosol particles by four common spectral techniques,which are known as Raman/electrodynamic balance,Fourier transform infrared/aerosol flow tube,Fourier transform infrared/attenuated total reflection,and confocal Raman on a quartz substrate.

14. Concentrations, size distributions and temporal variations of fluorescent biological aerosol particles in southern tropical India

Science.gov (United States)

Valsan, Aswathy; Krishna R, Ravi; CV, Biju; Huffman, Alex; Poschl, Ulrich; Gunthe, Sachin

2015-04-01

Biological aerosols constitute a wide range of dead and alive biological materials and structures that are suspended in the atmosphere. They play an important role in the atmospheric physical, chemical and biological processes and health of living being by spread of diseases among humans, plants, and, animals. The atmospheric abundance, sources, physical properties of PBAPs as compared to non-biological aerosols, however, is poorly characterized. The Indian tropical region, where large fraction of the world's total population is residing, experiences a distinctive meteorological phenomenon by means of Indian Summer Monsoon (IMS). Thus, the properties and characteristics of biological aerosols are also expected to be very diverse over the Indian subcontinent depending upon the seasons. Here we characterize the number concentration and size distribution of Fluorescent Biological Aerosol Particles (FBAP) at a high altitude continental site, Munnar (10.09 N, 77.06 E; 1605 m asl) in South India during the South-West monsoon, which constitute around 80 percent of the annual rainfall in Munnar. Continuous three months measurements (from 01 June 2014 to 21 Aug 2104) FBAPs were carried out at Munnar using Ultra Violet Aerodynamic Particle Sizer (UVAPS) during IMS. The mean number and mass concentration of coarse FBAP averaged over the entire campaign was 1.7 x 10-2 cm-3 and 0.24 µg m-3 respectively, which corresponds to 2 percent and 6 percent of total aerosol particle number and mass concentration. In agreement to other previous measurements the number size distribution of FBAP also peaks at 3.2 micron indicating the strong presence of fungal spores. This was also supported by the Scanning Electron Microscopic analysis of bioaerosols on filter paper. They also displayed a strong diurnal cycle with maximum concentration occurring at early morning hours. During periods of heavy and continuous rain where the wind is consistently blowing from South-West direction it was

15. Investigate the relationship between multiwavelength lidar ratios and aerosol size distributions using aerodynamic particle sizer spectrometer

Science.gov (United States)

Zhao, Hu; Hua, Dengxin; Mao, Jiandong; Zhou, Chunyan

2017-02-01

The real aerosol size distributions were obtained by aerodynamic particle sizer spectrometer (APS) in China YinChuan. The lidar ratios at wavelengths of 355 nm, 532 nm and 1064 nm were calculated using Mie theory. The effective radius of aerosol particles reff and volume C/F ratio (coarse/fine) Vc/f were retrieved from the real aerosol size distributions. The relationship between multiwavelength lidar ratios and particle reff and Vc/f were investigated. The results indicate that the lidar ratio is positive correlated to the particle reff and Vc/f. The lidar ratio is more sensitive to the coarse particles. The short wavelength lidar ratio is more sensitive to the particle Vc/f and the long wavelength lidar ratio is more sensitive to the particle reff. The wavelength dependency indicated that the lidar ratios decrease with increasing the wavelength. The lidar ratios are almost irrelevant to the shape and total particles of aerosol size distributions.

16. Characterization of Atmospheric Aerosol Particles from a Mining City in Southwest China Using Electron Probe microanalysis

Science.gov (United States)

Cheng, X.; Huang, Y.; Lu, H., III; Liu, Z., IV; Wang, N. V.

2015-12-01

Xin Cheng1, Yi Huang1*, Huilin Lu2, Zaidong Liu2, Ningming Wang21 Key Laboratory of Geological Nuclear Technology of Sichuan Province, College of Earth Science, Chengdu University of Technology, Chengdu 610059, China. ; E-mail:chengxin_cdut@163.com 2 College of Earth Science, Chengdu University of Technology, Chengdu 610059, China. ; *Corresponding author: E-mail: huangyi@cdut.cn Panzhihua is a mining city located at Pan-Xi Rift valley, southwest China. It has a long industrial history of vanadium-titanium magnetite mining, iron and steel smelting, and coal-fired power plants. Atomospheric environment has been seriously contaminated with airborne paticles, which is threatening human health.The harmful effects of aerosols are dependent on certain characteristics such as microphysical properties. However, few studsies have been carried out on morphological information contained on single atmospheric particles in this area. In this study, we provide a detailed morphologically and chemically characterization of airborne particles collected at Panzhihua city in October, 2014, using a quantitative single particle analysis based on EPXMA. The results indicate that based on their chemical composition, five major types of particles were identified. Among these, aluminosilicate particles have typical spherical shapes and are produced during the high-temperature combustion; Fe-containing particles contains high level of Mn, and more likely originated from mineralogical and steel industry; Si-containing particles can originate from mineralogical source; V-Ti-Mn-containing particles are also produced by steel industry; Ca-containing particles,these particles are CaCO3, mainly from the mining of limestone mine. The results help us on tracing and partitioning different sources of atomospheric particles in the industrial area. Fig.1 Fe-rich shperical particles

17. Airborne measurements of aerosol optical properties related to early spring transport of mid-latitude sources into the Arctic

Directory of Open Access Journals (Sweden)

2009-12-01

Full Text Available Airborne lidar and in-situ measurements of the aerosol properties were conducted between Svalbard Island and Scandinavia in April 2008. Evidence of aerosol transport from Europe and Asia is given. The analysis of the aerosol optical properties based on a multiwavelength lidar (355, 532, 1064 nm including depolarization at 355 nm aims at distinguishing the role of the different aerosol sources (Siberian wild fires, Eastern Asia and European anthropogenic emissions. Combining, first aircraft measurements, second FLEXPART simulations with a calculation of the PBL air fraction originating from the three different mid-latitude source regions, and third level-2 CALIPSO data products (i.e. backscatter coefficient, depolarisation and color ratio in aerosol layers along the transport pathways, appears a valuable approach to identify the role of the different aerosol sources even after a transport time larger than 4 days. Above Asia, CALIPSO data indicate more depolarisation (up to 15% and largest color ratio (>0.5 for the northeastern Asia emissions (i.e. an expected mixture of Asian pollution and dust, while low depolarisation together with smaller and quasi constant color ratio (≈0.3 are observed for the Siberian biomass burning emissions. A similar difference is visible between two layers observed by the aircraft above Scandinavia. The analysis of the time evolution of the aerosol optical properties revealed by CALIPSO between Asia and Scandinavia shows a gradual decrease of the aerosol backscatter, depolarisation ratio and color ratio which suggests the removal of the largest particles in the accumulation mode. A similar study conducted for a European plume has shown aerosol optical properties intermediate between the two Asian sources with color ratio never exceeding 0.4 and moderate depolarisation ratio being always less than 8%, i.e. less aerosol from the accumulation mode.

18. Review: engineering particles using the aerosol-through-plasma method

Energy Technology Data Exchange (ETDEWEB)

Phillips, Jonathan [Los Alamos National Laboratory; Luhrs, Claudia C [UNM; Richard, Monique [TEMA

2009-01-01

For decades, plasma processing of materials on the nanoscale has been an underlying enabling technology for many 'planar' technologies, particularly virtually every aspect of modern electronics from integrated-circuit fabrication with nanoscale elements to the newest generation of photovoltaics. However, it is only recent developments that suggest that plasma processing can be used to make 'particulate' structures of value in fields, including catalysis, drug delivery, imaging, higher energy density batteries, and other forms of energy storage. In this paper, the development of the science and technology of one class of plasma production of particulates, namely, aerosol-through-plasma (A-T-P), is reviewed. Various plasma systems, particularly RF and microwave, have been used to create nanoparticles of metals and ceramics, as well as supported metal catalysts. Gradually, the complexity of the nanoparticles, and concomitantly their potential value, has increased. First, unique two-layer particles were generated. These were postprocessed to create unique three-layer nanoscale particles. Also, the technique has been successfully employed to make other high-value materials, including carbon nanotubes, unsupported graphene, and spherical boron nitride. Some interesting plasma science has also emerged from efforts to characterize and map aerosol-containing plasmas. For example, it is clear that even a very low concentration of particles dramatically changes plasma characteristics. Some have also argued that the local-thermodynamic-equilibrium approach is inappropriate to these systems. Instead, it has been suggested that charged- and neutral-species models must be independently developed and allowed to 'interact' only in generation terms.

19. Dissolution process of atmospheric aerosol particles into cloud droplets; Processus de dissolution des aerosols atmospheriques au sein des gouttes d'eau nuageuses

Energy Technology Data Exchange (ETDEWEB)

Desboeufs, K.

2001-01-15

Clouds affect both climate via the role they play in the Earth's radiation balance and tropospheric chemistry since they are efficient reaction media for chemical transformation of soluble species. Cloud droplets are formed in the atmosphere by condensation of water vapour onto aerosol particles, the cloud condensation nuclei (CCN). The water soluble fraction of these CCN governs the cloud micro-physics, which is the paramount factor playing on the radiative properties of clouds. Moreover, this soluble fraction is the source of species imply in the oxidation/reduction reactions in the aqueous phase. Thus, it is of particular importance to understand the process controlling the solubilization of aerosols in the cloud droplets. The main purpose of this work is to investigate experimentally and theoretically the dissolution of particles incorporated in the aqueous phase. From the studies conducted up to now, we have identify several factors playing on the dissolution reaction of aerosols. However, the quantification of the effects of these factors is difficult since the current means of study are not adapted to the complexity of cloud systems. First, this work consisted to perform a experimental system, compound by an open flow reactor, enabling to follow the kinetic of dissolution in conditions representative of cloud. This experimental device is used to a systematic characterisation of the known factors playing on the dissolution, i.e. pH, aerosol nature, aerosol weathering... and also for the identification and the quantification of the effects of other factors: ionic strength, acid nature, clouds processes. These experiments gave quantitative results, which are used to elaborate a simple model of aerosol dissolution in the aqueous phase. This model considers the main factors playing on the dissolution and results in a general mechanism of aerosol dissolution extrapolated to the cloud droplets. (author)

20. Ozone oxidation of sulfur in sea-salt aerosol particles during the Azores Marine Aerosol and Gas Exchange experiment

Science.gov (United States)

Sievering, H.; Gorman, E.; Ley, T.; Pszenny, A.; Springer-Young, M.; Boatman, J.; Kim, Y.; Nagamoto, C.; Wellman, D.

1995-11-01

Sea-salt aerosol particles in the lowest tens of meters above the ocean are, typically, more than three-fourths water on a volume basis. Calculations herein indicate that aqueous-phase conversion of sulfur dioxide dissolved in the water associated with sea-salt particles (sea-salt aerosol water) supported the production of 2-8 nmol m-3 of nonsea-salt sulfate (nssSO4=) during the Marine Aerosol and Gas Exchange (MAGE) experiment intensives. This production is based on ozone oxidation of dissolved SO2 in sea-salt aerosol water and accounts for sulfur gas and ozone mass transfer limitations as a function of sea-salt particle size. Measurements showed that 1-15 nmol m-3 of nssSO4= was actually present in the sea-salt particle mode except for four enhanced concentration cases due to continental sulfur input. The range in predicted, as well as observed, nssSO4= was primarily due to variability in sea-salt aerosol water volume. The nssSO4= produced by ozone oxidation of sulfur dioxide, being in the sea-salt particle mode with observed volume geometric median diameter of 3.5-5 μm, is dry deposited at a fairly rapid rate. The remainder, being large-particle cloud condensation nuclei, may contribute little to cloud albedo over the global oceans. The two papers following this one, Kim et al. (this issue) on aerosol size distribution and water content and Parfai et al. (this issue) on compositional variations of sea-salt-mode aerosol particles observed by electron microscopy, complement and support results presented here. All three present results of the MAGE experiment and precede a forthcoming special issue of the Journal of Geophysical Research-Atmospheres on MAGE (B. Huebert, guest editor).

1. New aerosol particles formation in the Sao Paulo Metropolitan Area

Science.gov (United States)

Vela, Angel; Andrade, Maria de Fatima; Ynoue, Rita

2016-04-01

The Sao Paulo Metropolitan Area (SPMA), in the southeast region of Brazil, is considered a megalopolis comprised of Sao Paulo city and more 38 municipalities. The air pollutant emissions in the SPMA are related to the burning of the fuels: etanol, gasohol (gasoline with 25% ethanol) and diesel. According to CETESB (2013), the road vehicles contributed up to about 97, 87, and 80% of CO, VOCs and NOx emissions in 2012, respectively, being most of NOx associated to diesel combustion and most of CO and VOCs from gasohol and ethanol combustion. Studies conducted on ambient air pollution in the SPMA have shown that black carbon (BC) explains 21% of mass concentration of PM2.5 compared with 40% of organic carbon (OC), 20% of sulfates, and 12% of soil dust (Andrade et al., 2012). Most of the observed ambient PM2.5 mass concentration usually originates from precursors gases such as sulphur dioxide (SO2), ammonia (NH3), nitrogen oxides (NOx) and VOCs as well as through the physico-chemical processes such as the oxidation of low volatile hydrocarbons transferring to the condensed phase (McMurry et al., 2004). The Weather Research and Forecasting with Chemistry model (WRF-Chem; Grell et al. 2005), configured with three nested grid cells: 75, 15, and 3 km, is used as photochemical modeling to describe the physico-chemical processes leading to evolution of particles number and mass size distribution from a vehicular emission model developed by the IAG-USP laboratory of Atmospheric Processes and based on statistical information of vehicular activity. The spatial and temporal distributions of emissions in the finest grid cell are based on road density products compiled by the OpenStreetMap project and measurements performed inside tunnels in the SPMA, respectively. WRF-Chem simulation with coupled primary aerosol (dust and sea-salt) and biogenic emission modules and aerosol radiative effects turned on is conducted as the baseline simulation (Case_0) to evaluate the model

2. Deposition flux of aerosol particles and 15 polycyclic aromatic hydrocarbons in the North China Plain.

Science.gov (United States)

Wang, Xilong; Liu, Shuzhen; Zhao, Jingyu; Zuo, Qian; Liu, Wenxin; Li, Bengang; Tao, Shu

2014-04-01

The present study examined deposition fluxes of aerosol particles and 15 polycyclic aromatic hydrocarbons (PAHs) associated with the particles in the North China Plain. The annual mean deposition fluxes of aerosol particles and 15 PAHs were 0.69 ± 0.46 g/(m(2) ×d) and 8.5 ± 6.2 μg/(m(2) ×d), respectively. Phenanthrene, fluoranthene, pyrene, chrysene, benzo[b]fluoranthene, and benzo[k]fluoranthene were the dominant PAHs bound to deposited aerosol particles throughout the year. The total concentration of 15 PAHs in the deposited aerosol particles was the highest in winter but lowest in spring. The highest PAH concentration in the deposited aerosol particles in winter was because the heating processes highly increased the concentration in atmospheric aerosol particles. Low temperature and weak sunshine in winter reduced the degradation rate of deposited aerosol particle-bound PAHs, especially for those with low molecular weight. The lowest PAH concentration in deposited aerosol particles in spring resulted from the frequently occurring dust storms, which diluted PAH concentrations. The mean deposition flux of PAHs with aerosol particles in winter (16 μg/[m(2) ×d]) reached 3 times to 5 times that in other seasons (3.5-5.0 μg/[m(2) ×d]). The spatial variation of the deposition flux of PAHs with high molecular weight (e.g., benzo[a]pyrene) was consistent with their concentrations in the atmospheric aerosol particles, whereas such a phenomenon was not observed for those with low molecular weight (e.g., phenanthrene) because of their distinct hydrophobicity, Henry's law constant, and the spatially heterogeneous meteorological conditions.

3. Sources for charged particles; Les sources de particules chargees

Energy Technology Data Exchange (ETDEWEB)

Arianer, J.

1997-09-01

This document is a basic course on charged particle sources for post-graduate students and thematic schools on large facilities and accelerator physics. A simple but precise description of the creation and the emission of charged particles is presented. This course relies on every year upgraded reference documents. Following relevant topics are considered: electronic emission processes, technological and practical considerations on electron guns, positron sources, production of neutral atoms, ionization, plasma and discharge, different types of positive and negative ion sources, polarized particle sources, materials for the construction of ion sources, low energy beam production and transport. (N.T.).

4. Determination of aerosol extinction coefficient and mass extinction efficiency by DOAS with a flashlight source

Institute of Scientific and Technical Information of China (English)

Si Fu-Qi; Liu Jian-Guo; Xie Pin-Hua; Zhang Yu-Jun; Liu Wen-Qing; Hiroaki Kuze; Liu Cheng; Nofel Lagrosas; Nobuo Takeuchi

2005-01-01

With the method of differential optical absorption spectroscopy (DOAS), average concentrations of aerosol particles along light path were measured with a flashlight source in Chiba area during the period of one month. The optical thickness at 550 nm is compared with the concentration of ground-measured suspended particulate matter (SPM). Good correlations are found between the DOAS and SPM data, leading to the determination of the aerosol mass extinction efficiency (MEE) to be possible in the lower troposphere. The average MEE value is about 7.6m2.g-1, and the parameter exhibits a good correlation with the particle size as determined from the wavelength dependence of the DOAS signal intensity.

5. Heterogeneous OH oxidation of palmitic acid in single component and internally mixed aerosol particles: vaporization and the role of particle phase

Directory of Open Access Journals (Sweden)

C. B. Stipe

2008-09-01

Full Text Available We studied the OH oxidation of submicron aerosol particles consisting of pure palmitic acid (PA or thin (near monolayer coatings of PA on aqueous and effloresced inorganic salt particles. Experiments were performed as a function of particle size and OH exposure using a continuous-flow photochemical reaction chamber coupled to a chemical ionization mass spectrometer (CIMS system, for detection of gas and particle-bound organics, and a DMA/CPC for monitoring particle size distributions. The loss rate of PA observed for pure PA aerosols and PA on crystalline NaCl aerosols indicates that the OH oxidation of PA at the gas-aerosol interface is efficient. The pure PA oxidation data are well represented by a model consisting of four main processes: 1 surface-only reactions between OH and palmitic acid, 2 secondary reactions between palmitic acid and OH oxidation products, 3 volatilization of condensed-phase mass, and 4 a surface renewal process. Using this model we infer a value of γOH between 0.8 and 1. The oxidation of palmitic acid in thin film coatings of salt particles is also efficient, though the inferred γOH is lower, ranging from ~0.3+0.1/−0.05 for coatings on solid NaCl and ~0.05 (±0.01 on aqueous NaCl particles. These results, together with simultaneous data on particle size change and volatilized oxidation products, provide support for the ideas that oxidative aging of aliphatic organic aerosol is a source of small oxidized volatile organic compounds (OVOCs, and that OH oxidation may initiate secondary condensed-phase reactions.

6. The heterogeneous OH oxidation of palmitic acid in single component and internally mixed aerosol particles: vaporization, secondary chemistry, and the role of particle phase

Directory of Open Access Journals (Sweden)

V. F. McNeill

2008-03-01

Full Text Available We studied the OH oxidation of submicron aerosol particles consisting of pure palmitic acid (PA or thin (near monolayer coatings of PA on aqueous and effloresced inorganic salt particles. Experiments were performed as a function of particle size and OH exposure using a continuous-flow photochemical reaction chamber coupled to a chemical ionization mass spectrometer (CIMS system, for detection of gas and particle-bound organics, and a DMA/CPC for monitoring particle size distributions. The loss rate of PA observed for pure PA aerosols and PA on crystalline NaCl aerosols indicates that the OH oxidation of PA at the gas-aerosol interface is efficient. The pure PA oxidation data are well represented by a model consisting of four main processes: 1 surface-only reactions between OH and palmitic acid, 2 secondary reactions between palmitic acid and OH oxidation products, 3 volatilization of condensed-phase mass, and 4 a surface renewal process. Using this model we infer a value of γOH between 0.8 and 1. The oxidation of palmitic acid in thin film coatings of salt particles is also efficient, though the inferred γOH is lower, ranging from ~0.3 (+0.1/−0.05 for coatings on solid NaCl and ~0.05 (±0.01 on aqueous NaCl particles. These results, together with simultaneous data on particle size change and volatilized oxidation products, provide support for the ideas that oxidative aging of aliphatic organic aerosol is a source of small oxidized volatile organic compounds (OVOCs, and that OH oxidation may initiate secondary condensed-phase reactions.

7. Real-time measurement of aerosol particle concentration at high temperatures; Hiukkaspitoisuuden reaaliaikainen mittaaminen korkeassa laempoetilassa

Energy Technology Data Exchange (ETDEWEB)

Keskinen, J.; Hautanen, J.; Laitinen, A. [Tampere Univ. of Technology (Finland). Physics

1997-10-01

The aim of this project is to develop a new method for continuous aerosol particle concentration measurement at elevated temperatures (up to 800-1000 deg C). The measured property of the aerosol particles is the so called Fuchs surface area. This quantity is relevant for diffusion limited mass transfer to particles. The principle of the method is as follows. First, aerosol particles are charged electrically by diffusion charging process. The charging takes place at high temperature. After the charging, aerosol is diluted and cooled. Finally, aerosol particles are collected and the total charge carried by the aerosol particles is measured. Particle collection and charge measurement take place at low temperature. Benefits of this measurement method are: particles are charged in-situ, charge of the particles is not affected by the temperature and pressure changes after sampling, particle collection and charge measurement are carried out outside the process conditions, and the measured quantity is well defined. The results of this study can be used when the formation of the fly ash particles is studied. Another field of applications is the study and the development of gasification processes. Possibly, the method can also be used for the monitoring the operation of the high temperature particle collection devices. (orig.)

8. Global combustion sources of organic aerosols: model comparison with 84 AMS factor-analysis data sets

Science.gov (United States)

Tsimpidi, Alexandra P.; Karydis, Vlassis A.; Pandis, Spyros N.; Lelieveld, Jos

2016-07-01

Emissions of organic compounds from biomass, biofuel, and fossil fuel combustion strongly influence the global atmospheric aerosol load. Some of the organics are directly released as primary organic aerosol (POA). Most are emitted in the gas phase and undergo chemical transformations (i.e., oxidation by hydroxyl radical) and form secondary organic aerosol (SOA). In this work we use the global chemistry climate model ECHAM/MESSy Atmospheric Chemistry (EMAC) with a computationally efficient module for the description of organic aerosol (OA) composition and evolution in the atmosphere (ORACLE). The tropospheric burden of open biomass and anthropogenic (fossil and biofuel) combustion particles is estimated to be 0.59 and 0.63 Tg, respectively, accounting for about 30 and 32 % of the total tropospheric OA load. About 30 % of the open biomass burning and 10 % of the anthropogenic combustion aerosols originate from direct particle emissions, whereas the rest is formed in the atmosphere. A comprehensive data set of aerosol mass spectrometer (AMS) measurements along with factor-analysis results from 84 field campaigns across the Northern Hemisphere are used to evaluate the model results. Both the AMS observations and the model results suggest that over urban areas both POA (25-40 %) and SOA (60-75 %) contribute substantially to the overall OA mass, whereas further downwind and in rural areas the POA concentrations decrease substantially and SOA dominates (80-85 %). EMAC does a reasonable job in reproducing POA and SOA levels during most of the year. However, it tends to underpredict POA and SOA concentrations during winter indicating that the model misses wintertime sources of OA (e.g., residential biofuel use) and SOA formation pathways (e.g., multiphase oxidation).

9. Interannual Variations in Aerosol Sources and Their Impact on Orographic Precipitation Over California's Central Sierra Nevada

Science.gov (United States)

Creamean, J. M.; Ault, A. P.; White, A. B.; Neiman, P. J.; Ralph, F. M.; Minnis, Patrick; Prather, K. A.

2014-01-01

Aerosols that serve as cloud condensation nuclei (CCN) and ice nuclei (IN) have the potential to profoundly influence precipitation processes. Furthermore, changes in orographic precipitation have broad implications for reservoir storage and flood risks. As part of the CalWater I field campaign (2009-2011), the impacts of aerosol sources on precipitation were investigated in the California Sierra Nevada. In 2009, the precipitation collected on the ground was influenced by both local biomass burning (up to 79% of the insoluble residues found in precipitation) and long-range transported dust and biological particles (up to 80% combined), while in 2010, by mostly local sources of biomass burning and pollution (30-79% combined), and in 2011 by mostly long-range transport from distant sources (up to 100% dust and biological). Although vast differences in the source of residues was observed from year-to-year, dust and biological residues were omnipresent (on average, 55% of the total residues combined) and were associated with storms consisting of deep convective cloud systems and larger quantities of precipitation initiated in the ice phase. Further, biological residues were dominant during storms with relatively warm cloud temperatures (up to -15 C), suggesting these particles were more efficient IN compared to mineral dust. On the other hand, lower percentages of residues from local biomass burning and pollution were observed (on average 31% and 9%, respectively), yet these residues potentially served as CCN at the base of shallow cloud systems when precipitation quantities were low. The direct connection of the source of aerosols within clouds and precipitation type and quantity can be used in models to better assess how local emissions versus long-range transported dust and biological aerosols play a role in impacting regional weather and climate, ultimately with the goal of more accurate predictive weather forecast models and water resource management.

10. Source apportionment of the summer time carbonaceous aerosol at Nordic rural background sites

Directory of Open Access Journals (Sweden)

K. E. Yttri

2011-12-01

Full Text Available In the present study, natural and anthropogenic sources of particulate organic carbon (OCp and elemental carbon (EC have been quantified based on weekly filter samples of PM10 (particles with aerodynamic diameter <10 μm collected at four Nordic rural background sites [Birkenes (Norway, Hyytiälä (Finland, Vavihill (Sweden, Lille Valby, (Denmark] during late summer (5 August–2 September 2009. Levels of source specific tracers, i.e. cellulose, levoglucosan, mannitol and the 14C/12C ratio of total carbon (TC, have been used as input for source apportionment of the carbonaceous aerosol, whereas Latin Hypercube Sampling (LHS was used to statistically treat the multitude of possible combinations resulting from this approach. The carbonaceous aerosol (here: TCp; i.e. particulate TC was totally dominated by natural sources (69–86%, with biogenic secondary organic aerosol (BSOA being the single most important source (48–57%. Interestingly, primary biological aerosol particles (PBAP were the second most important source (20–32%. The anthropogenic contribution was mainly attributed to fossil fuel sources (OCff and ECff (10–24%, whereas no more than 3–7% was explained by combustion of biomass (OCbb and ECbb in this late summer campaign i.e. emissions from residential wood burning and/or wild/agricultural fires. Fossil fuel sources totally dominated the ambient EC loading, which accounted for 4–12% of TCp, whereas <1.5% of EC was attributed to combustion of biomass. The carbonaceous aerosol source apportionment showed only minor variation between the four selected sites. However, Hyytiälä and Birkenes showed greater resemblance to each other, as did Lille Valby and Vavihill, the two latter being somewhat more influenced by anthropogenic sources. Ambient levels of organosulphates and nitrooxy-organosulphates in the Nordic rural

11. Formation of highly porous aerosol particles by atmospheric freeze-drying in ice clouds.

Science.gov (United States)

Adler, Gabriela; Koop, Thomas; Haspel, Carynelisa; Taraniuk, Ilya; Moise, Tamar; Koren, Ilan; Heiblum, Reuven H; Rudich, Yinon

2013-12-17

The cycling of atmospheric aerosols through clouds can change their chemical and physical properties and thus modify how aerosols affect cloud microphysics and, subsequently, precipitation and climate. Current knowledge about aerosol processing by clouds is rather limited to chemical reactions within water droplets in warm low-altitude clouds. However, in cold high-altitude cirrus clouds and anvils of high convective clouds in the tropics and midlatitudes, humidified aerosols freeze to form ice, which upon exposure to subsaturation conditions with respect to ice can sublimate, leaving behind residual modified aerosols. This freeze-drying process can occur in various types of clouds. Here we simulate an atmospheric freeze-drying cycle of aerosols in laboratory experiments using proxies for atmospheric aerosols. We find that aerosols that contain organic material that undergo such a process can form highly porous aerosol particles with a larger diameter and a lower density than the initial homogeneous aerosol. We attribute this morphology change to phase separation upon freezing followed by a glass transition of the organic material that can preserve a porous structure after ice sublimation. A porous structure may explain the previously observed enhancement in ice nucleation efficiency of glassy organic particles. We find that highly porous aerosol particles scatter solar light less efficiently than nonporous aerosol particles. Using a combination of satellite and radiosonde data, we show that highly porous aerosol formation can readily occur in highly convective clouds, which are widespread in the tropics and midlatitudes. These observations may have implications for subsequent cloud formation cycles and aerosol albedo near cloud edges.

12. Urban background levels of particle number concentration and sources in Vilnius, Lithuania

Science.gov (United States)

Byčenkienė, Steigvilė; Plauškaitė, Kristina; Dudoitis, Vadimas; Ulevicius, Vidmantas

2014-06-01

This study presents results of research on urban aerosol particles with a focus on the aerosol particle number concentration (PNC) and the particle size distribution. The real time measurements of aerosol PNC (> 4.5 nm) and number size distributions (9-840 nm) were performed. The seasonal variations essentially comprised the minimum monthly mean in October 2010 (3400 ± 3000 cm- 3) and the maximum in April 2011 (19,000 ± 15,000 cm- 3). The mean annual PNC was 10,000 ± 8000 cm- 3 with an average mode size of 30-50 nm. The presence of strong diurnal patterns in aerosol PNC was evident as a direct effect of three sources of aerosol particles (nucleation, traffic, and residential heating). Hybrid receptor modeling potential source contribution function (PSCF) and concentration weighted trajectory (CWT) were used by incorporating 72-h backward trajectories and measurements of PNC in Vilnius. The results of trajectory clustering and the PSCF method demonstrated that possible additional source areas contributing to the elevated particle number concentration in Vilnius could be industrial areas in central Europe. Principal component analysis (PCA) revealed highest loadings for PNC, PM10, NOx, NO, NO2 and SO2 concentrations, indicating combustion processes occurring in vehicle engines and use of sulfur-containing fossil fuels for residential heating.

13. Modeling global impacts of heterogeneous loss of HO2 on cloud droplets, ice particles and aerosols

Directory of Open Access Journals (Sweden)

V. Huijnen

2014-03-01

Full Text Available The abundance and spatial variability of the hydroperoxyl radical (HO2 in the troposphere strongly affects atmospheric composition through tropospheric ozone production and associated HOx chemistry. One of the largest uncertainties in the chemical HO2 budget is its heterogeneous loss on the surface of cloud droplets, ice particles and aerosols. We quantify the importance of the heterogeneous HO2 loss at global scale using the latest recommendations on the scavenging efficiency on various surfaces. For this we included the simultaneous loss on cloud droplets and ice particles as well as aerosol in the Composition-Integrated Forecast System (C-IFS. We show that cloud surface area density (SAD is typically an order of magnitude larger than aerosol SAD, using assimilated satellite retrievals to constrain both meteorology and global aerosol distributions. Depending on the assumed uptake coefficients, loss on liquid water droplets and ice particles accounts for ∼53–70% of the total heterogeneous loss of HO2, due to the ubiquitous presence of cloud droplets. This indicates that HO2 uptake on cloud should be included in chemistry transport models that already include uptake on aerosol. Our simulations suggest that the zonal mean mixing ratios of HO2 are reduced by ∼25% in the tropics and up to ∼50% elsewhere. The subsequent decrease in oxidative capacity leads to a global increase of the tropospheric carbon monoxide (CO burden of up to 7%, and an increase in the ozone tropospheric lifetime of ∼6%. This increase results in an improvement in the global distribution when compared against CO surface observations over the Northern Hemisphere, although it does not fully resolve the wintertime bias in the C-IFS. There is a simultaneous increase in the high bias in C-IFS for tropospheric CO over the Southern Hemisphere, which constrains on the assumptions regarding HO2 uptake on a global scale. We show that enhanced HO2 uptake on aerosol types

14. A marine biogenic source of atmospheric ice-nucleating particles

Energy Technology Data Exchange (ETDEWEB)

Wilson, T. W.; Ladino, L. A.; Alpert, Peter A.; Breckels, M. N.; Brooks, I. M.; Browse, J.; Burrows, Susannah M.; Carslaw, K. S.; Huffman, J. A.; Judd, C.; Kilthau, W. P.; Mason, R. H.; McFiggans, Gordon; Miller, L. A.; Najera, J.; Polishchuk, E. A.; Rae, S.; Schiller, C. L.; Si, M.; Vergara Temprado, J.; Whale, Thomas; Wong, J P S; Wurl, O.; Yakobi-Hancock, J. D.; Abbatt, JPD; Aller, Josephine Y.; Bertram, Allan K.; Knopf, Daniel A.; Murray, Benjamin J.

2015-09-09

The formation of ice in clouds is facilitated by the presence of airborne ice nucleating particles1,2. Sea spray is one of the major global sources of atmospheric particles, but it is unclear to what extent these particles are capable of nucleating ice3–11. Here we show that material in the sea surface microlayer, which is enriched in surface active organic material representative of that found in sub-micron sea- spray aerosol12–21, nucleates ice under conditions that occur in mixed-phase clouds and high-altitude ice clouds. The ice active material is likely biogenic and is less than ~0.2 ?m in size. We also show that organic material (exudate) released by a common marine diatom nucleates ice when separated from cells and propose that organic material associated with phytoplankton cell exudates are a candidate for the observed ice nucleating ability of the microlayer samples. By combining our measurements with global model simulations of marine organic aerosol, we show that ice nucleating particles of marine origin are dominant in remote marine environments, such as the Southern Ocean, the North Pacific and the North Atlantic.

15. Chamber bioaerosol study: human emissions of size-resolved fluorescent biological aerosol particles.

Science.gov (United States)

Bhangar, S; Adams, R I; Pasut, W; Huffman, J A; Arens, E A; Taylor, J W; Bruns, T D; Nazaroff, W W

2016-04-01

Humans are a prominent source of airborne biological particles in occupied indoor spaces, but few studies have quantified human bioaerosol emissions. The chamber investigation reported here employs a fluorescence-based technique to evaluate bioaerosols with high temporal and particle size resolution. In a 75-m(3) chamber, occupant emission rates of coarse (2.5-10 μm) fluorescent biological aerosol particles (FBAPs) under seated, simulated office-work conditions averaged 0.9 ± 0.3 million particles per person-h. Walking was associated with a 5-6× increase in the emission rate. During both walking and sitting, 60-70% or more of emissions originated from the floor. The increase in emissions during walking (vs. while sitting) was mainly attributable to release of particles from the floor; the associated increased vigor of upper body movements also contributed. Clothing, or its frictional interaction with human skin, was demonstrated to be a source of coarse particles, and especially of the highly fluorescent fraction. Emission rates of FBAPs previously reported for lecture classes were well bounded by the experimental results obtained in this chamber study. In both settings, the size distribution of occupant FBAP emissions had a dominant mode in the 3-5 μm diameter range.

16. Single Particle Characterization of Free Tropospheric Aerosols at the Pico Mountain Observatory over the North Atlantic

Science.gov (United States)

Mazzoleni, C.; China, S.; Scarnato, B. V.; Moffet, R.; OBrien, R. E.; Gilles, M. K.; Fialho, P. J.; Ampadu, M.; Kumar, S.; Dzepina, K.; Wright, K.; Sharma, N.; Zhang, B.; Owen, R. C.; Perlinger, J. A.; Jacques, H.; Helmig, D.; Dziobak, M.; Kramer, L. J.; Mazzoleni, L. R.

2014-12-01

Free tropospheric aerosols are being studied at the Pico Mountain Observatory, located near the top of the Pico volcano in the Azores, Portugal (38.47°N, 28.40°W, 2225m asl). Typically above the marine boundary layer in the summer, this is an ideal site to study aerosol transported over long distances across the Atlantic Ocean. Aerosols reaching the Observatory often originate from North America and sometimes from Africa and Europe. Aerosols instrumentation deployed at the site include: a) an optical particle counter, b) a 7-wavelength aethalometer to measure black carbon equivalent mass concentration, c) a 3-wavelength nephelometer to measure total and backward light scattering, d) four high volume samplers for aerosol chemical characterization, and e) a sequential aerosol sampler and a 4-stage impactor to collect particles on different substrates for microscopy analysis. The origin and transport pathways of the air masses sampled at the site are determined using FLEXible PARTicle (FLEXPART) dispersion modeling retroplume analysis. Single particle morphology and mixing states were determined using electron microscopy, energy dispersive X-ray spectroscopy, and scanning transmission x-ray microscopy. This study provides an overview of different types of aerosol collected at Pico Mountain Observatory. We investigated morphology and mixing of various types of particles, including dust, soot, salt and organic particles transported to the Observatory. Soot particles were often mixed/coated with other material and exhibited very compact shape. Dust particles were often mixed with sulfur containing species. We also observed dust particles that were mixed with coated soot particles. During some events, we observed soot and sulfate aerosol trapped within organic matter. The results of this study have implications on how aerosol particles and their internal mixing can be represented in numerical models for remote regions of the free troposphere.

17. Hygroscopic growth of atmospheric aerosol particles and its relation to nucleation scavenging in clouds

Energy Technology Data Exchange (ETDEWEB)

Svenningsson, B.

1997-11-01

Aerosol particles in the atmosphere are important in several aspects. Some major aerosol constituents that are deposited in ecosystems are acidic or fertilizers and some minor or trace constituents are toxic. Aerosol particles are also involved in the earths radiation balance, both directly by scattering the sunlight and indirectly by influencing the clouds. All these effects are influenced by the interaction between the aerosol particles and water vapour. A tandem differential mobility analyser (TDMA) has been designed to measure hygroscopic growth, i.e. the particle diameter change due to uptake of water at well defined relative humidities below 100%. Tests of the instrument performance have been made using aerosol particles of pure inorganic salts. Three field experiments have been performed as parts of large fog and cloud experiments. Bimodal hygroscopic growth spectra were found: less-hygroscopic particles containing a few percent and more-hygroscopic particles around 50% by volume of hygroscopically active material. In general the fraction of less-hygroscopic particles decreases with particle size and it is larger in polluted continental aerosols than in remote background aerosols. This external mixing cannot be fully understood using present views on the formation of aerosols. Evidence or the importance of the external mixing on the cloud nucleating properties of the particles are found in comparisons between hygroscopic growth spectra for the total aerosol, the interstitial aerosol in clouds, and cloud drop residuals. Cloud condensation nuclei spectra, calculated using aerosol particle size distributions and hygroscopic growth spectra, in combination with information on the major inorganic ions are presented. These CCN spectra reveal for instance that the influence of less-hygroscopic particles on the cloud droplets increases with increasing peak supersaturation. The fraction of the particles that were scavenged to cloud drops, as a function of particle

18. The characterization of atmospheric aerosols: Application to heterogeneous gas-particle reactions

Energy Technology Data Exchange (ETDEWEB)

Robinson, J.M.; Henson, B.F.; Wilson, K.R. [Los Alamos National Lab., NM (United States); Prather, K.A.; Noble, C.A. [Univ. of California, Riverside, CA (United States)

1998-12-31

This is the final report of a three-year, Laboratory Directed Research and Development (LDRD) project of the Los Alamos National Laboratory (LANL). The objective of this collaborative research project is the measurement and modeling of atmospheric aerosols and heterogeneous (gas/aerosol) chemical reactions. The two major accomplishments are single particle characterization of tropospheric particles and experimental investigation of simulated stratospheric particles and reactions thereon. Using aerosol time-of-flight mass spectrometry, real-time and composition measurements of single particles are performed on ambient aerosol samples. This technique allows particle size distributions for chemically distinct particle types to be described. The thermodynamics and chemical reactivity of polar stratospheric clouds are examined using vapor deposited thin ice films. Employing nonlinear optical methods, as well as other techniques, phase transitions on both water and acid ices are monitored as a function of temperature or the addition of gases.

19. Interaction of aerosol particles with a standing wave optical field

Science.gov (United States)

Curry, John J.

2016-09-01

Trajectories of spherical dielectric particles carried across an optical standing wave by a flowing medium are investigated. Trajectories are determined by a three-dimensional Monte Carlo calculation that includes drag forces, Brownian motion, and optical gradient forces. We analyze the case of polystyrene particles with radii of order 100 nm carried across a Gaussian-mode standing wave by slowly flowing air. Particles are injected into the flowing air from a small source area such as the end of a capillary tube. Different sizes are dispersed continuously in space on the opposite side of the standing wave, demonstrating a practical way to sort particles. Certain discrete values of particle size show no interaction with the optical field, independent of intensity. These particles can be sorted with exceptionally high resolution. For example, particles with radii of 275 nm can be sorted with 1 nm resolution. This sorting scheme has the advantages of accommodating a high throughput, producing a continuous stream of continuously dispersed particles, and exhibiting excellent size resolution. The Monte Carlo results are in agreement with those obtained by a much simpler, and faster, fluid calculation based on effective velocities and effective diffusion coefficients, both obtained by averaging trajectories over multiple fringes of the optical field.

20. Observations and Modeling of the Green Ocean Amazon 2014/15: Transmission Electron Microscopy Analysis of Aerosol Particles Field Campaign Report

Energy Technology Data Exchange (ETDEWEB)

Buseck, Peter [Arizona State Univ., Tempe, AZ (United States)

2016-03-01

During two Intensive Operational Periods (IOP), we collected samples at 3-hour intervals for transmission electron microscopy analysis. The resulting transmission electron microscopy images and compositions were analyzed for the samples of interest. Further analysis will be done especially for the plume of interest. We found solid spherical organic particles from rebounded samples collected with Professor Scot Martin’s group (Harvard University). Approximately 30% of the rebounded particles at 95% relative humidity were spherical organic particles. Their sources and formation process are not known, but such spherical particles could be solid and will have heterogeneous chemical reactions. We observed many organic particles that are internally mixed with inorganic elements such as potassium and nitrogen. They are either homogeneously mixed or have inorganic cores with organic aerosol coatings. Samples collected from the Manaus, Brazil, pollution plume included many nano-size soot particles mixed with organic material and sulfate. Aerosol particles from clean periods included organic aerosol particles, sulfate, sea salt, dust, and primary biogenic aerosol particles. There was more dust, primary biogenic aerosol, and tar balls in samples taken during IOP1 than those taken during IOP2. Many dust particles were found between March 2 and 3.

1. Single particle characterization of biomass burning organic aerosol (BBOA: evidence for non-uniform mixing of high molecular weight organics and potassium

Directory of Open Access Journals (Sweden)

A. K. Y. Lee

2015-11-01

Full Text Available Biomass burning is a major source of black carbon (BC and primary organic aerosol globally. In particular, biomass burning organic aerosol (BBOA is strongly associated with atmospheric brown carbon (BrC that absorbs near ultraviolet and visible light, resulting in significant impacts on regional visibility degradation and radiative forcing. The mixing state of BBOA can play a critical role in the prediction of aerosol optical properties. In this work, single particle measurements from a soot-particle aerosol mass spectrometer coupled with a light scattering module (LS-SP-AMS were performed to examine the mixing state of BBOA, refractory black carbon (rBC and potassium (K+, a tracer for biomass burning aerosol in an air mass influenced by aged biomass burning. Cluster analysis of single particle measurements identified five BBOA-related particle types. rBC accounted for 3–14 w.t. % of these particle types on average. Only one particle type exhibited a strong ion signal for K+, with mass spectra characterized by low molecular weight organic species. The remaining four particle types were classified based on the apparent molecular weight of the BBOA constituents. Two particle types were associated with low potassium content and significant amounts of high molecular weight (HMW organic compounds. Our observations indicate non-uniform mixing of particles within a biomass burning plume in terms of molecular weight and illustrate that HMW BBOA can be a key contributor to low-volatility BrC observed in BBOA particles.

2. Characteristics of mass distributions of aerosol particle and its inorganic water-soluble ions in summer over a suburb farmland in Beijing

Institute of Scientific and Technical Information of China (English)

ZHAO Peng; ZHU Tong; LIANG Baosheng; HU Min; KANG Ling; GONG Jicheng

2007-01-01

Agricultural activity is one of the most important sources of aerosol particles.To understand the mass distribution and sources of aerosol particles and their inorganic water-soluble ions in a suburb farmland of Beijing,particle samples were collected using a microoririce uniform deposit impactor(MOUDI)in the summer of 2004 in a suburb vegetable field.The distribution of the particles and their inorganic water-soluble ions in the diameter range of 0.18-18 μm were measured.The dominant fine particle ions were SO42-,NO3-,and NH4+.The association of day-to-day variation of the concentration of these ions with temperature,humidity,and solar radiation suggested that they ate formed by the reaction of NH3 released from the vegetable field with the acid species produced from photochemical reactions.Fine particle K+ is likely from vegetation emission and biomass burning.Coarse particles like Ca2+,Mg2+,NO3-,and SO42- are suggested to come from the mechanical process by which the soil particle entered the atmosphere,and from the reaction of the acid species at the surface of the soil particle.The results show that fertilizer and soil are important factors determining the aerosol particle over agricultural fields,and vegetable fields in suburban Beijing contribute significantly to the aerosol particle.

3. Atmospheric aerosol compositions and sources at two national background sites in northern and southern China

Science.gov (United States)

Zhu, Qiao; He, Ling-Yan; Huang, Xiao-Feng; Cao, Li-Ming; Gong, Zhao-Heng; Wang, Chuan; Zhuang, Xin; Hu, Min

2016-08-01

Although China's severe air pollution has become a focus in the field of atmospheric chemistry and the mechanisms of urban air pollution there have been researched extensively, few field sampling campaigns have been conducted at remote background sites in China, where air pollution characteristics on a larger scale are highlighted. In this study, an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), together with an Aethalometer, was deployed at two of China's national background sites in northern (Lake Hongze site; 33.23° N, 118.33° E; altitude 21 m) and southern (Mount Wuzhi site; 18.84° N, 109.49° E; altitude 958 m) China in the spring seasons in 2011 and 2015, respectively, in order to characterize submicron aerosol composition and sources. The campaign-average PM1 concentration was 36.8 ± 19.8 µg m-3 at the northern China background (NCB) site, which was far higher than that at the southern China background (SCB) site (10.9 ± 7.8 µg m-3). Organic aerosol (OA) (27.2 %), nitrate (26.7 %), and sulfate (22.0 %) contributed the most to the PM1 mass at NCB, while OA (43.5 %) and sulfate (30.5 %) were the most abundant components of the PM1 mass at SCB, where nitrate only constituted a small fraction (4.7 %) and might have contained a significant amount of organic nitrates (5-11 %). The aerosol size distributions and organic aerosol elemental compositions all indicated very aged aerosol particles at both sites. The OA at SCB was more oxidized with a higher average oxygen to carbon (O / C) ratio (0.98) than that at NCB (0.67). Positive matrix factorization (PMF) analysis was used to classify OA into three components, including a hydrocarbon-like component (HOA, attributed to fossil fuel combustion) and two oxygenated components (OOA1 and OOA2, attributed to secondary organic aerosols from different source areas) at NCB. PMF analysis at SCB identified a semi-volatile oxygenated component (SV-OOA) and a low-volatility oxygenated

4. Method and device for detecting and identifying bio-aerosol particles in the air

NARCIS (Netherlands)

Stowers. M.A.; Wuijckhuijse, A.L.; Marijnissen, J.C.; Kientz, C.E.

2002-01-01

In a method for detecting and identifying bioaerosol particles in the air, the bioaerosol particles in a particle stream are selected in an ATOFMS (aerosol time-of-flight mass spectrometer) by means of fluorescence techniques, and only the selected bioaerosol particles are ionized, for instance on t

5. Chemical composition, sources, and processes of urban aerosols during summertime in Northwest China: insights from High Resolution Aerosol Mass Spectrometry

Science.gov (United States)

Xu, J.; Zhang, Q.; Chen, M.; Ge, X.; Ren, J.; Qin, D.

2014-06-01

An aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed along with a Scanning Mobility Particle Sizer (SMPS) and a Multi Angle Absorption Photometers (MAAP) to measure the temporal variations of the mass loading, chemical composition, and size distribution of sub-micrometer particulate matter (PM1) in Lanzhou, northwest China, during 12 July-7 August 2012. The average PM1 mass concentration including non-refractory PM1 (NR-PM1) measured by HR-ToF-AMS and black carbon (BC) measured by MAAP during this study was 24.5 μg m-3 (ranging from 0.86 to 105μg m-3), with a mean composition consisting of 47% organics, 16% sulfate, 12% BC, 11% ammonium, 10% nitrate, and 4% chloride. The organics was consisted of 70% carbon, 21% oxygen, 8% hydrogen, and 1% nitrogen, with the average oxygen-to-carbon ratio (O / C) of 0.33 and organic mass-to-carbon ratio (OM / OC) of 1.58. Positive matrix factorization (PMF) of the high-resolution mass spectra of organic aerosols (OA) identified four distinct factors which represent, respectively, two primary OA (POA) emission sources (traffic and food cooking) and two secondary OA (SOA) types - a fresher, semi-volatile oxygenated OA (SV-OOA) and a more aged, low-volatility oxygenated OA (LV-OOA). Traffic-related hydrocarbon-like OA (HOA) and BC displayed distinct diurnal patterns both with peak at ~07:00-11:00 (BJT: UTC +8) corresponding to the morning rush hours, while cooking OA (COA) peaked during three meal periods. The diurnal profiles of sulfate and LV-OOA displayed a broad peak between ∼07:00-15:00, while those of nitrate, ammonium, and SV-OOA showed a narrower peak at ~08:00-13:00. The later morning and early afternoon peak in the diurnal profiles of secondary aerosol species was likely caused by mixing down of pollutants aloft, which were likely produced in the residual layer decoupled from the boundary layer during night time. The mass spectrum of SV-OOA also showed similarity with that of

6. COLLABORATIVE RESEARCH: Study of Aerosol Sources and Processing at the GVAX Pantnagar Supersite

Energy Technology Data Exchange (ETDEWEB)

Thornton, Joel A. [Univ. of Washington, Seattle, WA (United States); Worsnop, Douglas [Aerodyne Research, Billerica, MA (United States)

2016-09-22

This project was part of a collaborative campaign, including the participation of scientists from seven research groups as part of the Winter Intensive Operating Period (January-February 2012) of the Clean Air for London (ClearfLo) campaign at a rural site in Detling, UK, 45 km southeast of central London to study wintertime sources of urban particulate matter. The UW contribution by PI Thornton’s group was to make the first deployment of a chemical ionization mass spectrometer instrument (MOVI-CI-ToFMS) to measure both particle and gas phase organic acids. The new instrument ran nearly continuously during the ClearfLo WINTER IOP at the Detling site, producing a first-ever data set of molecular composition information that can be used for source apportionment and process studies. The UW group published a paper in Environmental Science and Technology and contributed to another (Bohnenstengel et al BAMS 2015) detailing a direct molecular connection between biomass/biofuel burning particles and aerosol light absorption. The ES&T paper (Mohr, et al ES&T 2013) has received 42 citations in just 3 years indicative of its significant impact on the field. These measurements of urban and rural aerosol properties will contribute to improved modeling of regional aerosol emissions, and of atmospheric aging and removal.

7. Source apportionment of submicron organic aerosols at an urban site by linear unmixing of aerosol mass spectra

Directory of Open Access Journals (Sweden)

V. A. Lanz

2006-11-01

Full Text Available Submicron ambient aerosol was characterized in summer 2005 at an urban background site in Zurich, Switzerland, during a three-week measurement campaign. Highly time-resolved samples of non-refractory aerosol components were analyzed with an Aerodyne aerosol mass spectrometer (AMS. Positive matrix factorization (PMF was used for the first time for AMS data to identify the main components of the total organic aerosol and their sources. The PMF retrieved factors were compared to measured reference mass spectra and were correlated with tracer species of the aerosol and gas phase measurements from collocated instruments. Six factors were found to explain virtually all variance in the data and could be assigned either to sources or to aerosol components such as oxygenated organic aerosol (OOA. Our analysis suggests that at the measurement site only a small (<10% fraction of organic PM1 originates from freshly emitted fossil fuel combustion. Other primary sources identified to be of similar or even higher importance are charbroiling (10–15% and wood burning (~10%, along with a minor source interpreted to be influenced by food cooking (6%. The fraction of all identified primary sources is considered as primary organic aerosol (POA. This interpretation is supported by calculated ratios of the modelled POA and measured primary pollutants such as elemental carbon (EC, NOx, and CO, which are in good agreement to literature values. A high fraction (60–69% of the measured organic aerosol mass is OOA which is interpreted mostly as secondary organic aerosol (SOA. This oxygenated organic aerosol can be separated into a highly aged fraction, OOA I, (40–50% with low volatility and a mass spectrum similar to fulvic acid, and a more volatile and probably less processed fraction, OOA II (on average 20%. This is the first publication of a multiple component analysis technique to AMS organic spectral data and also the first report of the

8. Characteristics, sources, and transport of aerosols measured in spring 2008 during the aerosol, radiation, and cloud processes affecting Arctic Climate (ARCPAC) Project

Science.gov (United States)

Brock, C. A.; Cozic, J.; Bahreini, R.; Froyd, K. D.; Middlebrook, A. M.; McComiskey, A.; Brioude, J.; Cooper, O. R.; Stohl, A.; Aikin, K. C.; de Gouw, J. A.; Fahey, D. W.; Ferrare, R. A.; Gao, R.-S.; Gore, W.; Holloway, J. S.; Hübler, G.; Jefferson, A.; Lack, D. A.; Lance, S.; Moore, R. H.; Murphy, D. M.; Nenes, A.; Novelli, P. C.; Nowak, J. B.; Ogren, J. A.; Peischl, J.; Pierce, R. B.; Pilewskie, P.; Quinn, P. K.; Ryerson, T. B.; Schmidt, K. S.; Schwarz, J. P.; Sodemann, H.; Spackman, J. R.; Stark, H.; Thomson, D. S.; Thornberry, T.; Veres, P.; Watts, L. A.; Warneke, C.; Wollny, A. G.

2011-03-01

We present an overview of the background, scientific goals, and execution of the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) project of April 2008. We then summarize airborne measurements, made in the troposphere of the Alaskan Arctic, of aerosol particle size distributions, composition, and optical properties and discuss the sources and transport of the aerosols. The aerosol data were grouped into four categories based on gas-phase composition. First, the background troposphere contained a relatively diffuse, sulfate-rich aerosol extending from the top of the sea-ice inversion layer to 7.4 km altitude. Second, a region of depleted (relative to the background) aerosol was present within the surface inversion layer over sea-ice. Third, layers of dense, organic-rich smoke from open biomass fires in southern Russia and southeastern Siberia were frequently encountered at all altitudes from the top of the inversion layer to 7.1 km. Finally, some aerosol layers were dominated by components originating from fossil fuel combustion. Of these four categories measured during ARCPAC, the diffuse background aerosol was most similar to the average springtime aerosol properties observed at a long-term monitoring site at Barrow, Alaska. The biomass burning (BB) and fossil fuel layers were present above the sea-ice inversion layer and did not reach the sea-ice surface during the course of the ARCPAC measurements. The BB aerosol layers were highly scattering and were moderately hygroscopic. On average, the layers produced a noontime net heating of ~0.1 K day-1 between 3 and 7 km and a slight cooling at the surface. The ratios of particle mass to carbon monoxide (CO) in the BB plumes, which had been transported over distances >5000 km, were comparable to the high end of literature values derived from previous measurements in wildfire smoke. These ratios suggest minimal precipitation scavenging and removal of the BB particles between the time they were

9. Characteristics, sources, and transport of aerosols measured in spring 2008 during the aerosol, radiation, and cloud processes affecting Arctic Climate (ARCPAC Project

Directory of Open Access Journals (Sweden)

C. A. Brock

2011-03-01

Full Text Available We present an overview of the background, scientific goals, and execution of the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC project of April 2008. We then summarize airborne measurements, made in the troposphere of the Alaskan Arctic, of aerosol particle size distributions, composition, and optical properties and discuss the sources and transport of the aerosols. The aerosol data were grouped into four categories based on gas-phase composition. First, the background troposphere contained a relatively diffuse, sulfate-rich aerosol extending from the top of the sea-ice inversion layer to 7.4 km altitude. Second, a region of depleted (relative to the background aerosol was present within the surface inversion layer over sea-ice. Third, layers of dense, organic-rich smoke from open biomass fires in southern Russia and southeastern Siberia were frequently encountered at all altitudes from the top of the inversion layer to 7.1 km. Finally, some aerosol layers were dominated by components originating from fossil fuel combustion.

Of these four categories measured during ARCPAC, the diffuse background aerosol was most similar to the average springtime aerosol properties observed at a long-term monitoring site at Barrow, Alaska. The biomass burning (BB and fossil fuel layers were present above the sea-ice inversion layer and did not reach the sea-ice surface during the course of the ARCPAC measurements. The BB aerosol layers were highly scattering and were moderately hygroscopic. On average, the layers produced a noontime net heating of ~0.1 K day−1 between 3 and 7 km and a slight cooling at the surface. The ratios of particle mass to carbon monoxide (CO in the BB plumes, which had been transported over distances >5000 km, were comparable to the high end of literature values derived from previous measurements in wildfire smoke. These ratios suggest minimal precipitation scavenging and removal of the BB

10. Characteristics, sources, and transport of aerosols measured in spring 2008 during the aerosol, radiation, and cloud processes affecting Arctic climate (ARCPAC project

Directory of Open Access Journals (Sweden)

C. A. Brock

2010-11-01

Full Text Available We present an overview of the background, scientific goals, and execution of the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC project of April 2008. We then summarize airborne measurements, made in the troposphere of the Alaskan Arctic, of aerosol particle size distributions, composition, and optical properties and discuss the sources and transport of the aerosols. The aerosol data were grouped into four categories based on gas-phase composition. First, the background troposphere contained a relatively diffuse, sulfate-rich aerosol extending from the top of the sea-ice inversion layer to 7.4 km altitude. Second, a region of depleted (relative to the background aerosol was present within the surface inversion layer over sea-ice. Third, layers of dense, organic-rich smoke from open biomass fires in Southern Russia and Southeastern Siberia were frequently encountered at all altitudes from the top of the inversion layer to 7.1 km. Finally, some aerosol layers were dominated by components originating from fossil fuel combustion.

Of these four categories measured during ARCPAC, the diffuse background aerosol was most similar to the average springtime aerosol properties observed at a long-term monitoring site at Barrow, Alaska. The biomass burning (BB and fossil fuel layers were present above the sea-ice inversion layer and did not reach the sea-ice surface during the course of the ARCPAC measurements. The BB aerosol layers were highly scattering and were moderately hygroscopic. On average, the layers produced a noontime net heating of ~0.1 K day−1 between 2 and 7 km and a~slight cooling at the surface. The ratios of particle mass to carbon monoxide (CO in the BB plumes, which had been transported over distances >5000 km, were comparable to the high end of literature values derived from previous measurements in fresh wildfire smoke. These ratios suggest minimal precipitation scavenging and removal of

11. Treatment of losses of ultrafine aerosol particles in long sampling tubes during ambient measurements

Science.gov (United States)

Kumar, Prashant; Fennell, Paul; Symonds, Jonathan; Britter, Rex

Long sampling tubes are often required for particle measurements in street canyons. This may lead to significant losses of the number of ultrafine (those below 100 nm) particles within the sampling tubes. Inappropriate treatment of these losses may significantly change the measured particle number distributions (PND), because most of the ambient particles, by number, exist in the ultrafine size range. Based on the Reynolds number (Re) in the sampling tubes, most studies treat the particle losses using the Gormley and Kennedy laminar flow model (Gormley, P.G., Kennedy, M., 1949. Diffusion from a stream following through a cylinderical tube. Proceedings of Royal Irish Academy 52, 163-169.) or the Wells and Chamberlain turbulent flow model (Wells, A.C., Chamberlain, A.C., 1967. Transport of small particles to vertical surfaces. British Journal of Applied Physics 18, 1793-1799.). Our experiments used a particle spectrometer with various lengths (1.00, 5.47, 5.55, 8.90 and 13.40 m) of sampling tube to measure the PNDs in the 5-2738 nm range. Experiments were performed under different operating conditions to measure the particle losses through silicone rubber tubes of circular cross-section (7.85 mm internal diameter). Sources of particles included emissions from an idling diesel engine car in a street canyon, emissions from a burning candle and those from the generation of salt aerosols using a nebuliser in the laboratory. Results showed that losses for particles below ≈20 nm were important and were largest for the smallest size range (5-10 nm), but were modest for particles above ≈20 nm. In our experiments the laminar flow model did not reflect the observations for small Re. This may be due to the sampling tubes not being kept straight or other complications. In situ calibration or comparison appears to be required.

12. Aerosol optical properties at a coastal site in Hong Kong, South China: temporal features, size dependencies and source analysis

Science.gov (United States)

Wang, Jiaping; Ding, Aijun; Virkkula, Aki; Lee, Shuncheng; Shen, Yicheng; Chi, Xuguang; Xu, Zheng

2016-04-01

Hong Kong is a typical coastal city adjacent to the Pearl River Delta (PRD) region in southern China, which is one of the regions suffering from severe air pollution. Atmospheric aerosols can affect the earth's radiative balance by scattering and absorbing incoming solar radiation. Black Carbon (BC) aerosol is a particularly emphasized component due to its strong light absorption. Aerosol transported from different source areas consists of distinct size distributions, leading to different optical properties. As the byproducts of the incomplete oxidation, BC and CO both have relatively long life time, their relationship is a good indicator for distinguishing different pollutant sources. In this study, temporal variations of aerosol optical properties and concentrations of BC and CO at a coastal background station in Hong Kong were investigated. Transport characteristics and origins of aerosol were elucidated by analyzing backward Lagrangian particle dispersion modeling (LPDM) results, together with related parameters including the relationships between optical properties and particle size, BC-CO correlations, ship location data and meteorological variables. From February 2012 to September 2013 and March 2014 to February 2015, continuous in-situ measurements of light scattering and absorption coefficients, particle size distribution and concentrations of BC and CO were conducted at Hok Tsui (HT), a coastal background station on the southeast tip of Hong Kong Island (22.22°N, 114.25°E, 60 m above the sea level) with few local anthropogenic activities. Affected by the Asian monsoon, this region is dominated by continental outflow in winter and by marine inflow from the South China Sea in summer, which is an ideal station for identifying the transport characteristics of aerosol and their effects on optical properties from different anthropogenic emission sources. 7-day backward Lagrangian particle dispersion modeling was performed for source identification. Three

13. On the composition of ammonia-sulfuric acid clusters during aerosol particle formation

CERN Document Server

Schobesberger, S; Bianchi, F; Rondo, L; Duplissy, J; Kürten, A; Ortega, I K; Metzger, A; Schnitzhofer, R; Almeida, J; Amorim, A; Dommen, J; Dunne, E M; Ehn, M; Gagné, S; Ickes, L; Junninen, H; Hansel, A; Kerminen, V-M; Kirkby, J; Kupc, A; Laaksonen, A; Lehtipalo, K; Mathot, S; Onnela, A; Petäjä, T; Riccobono, F; Santos, F D; Sipilä, M; Tomé, A; Tsagkogeorgas, G; Viisanen, Y; Wagner, P E; Wimmer, D; Curtius, J; Donahue, N M; Baltensperger, U; Kulmala, M; Worsnop, D R

2014-01-01

The formation of particles from precursor vapors is an important source of atmospheric aerosol. Research at the Cosmics Leaving OUtdoor Droplets (CLOUD) facility at CERN tries to elucidate which vapors are responsible for this new particle formation, and how in detail it proceeds. Initial measurement campaigns at the CLOUD stainless-steel aerosol chamber focused on investigating particle formation from ammonia (NH3) and sulfuric acid (H2SO4). Experiments were conducted in the presence of water, ozone and sulfur dioxide. Contaminant trace gases were suppressed at the technological limit. For this study, we mapped out the compositions of small NH3-H2SO4 clusters over a wide range of atmospherically relevant environmental conditions. We covered [NH3] in the range from 10. Positively charged clusters grew on average by Δm / Δn = 1.05 and were only observed at sufficiently high [NH3] / [H2SO4]. The H2SO4 molecules of these clusters are partially neutralized by NH3, in close resemblance to the acid-base bindings ...

14. Coupling aerosol-cloud-radiative processes in the WRF-Chem model: investigating the radiative impact of elevated point sources

Directory of Open Access Journals (Sweden)

E. G. Chapman

2008-08-01

Full Text Available The local and regional influence of elevated point sources on summertime aerosol forcing and cloud-aerosol interactions in northeastern North America was investigated using the WRF-Chem community model. The direct effects of aerosols on incoming solar radiation were simulated using existing modules to relate aerosol sizes and chemical composition to aerosol optical properties. Indirect effects were simulated by adding a prognostic treatment of cloud droplet number and adding modules that activate aerosol particles to form cloud droplets, simulate aqueous-phase chemistry, and tie a two-moment treatment of cloud water (cloud water mass and cloud droplet number to an existing radiation scheme. Fully interactive feedbacks thus were created within the modified model, with aerosols affecting cloud droplet number and cloud radiative properties, and clouds altering aerosol size and composition via aqueous processes, wet scavenging, and gas-phase-related photolytic processes. Comparisons of a baseline simulation with observations show that the model captured the general temporal cycle of aerosol optical depths (AODs and produced clouds of comparable thickness to observations at approximately the proper times and places. The model overpredicted SO2 mixing ratios and PM2.5 mass, but reproduced the range of observed SO2 to sulfate aerosol ratios, suggesting that atmospheric oxidation processes leading to aerosol sulfate formation are captured in the model. The baseline simulation was compared to a sensitivity simulation in which all emissions at model levels above the surface layer were set to zero, thus removing stack emissions. Instantaneous, site-specific differences for aerosol and cloud related properties between the two simulations could be quite large, as removing above-surface emission sources influenced when and where clouds formed within the modeling domain. When summed spatially over the finest resolution model

15. Sources and atmospheric processing of organic aerosol in the Mediterranean: insights from aerosol mass spectrometer factor analysis

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L. Hildebrandt

2011-12-01

Full Text Available Atmospheric particles were measured in the late winter (25 February–26 March 2009 at a remote coastal site on the island of Crete, Greece during the Finokalia Aerosol Measurement Experiment-2009. A quadrupole aerosol mass spectrometer (Q-AMS was employed to quantify the size-resolved chemical composition of non-refractory submicron aerosol, and a thermodenuder was used to analyze the organic aerosol (OA volatility. Complementary measurements included particle size distributions from a scanning mobility particle sizer, inorganic and organic particle composition from filter analysis, air ion concentrations, O3, NOx and NOy concentrations, and meteorological measurements. Factor analysis was performed on the OA mass spectra, and the variability in OA composition could best be explained with three OA components. The oxygenated organic aerosol (OOA was similar in composition and volatility to the summertime OA previously measured at this site and may represent an effective endpoint in particle-phase oxidation of organics. The two other OA components, one associated with amines (Amine-OA and the other probably associated with the burning of olive branches (OB-OA, had very low volatility but were less oxygenated. Hydrocarbon-like organic aerosol (HOA was not detected. The absence of OB-OA and Amine-OA in the summer data may be due to lower emissions and/or photochemical conversion of these components to OOA.

16. Sources and atmospheric processing of organic aerosol in the Mediterranean: insights from aerosol mass spectrometer factor analysis

Directory of Open Access Journals (Sweden)

L. Hildebrandt

2011-07-01

Full Text Available Atmospheric particles were measured in the winter at a remote coastal site on the island of Crete, Greece during the Finokalia Aerosol Measurement Experiment-2009. A Quadrupole aerosol mass spectrometer (Q-AMS was employed to quantify the size-resolved chemical composition of non-refractory submicron aerosol, and a thermodenuder was used to analyze the organic aerosol (OA volatility. Complementary measurements included particle size distributions from a scanning mobility particle sizer, inorganic and organic particle composition from filter analysis, concentrations of O3, NOx and NOy, and meteorological measurements. Factor analysis was performed on the OA mass spectra, and the variability in OA composition could best be explained with three OA components. The oxygenated organic aerosol (OOA was similar in composition and volatility to the summertime OA previously measured at this site and appears to represent an effective endpoint in particle-phase oxidation of organics. The two other OA components, one associated with amines (Amine-OA and the other probably associated with the burning of olive branches (OB-OA, had lower volatility but were less oxygenated. Hydrocarbon-like organic aerosol (HOA was not detected. The absence of OB-OA and Amine-OA in the summer data may be due to lower emissions and/or photochemical conversion of these components to OOA.

17. Global Modeling of the Oceanic Source of Organic Aerosols

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Stelios Myriokefalitakis

2010-01-01

Full Text Available The global marine organic aerosol budget is investigated by a 3-dimensional chemistry-transport model considering recently proposed parameterisations of the primary marine organic aerosol (POA and secondary organic aerosol (SOA formation from the oxidation of marine volatile organic compounds. MODIS and SeaWiFS satellite data of Chlorophyll-a and ECMWF solar incoming radiation, wind speed, and temperature are driving the oceanic emissions in the model. Based on the adopted parameterisations, the SOA and the submicron POA marine sources are evaluated at about 5 Tg yr−1 (∼1.5 Tg C yr−1 and 7 to 8 Tg yr−1 (∼4 Tg C yr−1, respectively. The computed marine SOA originates from the dimethylsulfide oxidation (∼78%, the potentially formed dialkyl amine salts (∼21%, and marine hydrocarbon oxidation (∼0.1%. Comparison of calculations with observations indicates an additional marine source of soluble organic carbon that could be partially encountered by marine POA chemical ageing.

18. Resuspension of Aerosol Particles from Evaporated Rain Drops to the Coarse Mode

Science.gov (United States)

Wang, H.; Easter, R. C.; Ganguly, D.; Singh, B.; Rasch, P. J.

2015-12-01

Precipitation scavenging (i.e., wet removal) has long been recognized as one of the major removal processes for tropospheric aerosol particles, and the dominant one for accumulation-mode size particles. When rain drops evaporate, the aerosol material contained in drops is resuspended, and this process has received much less attention. Unlike the resuspension from evaporated cloud droplets, the aerosol particles resuspended from evaporated rain drops have much larger sizes than most of the aerosol particles that acted as cloud condensation nuclei (CCN), became cloud borne, and then were collected by rain drops, because each rain drop generally collects thousands of cloud droplets. Here we present some aspects of this resuspension process obtained from modeling studies. First, we investigate some details of the process using a simple drop-size resolved model of raindrop evaporation in sub-saturated air below cloud base. Using these results, we then investigate different treatments of this process in a global aerosol and climate model that employs a modal aerosol representation. Compared to the model's original treatment of this process in which rain-borne aerosol is resuspended to the mode that it came from with its original size, the new treatment that resuspends to the coarse mode produces notable reductions in global CCN concentrations, as well as sulfate, black carbon, and organic aerosol mass, because the resuspended aerosol particles have much shorter lifetimes due to their larger sizes. Somewhat surprisingly, there are also notable reductions in coarse-mode sea salt and mineral dust burdens. These species are resuspended to the coarse mode in both the original and new treatments, but these resuspended particles are fewer in number and larger in size in the new treatment. This finding highlights some issues of the modal aerosol treatment for coarse mode particles.

19. Possible effect of extreme solar energetic particle events of September–October 1989 on polar stratospheric aerosols: a case study

Directory of Open Access Journals (Sweden)

I. A. Mironova

2013-02-01

Full Text Available The main ionization source of the middle and low Earth atmosphere is related to energetic particles coming from outer space. Usually it is ionization from cosmic rays that is always present in the atmosphere. But in a case of a very strong solar eruption some solar energetic particles (SEP can reach middle/low atmosphere increasing the ionization rate up to some orders of magnitude at polar latitudes. We continue investigating such a special class of solar events and their possible applications for natural variations of the aerosol content. After the case study of the extreme SEP event of January 2005 and its possible effect upon polar stratospheric aerosols, here we analyze atmospheric applications of the second sequence of several events that took place over the Autumn 1989. Using aerosol data obtained over polar regions from two satellites with space-borne optical instruments SAGE II and SAM II that were operating during September–October 1989, we found that an extreme major SEP event might have led to formation of new particles and/or growth of preexisting ultrafine particles in the polar stratospheric region. However, the effect of the additional ambient air ionization on the aerosol formation is minor, in comparison with temperature effect, and can take place only in the cold polar atmospheric conditions.

20. Improved Tandem Measurement Techniques for Aerosol Particle Analysis

Science.gov (United States)

Rawat, Vivek Kumar

Non-spherical, chemically inhomogeneous (complex) nanoparticles are encountered in a number of natural and engineered environments, including combustion systems (which produces highly non-spherical aggregates), reactors used in gas-phase materials synthesis of doped or multicomponent materials, and in ambient air. These nanoparticles are often highly diverse in size, composition and shape, and hence require determination of property distribution functions for accurate characterization. This thesis focuses on development of tandem mobility-mass measurement techniques coupled with appropriate data inversion routines to facilitate measurement of two dimensional size-mass distribution functions while correcting for the non-idealities of the instruments. Chapter 1 provides the detailed background and motivation for the studies performed in this thesis. In chapter 2, the development of an inversion routine is described which is employed to determine two dimensional size-mass distribution functions from Differential Mobility Analyzer-Aerosol Particle Mass analyzer tandem measurements. Chapter 3 demonstrates the application of the two dimensional distribution function to compute cumulative mass distribution function and also evaluates the validity of this technique by comparing the calculated total mass concentrations to measured values for a variety of aerosols. In Chapter 4, this tandem measurement technique with the inversion routine is employed to analyze colloidal suspensions. Chapter 5 focuses on application of a transverse modulation ion mobility spectrometer coupled with a mass spectrometer to study the effect of vapor dopants on the mobility shifts of sub 2 nm peptide ion clusters. These mobility shifts are then compared to models based on vapor uptake theories. Finally, in Chapter 6, a conclusion of all the studies performed in this thesis is provided and future avenues of research are discussed.

1. Source apportionment of the summer time carbonaceous aerosol at Nordic rural background sites

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K. E. Yttri

2011-06-01

Full Text Available In the present study, natural and anthropogenic sources of particulate organic carbon (OCp and elemental carbon (EC have been quantified based on weekly filter samples of PM10 collected at four Nordic rural background sites (Birkenes (Norway, Hyytiälä (Finland Vavihill (Sweden, Lille Valby (Denmark during late summer (5 August–2 September 2009. Levels of source specific tracers, i.e. cellulose, levoglucosan, mannitol and the 14C/12C ratio of total carbon (TC, have been used as input for source apportionment of the carbonaceous aerosol, whereas Latin Hypercube Sampling (LHS was used to statistically treat the multitude of possible combinations resulting from this approach.

The carbonaceous aerosol (here: TCp; i.e. particulate TC was totally dominated by natural sources (69–86 %, with biogenic secondary organic aerosol (BSOA being the single most important source (48–57 %. Interestingly, primary biological aerosol particles (PBAP were the second most important source (20–32 %. The anthropogenic contribution was mainly attributed to fossil fuel sources (OCff and ECff (10–24 %, whereas no more than 3–7 % was explained by combustion of biomass (OCbb and ECbb in this late summer campaign i.e. emissions from residential wood burning and/or wild/agricultural fires. Fossil fuel sources totally dominated the ambient EC loading, accounting for 4–12 % of TCp, whereas <1.5 % was attributed to combustion of biomass. The carbonaceous aerosol source apportionment showed only minor variation between the four selected sites. However, Hyytiälä and Birkenes showed greater resemblance to each other, as did Lille Valby and Vavihill, the two latter being somewhat more influenced by anthropogenic sources.

Ambient levels of organosulphates and nitrooxy-organosulphates in the Nordic rural background environment are reported for

2. Chemical characterization of submicron aerosol and particle growth events at a national background site (3295 m a.s.l. in the Tibetan Plateau

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W. Du

2015-05-01

Full Text Available Atmospheric aerosols exert highly uncertain impacts on radiative forcing and also have detrimental effects on human health. While aerosol particles are widely characterized in megacities in China, aerosol composition, sources and particle growth in rural areas in the Tibetan Plateau remain less understood. Here we present the results from an autumn study that was conducted from 5 September to 15 October 2013 at a national background monitoring station (3295 m a.s.l. in the Tibetan Plateau. The submicron aerosol composition and particle number size distributions were measured in situ with an Aerodyne Aerosol Chemical Speciation Monitor (ACSM and a Scanning Mobility Particle Sizer (SMPS. The average mass concentration of submicron aerosol (PM1 is 11.9 μg m−3 (range: 1.0–78.4 μg m−3 for the entire study, which is much lower than those observed at urban and rural sites in eastern China. Organics dominated PM1 on average accounting for 43%, followed by sulfate (28% and nitrate (1%. Positive matrix factorization analysis of ACSM organic aerosol (OA mass spectra identified an oxygenated OA (OOA and a biomass burning OA (BBOA. The OOA dominated OA composition accounting for 85% on average, 17% of which was inferred from aged BBOA. The BBOA contributed a considerable fraction of OA (15% due to the burning of cow dung and straws in September. New particle formation and growth events were frequently observed (80% of time throughout the study. The average particle growth rate is 2.0 nm h−1 (range: 0.8–3.2 nm h−1. By linking the evolution of particle number size distribution to aerosol composition, we found an elevated contribution of organics during particle growth periods and also a positive relationship between the growth rate and the fraction of OOA in OA, which potentially indicates an important role of organics in particle growth in the Tibetan Plateau.

3. Seasonal variations in aerosol particle composition at the puy-de-Dôme research station in France

Directory of Open Access Journals (Sweden)

E. J. Freney

2011-12-01

Full Text Available Detailed investigations of the chemical and microphysical properties of atmospheric aerosol particles were performed at the puy-de-Dôme (pdD research station (1465 m in autumn (September and October 2008, winter (February and March 2009, and summer (June 2010 using a compact Time-of-Flight Aerosol Mass Spectrometer (cToF-AMS. Over the three campaigns, the average mass concentrations of the non-refractory submicron particles ranged from 10 μg m−3 up to 27 μg m−3. Highest nitrate and ammonium mass concentrations were measured during the winter and during periods when marine modified airmasses were arriving at the site, whereas highest concentrations of organic particles were measured during the summer and during periods when continental airmasses arrived at the site. The measurements reported in this paper show that atmospheric particle composition is strongly influenced by both the season and the origin of the airmass. The total organic mass spectra were analysed using positive matrix factorisation to separate individual organic components contributing to the overall organic particle mass concentrations. These organic components include a low volatility oxygenated organic aerosol particle (LV-OOA and a semi-volatile organic aerosol particle (SV-OOA. Correlations of the LV-OOA components with fragments of m/z 60 and m/z 73 (mass spectral markers of wood burning during the winter campaign suggest that wintertime LV-OOA are related to aged biomass burning emissions, whereas organic aerosol particles measured during the summer are likely linked to biogenic sources. Equivalent potential temperature calculations, gas-phase, and LIDAR measurements define whether the research site is in the planetary boundary layer (PBL or in the free troposphere (FT/residual layer (RL. We observe that SV-OOA and nitrate particles are associated with air masses arriving from the PBL where as particle composition measured from RL

4. Identification of source contributions to visibility-reducing organic aerosols in the vicinity of Grand Canyon National Park. Interim final report

Energy Technology Data Exchange (ETDEWEB)

Mazurek, M.A.; Hallock, K.A.; Leach, M. [Brookhaven National Lab., Upton, NY (United States); Mason-Jones, M.; Mason-Jones, H.; Salmon, L.G.; Winner, D.A.; Cass, G.R. [California Inst. of Tech., Pasadena, CA (United States). Dept. of Environmental Engineering Science

1993-06-01

Sulfates and carbonaceous aerosols are the largest contributors to the fine particle burden in the atmosphere near Grand Canyon National Park. While the effects of sulfate particles on visibility at the Grand Canyon has been extensively studied, much less is known about the nature and origin of the carbonaceous aerosols that are present. This disparity in understanding arises from at least two causes: aerosol carbon data for the region are less plentiful and many of the sources that could contribute to that organic aerosol are both diverse and not well characterized. The objective of this present study is to examine the origin of the carbonaceous aerosol at Grand Canyon National Park during the summer season based on molecular tracer techniques applied to source and ambient samples collected specifically for this purpose.

5. Regional source identification of atmospheric aerosols in Beijing based on sulfur isotopic compositions

Science.gov (United States)

Lianfang, Wei; Pingqing, Fu; Xiaokun, Han; Qingjun, Guo; Yele, Sun; Zifa, Wang

2016-04-01

65 daily PM2.5 (aerosol particle with aerodynamic diameter less than 2.5 μm) samples were collected from an urban site in Beijing in four months representing the four seasons between September 2013 and July 2014. Inorganic ions, organic/elemental carbon and stable sulfur isotopes of sulfate aerosols were analyzed systematically. The "fingerprint" characteristics of the stable sulfur isotopic composition, together with trajectory clustering modeled by HYSPLIT-4 and potential source contribution function (PSCF), were employed for identifying potential regional sources. Results obviously exhibited the distinctive seasonality for various aerosol speciation associated with PM2.5 in Beijing with sulfate, nitrate, ammonium, organic matter, and element carbon being the dominant species. Elevated chloride associated with higher concentration of organics were found in autumn and winter, due to enhanced coal combustion emissions. The δ34S values of Beijing aerosol samples ranged from 2.94‰ to 10.2‰ with an average value of 6.18±1.87‰ indicating that the major sulfur source is direct fossil fuel burning-related emissions. Owning to a temperature-dependent fractionation and elevated biogenic sources of isotopically light sulfur in summer, the δ34S values had significant seasonal variations with a winter maximum ( 8.6‰)and a summer minimum ( 5.0‰). The results of trajectory clustering and the PSCF method demonstrated that higher concentrations of sulfate with lower sulfur isotope ratios ( 4.83‰) were associated with air masses from the south, southeast or east, whereas lower sulfate concentrations with higher δ34S values ( 6.69‰) when the air masses were mainly from north or northwest. These results suggested two main different kinds of regional coal combustion sources contributed to the pollution in Beijing.

6. Long-term Chemical Characterization of Submicron Aerosol Particles in the Amazon Forest - ATTO Station

Science.gov (United States)

Carbone, S.; Brito, J.; Rizzo, L. V.; Holanda, B. A.; Cirino, G. G.; Saturno, J.; Krüger, M. L.; Pöhlker, C.; Ng, N. L.; Xu, L.; Andreae, M. O.; Artaxo, P.

2015-12-01

The study of the chemical composition of aerosol particles in the Amazon forest represents a step forward to understand the strong coupling between the atmosphere and the forest. For this reason submicron aerosol particles were investigated in the Amazon forest, where biogenic and anthropogenic aerosol particles coexist at the different seasons (wet/dry). The measurements were performed at the ATTO station, which is located about 150 km northeast of Manaus. At ATTO station the Aerosol chemical speciation monitor (ACSM, Aerodyne) and the Multiangle absorption photometer (MAAP, Thermo 5012) have been operated continuously from March 2014 to July 2015. In this study, long-term measurements (near-real-time, ~30 minutes) of PM1 chemical composition were investigated for the first time in this environment.The wet season presented lower concentrations than the dry season (~5 times). In terms of chemical composition, both seasons were dominated by organics (75 and 63%) followed by sulfate (11 and 13%). Nitrate presented different ratio values between the mass-to-charges 30 to 46 (main nitrate fragments) suggesting the presence of nitrate as inorganic and organic nitrate during both seasons. The results indicated that about 75% of the nitrate signal was from organic nitrate during the dry season. In addition, several episodes with elevated amount of chloride, likely in the form of sea-salt from the Atlantic Ocean, were observed during the wet season. During those episodes, chloride comprised up to 7% of the PM1. During the dry season, chloride was also observed; however, with different volatility, which suggested that Chloride was present in different form and source. Moreover, the constant presence of sulfate and BC during the wet season might be related to biomass burning emissions from Africa. BC concentration was 2.5 times higher during the dry season. Further characterization of the organic fraction was accomplished with the positive matrix factorization (PMF), which

7. Method and device for detecting and identifying bio-aerosol particles in the air

OpenAIRE

Stowers. M.A.; van Wuijckhuijse, A.L.; Marijnissen, J.C.; Kientz, C. E.

2002-01-01

In a method for detecting and identifying bioaerosol particles in the air, the bioaerosol particles in a particle stream are selected in an ATOFMS (aerosol time-of-flight mass spectrometer) by means of fluorescence techniques, and only the selected bioaerosol particles are ionized, for instance on the basis of MALDI (matrix-assisted laser desorption/ionization), after which the resulting ions are detected and the bioaerosol particles are identified.; The selection of bioaerosol particles take...

8. Possible effect of extreme solar energetic particle event of 20 January 2005 on polar stratospheric aerosols: direct observational evidence

Directory of Open Access Journals (Sweden)

I. A. Mironova

2011-05-01

Full Text Available Energetic cosmic rays are the main source of ionization of the low-middle atmosphere, leading to associated changes in atmospheric properties. Via the hypothetical influence of ionization on aerosol growth and facilitated formation of cloud condensation nuclei, this may be an important indirect link relating solar variability to climate. This effect is highly debated, however, since the proposed theoretical mechanisms still remain illusive and qualitative, and observational evidence is inconclusive and controversial. Therefore, important questions regarding the existence and magnitude of the effect, and particularly the fraction of aerosol particles that can be formed and grow large enough to influence cloud condensation nuclei (CCN, are still open. Here we present empirical evidence of the possible effect caused by cosmic rays upon polar stratospheric aerosols, based on a case study of an extreme solar energetic particle (SEP event of 20 January 2005. Using aerosol data obtained over polar regions from different satellites with optical instruments that were operating during January 2005, such as the Stratospheric Aerosol and Gas Experiment III (SAGE III, and Optical Spectrograph and Infrared Imaging System (OSIRIS, we found a significant simultaneous change in aerosol properties in both the southern and northern polar regions in temporal association with the SEP event. We speculate that ionization of the atmosphere, which was abnormally high during this extreme SEP event, might have led to formation of new particles and/or growth of preexisting ultrafine particles up to the size of CCN. However, a detailed interpretation of the effect is left for subsequent studies. This is the first time high vertical resolution measurements have been used to provide evidence for the probable production of stratospheric CCN from cosmic ray induced ionization.

9. Electron mean free path from angle-dependent photoelectron spectroscopy of aerosol particles

CERN Document Server

Goldmann, Maximilian; West, Adam H C; Yoder, Bruce L; Signorell, Ruth

2015-01-01

We propose angle-resolved photoelectron spectroscopy of aerosol particles as an alternative way to determine the electron mean free path of low energy electrons in solid and liquid materials. The mean free path is obtained from fits of simulated photoemission images to experimental ones over a broad range of different aerosol particle sizes. The principal advantage of the aerosol approach is twofold. Firstly, aerosol photoemission studies can be performed for many different materials, including liquids. Secondly, the size-dependent anisotropy of the photoelectrons can be exploited in addition to size-dependent changes in their kinetic energy. These finite size effects depend in different ways on the mean free path and thus provide more information on the mean free path than corresponding liquid jet, thin film, or bulk data. The present contribution is a proof of principle employing a simple model for the photoemission of electrons and preliminary experimental data for potassium chloride aerosol particles.

10. Spectro-microscopy of Ambient Aerosol Particles: Observational Constraints on Mixing State Parameterization

Science.gov (United States)

OBrien, R. E.; Wang, B.; Laskin, A.; West, M.; Riemer, N. S.; Gilles, M. K.; Moffet, R.

2014-12-01

Individual aerosol particles are often mixtures of multiple components such as inorganic salts, soot or elemental carbon, and organic molecules. The amounts of the different components in each particle and the particle morphologies will impact the CCN activity and the radiative properties of the aerosol population. A recent parameterization of the mixing state developed by Nicole Riemer and Matthew West provides a clear transition between ambient measurements of aerosol components and particle mixing states employed in climate models. Single particle spectro-microscopy techniques including scanning transmission x-ray microscopy/near-edge x-ray absorption fine structure spectroscopy (STXM/NEXAFS) and computer controlled scanning electron microscopy/energy dispersive x-ray spectroscopy (CCSEM/EDX) are used to measure the composition of aerosol particles from the CARES campaign at both T0 and T1. Here, we present results from the application of the per particle composition to a parameterization of the mixing state and provide constraints on the mixing state of ambient aerosol particles. The two microscopy techniques yield complementary information on the mixing state of the aerosol populations; STXM/NEXAFS provides information on the mixing state of the organic fraction while CCSEM/EDX provides information on the inorganic fraction.

11. A combined particle trap/HTDMA hygroscopicity study of mixed inorganic/organic aerosol particles

Science.gov (United States)

Zardini, A. A.; Sjogren, S.; Marcolli, C.; Krieger, U. K.; Gysel, M.; Weingartner, E.; Baltensperger, U.; Peter, T.

2008-09-01

Atmospheric aerosols are often mixtures of inorganic and organic material. Organics can represent a large fraction of the total aerosol mass and are comprised of water-soluble and insoluble compounds. Increasing attention was paid in the last decade to the capability of mixed inorganic/organic aerosol particles to take up water (hygroscopicity). We performed hygroscopicity measurements of internally mixed particles containing ammonium sulfate and carboxylic acids (citric, glutaric, adipic acid) in parallel with an electrodynamic balance (EDB) and a hygroscopicity tandem differential mobility analyzer (HTDMA). The organic compounds were chosen to represent three distinct physical states. During hygroscopicity cycles covering hydration and dehydration measured by the EDB and the HTDMA, pure citric acid remained always liquid, adipic acid remained always solid, while glutaric acid could be either. We show that the hygroscopicity of mixtures of the above compounds is well described by the Zdanovskii-Stokes-Robinson (ZSR) relationship as long as the two-component particle is completely liquid in the ammonium sulfate/glutaric acid system; deviations up to 10% in mass growth factor (corresponding to deviations up to 3.5% in size growth factor) are observed for the ammonium sulfate/citric acid 1:1 mixture at 80% RH. We observe even more significant discrepancies compared to what is expected from bulk thermodynamics when a solid component is present. We explain this in terms of a complex morphology resulting from the crystallization process leading to veins, pores, and grain boundaries which allow for water sorption in excess of bulk thermodynamic predictions caused by the inverse Kelvin effect on concave surfaces.

12. HETEROGENEOUS SOOT NANOSTRUCTURE IN ATMOSPHERIC AND COMBUSTION SOURCE AEROSOLS

Science.gov (United States)

Microscopic images of soot emissions from wildfire and a wide range of anthropogenic combustion sources show that the nanostructures of individual particles in these emissions are predominantly heterogeneous, decidedly influenced by the fuel composition and by the particular comb...

13. Numerical advection of correlated tracers: preserving particle size/composition moment sequences during transport of aerosol mixtures

Energy Technology Data Exchange (ETDEWEB)

McGraw, Robert [Atmospheric Sciences Division, Environmental Sciences Department Brookhaven National Laboratory, Upton, NY 11973 (United States)

2007-07-15

Nonlinear transport algorithms designed to reduce numerical diffusion fail to preserve correlations between moments, isotope abundances, etc. when these scalar densities are transported in models as separate tracers. In case of the particle size/composition coordinates of an aerosol, such loss can give rise to unphysical moment sets. New statistical approaches to aerosol dynamics, which involve tracking moments directly, offer highly efficient alternatives to sectional and modal methods for representing aerosols in climate models, but it is essential that moment set integrity be preserved throughout a simulation. In this paper we review the problem and weaknesses of previous attempts at solution, including vector transport - a scheme in which the moments, as internal aerosol coordinates, are transported together with a single lead tracer such as number or mass. A non-negative least squares (NNLS) solution that finally eliminates the problem without requiring modification of the transport algorithm itself is presented. Following each transport step, new moment sets are resolved into sums of previously validated sets with non-negative coefficients using NNLS Transport errors are removed and the now guaranteed-to-be-valid moment sets are ready for passage to the aerosol dynamics module. In addition to moment set validation, the new scheme reduces numerical diffusion during transport and provides greater accuracy for the source apportionment of aerosol mixtures. The method is not limited to moment transport - similar improvements in accuracy are expected using NNLS in conjunction with modal and sectional methods.

14. The online chemical analysis of single particles using aerosol beams and time of flight mass spectroscopy

NARCIS (Netherlands)

Kievit, O.; Weiss, M.; Verheijen, P.J.T.; Marijnissen, J.C.M.; Scarlett, B.

This paper describes an on-line instrument, capable of measuring the size and chemical composition of single aerosol particles. Possible applications include monitoring aerosol reactors and studying atmospheric chemistry. The main conclusion is that a working prototype has been built and tested. It

15. Connecting Organic Aerosol Climate-Relevant Properties to Chemical Mechanisms of Sources and Processing

Energy Technology Data Exchange (ETDEWEB)

Thornton, Joel [Univ. of Washington, Seattle, WA (United States)

2015-01-26

The research conducted on this project aimed to improve our understanding of secondary organic aerosol (SOA) formation in the atmosphere, and how the properties of the SOA impact climate through its size, phase state, and optical properties. The goal of this project was to demonstrate that the use of molecular composition information to mechanistically connect source apportionment and climate properties can improve the physical basis for simulation of SOA formation and properties in climate models. The research involved developing and improving methods to provide online measurements of the molecular composition of SOA under atmospherically relevant conditions and to apply this technology to controlled simulation chamber experiments and field measurements. The science we have completed with the methodology will impact the simulation of aerosol particles in climate models.

16. Measurement of ambient aerosols in northern Mexico City by single particle mass spectrometry

Directory of Open Access Journals (Sweden)

R. C. Moffet

2008-08-01

Full Text Available Continuous ambient measurements with aerosol time-of-flight mass spectrometry (ATOFMS were made in an industrial/residential section in the northern part of Mexico City as part of the Mexico City Metropolitan Area-2006 campaign (MCMA-2006. Results are presented for the period of 15–27 March 2006. The submicron size mode contained both fresh and aged biomass burning, aged organic carbon (OC mixed with nitrate and sulfate, elemental carbon (EC, nitrogen-organic carbon, industrial metal, and inorganic NaK inorganic particles. Overall, biomass burning and aged OC particle types comprised 40% and 31%, respectively, of the submicron mode. In contrast, the supermicron mode was dominated by inorganic NaK particle types (42% which represented a mixture of dry lake bed dust and industrial NaK emissions mixed with soot. Additionally, aluminosilicate dust, transition metals, OC, and biomass burning contributed to the supermicron particles. Early morning periods (2–6 a.m. showed high fractions of inorganic particles from industrial sources in the northeast, composed of internal mixtures of Pb, Zn, EC and Cl, representing up to 73% of the particles in the 0.2–3μm size range. A unique nitrogen-containing organic carbon (NOC particle type, peaking in the early morning hours, was hypothesized to be amines from local industrial emissions based on the time series profile and back trajectory analysis. A strong dependence on wind speed and direction was observed in the single particle types that were present during different times of the day. The early morning (3:30–10 a.m. showed the greatest contributions from industrial emissions. During mid to late mornings (7–11 a.m., weak northerly winds were observed along with the most highly aged particles. Stronger winds from the south picked up in the late morning (after 11 a.m., resulting in a decrease in the concentrations of the major aged particle types and an increase in the number fraction of fresh

17. [Factors influencing particle measurement of aerosols and their retention in the lung].

Science.gov (United States)

Le Bouffant, L

1977-01-01

The dimensional characteristics of the particles of an aerosol depend on the means used for producing them. Mechanical spray and ultrasonic dispersion give polydispersed particles. On the other hand, centrifugal atomization produces a monodispersed aerosol. Particle retention in the lung system depends on the particle diameter. In addition, retention varies according to the respiratory characteristics: it is minimal for about 15 inspirations per minute. Using iron-59 labeled particles, it was shown that the degree of retention varies considerably from one individual to the other and accessibility to the depths of the lungs is decreased under the effect of certain lesions. Bronchial retention appears to be increased in smokers.

18. A new method to discriminate secondary organic aerosols from different sources using high-resolution aerosol mass spectra

Science.gov (United States)

Heringa, M. F.; Decarlo, P. F.; Chirico, R.; Tritscher, T.; Clairotte, M.; Mohr, C.; Crippa, M.; Slowik, J. G.; Pfaffenberger, L.; Dommen, J.; Weingartner, E.; Prévôt, A. S. H.; Baltensperger, U.

2012-02-01

Organic aerosol (OA) represents a significant and often major fraction of the non-refractory PM1 (particulate matter with an aerodynamic diameter da car and a two-stroke Euro 2 scooter were characterized with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and compared to SOA from α-pinene. The emissions were sampled from the chimney/tailpipe by a heated inlet system and filtered before injection into a smog chamber. The gas phase emissions were irradiated by xenon arc lamps to initiate photo-chemistry which led to nucleation and subsequent particle growth by SOA production. Duplicate experiments were performed for each SOA type, with the averaged organic mass spectra showing Pearson's r values >0.94 for the correlations between the four different SOA types after five hours of aging. High-resolution mass spectra (HR-MS) showed that the dominant peaks in the MS, m/z 43 and 44, are dominated by the oxygenated ions C2H3O+ and CO2+, respectively, similarly to the relatively fresh semi-volatile oxygenated OA (SV-OOA) observed in the ambient aerosol. The atomic O:C ratios were found to be in the range of 0.25-0.55 with no major increase during the first five hours of aging. On average, the diesel SOA showed the lowest O:C ratio followed by SOA from wood burning, α-pinene and the scooter emissions. Grouping the fragment ions revealed that the SOA source with the highest O:C ratio had the largest fraction of small ions. The HR data of the four sources could be clustered and separated using principal component analysis (PCA). The model showed a significant separation of the four SOA types and clustering of the duplicate experiments on the first two principal components (PCs), which explained 79% of the total variance. Projection of ambient SV-OOA spectra resolved by positive matrix factorization (PMF) showed that this approach could be useful to identify large contributions of the tested SOA sources to SV-OOA. The first results from this

19. Estimating marine aerosol particle volume and number from Maritime Aerosol Network data

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A. M. Sayer

2012-09-01

Full Text Available As well as spectral aerosol optical depth (AOD, aerosol composition and concentration (number, volume, or mass are of interest for a variety of applications. However, remote sensing of these quantities is more difficult than for AOD, as it is more sensitive to assumptions relating to aerosol composition. This study uses spectral AOD measured on Maritime Aerosol Network (MAN cruises, with the additional constraint of a microphysical model for unpolluted maritime aerosol based on analysis of Aerosol Robotic Network (AERONET inversions, to estimate these quantities over open ocean. When the MAN data are subset to those likely to be comprised of maritime aerosol, number and volume concentrations obtained are physically reasonable. Attempts to estimate surface concentration from columnar abundance, however, are shown to be limited by uncertainties in vertical distribution. Columnar AOD at 550 nm and aerosol number for unpolluted maritime cases are also compared with Moderate Resolution Imaging Spectroradiometer (MODIS data, for both the present Collection 5.1 and forthcoming Collection 6. MODIS provides a best-fitting retrieval solution, as well as the average for several different solutions, with different aerosol microphysical models. The "average solution" MODIS dataset agrees more closely with MAN than the "best solution" dataset. Terra tends to retrieve lower aerosol number than MAN, and Aqua higher, linked with differences in the aerosol models commonly chosen. Collection 6 AOD is likely to agree more closely with MAN over open ocean than Collection 5.1. In situations where spectral AOD is measured accurately, and aerosol microphysical properties are reasonably well-constrained, estimates of aerosol number and volume using MAN or similar data would provide for a greater variety of potential comparisons with aerosol properties derived from satellite or chemistry transport model data. However, without accurate AOD data and prior knowledge of

20. Ambient measurement of fluorescent aerosol particles with a WIBS in the Yangtze River Delta of China: potential impacts of combustion-related aerosol particles

Science.gov (United States)

Yu, Xiawei; Wang, Zhibin; Zhang, Minghui; Kuhn, Uwe; Xie, Zhouqing; Cheng, Yafang; Pöschl, Ulrich; Su, Hang

2016-09-01

Fluorescence characteristics of aerosol particles in a polluted atmosphere were studied using a wideband integrated bioaerosol spectrometer (WIBS-4A) in Nanjing, Yangtze River Delta area of China. We observed strong diurnal and day-to-day variations of fluorescent aerosol particles (FAPs). The average number concentrations of FAPs (1-15 µm) detected in the three WIBS measurement channels (FL1: 0.6 cm-3, FL2: 3.4 cm-3, FL3: 2.1 cm-3) were much higher than those observed in forests and rural areas, suggesting that FAPs other than bioaerosols were detected. We found that the number fractions of FAPs were positively correlated with the black carbon mass fraction, especially for the FL1 channel, indicating a large contribution of combustion-related aerosols. To distinguish bioaerosols from combustion-related FAPs, we investigated two classification schemes for use with WIBS data. Our analysis suggests a strong size dependence for the fractional contributions of different types of FAPs. In the FL3 channel, combustion-related particles seem to dominate the 1-2 µm size range while bioaerosols dominate the 2-5 µm range. The number fractions of combustion-related particles and non-combustion-related particles to total aerosol particles were ˜ 11 and ˜ 5 %, respectively.

1. Airborne measurements of aerosol optical properties related to early spring transport of mid-latitude sources into the Arctic

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R. A. de Villiers

2010-06-01

Full Text Available Airborne lidar and in-situ measurements of the aerosol properties were conducted between Svalbard Island and Scandinavia in April 2008. Evidence of aerosol transport from Europe and Asia is given. The analysis of the aerosol optical properties based on a multiwavelength lidar (355, 532, 1064 nm including volume depolarization at 355 nm aims at distinguishing the role of the different aerosol sources (Siberian wild fires, Eastern Asia and European anthropogenic emissions. Combining, first aircraft measurements, second FLEXPART simulations with a calculation of the PBL air fraction originating from the three different mid-latitude source regions, and third level-2 CALIPSO data products (i.e. backscatter coefficient 532 nm,volume depolarization and color ratio between 1064 and 532 nm in aerosol layers along the transport pathways, appears a valuable approach to identify the role of the different aerosol sources even after a transport time larger than 4 days. Optical depth of the aerosol layers are always rather small (<4% while transported over the Arctic and ratio of the total attenuated backscatter (i.e. including molecular contribution provide more stable result than conventional aerosol backscatter ratio. Above Asia, CALIPSO data indicate more depolarization (up to 15% and largest color ratio (>0.5 for the northeastern Asia emissions (i.e. an expected mixture of Asian pollution and dust, while low depolarization together with smaller and quasi constant color ratio (≈0.3 are observed for the Siberian biomass burning emissions. A similar difference is visible between two layers observed by the aircraft above Scandinavia. The analysis of the time evolution of the aerosol optical properties revealed by CALIPSO between Asia and Scandinavia shows a gradual decrease of the aerosol backscatter, depolarization ratio and color ratio which suggests the removal of the largest particles in the accumulation mode. A similar study conducted for a European

2. Experimentation and modelling of mineral aerosol dissolution as source of transition metals in cloud droplets

Science.gov (United States)

Desboeufs, K.; Sofikitis, A.; Velay, J.; Losno, R.; Dulac, F.; Colin, J.

2004-12-01

Even at nano-molar concentrations, transition metals (TMI) could play an important role in the radical chemistry of the atmospheric liquid phase. For instance, cloud chemistry model calculations suggest that depletion of HOx by reactions between TMI and HO2/O2- radicals significantly slows down O3 production in polluted clouds. TMI are transferred into the liquid phase from aerosol particles by dissolution processes which can be a slow reaction. The dissolution kinetic of the solid phase thus competes with chemical kinetics in the homogeneous aqueous phase. It is therefore of importance to consider the evolution of TMI concentrations into cloud droplets in order to quantify the atmospheric impact of aerosols on the aqueous chemistry. Mineral particles including soil-derived particles and fly-ash are important sources of TMI in the troposphere.In order to parameterize the dissolution kinetic and concentrations of TMI from mineral particles into cloud droplets, we have conducted experimental laboratory simulations which mimic particles/water interactions occurring into droplets. These simulations were carried out in an open-flow reactor for typical atmospheric conditions (pH, ionic strength.). Data on TMI dissolution kinetic are provided for two generic kinds of mineral matrices from anthropogenic and natural sources: alumino-silicated and carbonaceous particles (dust, fly-ash, or urban particles). The concentrations of TMI released depend on pH, matrix type and particle-water contact time. The metals coming from carbonaceous particles are adsorbed impurities or salts and are very soluble with dissolution hardly dependent on pH. On the opposite, the metals dissolved from alumino-silicated particles are less soluble, notably the ones constitutive of the matrix network (Fe, Mn), and their dissolution is highly influenced by the pH. However, at a given pH, the results on the kinetic of dissolution emphasize that whatever the matrix, the TMI dissolution rates decrease

3. The Formation of Porous Membranes by Filtration of Aerosol Nano-particles

DEFF Research Database (Denmark)

Andersen, Sune Klint; Johannessen, Tue; Mosleh, Majid

2002-01-01

Flame-generated aerosol particles of Al2O3 were deposited by gas filtration on two types of porous and ceramic tubes of α-Al2O3 with mean pore diameters of 450 and 2700 nm, respectively. The particles were aggregates with average mobility diameters in the range of 30¨¢100 nm and primary particle...

4. Sugar markers in aerosol particles from an agro-industrial region in Brazil

Science.gov (United States)

Urban, R. C.; Alves, C. A.; Allen, A. G.; Cardoso, A. A.; Queiroz, M. E. C.; Campos, M. L. A. M.

2014-06-01

This work aimed to better understand how aerosol particles from sugar cane burning contribute to the chemical composition of the lower troposphere in an agro-industrial region of São Paulo State (Brazil) affected by sugar and ethanol fuel production. During a period of 21 months, we collected 105 samples and quantified 20 saccharides by GC-MS. The average concentrations of levoglucosan (L), mannosan (M), and galactosan (G) for 24-h sampling were 116, 16, and 11 ng m-3 respectively. The three anhydrosugars had higher and more variable concentrations in the nighttime and during the sugar cane harvest period, due to more intense biomass burning practices. The calculated L/M ratio, which may serve as a signature for sugar cane smoke particles, was 9 ± 5. Although the total concentrations of the anhydrosugars varied greatly among samples, the relative mass size distributions of the saccharides were reasonably constant. Emissions due to biomass burning were estimated to correspond to 69% (mass) of the sugars quantified in the harvest samples, whereas biogenic emissions corresponded to 10%. In the non-harvest period, these values were 44 and 27%, respectively, indicating that biomass burning is an important source of aerosol to the regional atmosphere during the whole year.

5. Contribution of feldspar and marine organic aerosols to global ice nucleating particle concentrations

Science.gov (United States)

Vergara-Temprado, Jesús; Murray, Benjamin J.; Wilson, Theodore W.; O'Sullivan, Daniel; Browse, Jo; Pringle, Kirsty J.; Ardon-Dryer, Karin; Bertram, Allan K.; Burrows, Susannah M.; Ceburnis, Darius; DeMott, Paul J.; Mason, Ryan H.; O'Dowd, Colin D.; Rinaldi, Matteo; Carslaw, Ken S.

2017-03-01

Ice-nucleating particles (INPs) are known to affect the amount of ice in mixed-phase clouds, thereby influencing many of their properties. The atmospheric INP concentration changes by orders of magnitude from terrestrial to marine environments, which typically contain much lower concentrations. Many modelling studies use parameterizations for heterogeneous ice nucleation and cloud ice processes that do not account for this difference because they were developed based on INP measurements made predominantly in terrestrial environments without considering the aerosol composition. Errors in the assumed INP concentration will influence the simulated amount of ice in mixed-phase clouds, leading to errors in top-of-atmosphere radiative flux and ultimately the climate sensitivity of the model. Here we develop a global model of INP concentrations relevant for mixed-phase clouds based on laboratory and field measurements of ice nucleation by K-feldspar (an ice-active component of desert dust) and marine organic aerosols (from sea spray). The simulated global distribution of INP concentrations based on these two species agrees much better with currently available ambient measurements than when INP concentrations are assumed to depend only on temperature or particle size. Underestimation of INP concentrations in some terrestrial locations may be due to the neglect of INPs from other terrestrial sources. Our model indicates that, on a monthly average basis, desert dusts dominate the contribution to the INP population over much of the world, but marine organics become increasingly important over remote oceans and they dominate over the Southern Ocean. However, day-to-day variability is important. Because desert dust aerosol tends to be sporadic, marine organic aerosols dominate the INP population on many days per month over much of the mid- and high-latitude Northern Hemisphere. This study advances our understanding of which aerosol species need to be included in order to

6. Spectral Light Absorption and Scattering by Aerosol Particles in Central Amazonia

Science.gov (United States)

Artaxo, P.; Holanda, B. A.; Ferreira De Brito, J.; Carbone, S.; Barbosa, H. M.; Rizzo, L. V.; Cirino, G. G.; Andreae, M. O.; Saturno, J.; Pöhlker, C.; Martin, S. T.; Holben, B. N.; Schafer, J.

2015-12-01

As part of the GoAmazon2014/5, a detailed characterization of spectral light absorption and light scattering was performed at four research sites located in the central Amazon forest at different distances upwind and downwind of Manaus. The sites ATTO (T0a) and Embrapa (T0e) are located upwind of Manaus where it is possible to observe very pristine atmospheric conditions in wet season. The site Tiwa (T2) is being operated under the direct influence of the Manaus plume at 5 km downwind of Manaus and, finally, the Manacapuru (T3) site is located at about 60 km downwind of Manaus. The spectral dependence of light absorption and light scattering were measured using Aethalometers (7-wavelengths) and Nephelometers (3-wavelengths), respectively. By calculating the Absorption Angstrom Exponent (AAE), it was possible to get information about the source of the aerosol whereas the Scattering Angstrom Exponent (SAE) gives information about its size distribution. Sunphotometers from the AERONET network were set up at T3 and T0e sites to measure column Aerosol Optical Depth (AOD). For all the stations, much higher absorption and scattering coefficients were observed during the dry season in comparison to the wet season, as a result of the larger concentration of BC and OC present in the biomass burning events. Additionally, we also observed Manaus plume pollution that alters the BC signal. There is also an increase of the AAE during the dry season due to the larger amount of aerosols from biomass burning compared with urban pollution. High values of AAE are also observed during the wet season, attributed to the presence of long-range transport of aerosols from Africa. The SAE for all the sites are lower during the wet season, with the dominance of large biological particles, and increases during the dry season as a consequence of fine particles emitted from both biomass and fossil fuel burning. The AOD at T0e and T3 (Jan-Jun/2014) showed very similar values ranging from 0.05 to

7. Multi-Modal Spatial Analysis of Metals within Individual Aerosol Particles Sampled from the Asian Continental Outflow

Science.gov (United States)

Moffet, R.; Harder, T.; Williams, G.; Chen-Wiegart, Y. C. K.; Furutani, H.; Gilles, M. K.; Laskin, A.; Schoonen, M. A.; Thieme, J.; Uematsu, M.

2015-12-01

Aerosols represent an important source of iron and other metals into oceanic surface waters. In some regions of the ocean, the productivity is limited by iron. Thus, iron is an important variable in the carbon cycles of both marine and atmospheric environments. Here, we build upon previous work characterizing the source and oxidation state of iron in atmospheric particles to provide more information on the mineralogy of the iron phases using the newly built Sub-Micron Resolution X-ray Spectroscopy (SRX) beamline at the National Synchrotron Light Source II (NSLS II). The SRX beamline covers energies from 4.6 to 24 keV, allowing mapping of elements from Z=15 (P) to Z=95 (Am) at a sub-micrometer and a sub-100 nm spatial scale. This new method of aerosol analysis will provide outstanding performance for the spectromicroscopy of trace elements. Moreover, this technique will provide multiple modes of detection (fluorescence, absorption, diffraction, and tomographic imaging) to allow for a more complete characterization of the molecular nature of natural samples having nanometer scale structural features. Simultaneously measured X-ray absorption and fluorescence spectra from Asian mineral dust standards and deposited atmospheric particles will be presented. Application of this technique to atmospheric particle samples will broaden the scope of elements over which detailed spectral information can be obtained at a high spatial resolution and will complement existing imaging methods used to determine aerosol chemical and physical properties.

8. ATMOSPHERIC AEROSOL SOURCE-RECEPTOR RELATIONSHIPS: THE ROLE OF COAL-FIRED POWER PLANTS

Energy Technology Data Exchange (ETDEWEB)

Allen L. Robinson; Spyros N. Pandis; Cliff I. Davidson

2004-04-01

This report describes the technical progress made on the Pittsburgh Air Quality Study (PAQS) during the period of September 2003 through February 2004. Significant progress was made this project period on the analysis of ambient data, source apportionment, and deterministic modeling activities. Results highlighted in this report include chemical fractionation of the organic fraction to quantify the ratio of organic mass to organic carbon (OM/OC). The average OM/OC ratio for the 31 samples analyzed so far is 1.89, ranging between 1.62 and 2.53, which is consistent with expectations for an atmospherically processed regional aerosol. Analysis of the single particle data reveals that a on a particles in Pittsburgh consist of complex mixture of primary and secondary components. Approximately 79% of all particles measured with the instrument containing some form of carbon, with Carbonaceous Ammonium Nitrate (54.43%) being the dominant particle class. PMCAMx predictions were compared with data from more than 50 sites of the STN network located throughout the Eastern United States for the July 2001 period. OC and sulfate concentrations predicted by PMCAMx are within {+-}30% of the observed concentration at most of these sites. Spherical Aluminum Silicate particle concentrations (SAS) were used to estimate the contribution of primary coal emissions to fine particle levels at the central monitoring site. Primary emissions from coal combustion contribute on average 0.44 {+-} 0.3 {micro}g/m{sup 3} to PM{sub 2.5} at the site or 1.4 {+-} 1.3% of the total PM{sub 2.5} mass. Chemical mass balance analysis was performed to apportion the primary organic aerosol. About 70% of the primary OC emissions are from vehicular sources, with the gasoline contribution being on average three times greater than the diesel emissions in the summer.

9. Organic particle types by single-particle measurements using a time-of-flight aerosol mass spectrometer coupled with a light scattering module

Directory of Open Access Journals (Sweden)

S. Liu

2013-02-01

Full Text Available Chemical and physical properties of individual ambient aerosol particles can vary greatly, so measuring the chemical composition at the single-particle level is essential for understanding atmospheric sources and transformations. Here we describe 46 days of single-particle measurements of atmospheric particles using a time-of-flight aerosol mass spectrometer coupled with a light scattering module (LS-ToF-AMS. The light scattering module optically detects particles larger than 180 nm vacuum aerodynamic diameter (130 nm geometric diameter before they arrive at the chemical mass spectrometer and then triggers the saving of single-particle mass spectra. 271 641 particles were detected and sampled during 237 h of sampling in single-particle mode. By comparing timing of the predicted chemical ion signals from the light scattering measurement with the measured chemical ion signals by the mass spectrometer for each particle, particle types were classified and their number fractions determined as follows: prompt vaporization (46%, delayed vaporization (6%, and null (48%, where null was operationally defined as less than 6 ions per particle. Prompt and delayed vaporization particles with sufficient chemical information (i.e., more than 40 ions per particle were clustered based on similarity of organic mass spectra (using k-means algorithm to result in three major clusters: highly oxidized particles (dominated by m/z 44, relatively less oxidized particles (dominated by m/z 43, and particles associated with fresh urban emissions. Each of the three organic clusters had limited chemical properties of other clusters, suggesting that all of the sampled organic particle types were internally mixed to some degree; however, the internal mixing was never uniform and distinct particle types existed throughout the study. Furthermore, the single-particle mass spectra and time series of these clusters agreed well with mass-based components

10. Burning of olive tree branches: a major organic aerosol source in the Mediterranean

Directory of Open Access Journals (Sweden)

E. Kostenidou

2013-09-01

Full Text Available Aerosol produced during the burning of olive tree branches was characterized with both direct source sampling (using a mobile smog chamber and with ambient measurements during the burning season. The fresh particles were composed of 80% organic matter, 8–10% black carbon (BC, 5% potassium, 3–4% sulfate, 2–3% nitrate and 0.8% chloride. Almost half of the fresh olive tree branches burning organic aerosol (otBB-OA consisted of alkane groups. Their mode diameter was close to 70 nm. The oxygen to carbon (O : C ratio of the fresh otBB-OA was 0.29 ± 0.04. The mass fraction of levoglucosan in PM1 was 0.034–0.043, relatively low in comparison with most fuel types. This may lead to an underestimation of the otBB-OA contribution if levoglucosan is being used as a wood burning tracer. Chemical aging was observed during smog chamber experiments, as f44 and O : C ratio increased, due to reactions with OH radicals and O3. The otBB-OA AMS mass spectrum differs from the other published biomass burning spectra, with a main difference at m/z 60, used as levoglucosan tracer. In addition to particles, volatile organic compounds (VOCs such as methanol, acetonitrile, acrolein, benzene, toluene and xylenes are also emitted. Positive matrix factorization (PMF was applied to the ambient organic aerosol data and 3 factors could be identified: OOA (oxygenated organic aerosol, 55%, HOA (hydrocarbon-like organic aerosol, 11.3% and otBB-OA 33.7%. The fresh chamber otBB-OA AMS spectrum is close to the PMF otBB-OA spectrum and resembles the ambient mass spectrum during olive tree branches burning periods. We estimated an otBB-OA emission factor of 3.5 ± 0.9 g kg−1. Assuming that half of the olive tree branches pruned is burned in Greece, 2300 ± 600 tons of otBB-OA are emitted every year. This activity is one of the most important fine aerosol sources during the winter months in Mediterranean countries.

11. Burning of olive tree branches: a major organic aerosol source in the Mediterranean

Directory of Open Access Journals (Sweden)

E. Kostenidou

2013-03-01

Full Text Available Aerosol produced during the burning of olive tree branches was characterized with both direct source-sampling (using a mobile smog chamber and with ambient measurements during the burning season. The fresh particles were composed of 80% organic matter, 8–10% black carbon (BC, 5% potassium, 3–4% sulfate, 2–3% nitrate and 0.8% chloride. Almost half of the fresh olive tree branches burning organic aerosol (otBB-OA consisted of alkane groups. Their mode diameter was close to 70 nm. The oxygen to carbon (O:C ratio of the fresh otBB-OA was 0.29 ± 0.04. The mass fraction of levoglucosan in PM1 was 0.034–0.043, relatively low in comparison with most fuel types. This may lead to an underestimation of the otBB-OA contribution if levoglucosan is being used as a wood burning tracer. Chemical aging was observed during smog chamber experiments, as f44 and O:C ratio increased, due to reactions with OH radicals and O3. The otBB-OA AMS mass spectrum differs from the other published biomass burning spectra, with a main difference at m/z 60, used as levoglucosan tracer. In addition to particles, volatile organic compounds (VOCs such as methanol, acetonitrile, acrolein, benzene, toluene and xylenes are also emitted. Positive matrix factorization (PMF was applied to the ambient organic aerosol data and 3 factors could be identified: OOA (oxygenated organic aerosol, 55%, HOA (hydrocarbon-like organic aerosol, 11.3% and otBB-OA 33.7%. The fresh chamber otBB-OA AMS spectrum is close to the PMF otBB-OA spectrum and resembles the ambient mass spectrum during olive tree branches burning periods. We estimated an otBB-OA emission factor of 3.5 ± 0.2 g kg−1. Assuming that half of the olive tree branches pruned is burned in Greece 2280 ± 140 tons of otBB-OA are emitted every year. This activity is one of the most important fine aerosol sources during the winter months in the Mediterranean countries.

12. Sources and transformations of particle-bound polycyclic aromatic hydrocarbons in Mexico City

Directory of Open Access Journals (Sweden)

L. C. Marr

2006-01-01

Full Text Available Understanding sources, concentrations, and transformations of polycyclic aromatic hydrocarbons (PAHs in the atmosphere is important because of their potent mutagenicity and carcinogenicity. The measurement of particle-bound PAHs by three different methods during the Mexico City Metropolitan Area field campaign in April 2003 presents a unique opportunity for characterization of these compounds and intercomparison of the methods. The three methods are (1 collection and analysis of bulk samples for time-integrated gas- and particle-phase speciation by gas chromatography/mass spectrometry; (2 aerosol photoionization for fast detection of PAHs on particles' surfaces; and (3 aerosol mass spectrometry for fast analysis of size and chemical composition. This research represents the first time aerosol mass spectrometry has been used to measure ambient PAH concentrations and the first time that fast, real-time methods have been used to quantify PAHs alongside traditional filter-based measurements in an extended field campaign. Speciated PAH measurements suggest that motor vehicles and garbage and wood burning are important sources in Mexico City. The diurnal concentration patterns captured by aerosol photoionization and aerosol mass spectrometry are generally consistent. Ambient concentrations of particle-phase PAHs typically peak at ~110 ng m-3 during the morning rush hour and rapidly decay due to changes in source activity patterns and dilution as the boundary layer rises, although surface-bound PAH concentrations decay faster. The more rapid decrease in surface versus bulk PAH concentrations during the late morning suggests that freshly emitted combustion-related particles are quickly coated by secondary aerosol material in Mexico City's atmosphere and may also be transformed by heterogeneous reactions.

13. Comparison between CARIBIC aerosol samples analysed by accelerator-based methods and optical particle counter measurements

Directory of Open Access Journals (Sweden)

B. G. Martinsson

2014-04-01

Full Text Available Inter-comparison of results from two kinds of aerosol systems in the CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container passenger aircraft based observatory, operating during intercontinental flights at 9–12 km altitude, is presented. Aerosol from the lowermost stratosphere (LMS, the extra-tropical upper troposphere (UT and the tropical mid troposphere (MT were investigated. Aerosol particle volume concentration measured with an optical particle counter (OPC is compared with analytical results of the sum of masses of all major and several minor constituents from aerosol samples collected with an impactor. Analyses were undertaken with accelerator-based methods particle-induced X-ray emission (PIXE and particle elastic scattering analysis (PESA. Data from 48 flights during one year are used, leading to a total of 106 individual comparisons. The ratios of the particle volume from the OPC and the total mass from the analyses were in 84% within a relatively narrow interval. Data points outside this interval are connected with inlet-related effects in clouds, large variability in aerosol composition, particle size distribution effects and some cases of non-ideal sampling. Overall, the comparison of these two CARIBIC measurements based on vastly different methods show good agreement, implying that the chemical and size information can be combined in studies of the MT/UT/LMS aerosol.

14. A wavelength-dispersive instrument for characterizing fluorescence and scattering spectra of individual aerosol particles on a substrate

Science.gov (United States)

Huffman, Donald R.; Swanson, Benjamin E.; Huffman, J. Alex

2016-08-01

We describe a novel, low-cost instrument to acquire both elastic and inelastic (fluorescent) scattering spectra from individual supermicron-size particles in a multi-particle collection on a microscope slide. The principle of the device is based on a slitless spectroscope that is often employed in astronomy to determine the spectra of individual stars in a star cluster but had not been applied to atmospheric particles. Under excitation, most commonly by either a 405 nm diode laser or a UV light-emitting diode (LED), fluorescence emission spectra of many individual particles can be determined simultaneously. The instrument can also acquire elastic scattering spectra from particles illuminated by a white-light source. The technique also provides the ability to detect and rapidly estimate the number fraction of fluorescent particles that could contaminate a collection of non-fluorescent material, even without analyzing full spectra. Advantages and disadvantages of using black-and-white cameras compared to color cameras are given. The primary motivation for this work has been to develop an inexpensive technique to characterize fluorescent biological aerosol particles, especially particles such as pollen and mold spores that can cause allergies. An example of an iPhone-enabled device is also shown as a means for collecting data on biological aerosols at lower cost or by utilizing citizen scientists for expanded data collection.

15. Vertical Transport of Aerosol Particles across Mountain Topography near the Los Angeles Basin

Science.gov (United States)

Murray, J. J.; Schill, S.; Freeman, S.; Bertram, T. H.; Lefer, B. L.

2015-12-01

Transport of aerosol particles is known to affect air quality and is largely dependent on the characteristic topography of the surrounding region. To characterize this transport, aerosol number distributions were collected with an Ultra-High Sensitivity Aerosol Spectrometer (UHSAS, DMT) during the 2015 NASA Student Airborne Research Program (SARP) in and around the Los Angeles Basin in Southern California. Increases in particle number concentration and size were observed over mountainous terrain north of Los Angeles County. Chemical analysis and meteorological lagrangian trajectories suggest orographic lifting processes, known as the "chimney effect". Implications for spatial transport and distribution will be discussed.

16. Global modelling of direct and indirect effects of sea spray aerosol using a source function encapsulating wave state

Science.gov (United States)

Partanen, A.-I.; Dunne, E. M.; Bergman, T.; Laakso, A.; Kokkola, H.; Ovadnevaite, J.; Sogacheva, L.; Baisnée, D.; Sciare, J.; Manders, A.; O'Dowd, C.; de Leeuw, G.; Korhonen, H.

2014-11-01

Recently developed parameterizations for the sea spray aerosol source flux, encapsulating wave state, and its organic fraction were incorporated into the aerosol-climate model ECHAM-HAMMOZ to investigate the direct and indirect radiative effects of sea spray aerosol particles. Our simulated global sea salt emission of 805 Tg yr-1 (uncertainty range 378-1233 Tg yr-1) was much lower than typically found in previous studies. Modelled sea salt and sodium ion concentrations agreed relatively well with measurements in the smaller size ranges at Mace Head (annual normalized mean model bias -13% for particles with vacuum aerodynamic diameter Dva particles with aerodynamic diameter Da particles with Da particles with 2.5 μm biologically active months, suggesting a need to improve the parameterization of the organic sea spray fraction. Globally, the satellite-retrieved AOD over the oceans, using PARASOL data, was underestimated by the model (means over ocean 0.16 and 0.10, respectively); however, in the pristine region around Amsterdam Island the measured AOD fell well within the simulated uncertainty range. The simulated sea spray aerosol contribution to the indirect radiative effect was positive (0.3 W m-2), in contrast to previous studies. This positive effect was ascribed to the tendency of sea salt aerosol to suppress both the in-cloud supersaturation and the formation of cloud condensation nuclei from sulfate. These effects can be accounted for only in models with sufficiently detailed aerosol microphysics and physics-based parameterizations of cloud activation. However, due to a strong negative direct effect, the simulated effective radiative forcing (total radiative) effect was -0.2 W m-2. The simulated radiative effects of the primary marine organic emissions were small, with a direct effect of 0.03 W m-2 and an indirect effect of -0.07 W m-2.

17. The effects of mineral dust particles, aerosol regeneration and ice nucleation parameterizations on clouds and precipitation

Directory of Open Access Journals (Sweden)

A. Teller

2012-03-01

Full Text Available This study focuses on the effects of aerosol particles on the formation of convective clouds and precipitation in the Eastern Mediterranean sea with a special emphasis on the role of mineral dust particles in these processes. We used a new detailed numerical cloud microphysics scheme that has been implemented in the Weather Research and Forecast (WRF model in order to study aerosol-cloud interaction in 3-D configuration based on realistic meteorological data. Using a number of case studies we tested the contribution of mineral dust particles and different ice nucleation parameterizations to precipitation development. In this study we also investigated the importance of recycled (regenerated aerosols that had been released to the atmosphere following the evaporation of cloud droplets.

The results showed that increased aerosol concentration due to the presence of mineral dust enhanced the formation of ice crystals. The dynamic evolution of the cloud system sets the time periods and regions in which heavy or light precipitation occurred in the domain. The precipitation rate, the time and duration of precipitation were affected by the aerosol properties only at small area scales (with areas of about 20 km2. Changes of the ice nucleation scheme from ice supersaturation dependent parameterization to a recent approach of aerosol concentration and temperature dependent parameterization modified the ice crystals concentrations but did not affect the total precipitation in the domain. Aerosol regeneration modified the concentration of cloud droplets at cloud base by dynamic recirculation of the aerosols but also had only a minor effect on precipitation.

The major conclusion from this study is that the effect of mineral dust particles on clouds and total precipitation is limited by the properties of the atmospheric dynamics and the only effect of aerosol on precipitation may come from significant increase in the concentration

18. Seasonality of ultrafine and sub-micron aerosols and the inferences on particle formation processes

Science.gov (United States)

Cheung, H. C.; Chou, C. C.-K.; Chen, M.-J.; Huang, W.-R.; Huang, S.-H.; Tsai, C.-Y.; Lee, C. S.-L.

2015-08-01

suggested as a result of seasonally enhanced photochemical oxidation of SO2, which contributes to the production of H2SO4, and low level of PM10 (d ≤ 10 μm) that serves as the condensation sink. Regarding the sources of aerosol particles, correlation analysis upon the PNCs against NOx revealed that the local vehicular exhaust was the dominant contributor of the UFPs throughout a year. On the contrary, the Asian pollution outbreaks can have significant influence in the PNC of accumulation mode particles during the seasons of winter monsoons. The results of this study underline the significance of secondary organic aerosols in the seasonal variations of UFPs and the influences of continental pollution outbreaks in the downwind areas of Asian outflows.

19. Metal and silicate particles including nanoparticles are present in electronic cigarette cartomizer fluid and aerosol.

Directory of Open Access Journals (Sweden)

Monique Williams

Full Text Available Electronic cigarettes (EC deliver aerosol by heating fluid containing nicotine. Cartomizer EC combine the fluid chamber and heating element in a single unit. Because EC do not burn tobacco, they may be safer than conventional cigarettes. Their use is rapidly increasing worldwide with little prior testing of their aerosol.We tested the hypothesis that EC aerosol contains metals derived from various components in EC.Cartomizer contents and aerosols were analyzed using light and electron microscopy, cytotoxicity testing, x-ray microanalysis, particle counting, and inductively coupled plasma optical emission spectrometry.The filament, a nickel-chromium wire, was coupled to a thicker copper wire coated with silver. The silver coating was sometimes missing. Four tin solder joints attached the wires to each other and coupled the copper/silver wire to the air tube and mouthpiece. All cartomizers had evidence of use before packaging (burn spots on the fibers and electrophoretic movement of fluid in the fibers. Fibers in two cartomizers had green deposits that contained copper. Centrifugation of the fibers produced large pellets containing tin. Tin particles and tin whiskers were identified in cartridge fluid and outer fibers. Cartomizer fluid with tin particles was cytotoxic in assays using human pulmonary fibroblasts. The aerosol contained particles >1 µm comprised of tin, silver, iron, nickel, aluminum, and silicate and nanoparticles (<100 nm of tin, chromium and nickel. The concentrations of nine of eleven elements in EC aerosol were higher than or equal to the corresponding concentrations in conventional cigarette smoke. Many of the elements identified in EC aerosol are known to cause respiratory distress and disease.The presence of metal and silicate particles in cartomizer aerosol demonstrates the need for improved quality control in EC design and manufacture and studies on how EC aerosol impacts the health of users and bystanders.

20. Aerosol composition, oxidation properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation summit study

Science.gov (United States)

Xu, W. Q.; Sun, Y. L.; Chen, C.; Du, W.; Han, T. T.; Wang, Q. Q.; Fu, P. Q.; Wang, Z. F.; Zhao, X. J.; Zhou, L. B.; Ji, D. S.; Wang, P. C.; Worsnop, D. R.

2015-12-01

The mitigation of air pollution in megacities remains a great challenge because of the complex sources and formation mechanisms of aerosol particles. The 2014 Asia-Pacific Economic Cooperation (APEC) summit in Beijing serves as a unique experiment to study the impacts of emission controls on aerosol composition, size distributions, and oxidation properties. Herein, a high-resolution time-of-flight aerosol mass spectrometer was deployed in urban Beijing for real-time measurements of size-resolved non-refractory submicron aerosol (NR-PM1) species from 14 October to 12 November 2014, along with a range of collocated measurements. The average (±σ) PM1 was 41.6 (±38.9) μg m-3 during APEC, which was decreased by 53 % compared with that before APEC. The aerosol composition showed substantial changes owing to emission controls during APEC. Secondary inorganic aerosol (SIA: sulfate + nitrate + ammonium) showed significant reductions of 62-69 %, whereas organics presented much smaller decreases (35 %). The results from the positive matrix factorization of organic aerosol (OA) indicated that highly oxidized secondary organic aerosol (SOA) showed decreases similar to those of SIA during APEC. However, primary organic aerosol (POA) from cooking, traffic, and biomass-burning sources were comparable to those before APEC, indicating the presence of strong local source emissions. The oxidation properties showed corresponding changes in response to OA composition. The average oxygen-to-carbon level during APEC was 0.36 (±0.10), which is lower than the 0.43 (±0.13) measured before APEC, demonstrating a decrease in the OA oxidation degree. The changes in size distributions of primary and secondary species varied during APEC. SIA and SOA showed significant reductions in large accumulation modes with peak diameters shifting from ~ 650 to 400 nm during APEC, whereas those of POA remained relatively unchanged. The changes in aerosol composition, size distributions, and oxidation

1. The chemical composition of fine ambient aerosol particles in the Beijing area

Science.gov (United States)

Nekat, Bettina; van Pinxteren, Dominik; Iinuma, Yoshiteru; Gnauk, Thomas; Müller, Konrad; Herrmann, Hartmut

2010-05-01

The strong economical growth in China during the last few decades led to heavy air pollution caused by significantly increased particle emissions. The aerosol particles affect not only the regional air quality and visibility, but can also influence cloud formation processes and the radiative balance of the atmosphere by their optical and microphysical properties. The ability to act as Cloud Condensation Nuclei (CCN) is related to microphysical properties like the hygroscopic growth or the cloud droplet activation. The chemical composition of CCN plays an important role on these properties and varies strongly with the particle size and the time of day. Hygroscopic or surface active substances can increase the hygroscopicity and lower the surface tension of the particle liquid phase, respectively. The presence of such compounds may result in faster cloud droplet activation by faster water uptake. The DFG project HaChi (Haze in China) aimed at studying physical and chemical parameters of urban aerosol particles in the Beijing area in order to associate the chemical composition of aerosol particles with their ability to act as CCN. To this end, two measurement campaigns were performed at the Wuqing National Ordinary Meteorological Observing Station, which is a background site near Beijing. The winter campaign was realized in March 2009 and the summer campaign took place from mid July 2009 to mid August 2009. Fine particles with an aerodynamic diameter smaller than or equal 1 μm were continuously sampled for 24h over the two campaigns using a DIGITEL high volume sampler (DHA-80). The present contribution presents and discusses the results of the chemical characterization of the DIGITEL filters samples. The filters were analyzed for the mass concentration, inorganic ions and carbon sum parameters like elemental (EC), organic (OC) and water soluble organic carbon (WSOC). The WSOC fraction was further characterized for hygroscopic substances like low molecular

2. Laser ion source for particle accelerators

CERN Document Server

Sherwood, T R

1995-01-01

There is an interest in accelerating atomic nuclei to produce particle beams for medical therapy, atomic and nuclear physics, inertial confinement fusion and particle physics. Laser Ion Sources, in which ions are extracted from plasma created when a high power density laser beam pulse strikes a solid surface in a vacuum, are not in common use. However, some new developments in which heavy ions have been accelerated show that such sources have the potential to provide the beams required for high-energy accelerator systems.

3. Aerosol Source Attributions and Source-Receptor Relationships Across the Northern Hemisphere

Science.gov (United States)

Bian, Huisheng; Chin, Mian; Kucsera, Tom; Pan, Xiaohua; Darmenov, Anton; Colarco, Peter; Torres, Omar; Shults, Michael

2014-01-01

Emissions and long-range transport of air pollution pose major concerns on air quality and climate change. To better assess the impact of intercontinental transport of air pollution on regional and global air quality, ecosystems, and near-term climate change, the UN Task Force on Hemispheric Transport of Air Pollution (HTAP) is organizing a phase II activity (HTAP2) that includes global and regional model experiments and data analysis, focusing on ozone and aerosols. This study presents the initial results of HTAP2 global aerosol modeling experiments. We will (a) evaluate the model results with surface and aircraft measurements, (b) examine the relative contributions of regional emission and extra-regional source on surface PM concentrations and column aerosol optical depth (AOD) over several NH pollution and dust source regions and the Arctic, and (c) quantify the source-receptor relationships in the pollution regions that reflect the sensitivity of regional aerosol amount to the regional and extra-regional emission reductions.

4. SPM analysis on groups of single aerosol particles around steel plant

Institute of Scientific and Technical Information of China (English)

沙因; 王安璞; 等

1996-01-01

Several methods for preparing samples of dispersed single aeroslo particles used in scanning proton microprobe(SPM) analysis were tested.Many elements such as Al,Si,S,Cl,Ca,Ti,Cr,Mn,Fe,Ni,Cu and Zn in the groups of different single aerosol particles from the Capital Steel Plant area were analyzed by SPM,The distributions of elemental contents in the group of single particles were mapped with three dimensional contour and the isometric.A new approach to study the group of different single aerosol particles for air pollution is developed in the present work.The results are significant to assessing the environmental impact of the dispersed single aerosol particles.

5. Investigating the use of secondary organic aerosol as seed particles in simulation chamber experiments

Directory of Open Access Journals (Sweden)

J. F. Hamilton

2011-06-01

Full Text Available The use of β-caryophyllene secondary organic aerosol particles as seeds for smog chamber simulations has been investigated. A series of experiments were carried out in the Manchester photochemical chamber as part of the Aerosol Coupling in the Earth System (ACES project to study the effect of seed particles on the formation of secondary organic aerosol (SOA from limonene photo-oxidation. Rather than use a conventional seed aerosol containing ammonium sulfate or diesel particles, a method was developed to use in-situ chamber generated seed particles from β-caryophyllene photo-oxidation, which were then diluted to a desired mass loading (in this case 4–13 μg m−3. Limonene was then introduced into the chamber and oxidised, with the formation of SOA seen as a growth in the size of oxidised organic seed particles from 150 to 325 nm mean diameter. The effect of the partitioning of limonene oxidation products onto the seed aerosol was assessed using aerosol mass spectrometry during the experiment and the percentage of m/z 44, an indicator of degree of oxidation, increased from around 5 to 8 %. The hygroscopicity of the aerosol also changed, with the growth factor for 200 nm particles increasing from less than 1.05 to 1.25 at 90 % RH. The detailed chemical composition of the limonene SOA could be extracted from the complex β-caryophyllene matrix using two-dimensional gas chromatography (GC × GC and liquid chromatography coupled to mass spectrometry. High resolution Fourier Transform Ion Cyclotron Resonance Mass Spectrometry (FTICR-MS was used to determine exact molecular formulae of the seed and the limonene modified aerosol. The average O:C ratio was seen to increase from 0.32 to 0.37 after limonene oxidation products had condensed onto the organic seed.

6. Investigating the use of secondary organic aerosol as seed particles in simulation chamber experiments

Directory of Open Access Journals (Sweden)

J. F. Hamilton

2010-10-01

Full Text Available The use of β-caryophyllene secondary organic aerosol particles as seeds for smog chamber simulations has been investigated. A series of experiments were carried out in the Manchester photochemical chamber as part of the Aerosol Coupling in the Earth System (ACES project to study the effect of seed particles on the formation of secondary organic aerosol (SOA from limonene photo-oxidation. Rather than use a conventional seed aerosol containing ammonium sulphate or diesel particles, a method was developed to use in situ chamber generated seed particles from β-caryophyllene photo-oxidation, which were then diluted to a desired mass loading (in this case 4–13 μg m-3. Limonene was then introduced into the chamber and oxidised, with the formation of SOA seen as a growth in the size of oxidised organic seed particles from 150 to 325 nm mean diameter. The effect of the partitioning of limonene oxidation products onto the seed aerosol was assessed using aerosol mass spectrometry during the experiment and the percentage of m/z 44, an indicator of degree of oxidation, increased from around 5 to 8%. The hygroscopicity of the aerosol also changed, with the growth factor for 200 nm particles increasing from less than 1.05 to 1.25 at 90% RH. The detailed chemical composition of the limonene SOA could be extracted from the complex β-caryophyllene matrix using two-dimensional gas chromatography (GC×GC and liquid chromatography coupled to mass spectrometry. High resolution Fourier Transform Ion Cyclotron Resonance Mass Spectrometry (FTICR-MS was used to determine exact molecular formulae of the seed and the limonene modified aerosol. The average O:C ratio was seen to increase from 0.32 to 0.37 after limonene oxidation products had condensed onto the organic seed.

7. Single particle characterization using a light scattering module coupled to a time-of-flight aerosol mass spectrometer

Directory of Open Access Journals (Sweden)

E. S. Cross

2008-12-01

Full Text Available We present the first single particle results obtained using an Aerodyne time-of-flight aerosol mass spectrometer coupled with a light scattering module (LS-ToF-AMS. The instrument was deployed at the T1 ground site approximately 40 km northeast of the Mexico City Metropolitan Area (MCMA as part of the MILAGRO field study in March of 2006. The instrument was operated as a standard AMS from 12–30 March, acquiring average chemical composition and size distributions for the ambient aerosol, and in single particle mode from 27–30 March. Over a 75-h sampling period, 12 853 single particle mass spectra were optically triggered, saved, and analyzed. The correlated optical and chemical detection allowed detailed examination of single particle collection and quantification within the LS-ToF-AMS. The single particle data enabled the mixing states of the ambient aerosol to be characterized within the context of the size-resolved ensemble chemical information.

The particulate mixing states were examined as a function of sampling time and most of the particles were found to be internal mixtures containing many of the organic and inorganic species identified in the ensemble analysis. The single particle mass spectra were deconvolved, using techniques developed for ensemble AMS data analysis, into HOA, OOA, NH4NO3, (NH42SO4, and NH4Cl fractions. Average single particle mass and chemistry measurements are shown to be in agreement with ensemble MS and PTOF measurements. While a significant fraction of ambient particles were internal mixtures of varying degrees, single particle measurements of chemical composition allowed the identification of time periods during which the ambient ensemble was externally mixed. In some cases the chemical composition of the particles suggested a likely source. Throughout the full sampling period, the ambient ensemble was an external mixture of combustion

8. A new method to discriminate secondary organic aerosols from different sources using high-resolution aerosol mass spectra

Directory of Open Access Journals (Sweden)

M. F. Heringa

2012-02-01

Full Text Available Organic aerosol (OA represents a significant and often major fraction of the non-refractory PM1 (particulate matter with an aerodynamic diameter da < 1 μm mass. Secondary organic aerosol (SOA is an important contributor to the OA and can be formed from biogenic and anthropogenic precursors. Here we present results from the characterization of SOA produced from the emissions of three different anthropogenic sources. SOA from a log wood burner, a Euro 2 diesel car and a two-stroke Euro 2 scooter were characterized with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS and compared to SOA from α-pinene.

The emissions were sampled from the chimney/tailpipe by a heated inlet system and filtered before injection into a smog chamber. The gas phase emissions were irradiated by xenon arc lamps to initiate photo-chemistry which led to nucleation and subsequent particle growth by SOA production.

Duplicate experiments were performed for each SOA type, with the averaged organic mass spectra showing Pearson's r values >0.94 for the correlations between the four different SOA types after five hours of aging. High-resolution mass spectra (HR-MS showed that the dominant peaks in the MS, m/z 43 and 44, are dominated by the oxygenated ions C2H3O+ and CO2+, respectively, similarly to the relatively fresh semi-volatile oxygenated OA (SV-OOA observed in the ambient aerosol. The atomic O:C ratios were found to be in the range of 0.25–0.55 with no major increase during the first five hours of aging. On average, the diesel SOA showed the lowest O:C ratio followed by SOA from wood burning, α-pinene and the scooter emissions. Grouping the fragment ions revealed that the SOA source with the highest O:C ratio had the largest fraction of small ions.

The HR data of the four sources could be clustered and separated using

9. A new method to discriminate secondary organic aerosols from different sources using high-resolution aerosol mass spectra

Directory of Open Access Journals (Sweden)

M. F. Heringa

2011-10-01

Full Text Available Organic aerosol (OA represents a significant and often major fraction of the non-refractory PM1 (particulate matter with an aerodynamic diameter da < 1 μm mass. Secondary organic aerosol (SOA is an important contributor to the OA and can be formed from biogenic and anthropogenic precursors. Here we present results from the characterization of SOA produced from the emissions of three different anthropogenic sources. SOA from a log wood burner, a Euro 2 diesel car and a two-stroke Euro 2 scooter were characterized with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS and compared to SOA from α-pinene.

The emissions were sampled from the chimney/tailpipe by a heated inlet system and filtered before injection into a smog chamber. The gas phase emissions were irradiated by xenon arc lamps to initiate photo-chemistry which led to nucleation and subsequent particle growth by SOA production.

Duplicate experiments were performed for each SOA type, with the averaged organic mass spectra in the m/z range 12–250 showing Pearson's r values >0.94 for the correlations between the different SOA types after 5 h of aging. High-resolution mass spectra (HR-MS showed that the dominant peaks in the MS, m/z 43 and 44, are dominated by the oxygenated ions C2H3O+ and CO2+, respectively, similarly to the relatively fresh semi-volatile oxidized OA (SV-OOA observed in the ambient aerosol. The atomic O : C ratios were found to be in the range of 0.25–0.55 with no major increase during the first 5 h of aging. On average, the diesel SOA showed the lowest O : C ratio followed by SOA from wood burning, α-pinene and the scooter emissions. Grouping the fragment ions based on their carbon number revealed that the SOA source with the highest O : C ratio had the largest fraction of small ions. Fragment ions

10. Glyoxal processing outside clouds: towards a kinetic modeling framework of secondary organic aerosol formation in aqueous particles

Directory of Open Access Journals (Sweden)

B. Ervens

2010-05-01

from glyoxal: (1 time scales to reach equilibrium states (as opposed to assuming instantaneous equilibrium, (2 particle pH, (3 chemical composition of the bulk aerosol, (4 particle surface composition, and (5 particle liquid water content that is mostly determined by the amount and hygroscopicity of aerosol mass and to a lesser extent by the ambient relative humidity.

Glyoxal serves as an example molecule, and the conclusions about SOA formation in aqueous particles can serve for comparative studies also of other molecules that form SOA as the result of multiphase chemical processing in aerosol water. This SOA source is currently underrepresented in atmospheric models; if included it is likely to bring SOA predictions (mass and O/C ratio into better agreement with field observations.

11. Sources and transformations of particle-bound polycyclic aromatic hydrocarbons in Mexico City

Directory of Open Access Journals (Sweden)

L. C. Marr

2005-12-01

Full Text Available Understanding sources, concentrations, and transformation of polycyclic aromatic hydrocarbons (PAHs in the atmosphere is important because of their potent mutagenicity and carcinogenicity. The measurement of particle-bound PAHs by three different methods during the Mexico City Metropolitan Area field campaign in April 2003 presents a unique opportunity for characterization of these compounds and assessment of the methods. The three methods are (1 collection and analysis of bulk samples for time-integrated gas- and particle-phase speciation by gas chromatography/mass spectrometry; (2 aerosol photoionization for fast detection of PAHs on particles' surfaces; and (3 aerosol mass spectrometry for fast analysis of size and chemical composition. This research represents the first time aerosol mass spectrometry has been used to measure ambient PAH concentrations and the first time that fast, real-time methods have been used to quantify PAHs alongside traditional filter-based measurements in an extended field campaign. Speciated PAH measurements suggest that motor vehicles and garbage and wood burning are important sources in Mexico City. The diurnal concentration patterns captured by aerosol photoionization and aerosol mass spectrometry are generally consistent. Ambient concentrations typically peak at ~110 ng m−3 during the morning rush hour and rapidly decay due to changes in source activity patterns and dilution as the boundary layer rises, although surface-bound PAH concentrations decay faster. The more rapid decrease in surface versus bulk PAH concentrations during the late morning suggests that freshly emitted combustion-related particles are quickly coated by secondary aerosol material in Mexico City's atmosphere and may also be transformed by heterogeneous reactions.

12. Study of real time detection and size distribution measurement of ultrafine aerosol with a particle growth system (PGS)

Energy Technology Data Exchange (ETDEWEB)

Rebours, A.

1994-06-29

First, the theoretical knowledge on condensation phenomena of a supersaturated vapor in a cylindrical duct where an ultrafine aerosol of nanometers size is flowing, is recalled. Then, a Particle Growth-System (PGS) of original design is developed: the aerosol is confined in a region with a uniform vapor supersaturation profile. When imperfectly filtered atmospheric air is used as source of condensation nuclei, the produced droplets are found to be monodisperse. Therefore, our PGS offers a simple method of calibrating Optical Particle Counters because the size distribution of theses droplets is controlled. After an experimental study validated by a theoretical model, we establish that, under certain supersaturation conditions, the droplet size in our PGS is a function of ultrafine particle size on which the vapor condenses. Furthermore, when the sampled aerosol is constituted of an ultrafine fraction and a fine fraction, we show that the size distribution of the droplets that come out from the PGS is bimodal too. Finally, a simple redesign of our fluids inlet system should reduce particles losses in the PGS due to brownian diffusion and, in that manner improve their detection. (author). 72 refs., 46 figs., 8 tabs., 4 appends.

13. Source apportionment of PM2.5 carbonaceous aerosol in Baghdad, Iraq

Science.gov (United States)

Hamad, Samera Hussein; Schauer, James Jay; Heo, Jongbae; Kadhim, Ahmed K. H.

2015-04-01

Baghdad is the second largest city in the Middle East and suffers from severe air quality degradation due to the high levels of the atmospheric particulate matter (PM). Limited information exists regarding the sources of PM in Baghdad, and the lack of information on sources inhibits the development of control strategies to reduce air pollution. To better understand the nature of fine particulate matter (PM2.5) in Baghdad and the Middle East, a one year sampling campaign to collect PM2.5 was conducted from September 2012 through September 2013, missing August 2013 samples due to the security situation. 24-hour integrated samples collected on a 1-in-6 day schedule were analyzed for the major components, and monthly average samples were analyzed by gas chromatography mass spectrometry (GCMS) methods to measure particle-phase organic molecular markers. The results of organic molecular markers were used in a chemical mass balance (CMB) model to quantify the sources of PM2.5 organic carbon (OC) and PM2.5 mass. Primary sources accounted for 44% of the measured PM2.5, and secondary sources were estimated to make up 28% of the measured PM2.5. Picene, a tracer of coal combustion detected in Baghdad where there is no evidence for coal combustion, can be attributed to burning crude oil and other low quality fuels in Baghdad. Source apportionment results showed that the dominant sources of the carbonaceous aerosols in Baghdad are gasoline (37 ± 6%) and diesel engines (17 ± 3%) which can be attributed to the extensive use of gasoline and diesel powered generators in Baghdad. Wood burning and residual oil combustion contributed to 5 ± 0.4 and 1 ± 0.2% respectively of OC. The unresolved sources contributed to 42 ± 19% of the OC which represented the secondary organic aerosol (SOA) and the unidentified sources.

14. Evaluation of a global aerosol microphysics model against size-resolved particle statistics in the marine atmosphere

Directory of Open Access Journals (Sweden)

D. V. Spracklen

2007-01-01

Full Text Available A statistical synthesis of marine aerosol measurements from experiments in four different oceans is used to evaluate a global aerosol microphysics model (GLOMAP. We compare the model against observed size resolved particle concentrations, probability distributions, and the temporal persistence of different size particles. We attempt to explain the observed sub-micrometre size distributions in terms of sulfate and sea spray and quantify the possible contributions of anthropogenic sulfate and carbonaceous material to the number and mass distribution. The model predicts a bimodal size distribution that agrees well with observations as a grand average over all regions, but there are large regional differences. Notably, observed Aitken mode number concentrations are more than a factor 10 higher than in the model for the N Atlantic but a factor 7 lower than the model in the NW Pacific. We also find that modelled Aitken mode and accumulation mode geometric mean diameters are generally smaller in the model by 10–30%. Comparison with observed free tropospheric Aitken mode distributions suggests that the model underpredicts growth of these particles during descent to the marine boundary layer (MBL. Recent observations of a substantial organic component of free tropospheric aerosol could explain this discrepancy. We find that anthropogenic continental material makes a substantial contribution to N Atlantic MBL aerosol, with typically 60–90% of sulfate across the particle size range coming from anthropogenic sources, even if we analyse air that has spent an average of >120 h away from land. However, anthropogenic primary black carbon and organic carbon particles (at the emission size and quantity assumed here do not explain the large discrepancies in Aitken mode number. Several explanations for the discrepancy are suggested. The lack of lower atmospheric particle formation in the model may explain low N Atlantic particle concentrations. However, the

15. Evaluation of a global aerosol microphysics model against size-resolved particle statistics in the marine atmosphere

Science.gov (United States)

Spracklen, D. V.; Pringle, K. J.; Carslaw, K. S.; Mann, G. W.; Manktelow, P.; Heintzenberg, J.

2007-04-01

A statistical synthesis of marine aerosol measurements from experiments in four different oceans is used to evaluate a global aerosol microphysics model (GLOMAP). We compare the model against observed size resolved particle concentrations, probability distributions, and the temporal persistence of different size particles. We attempt to explain the observed sub-micrometre size distributions in terms of sulfate and sea spray and quantify the possible contributions of anthropogenic sulfate and carbonaceous material to the number and mass distribution. The model predicts a bimodal size distribution that agrees well with observations as a grand average over all regions, but there are large regional differences. Notably, observed Aitken mode number concentrations are more than a factor 10 higher than in the model for the N Atlantic but a factor 7 lower than the model in the NW Pacific. We also find that modelled Aitken mode and accumulation mode geometric mean diameters are generally smaller in the model by 10-30%. Comparison with observed free tropospheric Aitken mode distributions suggests that the model underpredicts growth of these particles during descent to the marine boundary layer (MBL). Recent observations of a substantial organic component of free tropospheric aerosol could explain this discrepancy. We find that anthropogenic continental material makes a substantial contribution to N Atlantic MBL aerosol, with typically 60-90% of sulfate across the particle size range coming from anthropogenic sources, even if we analyse air that has spent an average of >120 h away from land. However, anthropogenic primary black carbon and organic carbon particles (at the emission size and quantity assumed here) do not explain the large discrepancies in Aitken mode number. Several explanations for the discrepancy are suggested. The lack of lower atmospheric particle formation in the model may explain low N Atlantic particle concentrations. However, the observed and modelled

16. Source and composition of size fractionated aerosols collected in the Central Valley

Science.gov (United States)

Allen, G.; Kelly, P. B.; Buchholz, B. A.; Clifford, A.

2013-12-01

The Central Valley in California has historically had high levels of atmospheric particulate matter (PM), resulting in significant adverse health effects. The three sources of atmospheric PM in the Central Valley are vehicle exhaust emissions, agricultural activity and residential wood burning. Ambient PM was collected during the winter of 2011 and 2012 in Davis, CA using a DRUM impact analyzer to determine the contributions of the various sources to the size fractionated aerosols. Laser desorption ionization time-of-flight mass spectrometry (LDI-TOF MS) and radiocarbon accelerator mass spectrometry (AMS) were performed on size fractionated atmospheric PM. The results show that as particle size decreases the amount of organic carbon increases. In the smallest size fraction (0.09 - 1.2 μm) the organic carbon encompasses approximately 70% of the LDI-TOF signal intensity. A comparison of the size fraction PM LDI-TOF spectra showed that there was a significant difference in the chemical composition with particle size. Three distinct chemical composition modes were observed in the LDI-TOF analysis: 0.09 to 0.34 μm, 0.34 to 0.56 μm and >0.56 μm. The particles 0.5 μm. The chemical difference in the PM is driven by the large amount of secondary organic aerosol. Dicarboxylic acids, aromatic acids and nitrated aromatics were predominately found in particles <0.34 μm. The effect on human health of these compounds needs to be further explored. The difference in the chemical composition between the respirable and larger PM needs to be considered when associating health effects with PM exposure. The radiocarbon AMS analysis showed that the size fractionated total carbonaceous particulate matter was mainly biogenic in origin, having an average fraction modern (F14C) = 0.753 × 0.006. The F14C from both sample collections were similar and there wasn't a significant change in fraction modern as particle size decreased. The high fraction modern in the small PM points to the

17. Hygroscopicity of aerosol particles and CCN activity of nearly hydrophobic particles in the urban atmosphere over Japan during summer

Science.gov (United States)

Ogawa, Shuhei; Setoguchi, Yoshitaka; Kawana, Kaori; Nakayama, Tomoki; Ikeda, Yuka; Sawada, Yuuki; Matsumi, Yutaka; Mochida, Michihiro

2016-06-01

We investigated the hygroscopicity of 150 nm particles and the number-size distributions and the cloud condensation nuclei (CCN) activity of nearly hydrophobic particles in aerosols over Nagoya, Japan, during summer. We analyzed the correlations between the number concentrations of particles in specific hygroscopic growth factor (g) ranges and the mass concentrations of chemical components. This analysis suggests the association of nearly hydrophobic particles with hydrocarbon-like organic aerosol, elemental carbon and semivolatile oxygenated organic aerosol (SV-OOA), that of less hygroscopic particles with SV-OOA and nitrate and that of more hygroscopic particles with low-volatile oxygenated organic aerosol (LV-OOA) and sulfate. The hygroscopicity parameter (κ) of organics was derived based on the g distributions and chemical composition of 150 nm particles. The κ of the organics correlated positively with the fraction of the total organic mass spectral signal at m/z 44 and the volume fraction of the LV-OOA to the organics, indicating that organics with highly oxygenated structures including carboxylic acid groups contribute to the water uptake. The number-size distributions of the nearly hydrophobic particles with g around 1.0 and 1.1 correlated with the mass concentrations of chemical components. The results show that the chemical composition of the particles with g around 1.0 was different between the Aitken mode and the accumulation mode size ranges. An analysis for a parameter Fmax of the curves fitted to the CCN efficiency spectra of the particles with g around 1.0 suggests that the coating by organics associated with SV-OOA elevated the CCN activity of these particles.

18. Real-time detection of individual secondary organic aerosol particle from photooxidation of toluene using aerosol time of flight mass spectrometer

Institute of Scientific and Technical Information of China (English)

WANG Zhenya; HAO Liqing; ZHOU Liuzhu; GUO Xiaoyong; ZHAO Wenwu; FANG Li; ZHANG Weijun

2006-01-01

Photooxidation of the aromatic hydrocarbon toluene and its subsequent reactions were carried out using UV-irradiation of toluene/CH3ONO/NO/air mixtures in a home-made smog chamber.The secondary organic aerosols could be formed after those oxidation products of semi-volatile or-ganic compounds were partitioned between gas phase and particle phase. The aerosol time of flight mass spectrometer (ATOFMS) was used to measure size and molecular composition of individual secondary organic aerosol particle. Size distribution and chemical composition of secondary organic aerosol were got in real time.

19. Source attribution of aerosol size distributions and model evaluation using Whistler Mountain measurements and GEOS-Chem-TOMAS simulations

Science.gov (United States)

D'Andrea, S. D.; Ng, J. Y.; Kodros, J. K.; Atwood, S. A.; Wheeler, M. J.; Macdonald, A. M.; Leaitch, W. R.; Pierce, J. R.

2016-01-01

Remote and free-tropospheric aerosols represent a large fraction of the climatic influence of aerosols; however, aerosol in these regions is less characterized than those polluted boundary layers. We evaluate aerosol size distributions predicted by the GEOS-Chem-TOMAS global chemical transport model with online aerosol microphysics using measurements from the peak of Whistler Mountain, British Columbia, Canada (2182 m a.s.l., hereafter referred to as Whistler Peak). We evaluate the model for predictions of aerosol number, size, and composition during periods of free-tropospheric (FT) and boundary-layer (BL) influence at "coarse" 4° × 5° and "nested" 0.5° × 0.667° resolutions by developing simple FT/BL filtering techniques. We find that using temperature as a proxy for upslope flow (BL influence) improved the model-measurement comparisons. The best threshold temperature was around 2 °C for the coarse simulations and around 6 °C for the nested simulations, with temperatures warmer than the threshold indicating boundary-layer air. Additionally, the site was increasingly likely to be in cloud when the measured relative humidity (RH) was above 90 %, so we do not compare the modeled and measured size distributions during these periods. With the inclusion of these temperature and RH filtering techniques, the model-measurement comparisons improved significantly. The slope of the regression for N80 (the total number of particles with particle diameter, Dp, > 80 nm) in the nested simulations increased from 0.09 to 0.65, R2 increased from 0.04 to 0.46, and log-mean bias improved from 0.95 to 0.07. We also perform simulations at the nested resolution without Asian anthropogenic emissions and without biomass-burning emissions to quantify the contribution of these sources to aerosols at Whistler Peak (through comparison with simulations with these emissions on). The long-range transport of Asian anthropogenic aerosol was found to be significant throughout all particle

20. Size distribution of the secondary organic aerosol particles from the photooxidation of toluene

Institute of Scientific and Technical Information of China (English)

HAO Li-qing; WANG Zhen-ya; HUANG Ming-qiang; PEI Shi-xin; YANG Yong; ZHANG Wei-jun

2005-01-01

In a smog chamber, the photooxidation of toluene was initiated by hydroxyl radical (OH·) under different experimental conditions. The size distribution of secondary organic aerosol(SOA) particles from the above reaction was measured using aerodynamic particle sizer spectrometer. It was found from our experimental results that the number of SOA particles increased with increasing the concentration of toluene. As the reaction time prolonged, the sum of SOA particles was also increased. After a reaction time of 130 min,the concentration of secondary organic aerosol particles would be kept constant at 2300 particles/cm3 . Increasing illumination power of blacklamps could significantly induce a higher concentration of secondary organic aerosol particle. The density of SOA particles would also be increased with increasing concentration of CH3 ONO, however, it would be decreased as soon as the concentration of CH3 ONO was larger than 225.2 ppm. Nitrogen oxide with initial concentration higher than 30.1 ppm was also found to have little effect on the formation of secondary organic aerosol.

1. An overview of differential mobility analyzers for size classification of nanometer-sized aerosol particles

Directory of Open Access Journals (Sweden)

Nakorn Tippayawong

2008-03-01

Full Text Available Size classification of nanoparticles is an important process in the electrical mobility particle size analyzer. The differential mobility analyzer (DMA is one of the most commonly used devices for classifying and measuring nanometersized aerosol particles between 1 nm to 1 μm in diameter, based on their electrical mobility. The DMA can be described as an assembly of two concentrically cylindrical electrodes with an air gap between the walls. In the DMA, air and aerosol flows enter from one end, pass through the annulus and exit the other end. An electric field is applied between the inner and outer electrodes. Particles having a specific mobility exit with the monodisperse air flow through a small slit located at the bottom of the inner electrode. These particles are transferred to a particle counter to determine the particle number concentration. In the past several decades, there have been numerous extensive studies and developments on the DMA. Nonetheless, they are different in terms of specific applications, construction, particle size range, as well as time response and resolution. The purpose of this article is to provide an overview of the state-of-the-art existing cylindrical DMAs for aerosol particle size classification as well as for the generation of monodisperse aerosol in nanometer size range. A description of the operating principles, detailed physical characteristics of these DMAs, including the single-channel and multi-channel DMAs, as well as some examples of applications to nanotechnology are given.

2. Quantification of bitumen particles in aerosol and soil samples using HP-GPC

DEFF Research Database (Denmark)

Fauser, Patrik; Tjell, Jens Christian; Mosbæk, Hans;

2000-01-01

A method for identifying and quantifying bitumen particles, generated from the wear of roadway asphalts, in aerosol and soil samples has been developed. Bitumen is found to be the only contributor to airborne particles containing organic molecules with molecular weights larger than 2000 g pr. mol...

3. Tire-tread and bitumen particle concentrations in aerosol and soil samples

DEFF Research Database (Denmark)

Fauser, Patrik; Tjell, Jens Christian; Mosbæk, Hans;

2002-01-01

ire and bitumen particle concentrations are determined in aerosol and soil samples. They each constitute about 5 wt-% of the total suspended particulate matter (TSP) in inner city air, collected with a Berner low pressure impactor, 5 m from a road. The particle size distribution shows that 92% of...

4. Particle Morphology and Size Results from the Smoke Aerosol Measurement Experiment-2

Science.gov (United States)

Urban, David L.; Ruff, Gary A.; Greenberg, Paul S.; Fischer, David; Meyer, Marit; Mulholland, George; Yuan, Zeng-Guang; Bryg, Victoria; Cleary, Thomas; Yang, Jiann

2012-01-01

Results are presented from the Reflight of the Smoke Aerosol Measurement Experiment (SAME-2) which was conducted during Expedition 24 (July-September 2010). The reflight experiment built upon the results of the original flight during Expedition 15 by adding diagnostic measurements and expanding the test matrix. Five different materials representative of those found in spacecraft (Teflon, Kapton, cotton, silicone rubber and Pyrell) were heated to temperatures below the ignition point with conditions controlled to provide repeatable sample surface temperatures and air flow. The air flow past the sample during the heating period ranged from quiescent to 8 cm/s. The smoke was initially collected in an aging chamber to simulate the transport time from the smoke source to the detector. This effective transport time was varied by holding the smoke in the aging chamber for times ranging from 11 to 1800 s. Smoke particle samples were collected on Transmission Electron Microscope (TEM) grids for post-flight analysis. The TEM grids were analyzed to observe the particle morphology and size parameters. The diagnostics included a prototype two-moment smoke detector and three different measures of moments of the particle size distribution. These moment diagnostics were used to determine the particle number concentration (zeroth moment), the diameter concentration (first moment), and the mass concentration (third moment). These statistics were combined to determine the diameter of average mass and the count mean diameter and, by assuming a log-normal distribution, the geometric mean diameter and the geometric standard deviations can also be calculated. Overall the majority of the average smoke particle sizes were found to be in the 200 nm to 400 nm range with the quiescent cases producing some cases with substantially larger particles.

5. Chemical composition, sources, and processes of urban aerosols during summertime in Northwest China: insights from High Resolution Aerosol Mass Spectrometry

Directory of Open Access Journals (Sweden)

J. Xu

2014-06-01

Full Text Available An aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS was deployed along with a Scanning Mobility Particle Sizer (SMPS and a Multi Angle Absorption Photometers (MAAP to measure the temporal variations of the mass loading, chemical composition, and size distribution of sub-micrometer particulate matter (PM1 in Lanzhou, northwest China, during 12 July–7 August 2012. The average PM1 mass concentration including non-refractory PM1 (NR-PM1 measured by HR-ToF-AMS and black carbon (BC measured by MAAP during this study was 24.5 μg m−3 (ranging from 0.86 to 105μg m−3, with a mean composition consisting of 47% organics, 16% sulfate, 12% BC, 11% ammonium, 10% nitrate, and 4% chloride. The organics was consisted of 70% carbon, 21% oxygen, 8% hydrogen, and 1% nitrogen, with the average oxygen-to-carbon ratio (O / C of 0.33 and organic mass-to-carbon ratio (OM / OC of 1.58. Positive matrix factorization (PMF of the high-resolution mass spectra of organic aerosols (OA identified four distinct factors which represent, respectively, two primary OA (POA emission sources (traffic and food cooking and two secondary OA (SOA types – a fresher, semi-volatile oxygenated OA (SV-OOA and a more aged, low-volatility oxygenated OA (LV-OOA. Traffic-related hydrocarbon-like OA (HOA and BC displayed distinct diurnal patterns both with peak at ~07:00–11:00 (BJT: UTC +8 corresponding to the morning rush hours, while cooking OA (COA peaked during three meal periods. The diurnal profiles of sulfate and LV-OOA displayed a broad peak between ∼07:00–15:00, while those of nitrate, ammonium, and SV-OOA showed a narrower peak at ~08:00–13:00. The later morning and early afternoon peak in the diurnal profiles of secondary aerosol species was likely caused by mixing down of pollutants aloft, which were likely produced in the residual layer decoupled from the boundary layer during night time. The mass spectrum of SV-OOA also showed similarity

6. Ice Nucleating Particle Properties in the Saharan Air Layer Close to the Dust Source

Science.gov (United States)

Boose, Y.; Garcia, I. M.; Rodríguez, S.; Linke, C.; Schnaiter, M.; Nickovic, S.; Lohmann, U.; Kanji, Z. A.; Sierau, B.

2015-12-01

In August 2013 and 2014 measurements of ice nucleating particle (INP) concentrations, aerosol particle size distributions, chemistry and fluorescence were conducted at the Izaña Atmospheric Observatory located at 2373 m asl on Tenerife, west off the African shore. During summer, the observatory is frequently within the Saharan Air Layer and thus often exposed to dust. Absolute INP concentrations and activated fractions at T=-40 to -15°C and RHi=100-150 % were measured. In this study, we discuss the in-situ measured INP properties with respect to changes in the chemical composition, the biological content, the source regions as well as transport pathways and thus aging processes of the dust aerosol. For the first time, ice crystal residues were also analyzed with regard to biological content by means of their autofluorescence signal close to a major dust source region. Airborne dust samples were collected with a cyclone for additional offline analysis in the laboratory under similar conditions as in the field. Both, in-situ and offline dust samples were chemically characterized using single-particle mass spectrometry. The DREAM8 dust model extended with dust mineral fractions was run to simulate meteorological and dust aerosol conditions for ice nucleation. Results show that the background aerosol at Izaña was dominated by carbonaceous particles, which were hardly ice-active under the investigated conditions. When Saharan dust was present, INP concentrations increased by up to two orders of magnitude even at water subsaturated conditions at T≤-25°C. Differences in the ice-activated fraction were found between different dust periods which seem to be linked to variations in the aerosol chemical composition (dust mixed with changing fractions of sea salt and differences in the dust aerosol itself). Furthermore, two biomass burning events in 2014 were identified which led to very low INP concentrations under the investigated temperature and relative humidity

7. Complex anthropogenic sources of platinum group elements in aerosols on Cape Cod, USA.

Science.gov (United States)

Sen, Indra S; Peucker-Ehrenbrink, Bernhard; Geboy, Nicholas

2013-09-17

Platinum group elements (PGE) of anthropogenic origin have been reported in rainwater, snow, roadside soil and vegetation, industrial waste, and urban airborne particles around the world. As recent studies have shown that PGE are bioavailable in the environment and pose health risks at chronic levels, the extent of PGE pollution is of global concern. In this study, we report PGE concentrations and osmium isotope ((187)Os/(188)Os) ratios of airborne particles (particulate matter, PM10) collected in Woods Hole, a small coastal village on Cape Cod, Massachusetts, U.S.A. The sampling site is more than 100 km away from the nearest urban centers (Boston, Providence) and has no large industrial emission center within a 30 km radius. The study reveals that, although PGE concentrations in rural airborne particulate matter are orders of magnitude lower than in urban aerosols, 69% of the total osmium is of anthropogenic origin. Anthropogenic PGE signatures in airborne particles are thus not restricted to large cities with high traffic flows and substantial industries; they can also be found in rural environments. We further conclude that the combination of Pt/Rh concentration ratios and (187)Os/(188)Os composition can be used to trace PGE sources. The Pt/Rh and (187)Os/(188)Os composition of Woods Hole aerosols indicate that the anthropogenic PGE fraction is primarily sourced from ore smelting processes, with possible minor contributions from fossil fuel burning and automobile catalyst-derived materials. Our results further substantiate the use of (187)Os/(188)Os in source apportionment studies on continental scales.

8. LOAC (Light Optical Particle Counter): a new small aerosol counter with particle characterization capabilities for surface and airborne measurements

Science.gov (United States)

Renard, Jean-Baptiste; Berthet, Gwenael; Jégou, Fabrice; Jeannot, Matthieu; Jourdain, Line; Dulac, François; Mallet, Marc; Dupont, Jean-Charles; Thaury, Claire; Tonnelier, Thierry; Verdier, Nicolas; Charpentier, Patrick

2013-04-01

The determination of the size distribution of tropospheric and stratospheric aerosols with conventional optical counters is difficult when different natures of particles are present (droplets, soot, mineral dust, secondary organic or mineral particles...). Also, a light and cheap aerosol counter that can be used at ground, onboard drones or launched under all kinds of atmospheric balloons can be very useful during specific events as volcanic plumes, desert dust transport or local pollution episodes. These goals can be achieved thanks to a new generation of aerosol counter, called LOAC (Light Optical Aerosol Counter). The instrument was developed in the frame of a cooperation between French scientific laboratories (CNRS), the Environnement-SA and MeteoModem companies and the French Space Agency (CNES). LOAC is a small optical particle counter/sizer of ~250 grams, having a low electrical power consumption. The measurements are conducted at two scattering angles. The first one, at 12°, is used to determine the aerosol particle concentrations in 19 size classes within a diameter range of 0.3-100 micrometerers. At such an angle close to forward scattering, the signal is much more intense and the measurements are the least sensitive to the particle nature. The second angle is at 60°, where the scattered light is strongly dependent on the particle refractive index and thus on the nature of the aerosols. The ratio of the measurements at the two angles is used to discriminate between the different types of particles dominating the nature of the aerosol particles in the different size classes. The sensor particularly discriminates wet or liquid particles, soil dust and soot. Since 2011, we have operated LOAC in various environments (Arctic, Mediterranean, urban and peri-urban…) under different kinds of balloons including zero pressure stratospheric, tethered, drifting tropospheric, and meteorological sounding balloons. For the last case, the total weight of the gondola

9. Characterization of aerosol particles from grass mowing by joint deployment of ToF-AMS and ATOFMS instruments

Science.gov (United States)

Drewnick, Frank; Dall'Osto, Manuel; Harrison, Roy

During a measurement campaign at a semi-urban/industrial site a grass-cutting event was observed, when the lawn in the immediate surrounding of the measurement site was mowed. Using a wide variety of state-of-the-art aerosol measurement technology allowed a broad characterization of the aerosol generated by the lawn mowing. The instrumentation included two on-line aerosol mass spectrometers: an Aerodyne Time-of-Flight Aerosol Mass Spectrometer (ToF-AMS) and a TSI Aerosol Time-of-Flight Mass Spectrometer (ATOFMS); in addition, a selection of on-line aerosol concentration and size distribution instruments (OPC, APS, SMPS, CPC, FDMS-TEOM, MAAP) was deployed. From comparison of background aerosol measurements during most of the day with the aerosol measured during the lawn mowing, the grass cutting was found to generate mainly two different types of aerosol particles: an intense ultrafine particle mode (1 h average: 4 μg m -3) of almost pure hydrocarbon-like organics and a distinct particle mode in the upper sub-micrometer size range containing particles with potassium and nitrogen-organic compounds. The ultrafine particles are probably lubricating oil particles from the lawn mower exhaust; the larger particles are swirled-up plant debris particles from the mowing process. While these particle types were identified in the data from the two mass spectrometers, the on-line aerosol concentration and size distribution data support these findings. The results presented here show that the combination of quantitative aerosol particle ensemble mass spectrometry (ToF-AMS) and single particle mass spectrometry (ATOFMS) provides much deeper insights into the nature of the aerosol properties than each of the instruments could do alone. Therefore a combined deployment of both types of instruments is strongly recommended.

10. Measurements of Ultra-fine and Fine Aerosol Particles over Siberia: Large-scale Airborne Campaigns

Science.gov (United States)

Arshinov, Mikhail; Paris, Jean-Daniel; Stohl, Andreas; Belan, Boris; Ciais, Philippe; Nédélec, Philippe

2010-05-01

In this paper we discuss the results of in-situ measurements of ultra-fine and fine aerosol particles carried out in the troposphere from 500 to 7000 m in the framework of several International and Russian State Projects. Number concentrations of ultra-fine and fine aerosol particles measured during intensive airborne campaigns are presented. Measurements carried over a great part of Siberia were focused on particles with diameters from 3 to 21 nm to study new particle formation in the free/upper troposphere over middle and high latitudes of Asia, which is the most unexplored region of the Northern Hemisphere. Joint International airborne surveys were performed along the following routes: Novosibirsk-Salekhard-Khatanga-Chokurdakh-Pevek-Yakutsk-Mirny-Novosibirsk (YAK-AEROSIB/PLARCAT2008 Project) and Novosibirsk-Mirny-Yakutsk-Lensk-Bratsk-Novosibirsk (YAK-AEROSIB Project). The flights over Lake Baikal was conducted under Russian State contract. Concentrations of ultra-fine and fine particles were measured with automated diffusion battery (ADB, designed by ICKC SB RAS, Novosibirsk, Russia) modified for airborne applications. The airborne ADB coupled with CPC has an additional aspiration unit to compensate ambient pressure and changing flow rate. It enabled to classify nanoparticles in three size ranges: 3-6 nm, 6-21 nm, and 21-200 nm. To identify new particle formation events we used similar specific criteria as Young et al. (2007): (1) N3-6nm >10 cm-3, (2) R1=N3-6/N621 >1 and R2=N321/N21200 >0.5. So when one of the ratios R1 or R2 tends to decrease to the above limits the new particle formation is weakened. It is very important to notice that space scale where new particle formation was observed is rather large. All the events revealed in the FT occurred under clean air conditions (low CO mixing ratios). Measurements carried out in the atmospheric boundary layer over Baikal Lake did not reveal any event of new particle formation. Concentrations of ultra

11. The formation of aerosol particles during combustion of biomass and waste. Final report

Energy Technology Data Exchange (ETDEWEB)

Hjerrild Zeuthen, J.

2007-05-15

This thesis describes the formation of aerosol particles during combustion of biomass and waste. The formation of aerosol particles is investigated by studying condensation of alkali salts from synthetic flue gasses in a laboratory tubular furnace. In this so-called laminar flow aerosol condenser-furnace gaseous alkali chlorides are mixed with sulphur dioxide, water vapour and oxygen. At high temperatures the alkali chloride reacts with sulphur dioxide to form alkali sulphate. During subsequent cooling of the synthetic flue gas the chlorides and sulphates condense either as deposits on walls or on other particles or directly from the gas phase by homogenous nucleation. A previously developed computer code for simulation of one-component nucleation of particles in a cylindrical laminar flow is extended to include a homogeneous gas phase reaction to produce gaseous alkali sulphate. The formation of aerosol particles during full-scale combustion of wheat straw is investigated in a 100 MW grate-fired boiler. Finally, aerosols from incineration of waste are investigated during full-scale combustion of municipal waste in a 22 MW grate-fired unit. (BA)

12. [Concentration and Particle Size Distribution of Microbiological Aerosol During Haze Days in Beijing].

Science.gov (United States)

Hu, Ling-fei; Zhang, Ke; Wang, Hong-bao; Li, Na; Wang, Jie; Yang, Wen-hui; Yin, Zhe; Jiao, Zhou-guang; Wen, Zhan-bo; Li, Jin-song

2015-09-01

In this study, we evaluated the bacterial, fungal aerosol concentration, and particle size distribution using microbiological aerosol sampler, and analyzed the particles count concentration of PM1.0, PM2.5, PM5.0 and PM10.0 using aerodynamic particle sizer during clear and haze days in Beijing during Jan 8th, 2013 to Feb 4th, 2013. The concentration of bacterial, fungal aerosol, air particulate matter and aerosol distribution were compared between haze days and clear days. Our results indicated that the proportion of fungal particles smaller than 5 micron, which could deposit in lungs or deeper regions, was much higher than bacterial particles. The biological concentration of bacteria and fungi were higher in clear days than in haze days, and there was no statistic difference of the microbiological aerosol distribution. The concentration of air particulate matter were higher in haze days than in clear days, PM10 was the main particulate matters both in clear days and haze days.

13. Stratospheric aerosol particle size information in Odin-OSIRIS limb scatter spectra

Directory of Open Access Journals (Sweden)

L. A. Rieger

2013-06-01

Full Text Available The Optical Spectrograph and InfraRed Imaging System (OSIRIS on-board the Odin satellite has now taken over a decade of limb scatter measurements that have been used to retrieve the Version 5 stratospheric aerosol extinction product. This product is retrieved using a representative particle size distribution to calculate scattering cross sections and scattering phase functions for the forward model calculations. In this work the information content of OSIRIS measurements with respect to stratospheric aerosol is systematically examined for the purpose of retrieving particle size information along with the extinction coefficient. The benefit of using measurements at different wavelengths and scattering angles in the retrieval is studied and it is found that incorporation of the 1530 nm radiance measurement is key for a robust retrieval of particle size information. It is also found that using OSIRIS measurements at different solar geometries simultaneously provides little additional benefit. Based on these results, an improved aerosol retrieval algorithm is developed that couples the retrieval of aerosol extinction and mode radius of a log-normal particle size distribution. Comparison of these results with coincident measurements from SAGE III show agreement in retrieved extinction to within approximately 10% over the bulk of the aerosol layer, which is comparable to Version 5. The retrieved particle size, when converted to Ångström coefficient, shows good qualitative agreement with SAGE II measurements made at somewhat shorter wavelengths.

14. Fluorescence from atmospheric aerosol detected by a lidar indicates biogenic particles in the lowermost stratosphere

Directory of Open Access Journals (Sweden)

F. Immler

2005-01-01

Full Text Available With a lidar system that was installed in Lindenberg/Germany, we observed in June 2003 an extended aerosol layer at 13km altitude in the lowermost stratosphere. This layer created an inelastic backscatter signal that we detected with a water vapour Raman channel, but that was not produced by Raman scattering. Also, we find evidence for inelastic scattering from a smoke plume from a forest fire that we observed in the troposphere. We interpret the unexpected properties of these aerosols as fluorescence induced by the laser beam at organic components of the aerosol particles. Fluorescence from ambient aerosol had not yet been considered detectable by lidar systems. However, organic compounds such as polycyclic aromatic hydrocarbons sticking to the aerosol particles, or bioaerosol such as bacteria, spores or pollen fluoresce when excited with UV-radiation in a way that is detectable by our lidar system. Therefore, we conclude that fluorescence from organic material released by biomass burning creates, inelastic backscatter signals that we measured with our instrument and thus demonstrate a new and powerful way to characterize aerosols by a remote sensing technique. The stratospheric aerosol layer that we have observed in Lindenberg for three consecutive days is likely to be a remnant from Siberian forest fire plumes lifted across the tropopause and transported around the globe.

15. The response of reworked aerosols to climate through estimation of inter-particle forces

OpenAIRE

2016-01-01

This paper describes the first use of inter-particle force measurement in reworked aerosols to better understand the mechanics of dust deflation and its consequent ecological ramifications. Dust is likely to carry hydrocarbons and micro-organisms including human pathogens and cultured microbes and thereby is a threat to plants, animals and human. Present-day global aerosol emissions are substantially greater than in 1850; however, the projected influx rates are highly disputable. This uncerta...

16. Explaining global surface aerosol number concentrations in terms of primary emissions and particle formation

Directory of Open Access Journals (Sweden)

D. V. Spracklen

2010-05-01

Full Text Available We synthesised observations of total particle number (CN concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300–2000 cm−3 in the marine boundary layer and free troposphere (FT and 1000–10 000 cm−3 in the continental boundary layer (BL. Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2–10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R2=0.46 but fail to explain the observed seasonal cycle (R2=0.1. The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=−88% unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=−25%. Simulated CN concentrations in the continental BL were also biased low (NMB=−74% unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J, proportional to gas-phase sulfuric acid concentration to the power one or kinetic-type mechanism (J proportional to sulfuric acid to the power two with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R2=0.3 than by increasing the number emission from primary anthropogenic sources (R2=0.18. The nucleation constants that resulted in best overall match between model and observed CN concentrations were

17. Organic matter and non-refractory aerosol over the remote Southeast Pacific: oceanic and combustion sources

Directory of Open Access Journals (Sweden)

L. M. Shank

2012-01-01

Full Text Available Submicron aerosol physical and chemical properties in remote marine air were measured from aircraft over the Southeast Pacific during VOCALS-REx in 2008 and the North Pacific during IMPEX in 2006, and aboard a ship in the Equatorial Pacific in 2009. A High Resolution – Particle Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS measured non-refractory submicron aerosol composition during all campaigns. Sulfate (SO4 and organics (Org, during VOCALS and the cruise show lower absolute values than those reported for previous "clean air" studies. In the marine boundary layer, average concentrations for SO4 were 0.52 μg m−3 for the VOCALS region and 0.85 μg m−3 for the equatorial region while average Org concentrations were 0.10 and 0.07 μg m−3, respectively. Campaign average Org/SO4 ratios were 0.19 (VOCALS and 0.08 (equatorial Pacific. Black carbon (BC measurements from a single particle soot photometer (SP2 and carbon monoxide (CO concentrations over the Southeast Pacific provided sensitive indicators of pollution. CO and BC were used to identify the least polluted air, which had average concentrations of SO4 and Org of 0.14 and 0.01 μg m−3, respectively, with an average Org/SO4 of 0.08. Data from IMPEX was constrained to similar clean air criterion, and resulted in an average Org/SO4 ratio of 0.19. Under the cleanest MBL conditions during VOCALS, identified by CO below 61 ppbv, a robust linear relationship between Org and BC concentrations revealed that even at very low pollution levels, combustion sources dominated organic aerosol, suggesting little to no marine source of submicrometer Org to the atmosphere over the eastern South Pacific. This means marine organics cannot be identified by merely setting a standard for background conditions below which anthropogenic influence can be disregarded. Other methods must be used

18. Experimental and modeling studies on number and size spectrum evolutions of aerosol particles within a chamber

Institute of Scientific and Technical Information of China (English)

SUN Zai; HUANG Zhen; WANG JiaSong

2007-01-01

A size-specific aerosol dynamic model is set up to predict the evolution of particle number concentration within a chamber. Particle aggregation is based on the theory of Brownian coagulation, and the model not only comprises particle loss due to coagulation, but also considers the formation of large particles by collision. To validate the model, three different groups of chamber experiments with SMPS (Scanning Mobility Particle Sizer) are conducted. The results indicate that the advantage of the model over the past simple size bin model is its provision of detailed information of size spectrum evolution,and the results can be used to analyze the variations of number concentration and CMD (Count Median Diameter). Furthermore, some aerosol dynamic mechanisms that cannot be measured by instrument can be analyzed by the model simulation, which is significant for better understanding the removal and control mechanisms of ultrafine particles.

19. Mixing state of particles with secondary species by single particle aerosol mass spectrometer in an atmospheric pollution event

Science.gov (United States)

Xu, Lingling; Chen, Jinsheng

2016-04-01

Single particle aerosol mass spectrometer (SPAMS) was used to characterize size distribution, chemical composition, and mixing state of particles in an atmospheric pollution event during 20 Oct. - 5 Nov., 2015 in Xiamen, Southeast China. A total of 533,012 particle mass spectra were obtained and clustered into six groups, comprising of industry metal (4.5%), dust particles (2.6%), carbonaceous species (70.7%), K-Rich particles (20.7%), seasalt (0.6%) and other particles (0.9%). Carbonaceous species were further divided into EC (70.6%), OC (28.5%), and mixed ECOC (0.9%). There were 61.7%, 58.3%, 4.0%, and 14.6% of particles internally mixed with sulfate, nitrate, ammonium and C2H3O, respectively, indicating that these particles had undergone significant aging processing. Sulfate was preferentially mixed with carbonaceous particles, while nitrate tended to mix with metal-containing and dust particles. Compared to clear days, the fractions of EC-, metal- and dust particles remarkably increased, while the fraction of OC-containing particles decreased in pollution days. The mixing state of particles, excepted for OC-containing particles with secondary species was much stronger in pollution days than that in clear days, which revealed the significant influence of secondary particles in atmospheric pollution. The different activity of OC-containing particles might be related to their much smaller aerodynamic diameter. These results could improve our understanding of aerosol characteristics and could be helpful to further investigate the atmospheric process of particles.

20. Applications of aerosol model in the reactor containment

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2014-10-01

For spatially homogeneous aerosol of uniform chemical composition, the aerosol dynamic equation is solved in closed volume to simulate the radionuclide particle transport in the containment. The effects of initial conditions on the aerosol distribution, boundary layer thickness and the aerosol behaviour under source reinforcement (external source are considered.

1. Internally mixed soot, sulfates, and organic matter in aerosol particles from Mexico City

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2008-11-01

Full Text Available Soot particles, which are aggregated carbonaceous spherules with graphitic structures, are major aerosol constituents that result from burning of fossil fuel, biofuel, and biomass. Their properties commonly change through reaction with other particles or gases, resulting in complex internal mixtures. Using a transmission electron microscope (TEM for both imaging and chemical analysis, we measured ~8000 particles (25 samples with aerodynamic diameters from 0.05 to 0.3 μm that were collected in March 2006 from aircraft over Mexico City (MC and adjacent areas. Most particles are coated, consist of aggregates, or both. For example, almost all analyzed particles contain S and 70% also contain K, suggesting coagulation and condensation of sulfates and particles derived from biomass and biofuel burning. In the MC plumes, over half of all particles contained soot coated by organic matter and sulfates. The median value of the soot volume fraction in such coated particles is about 15%. In contrast to the assumptions used in many climate models, the soot particles did not become compact even when coated. Moreover, about 80% by volume of the particles consisting of organic matter with sulfate also contained soot, indicating the important role of soot in the formation of secondary aerosol particles. Coatings on soot particles can amplify their light absorption, and coagulation with sulfates changes their hygroscopic properties, resulting in shorter lifetimes. Through changes in their optical and hygroscopic properties, internally mixed soot particles have a greater effect on the regional climate of MC than uncoated soot particles.

2. Individual aerosol particles in ambient and updraft conditions below convective cloud bases in the Oman mountain region

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Semeniuk, T. A.; Bruintjes, R. T.; Salazar, V.; Breed, D. W.; Jensen, T. L.; Buseck, P. R.

2014-03-01

An airborne study of cloud microphysics provided an opportunity to collect aerosol particles in ambient and updraft conditions of natural convection systems for transmission electron microscopy (TEM). Particles were collected simultaneously on lacey carbon and calcium-coated carbon (Ca-C) TEM grids, providing information on particle morphology and chemistry and a unique record of the particle's physical state on impact. In total, 22 particle categories were identified, including single, coated, aggregate, and droplet types. The fine fraction comprised up to 90% mixed cation sulfate (MCS) droplets, while the coarse fraction comprised up to 80% mineral-containing aggregates. Insoluble (dry), partially soluble (wet), and fully soluble particles (droplets) were recorded on Ca-C grids. Dry particles were typically silicate grains; wet particles were mineral aggregates with chloride, nitrate, or sulfate components; and droplets were mainly aqueous NaCl and MCS. Higher numbers of droplets were present in updrafts (80% relative humidity (RH)) compared with ambient conditions (60% RH), and almost all particles activated at cloud base (100% RH). Greatest changes in size and shape were observed in NaCl-containing aggregates (>0.3 µm diameter) along updraft trajectories. Their abundance was associated with high numbers of cloud condensation nuclei (CCN) and cloud droplets, as well as large droplet sizes in updrafts. Thus, compositional dependence was observed in activation behavior recorded for coarse and fine fractions. Soluble salts from local pollution and natural sources clearly affected aerosol-cloud interactions, enhancing the spectrum of particles forming CCN and by forming giant CCN from aggregates, thus, making cloud seeding with hygroscopic flares ineffective in this region.

3. Mixing state of aerosols and direct observation of carbonaceous and marine coatings on African dust by individual particle analysis

Science.gov (United States)

Deboudt, Karine; Flament, Pascal; ChoëL, Marie; Gloter, Alexandre; Sobanska, Sophie; Colliex, Christian

2010-12-01

The mixing state of aerosols collected at M'Bour, Senegal, during the Special Observing Period conducted in January-February 2006 (SOP-0) of the African Monsoon Multidisciplinary Analysis project (AMMA), was studied by individual particle analysis. The sampling location on the Atlantic coast is particularly adapted for studying the mixing state of tropospheric aerosols since it is (1) located on the path of Saharan dust plumes transported westward over the northern tropical Atlantic, (2) influenced by biomass burning events particularly frequent from December to March, and (3) strongly influenced by anthropogenic emissions from polluted African cities. Particle size, morphology, and chemical composition were determined for 12,672 particles using scanning electron microscopy (automated SEM-EDX). Complementary analyses were performed using transmission electron microscopy combined with electron energy loss spectrometry (TEM-EELS) and Raman microspectrometry. Mineral dust and carbonaceous and marine compounds were predominantly found externally mixed, i.e., not present together in the same particles. Binary internally mixed particles, i.e., dust/carbonaceous, carbonaceous/marine, and dust/marine mixtures, accounted for a significant fraction of analyzed particles (from 10.5% to 46.5%). Western Sahara was identified as the main source of mineral dust. Two major types of carbonaceous particles were identified: "tar balls" probably coming from biomass burning emissions and soot from anthropogenic emissions. Regarding binary internally mixed particles, marine and carbonaceous compounds generally formed a coating on mineral dust particles. The carbonaceous coating observed at the particle scale on African dust was evidenced by the combined use of elemental and molecular microanalysis techniques, with the identification of an amorphous rather than crystallized carbon structure.

4. Quantitative evaluation of emission controls on primary and secondary organic aerosol sources during Beijing 2008 Olympics

Science.gov (United States)

Guo, S.; Hu, M.; Guo, Q.; Zhang, X.; Schauer, J. J.; Zhang, R.

2013-08-01

To assess the primary and secondary sources of fine organic aerosols after the aggressive implementation of air pollution controls during the 2008 Beijing Olympic Games, 12 h PM2.5 values were measured at an urban site at Peking University (PKU) and an upwind rural site at Yufa during the CAREBEIJING-2008 (Campaigns of Air quality REsearch in BEIJING and surrounding region) summer field campaign. The average PM2.5 concentrations were 72.5 ± 43.6 μg m-3 and 64.3 ± 36.2 μg m-3 (average ± standard deviation, below as the same) at PKU and Yufa, respectively, showing the lowest concentrations in recent years. Combining the results from a CMB (chemical mass balance) model and secondary organic aerosol (SOA) tracer-yield model, five primary and four secondary fine organic aerosol sources were compared with the results from previous studies in Beijing. The relative contribution of mobile sources to PM2.5 concentrations was increased in 2008, with diesel engines contributing 16.2 ± 5.9% and 14.5 ± 4.1% and gasoline vehicles contributing 10.3 ± 8.7% and 7.9 ± 6.2% to organic carbon (OC) at PKU and Yufa, respectively. Due to the implementation of emission controls, the absolute OC concentrations from primary sources were reduced during the Olympics, and the contributions from secondary formation of OC represented a larger relative source of fine organic aerosols. Compared with the non-controlled period prior to the Olympics, primary vehicle contributions were reduced by 30% at the urban site and 24% at the rural site. The reductions in coal combustion contributions were 57% at PKU and 7% at Yufa. Our results demonstrate that the emission control measures implemented in 2008 significantly alleviated the primary organic particle pollution in and around Beijing. However, additional studies are needed to provide a more comprehensive assessment of the emission control effectiveness on SOA formation.

5. Quantitative evaluation of emission controls on primary and secondary organic aerosol sources during Beijing 2008 Olympics

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S. Guo

2013-08-01

Full Text Available To assess the primary and secondary sources of fine organic aerosols after the aggressive implementation of air pollution controls during the 2008 Beijing Olympic Games, 12 h PM2.5 values were measured at an urban site at Peking University (PKU and an upwind rural site at Yufa during the CAREBEIJING-2008 (Campaigns of Air quality REsearch in BEIJING and surrounding region summer field campaign. The average PM2.5 concentrations were 72.5 ± 43.6 μg m−3 and 64.3 ± 36.2 μg m−3 (average ± standard deviation, below as the same at PKU and Yufa, respectively, showing the lowest concentrations in recent years. Combining the results from a CMB (chemical mass balance model and secondary organic aerosol (SOA tracer-yield model, five primary and four secondary fine organic aerosol sources were compared with the results from previous studies in Beijing. The relative contribution of mobile sources to PM2.5 concentrations was increased in 2008, with diesel engines contributing 16.2 ± 5.9% and 14.5 ± 4.1% and gasoline vehicles contributing 10.3 ± 8.7% and 7.9 ± 6.2% to organic carbon (OC at PKU and Yufa, respectively. Due to the implementation of emission controls, the absolute OC concentrations from primary sources were reduced during the Olympics, and the contributions from secondary formation of OC represented a larger relative source of fine organic aerosols. Compared with the non-controlled period prior to the Olympics, primary vehicle contributions were reduced by 30% at the urban site and 24% at the rural site. The reductions in coal combustion contributions were 57% at PKU and 7% at Yufa. Our results demonstrate that the emission control measures implemented in 2008 significantly alleviated the primary organic particle pollution in and around Beijing. However, additional studies are needed to provide a more comprehensive assessment of the emission control effectiveness on SOA formation.

6. Complex refractive index of aerosols during LACE 98 as derived from the analysis of individual particles

Science.gov (United States)

Ebert, , M.; Weinbruch, , S.; Rausch, , A.; Gorzawski, , G.; Helas, , G.; Hoffmann, , P.; Wex, H.

2002-11-01

During the Lindenberger Aerosol Characterization Experiment (LACE 98), impactor sampling of aerosol particles in the size range of 0.1 to 25 μm was performed. The atmospheric concentrations of the elements sodium to lead (11 ≤ Z ≤ 83) were determined by total reflection X-ray fluorescence analysis. Approximately 15,500 individual particles were examined by high-resolution scanning electron microscopy and energy-dispersive X-ray microanalysis, and about 3800 particles were examined by transmission electron microscopy combined with energy-dispersive X-ray microanalysis. On the basis of morphology and chemical composition the particles were classified into 10 different groups: ammonium sulfates, calcium sulfates, sea salt, metal oxides/hydroxides, carbonates, silicates, soot, biological particles, carbon/sulfate mixed particles, and rest of carbon-rich particles Crest. The phases present in the different particle groups were determined by selected area electron diffraction in the transmission electron microscope. In addition, the heterogeneous phase composition of agglomerates was studied in detail. On the basis of the size distribution and the relative abundance of the particle groups, the average and size-resolved complex refractive index of the total aerosol were calculated. The real part of the average refractive index mainly depends on the abundance of metal oxide/hydroxide particles and varied between 1.52 and 1.57 on the different sampling days. The average imaginary part varied between 0.031 and 0.057 depending on the amounts of soot and carbon/sulfate mixed particles. The average complex refractive index deduced from the analysis of individual aerosol particles is in good agreement with the results of photometer measurements of dried filter samples.

7. New insights on aerosol sources and properties of Organics in the west Mediterranean basin

Science.gov (United States)

Nicolas, José B.; Sciare, Jean; Petit, Jean-Eudes; Bonnaire, Nicolas; Féron, Anais; Dulac, François; Hamonou, Eric; Gros, Valérie; Mallet, Marc; Lambert, Dominique; Sauvage, Stéphane; Léonardis, Thierry; Tison, Emmanuel; Colomb, Aurélie; Fresney, Evelyn; Pichon, Jean-Marc; Bouvier, Laetitia; Bourrianne, Thierry; Roberts, Gregory

2013-04-01

The Mediterranean basin exhibits high PM concentrations for a marine area, in particular during the dry season (summer), associated with high photochemistry. The large population of the basin is impacted by both natural and anthropogenic aerosols of various sources from Europe and North Africa. Simulations predict significant climate changes in that area, with less precipitation and hotter temperatures, reinforced by an increasing anthropogenic pressure, which will be linked by higher emissions of pollutants and also by higher impacts on the health. Nevertheless the aerosol models in that area currently suffer from large uncertainties, due to a lack of knowledge in organic aerosol (OA) sources and processes. As part of the French program ChArMEx (The Chemistry-Aerosol Mediterranean Experiment, http://charmex.lsce.ipsl.fr), a 5-week intensive campaign has been performed in June - July 2012 at the new Cape Corsica station (see Dulac et al. in that session), and aiming at a better characterization of anthropogenic versus biogenic aerosols, long range transport versus local influence, with a focus on fine OA. A complete instrumental strategy was deployed thanks to the contribution of a large French community: PM1 concentration every 6 min with a TEOM-FDMS 1405 (Thermo), major aerosol components in PM1 every 30 min (Organics, SO4, NO3, NH4) by Aerosol Chemical Speciation Monitor (Aerodyne), Equivalent Black Carbon every 5 min with a 7-? aethalometer AE31 (Magee Scientific), on-line major anions and cations (incl. light organics like oxalate & MSA) every 10 min with Particle-Into-Liquid Sampler (PILS, Metrohm) coupled with Ion Chromatographs (Dionex), on-line water-soluble organic carbon (WSOC) every 4 min with a PILS (Applikon) coupled with a Total Organic Carbon instrument (Ionics). Filter sampling in PM2.5 and PM10 was also performed every 12h for quality purposes (PM, EC/OC, ions) and for complementary measurements (metals by ICP-MS and organic tracers by LC

8. On the composition of ammonia-sulfuric-acid ion clusters during aerosol particle formation

Science.gov (United States)

Schobesberger, S.; Franchin, A.; Bianchi, F.; Rondo, L.; Duplissy, J.; Kürten, A.; Ortega, I. K.; Metzger, A.; Schnitzhofer, R.; Almeida, J.; Amorim, A.; Dommen, J.; Dunne, E. M.; Ehn, M.; Gagné, S.; Ickes, L.; Junninen, H.; Hansel, A.; Kerminen, V.-M.; Kirkby, J.; Kupc, A.; Laaksonen, A.; Lehtipalo, K.; Mathot, S.; Onnela, A.; Petäjä, T.; Riccobono, F.; Santos, F. D.; Sipilä, M.; Tomé, A.; Tsagkogeorgas, G.; Viisanen, Y.; Wagner, P. E.; Wimmer, D.; Curtius, J.; Donahue, N. M.; Baltensperger, U.; Kulmala, M.; Worsnop, D. R.

2015-01-01

The formation of particles from precursor vapors is an important source of atmospheric aerosol. Research at the Cosmics Leaving OUtdoor Droplets (CLOUD) facility at CERN tries to elucidate which vapors are responsible for this new-particle formation, and how in detail it proceeds. Initial measurement campaigns at the CLOUD stainless-steel aerosol chamber focused on investigating particle formation from ammonia (NH3) and sulfuric acid (H2SO4). Experiments were conducted in the presence of water, ozone and sulfur dioxide. Contaminant trace gases were suppressed at the technological limit. For this study, we mapped out the compositions of small NH3-H2SO4 clusters over a wide range of atmospherically relevant environmental conditions. We covered [NH3] in the range from 10. Positively charged clusters grew on average by Δm/Δn = 1.05 and were only observed at sufficiently high [NH3] / [H2SO4]. The H2SO4 molecules of these clusters are partially neutralized by NH3, in close resemblance to the acid-base bindings of ammonium bisulfate. Supported by model simulations, we substantiate previous evidence for acid-base reactions being the essential mechanism behind the formation of these clusters under atmospheric conditions and up to sizes of at least 2 nm. Our results also suggest that electrically neutral NH3-H2SO4 clusters, unobservable in this study, have generally the same composition as ionic clusters for [NH3] / [H2SO4] > 10. We expect that NH3-H2SO4 clusters form and grow also mostly by Δm/Δn > 1 in the atmosphere's boundary layer, as [NH3] / [H2SO4] is mostly larger than 10. We compared our results from CLOUD with APi-TOF measurements of NH3-H2SO4 anion clusters during new-particle formation in the Finnish boreal forest. However, the exact role of NH3-H2SO4 clusters in boundary layer particle formation remains to be resolved.

9. On the composition of ammonia-sulfuric acid clusters during aerosol particle formation

Science.gov (United States)

Schobesberger, S.; Franchin, A.; Bianchi, F.; Rondo, L.; Duplissy, J.; Kürten, A.; Ortega, I. K.; Metzger, A.; Schnitzhofer, R.; Almeida, J.; Amorim, A.; Dommen, J.; Dunne, E. M.; Ehn, M.; Gagné, S.; Ickes, L.; Junninen, H.; Hansel, A.; Kerminen, V.-M.; Kirkby, J.; Kupc, A.; Laaksonen, A.; Lehtipalo, K.; Mathot, S.; Onnela, A.; Petäjä, T.; Riccobono, F.; Santos, F. D.; Sipilä, M.; Tomé, A.; Tsagkogeorgas, G.; Viisanen, Y.; Wagner, P. E.; Wimmer, D.; Curtius, J.; Donahue, N. M.; Baltensperger, U.; Kulmala, M.; Worsnop, D. R.

2014-05-01

The formation of particles from precursor vapors is an important source of atmospheric aerosol. Research at the Cosmics Leaving OUtdoor Droplets (CLOUD) facility at CERN tries to elucidate which vapors are responsible for this new particle formation, and how in detail it proceeds. Initial measurement campaigns at the CLOUD stainless-steel aerosol chamber focused on investigating particle formation from ammonia (NH3) and sulfuric acid (H2SO4). Experiments were conducted in the presence of water, ozone and sulfur dioxide. Contaminant trace gases were suppressed at the technological limit. For this study, we mapped out the compositions of small NH3-H2SO4 clusters over a wide range of atmospherically relevant environmental conditions. We covered [NH3] in the range from 10. Positively charged clusters grew on average by Δm / Δn = 1.05 and were only observed at sufficiently high [NH3] / [H2SO4]. The H2SO4 molecules of these clusters are partially neutralized by NH3, in close resemblance to the acid-base bindings of ammonium bisulfate. Supported by model simulations, we substantiate previous evidence for acid-base reactions being the essential mechanism behind the formation of these clusters under atmospheric conditions and up to sizes of at least 2 nm. Our results also suggest that yet unobservable electrically neutral NH3-H2SO4 clusters grow by generally the same mechanism as ionic clusters, particularly for [NH3] / [H2SO4]>10. We expect that NH3-H2SO4 clusters form and grow also mostly by Δm / Δn>1 in the atmosphere's boundary layer, as [NH3] / [H2SO4] is mostly larger than 10. We compared our results from CLOUD with APi-TOF measurements of NH3-H2SO4 anion clusters during new particle formation in the Finnish boreal forest. However, the exact role of NH3-H2SO4 clusters in boundary layer particle formation remains to be resolved.

10. Spontaneous Aerosol Ejection: Origin of Inorganic Particles in Biomass Pyrolysis.

Science.gov (United States)

Teixeira, Andrew R; Gantt, Rachel; Joseph, Kristeen E; Maduskar, Saurabh; Paulsen, Alex D; Krumm, Christoph; Zhu, Cheng; Dauenhauer, Paul J

2016-06-08

At high thermal flux and temperatures of approximately 500 °C, lignocellulosic biomass transforms to a reactive liquid intermediate before evaporating to condensable bio-oil for downstream upgrading to renewable fuels and chemicals. However, the existence of a fraction of nonvolatile compounds in condensed bio-oil diminishes the product quality and, in the case of inorganic materials, catalyzes undesirable aging reactions within bio-oil. In this study, ablative pyrolysis of crystalline cellulose was evaluated, with and without doped calcium, for the generation of inorganic-transporting aerosols by reactive boiling ejection from liquid intermediate cellulose. Aerosols were characterized by laser diffraction light scattering, inductively coupled plasma spectroscopy, and high-speed photography. Pyrolysis product fractionation revealed that approximately 3 % of the initial feed (both organic and inorganic) was transported to the gas phase as aerosols. Large bubble-to-aerosol size ratios and visualization of significant late-time ejections in the pyrolyzing cellulose suggest the formation of film bubbles in addition to the previously discovered jet formation mechanism.

11. Two-Photon Excited Fluorescence from Biological Aerosol Particles

Science.gov (United States)

2010-09-29

previously observed from serotonin (5-HT) and its precursor hyrdroxytryptophan (5- HTP ) using multi-photon excitation [17-19]. Visible emission from...Sivaprakasam, A. Huston, H.B. Lin, J.D. Eversole, P. Falkenstein and A. Schultz, “Field test results and ambient aerosol measurements using dual

12. The 2005 Study of Organic Aerosols at Riverside (SOAR-1: instrumental intercomparisons and fine particle composition

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K. S. Docherty

2011-02-01

Full Text Available Multiple state-of-the-art instruments sampled ambient aerosol in Riverside, California during the 2005 Study of Organic Aerosols at Riverside (SOAR to investigate sources and chemical composition of fine particles (PMf in the inland region of Southern California. This paper briefly summarizes the spatial, meteorological and gas-phase conditions during SOAR-1 (15 July–15 August and provides detailed intercomparisons of complementary measurements and average PMf composition during this period. Daily meteorology and gas-phase species concentrations were highly repetitive with meteorological and gas-phase species concentrations displaying clear diurnal cycles and weekday/weekend contrast, with organic aerosol (OA being the single largest component contributing approximately one-third of PMf mass. In contrast with historical characterizations of OA in the region, several independent source apportionment efforts attributed the vast majority (~80% of OA mass during SOAR-1 to secondary organic aerosol (SOA. Given the collocation of complementary aerosol measurements combined with a dominance of SOA during SOAR-1, this paper presents new results on intercomparisons among several complementary measurements and on PMf composition during this period. Total non-refractory submicron (NR-PM1 measurements from a high-resolution aerosol mass spectrometer (HR-AMS are compared with measurements by tapered element oscillating microbalances (TEOM including a filter dynamics measurement system (TEOMFDMS. NR-PM1 is highly correlated with PM2.5 TEOMFDMS measurements and accounts for the bulk of PM2.5 mass with the remainder contributed primarily by refractory material. In contrast, measurements from a heated TEOM show substantial losses of semi-volatile material, including ammonium nitrate and semi-volatile organic material. Speciated HR-AMS measurements are

13. Ice cloud processing of ultra-viscous/glassy aerosol particles leads to enhanced ice nucleation ability

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R. Wagner

2012-09-01

Full Text Available The ice nucleation potential of airborne glassy aqueous aerosol particles has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 247 and 216 K. Four different solutes were used as proxies for oxygenated organic matter found in the atmosphere: raffinose, 4-hydroxy-3-methoxy-DL-mandelic acid (HMMA, levoglucosan, and a multi-component mixture of raffinose with five dicarboxylic acids and ammonium sulphate. Similar to previous experiments with citric acid aerosols, all particles were found to nucleate ice heterogeneously before reaching the homogeneous freezing threshold provided that the freezing cycles were started well below the respective glass transition temperatures of the compounds; this is discussed in detail in a separate article. In this contribution, we identify a further mechanism by which glassy aerosols can promote ice nucleation below the homogeneous freezing limit. If the glassy aerosol particles are probed in freezing cycles started only a few degrees below their respective glass transition temperatures, they enter the liquid regime of the state diagram upon increasing relative humidity (moisture-induced glass-to-liquid transition before being able to act as heterogeneous ice nuclei. Ice formation then only occurs by homogeneous freezing at elevated supersaturation levels. When ice forms the remaining solution freeze concentrates and re-vitrifies. If these ice cloud processed glassy aerosol particles are then probed in a second freezing cycle at the same temperature, they catalyse ice formation at a supersaturation threshold between 5 and 30% with respect to ice. By analogy with the enhanced ice nucleation ability of insoluble ice nuclei like mineral dusts after they nucleate ice once, we refer to this phenomenon as pre-activation. We propose a number of possible explanations for why glassy aerosol particles that have re

14. Ice cloud processing of ultra-viscous/glassy aerosol particles leads to enhanced ice nucleation ability

Science.gov (United States)

Wagner, R.; Möhler, O.; Saathoff, H.; Schnaiter, M.; Skrotzki, J.; Leisner, T.; Wilson, T. W.; Malkin, T. L.; Murray, B. J.

2012-09-01

The ice nucleation potential of airborne glassy aqueous aerosol particles has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 247 and 216 K. Four different solutes were used as proxies for oxygenated organic matter found in the atmosphere: raffinose, 4-hydroxy-3-methoxy-DL-mandelic acid (HMMA), levoglucosan, and a multi-component mixture of raffinose with five dicarboxylic acids and ammonium sulphate. Similar to previous experiments with citric acid aerosols, all particles were found to nucleate ice heterogeneously before reaching the homogeneous freezing threshold provided that the freezing cycles were started well below the respective glass transition temperatures of the compounds; this is discussed in detail in a separate article. In this contribution, we identify a further mechanism by which glassy aerosols can promote ice nucleation below the homogeneous freezing limit. If the glassy aerosol particles are probed in freezing cycles started only a few degrees below their respective glass transition temperatures, they enter the liquid regime of the state diagram upon increasing relative humidity (moisture-induced glass-to-liquid transition) before being able to act as heterogeneous ice nuclei. Ice formation then only occurs by homogeneous freezing at elevated supersaturation levels. When ice forms the remaining solution freeze concentrates and re-vitrifies. If these ice cloud processed glassy aerosol particles are then probed in a second freezing cycle at the same temperature, they catalyse ice formation at a supersaturation threshold between 5 and 30% with respect to ice. By analogy with the enhanced ice nucleation ability of insoluble ice nuclei like mineral dusts after they nucleate ice once, we refer to this phenomenon as pre-activation. We propose a number of possible explanations for why glassy aerosol particles that have re-vitrified in contact

15. Aerosol composition, oxidative properties, and sources in Beijing: results from the 2014 Asia-Pacific Economic Cooperation Summit study

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W. Q. Xu

2015-08-01

Full Text Available The mitigation of air pollution in megacities remains a great challenge because of the complex sources and formation mechanisms of aerosol particles. The 2014 Asia- Pacific Economic Cooperation (APEC summit in Beijing serves as a unique experiment to study the impacts of emission controls on aerosol composition, size distributions, and oxidative properties. Herein, a high-resolution time-of-flight aerosol mass spectrometer was deployed in urban Beijing for real-time measurements of size-resolved non-refractory submicron aerosol (NR-PM1 species from 14 October to 12 November 2014, along with a range of collocated measurements. The average (±σ PM1 was 41.6 (±38.9 μg m−3 during APEC, which was decreased by 53 % compared with that before APEC. The aerosol composition showed substantial changes owing to emission controls during APEC. Secondary inorganic aerosols (SIA = sulfate + nitrate + ammonium showed significant reductions of 62–69 %, whereas organics presented much smaller decreases (35 %. The results from the positive matrix factorization of organic aerosols (OA indicated that highly oxidized secondary OA (SOA showed decreases similar to those of SIA during APEC. However, primary OA (POA from cooking, traffic, and biomass burning sources were comparable to those before APEC, indicating the presence of strong local source emissions. The oxidation properties showed corresponding changes in response to OA composition. The average oxygen-to-carbon level during APEC was 0.36 (±0.10, which is lower than the 0.43 (±0.13 measured before APEC, demonstrating a decrease in the OA oxidation degree. The changes in size distributions of primary and secondary species varied during APEC. SIA and SOA showed significant reductions in large accumulation modes with peak diameters shifting from ~ 650 to 400 nm during APEC, whereas those of POA remained relatively unchanged. The changes in aerosol composition, size distributions, and oxidation degrees

16. Development and experimental evaluation of an optical sensor for aerosol particle characterization

Energy Technology Data Exchange (ETDEWEB)

Somesfalean, G.

1998-03-01

A sensor for individual aerosol particle characterization, based on a single-mode semiconductor laser coupled to an external cavity is presented. The light emitting semiconductor laser acts as a sensitive optical detector itself, and the whole system has the advantage of using conventional optical components and providing a compact set-up. Aerosol particles moving through the sensing volume, which is located in the external cavity of a semiconductor laser, scatter and absorb light. Thereby they act as small disturbances on the electromagnetic field inside the dynamic multi-cavity laser system. From the temporal variation of the output light intensity, information about the number, velocity, size, and refractive index of the aerosol particles can be derived. The diffracted light in the near-forward scattering direction is collected and Fourier-transformed by a lens, and subsequently imaged on a CCD camera. The recorded Fraunhofer diffraction pattern provides information about the projected area of the scattering particle, and can thus be used to determine the size and the shape of aerosol particles. The sensor has been tested on fibers which are of interest in the field of working environment monitoring. The recorded output intensity variation has been analysed, and the relationship between the shape and the size of each fibre, and the resulting scattering profiles has been investigated. A simple one-dimensional model for the optical feedback variation due to the light-particle interaction in the external cavity is also discussed 34 refs, 26 figs, 6 tabs

17. Aerosols in the tropical and subtropical UT/LS: in-situ measurements of submicron particle abundance and volatility

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S. Borrmann

2010-06-01

compact enough to derive a parameterisation. The tropical profiles all show a broad maximum of particle mixing ratios (between Θ≈340 K and 390 K which extends from below the TTL to above the thermal tropopause. Thus these particles are a "reservoir" for vertical transport into the stratosphere. The ratio of non-volatile particle number density to total particle number density was also measured by COPAS. The vertical profiles of this ratio have a maximum of 50% above 370 K over Australia and West Africa and a pronounced minimum directly below. Without detailed chemical composition measurements a reason for the increase of non-volatile particle fractions cannot yet be given. However, half of the particles from the tropical "reservoir" contain compounds other than sulphuric acid and water. Correlations of the measured aerosol mixing ratios with N2O and ozone exhibit compact relationships for the tropical data from SCOUT-AMMA, TROCCINOX, and SCOUT-O3. Correlations with CO are more scattered probably because of the connection to different pollution source regions. We provide additional data from the long distance transfer flights to the campaign sites in Brazil, Australia, and West-Africa. These were executed during a time window of 17 months within a period of relative volcanic quiescence. Thus the data represent a "snapshot picture" documenting the status of a significant part of the global UT/LS fine aerosol at low concentration levels 15 years after the last major (i.e., the 1991 Mount Pinatubo eruption. The corresponding latitudinal distributions of the measured particle number densities are presented in this paper to provide data of the UT/LS background aerosol for modelling purposes.

18. Aerosols in the tropical and subtropical UT/LS: in-situ measurements of submicron particle abundance and volatility

Science.gov (United States)

Borrmann, S.; Kunkel, D.; Weigel, R.; Minikin, A.; Deshler, T.; Wilson, J. C.; Curtius, J.; Volk, C. M.; Homan, C. D.; Ulanovsky, A.; Ravegnani, F.; Viciani, S.; Shur, G. N.; Belyaev, G. V.; Law, K. S.; Cairo, F.

2010-06-01

parameterisation. The tropical profiles all show a broad maximum of particle mixing ratios (between Θ≍340 K and 390 K) which extends from below the TTL to above the thermal tropopause. Thus these particles are a "reservoir" for vertical transport into the stratosphere. The ratio of non-volatile particle number density to total particle number density was also measured by COPAS. The vertical profiles of this ratio have a maximum of 50% above 370 K over Australia and West Africa and a pronounced minimum directly below. Without detailed chemical composition measurements a reason for the increase of non-volatile particle fractions cannot yet be given. However, half of the particles from the tropical "reservoir" contain compounds other than sulphuric acid and water. Correlations of the measured aerosol mixing ratios with N2O and ozone exhibit compact relationships for the tropical data from SCOUT-AMMA, TROCCINOX, and SCOUT-O3. Correlations with CO are more scattered probably because of the connection to different pollution source regions. We provide additional data from the long distance transfer flights to the campaign sites in Brazil, Australia, and West-Africa. These were executed during a time window of 17 months within a period of relative volcanic quiescence. Thus the data represent a "snapshot picture" documenting the status of a significant part of the global UT/LS fine aerosol at low concentration levels 15 years after the last major (i.e., the 1991 Mount Pinatubo) eruption. The corresponding latitudinal distributions of the measured particle number densities are presented in this paper to provide data of the UT/LS background aerosol for modelling purposes.

19. Modelling non-equilibrium secondary organic aerosol formation and evaporation with the aerosol dynamics, gas- and particle-phase chemistry kinetic multilayer model ADCHAM

Energy Technology Data Exchange (ETDEWEB)

Roldin, P.; Eriksson, A. C.; Nordin, E. Z.; Hermansson, E.; Mogensen, Ditte; Rusanen, A.; Boy, Michael; Swietlicki, E.; Svenningsson, Birgitta; Zelenyuk, Alla; Pagels, J.

2014-08-11

We have developed the novel Aerosol Dynamics, gas- and particle- phase chemistry model for laboratory CHAMber studies (ADCHAM). The model combines the detailed gas phase Master Chemical Mechanism version 3.2, an aerosol dynamics and particle phase chemistry module (which considers acid catalysed oligomerization, heterogeneous oxidation reactions in the particle phase and non-ideal interactions between organic compounds, water and inorganic ions) and a kinetic multilayer module for diffusion limited transport of compounds between the gas phase, particle surface and particle bulk phase. In this article we describe and use ADCHAM to study: 1) the mass transfer limited uptake of ammonia (NH3) and formation of organic salts between ammonium (NH4+) and carboxylic acids (RCOOH), 2) the slow and almost particle size independent evaporation of α-pinene secondary organic aerosol (SOA) particles, and 3) the influence of chamber wall effects on the observed SOA formation in smog chambers.

20. The Influence of a Secondary Organic Aerosol Coating on the Heterogeneous Reaction of Squalane Particles with OH

Science.gov (United States)

Kolesar, K.; Cappa, C. D.; Buffaloe, G.; Chen, C. J.; Isaacman, G.; Nah, T.; Ruehl, C.; Goldstein, A. H.; Wilson, K. R.

2012-12-01

Reactions occurring in the condensed phase or at the surface of particles have the potential to alter their chemical and physical properties. The use of a model system such as the previously well-characterized heterogeneous oxidation of particulate squaqlane can facilitate understanding of the mechanisms associated with such reactions. The rate of squalane oxidation is determined from the frequency of hydroxyl radical collision with the particle surface and the probability that a collision will react. We now add a layer of complexity to the oxidation of particulate squalane by measuring the heterogeneous reactivity towards OH of the squalane after addition of a coating of secondary organic aerosol (SOA), generated from the reaction of α-pinene and ozone. Heterogeneous reaction rates and OH uptake coefficients for squalane within the resulting internally mixed particles were measured using a flow tube reactor coupled to the Vacuum Ultraviolet Aerosol Mass Spectrometer at Beamline 9.0.2 of the Advanced Light Source. The use of the relatively soft VUV ionization allowed for clear differentiation of squalane and its major oxidation products from that of the SOA in the measured mass spectra. This allows for direct, online measurement of the squalane decay rate in the presence of the SOA species and thus determination of the reaction rate constant for squalane with OH radicals. The decay of squalane in the internally mixed squalane/SOA particles was faster than that observed for pure squalane particles, by about a factor of 2, despite the fact that the SOA was coated onto the squalane particles. The apparent increase in the squalane loss rate is most likely due to increased loss of squalane via condensed-phase secondary chemical reactions in the mixed particles. This illustrates the important role the particle composition plays in determining the nature and extent of condensed phase reactions that occur within organic particles in the atmosphere that warrants further

1. Ice cloud processing of ultra-viscous/glassy aerosol particles leads to enhanced ice nucleation ability

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B. J. Murray

2012-04-01

Full Text Available The ice nucleation potential of airborne glassy aqueous aerosol particles has been investigated by controlled expansion cooling cycles in the AIDA aerosol and cloud chamber of the Karlsruhe Institute of Technology at temperatures between 247 and 216 K. Four different solutes were used as proxies for oxygenated organic matter found in the atmosphere: raffinose, 4-hydroxy-3-methoxy-DL-mandelic acid (HMMA, levoglucosan, and a multi-component mixture of raffinose with five dicarboxylic acids and ammonium sulphate. Similar to previous experiments with citric acid aerosols, all particles were found to nucleate ice heterogeneously before reaching the homogeneous freezing threshold provided that the freezing cycles were started well below the respective glass transition temperatures of the compounds; this is discussed in detail in a separate article. In this contribution, we identify a further mechanism by which glassy aerosols can promote ice nucleation below the homogeneous freezing limit. If the glassy aerosol particles are probed in freezing cycles started only a few degrees below their respective glass transition temperatures, they enter the liquid regime of the state diagram upon increasing relative humidity (moisture-induced glass-to-liquid transition before being able to act as heterogeneous ice nuclei. Ice formation then only occurs by homogeneous freezing at elevated supersaturation levels. When ice forms the remaining solution freeze concentrates and re-vitrifies. If these ice cloud processed glassy aerosol particles are then probed in a second freezing cycle at the same temperature, they catalyse ice formation at a supersaturation threshold between 5 and 30% with respect to ice. By analogy with the enhanced ice nucleation ability of insoluble ice nuclei like mineral dusts after they nucleate ice once, we refer to this phenomenon as pre-activation. We propose a number of possible explanations for why glassy aerosols that have re-vitrified in

2. Fabrication of a pure, uniform electroless silver film using ultrafine silver aerosol particles.

Science.gov (United States)

Byeon, Jeong Hoon; Kim, Jang-Woo

2010-07-20

To obtain evenly distributed pure Ag particles with a narrow size distribution on a polymer membrane, a novel activation procedure with an environmentally friendly, cost-effective method was utilized as a pretreatment before electroless Ag deposition. The pretreatment was first performed on an untreated membrane surface by collecting ultrafine ambient spark-generated Ag aerosol particles. After annealing, the electroless Ag film was fabricated on the collected aerosol particles in the Ag electroless bath. Experimental characterizations showed that the ultrafine Ag particles were uniformly anchored onto the membrane surface through pretreatment, resulting in a pure Ag film of closely packed particles with a narrow size distribution on the membrane, and the properties were comparable to those of an Ag film on wet Sn-Ag-activated membranes.

3. Characterisation of Fluorescent Biological Aerosol Particles during South-West Monsoon from a High Altitude Site in South India

Science.gov (United States)

Valsan, A. E.; R, R.; V, B. C.; Huffman, J. A.; Poeschl, U.; Gunthe, S. S.

2015-12-01

Biological aerosols (Bioaerosols) constitute a wide range of dead and alive biological materials that are suspended in the atmosphere. Though ubiquitous in earth's atmosphere, bioaerosols are poorly characterized in terms of their atmospheric abundance, sources and physical properties. Here we discuss the number concentration and size distribution of coarse mode (>1µm) biological aerosols measured at a relatively clean high altitude continental site, Munnar (10.09 N, 77.06 E; 1605 m asl) located in the Western Ghats mountain ranges of Southern Tropical India. The fluorescent biological aerosol particles (FBAP) were continuously measured using Ultra Violet Aerodynamic Particle Sizer (UVAPS) from 01 June to 21 August 2014 (South-West Monsoon Period) which showed some interesting patterns. The mean number and mass concentration of coarse FBAP during the campaign was observed to be 1.7 x 10-2cm-3 and 0.24µg m-3 respectively, which corresponds to 2% and 9% of coarse total aerosol particles (TAP) number and mass concentration. FBAP concentration decreased significantly during periods of heavy and continuous rain with constant South-West winds. This may be due to the clean marine influx coming from the ocean and continuous washout. The Relative Humidity (RH) and temperature remained consistent during this period without any strong diurnal pattern. When the wind fluctuated in North-West directions, the FBAP concentration increased to even an order of magnitude higher than the periods of South-West winds which can be attributed to the transported bioaerosols from the nearby vegetated area. In spite of variability in the number concentrations, the size distribution of FBAP exhibited a prominent peak at ~3 μm throughout the campaign, which should be fungal spores. They also exhibited a strong diurnal pattern with high concentrations occuring during the night time which peaks in the early morning hours.Biological aerosols (Bioaerosols) constitute a wide range of dead and

4. Fluorescence from atmospheric aerosol detected by a lidar indicates biogenic particles in the stratosphere

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F. Immler

2004-09-01

Full Text Available With a lidar system that was installed in Lindenberg/Germany, we observed in June 2003, an extended aerosol layer at 13 km altitude in the lowermost stratosphere. This layer created an inelastic backscatter signal which we interpret as laser induced fluorescence from aerosol particles. Also, we find evidence for inelastic scattering in a smoke plume from a forest fire that we observed in the troposphere. Fluorescence from ambient aerosol had not yet been considered detectable by lidar. However, organic compounds such as polycyclic aromatic hydrocarbons sticking to the aerosol particles, or bioaerosol such as bacteria, spores or pollen fluoresce when excited with UV-radiation in a way that is detectable by our lidar system. Therefore, we conclude that fluorescence from organic material released by biomass burning creates the inelastic backscatter signal that we measured with our instrument and thus demonstrate a new and powerful way to characterize aerosols by a remote sensing technique. The stratospheric aerosol layer that we have observed in Lindenberg for three consecutive days is likely to be a remnant from Siberian forest fire plumes lifted across the tropopause and transported around the globe.

5. Polar organic marker compounds in atmospheric aerosols: Determination, time series, size distributions and sources

Science.gov (United States)

Kourtchev, Ivan

Terrestrial vegetation releases substantial amounts of reactive volatile organic compounds (VOCs; e.g., isoprene, monoterpenes) into the atmosphere. The VOCs can be rapidly photooxidized under conditions of high solar radiation, yielding products that can participate in new particle formation and growth processes above forests. This thesis focuses on the characterization, identification and quantification of oxidation products of biogenic VOC (BVOCs) as well as other species (tracer compounds) that provide information on aerosol sources and source processes. Atmospheric aerosols from various forested sites (i.e., Hyytiala, southern Finland; Rondonia, Brazil; K-Puszta, Hungary and Julich, Germany) were analyzed with Gas Chromotography/Mass Spectrometry (GC/MS) using analytical procedure that targets polar organic compounds. The study demonstrated that isoprene (i.e., 2-methyerythritol, 2-methylthreitol, 2-methylglyceric acid and C5-alkene triols (2-methyl-1,3,4-trihydroxy-l-butene (cis and trans) and 3 methyl-2,3,4-trihydroxy-1-butene)) and monoterpene (pinic acid, norpinic acid, 3-hydroxyglutaric acid and 3-methyl-1,2,3-butanetricarboxylic acid) oxidation products were present in substantial concentrations in atmospheric aerosols suggesting that oxidation of BVOC from the vegetation is an important process in all studied sites. On the other hand, presence of levoglucosan, biomass burning marker, especially in Amazonian rain forest site at Rondonia, Brazil, pointed that all sites were affected by anthropogenic activities, namely biomass burning. Other identified compounds included plyols, arabitol, mannitol and erythritol, which are marker compounds for fungal spores and monosacharides, glucose and fructose, markers for plant polens. Temporal variations as well as mass size distributions of the detected species confirmed the possible formation mechanisms of marker compounds.

6. Development and characterization of a single particle laser ablation mass spectrometer (SPLAM for organic aerosol studies

Directory of Open Access Journals (Sweden)

F. Gaie-Levrel

2011-07-01

Full Text Available A single particle instrument has been developed for real-time analysis of organic aerosols. This instrument, named Single Particle Laser Ablation Mass Spectrometry (SPLAM, samples particles using an aerodynamic lens system for which the theoretical performances were calculated. At the outlet of this system, particle detection and sizing are realized using two continuous diode lasers operating at λ = 403 nm. Polystyrene Latex (PSL, sodium chloride (NaCl and dioctylphtalate (DOP particles were used to characterize and calibrate optical detection of SPLAM. The optical detection limit (DL and detection efficiency (DE were determined using size-selected DOP particles. The DE is ranging from 0.1 to 90 % for 100 and 350 nm DOP particles respectively and the SPLAM instrument is able to detect and size-resolve particles as small as 110–120 nm. Scattered light is detected by two photomultipliers and the detected signals are used to trigger a UV excimer laser (λ = 248 nm used for laser desorption ionization (LDI of individual aerosol particles. The formed ions are analyzed by a 1 m linear time-of-flight mass spectrometer in order to access to the chemical composition of individual particles. The TOF-MS detection limit for gaseous aromatic compounds was determined to be 0.85 attograms. DOP particles were also used to test the overall functioning of the instrument. The analysis of a secondary organic aerosol, formed in a smog chamber by the ozonolysis of indene, is presented as a first scientific application of the instrument. Single particle mass spectra are obtained with a global hit rate of 10 %. They are found to be very different from one particle to another, reflecting chemical differences of the analyzed particles, and most of the detected mass peaks are attributed to oxidized products of indene.

7. Morphology, Composition, and Mixing State of Individual Aerosol Particles in Northeast China during Wintertime

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Liang Xu

2017-02-01

Full Text Available Northeast China is located in a high latitude area of the world and undergoes a cold season that lasts six months each year. Recently, regional haze episodes with high concentrations of fine particles (PM2.5 have frequently been occurring in Northeast China during the heating period, but little information has been available. Aerosol particles were collected in winter at a site in a suburban county town (T1 and a site in a background rural area (T2. Morphology, size, elemental composition, and mixing state of individual aerosol particles were characterized by transmission electron microscopy (TEM. Aerosol particles were mainly composed of organic matter (OM and S-rich and certain amounts of soot and K-rich. OM represented the most abundant particles, accounting for 60.7% and 53.5% at the T1 and T2 sites, respectively. Abundant spherical OM particles were likely emitted directly from coal-burning stoves. Soot decreased from 16.9% at the T1 site to 4.6% at the T2 site and sulfate particles decrease from 35.9% at the T2 site to 15.7% at the T1 site, suggesting that long-range transport air masses experienced more aging processes and produced more secondary particles. Based on our investigations, we proposed that emissions from coal-burning stoves in most rural areas of the west part of Northeast China can induce regional haze episodes.

8. Characterizing the impact of urban emissions on regional aerosol particles; airborne measurements during the MEGAPOLI experiment

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E. J. Freney

2013-09-01

Full Text Available The MEGAPOLI experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS giving detailed information of the non-refractory submicron aerosol species. The mass concentration of BC, measured by a particle absorption soot photometer (PSAP, was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA, black carbon and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NOx. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (−log(NOx / NOy. Plotting the equivalent ratios for the Positive Matrix Factorization (PMF resolved species (LV-OOA, SV-OOA, and HOA illustrate that the increase in OA is a result of secondary organic aerosol (SOA. Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in Mexico city, Mexico and in New England, USA. Using the measured VOCs species together with recent organic aerosol formation yields we predicted ~ 50% of the measured organics. These airborne measurements during the MEGAPOLI experiment show that urban emissions contribute to the

9. A novel tandem differential mobility analyzer with organic vapor treatment of aerosol particles

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J. Joutsensaari

2001-01-01

Full Text Available A novel method to characterize the organic composition of aerosol particles has been developed. The method is based on organic vapor interaction with aerosol particles and it has been named an Organic Tandem Differential Mobility Analyzer (OTDMA. The OTDMA method has been tested for inorganic (sodium chloride and ammonium sulfate and organic (citric acid and adipic acid particles. Growth curves of the particles have been measured in ethanol vapor and as a comparison in water vapor as a function of saturation ratio. Measurements in water vapor show that sodium chloride and ammonium sulfate as well as citric acid particles grow at water saturation ratios (S of 0.8 and above, whereas adipic acid particles do not grow at S S = 0.75 and S = 0.79, respectively. Citric acid particles grow monotonously with increasing saturation ratios already at low saturation ratios and no clear deliquescence point is found. For sodium chloride and ammonium sulfate particles, no growth can be seen in ethanol vapor at saturation ratios below 0.93. In contrast, for adipic acid particles, the deliquescence takes place at around S = 0.95 in the ethanol vapor. The recrystallization of adipic acid takes place at S The results show that the working principles of the OTDMA are operational for single-component aerosols. Furthermore, the results indicate that the OTDMA method may prove useful in determining whether aerosol particles contain organic substances, especially if the OTDMA is operated in parallel with a hygroscopicity TDMA, as the growth of many substances is different in ethanol and water vapors.

10. Dynamic viscosity mapping of the oxidation of squalene aerosol particles.

OpenAIRE

Athanasiadis, Athanasios; Fitzgerald, Clare; Davidson, Nicholas M; Giorio, Chiara; Botchway, Stanley W; Ward, Andrew D.; Kalberer, Markus; Pope, Francis D.; Kuimova, Marina K.

2016-01-01

Organic aerosols (OAs) play important roles in multiple atmospheric processes, including climate change, and can impact human health. The physico-chemical properties of OAs are important for all these processes and can evolve through reactions with various atmospheric components, including oxidants. The dynamic nature of these reactions makes it challenging to obtain a true representation of their composition and surface chemistry. Here we investigate the microscopic viscosity of the model OA...

11. Size distribution dynamics reveal particle-phase chemistry in organic aerosol formation.

Science.gov (United States)

Shiraiwa, Manabu; Yee, Lindsay D; Schilling, Katherine A; Loza, Christine L; Craven, Jill S; Zuend, Andreas; Ziemann, Paul J; Seinfeld, John H

2013-07-16

Organic aerosols are ubiquitous in the atmosphere and play a central role in climate, air quality, and public health. The aerosol size distribution is key in determining its optical properties and cloud condensation nucleus activity. The dominant portion of organic aerosol is formed through gas-phase oxidation of volatile organic compounds, so-called secondary organic aerosols (SOAs). Typical experimental measurements of SOA formation include total SOA mass and atomic oxygen-to-carbon ratio. These measurements, alone, are generally insufficient to reveal the extent to which condensed-phase reactions occur in conjunction with the multigeneration gas-phase photooxidation. Combining laboratory chamber experiments and kinetic gas-particle modeling for the dodecane SOA system, here we show that the presence of particle-phase chemistry is reflected in the evolution of the SOA size distribution as well as its mass concentration. Particle-phase reactions are predicted to occur mainly at the particle surface, and the reaction products contribute more than half of the SOA mass. Chamber photooxidation with a midexperiment aldehyde injection confirms that heterogeneous reaction of aldehydes with organic hydroperoxides forming peroxyhemiacetals can lead to a large increase in SOA mass. Although experiments need to be conducted with other SOA precursor hydrocarbons, current results demonstrate coupling between particle-phase chemistry and size distribution dynamics in the formation of SOAs, thereby opening up an avenue for analysis of the SOA formation process.

12. Modeling Gas-Particle Partitioning of SOA: Effects of Aerosol Physical State and RH

Science.gov (United States)

Zuend, A.; Seinfeld, J.

2011-12-01

Aged tropospheric aerosol particles contain mixtures of inorganic salts, acids, water, and a large variety of organic compounds. In liquid aerosol particles non-ideal mixing of all species determines whether the condensed phase undergoes liquid-liquid phase separation or whether it is stable in a single mixed phase, and whether it contains solid salts in equilibrium with their saturated solution. The extended thermodynamic model AIOMFAC is able to predict such phase states by representing the variety of organic components using functional groups within a group-contribution concept. The number and composition of different condensed phases impacts the diversity of reaction media for multiphase chemistry and the gas-particle partitioning of semivolatile species. Recent studies show that under certain conditions biogenic and other organic-rich particles can be present in a highly viscous, semisolid or amorphous solid physical state, with consequences regarding reaction kinetics and mass transfer limitations. We present results of new gas-particle partitioning computations for aerosol chamber data using a model based on AIOMFAC activity coefficients and state-of-the-art vapor pressure estimation methods. Different environmental conditions in terms of temperature, relative humidity (RH), salt content, amount of precursor VOCs, and physical state of the particles are considered. We show how modifications of absorptive and adsorptive gas-particle mass transfer affects the total aerosol mass in the calculations and how the results of these modeling approaches compare to data of aerosol chamber experiments, such as alpha-pinene oxidation SOA. For a condensed phase in a mixed liquid state containing ammonium sulfate, the model predicts liquid-liquid phase separation up to high RH in case of, on average, moderately hydrophilic organic compounds, such as first generation oxidation products of alpha-pinene. The computations also reveal that treating liquid phases as ideal

13. Synthesizing Scientific Progress: Outcomes from US EPA’s Carbonaceous Aerosols and Source Apportionment STAR Grants

Science.gov (United States)

ABSTRACTA number of studies in the past decade have transformed the way we think about atmospheric aerosols. The advances include, but are not limited to, source apportionment of organics using aerosol mass spectrometer data, the volatility basis set approach, quantifying isopre...

14. Characteristics and source of aerosols at Shiyi Glacier,Qilian Mountains, China

Institute of Scientific and Technical Information of China (English)

2016-01-01

Aerosol samples were collected in the Shiyi Glacier, Qilian Mountains from July 24 to August 19, 2012 and analyzed formajor water-soluble ionic species （F-, Cl-, NO2-, NO3-, SO42-, Na＋, NH4＋, K＋, Mg2＋ and Ca2＋） by ion chromatography.SO42- and NH4＋ were the most abundant components of all the anions and cations, with average concentrations of 94.72and 54.26 neq/m3, respectively, accounting for 34% and 20% of the total water-soluble ions analyzed. These mean ionconcentrations were generally comparable with the background conditions in remote sites of the Qilian Mountains, butwere much lower than those in certain cities in China. The particles were grouped into two dominant types according totheir morphology and EDX signal： Si-rich particles and Fe-rich particles. Backward air mass trajectory analysis suggestedthat inland cities may contribute some anthropogenic pollution to this glacier, while the arid and semi-arid regions ofcentral Asia were the primary sources of the mineral particles.

15. Production, Organic Characterization, and Phase Transformations of Marine Particles Aerosolized from a Laboratory Mesocosm Phytoplankton Bioreactor

Science.gov (United States)

Alpert, P. A.; Knopf, D. A.; Aller, J. Y.; Radway, J.; Kilthau, W.

2012-12-01

Previous studies have shown that particles emitted from bubble bursting and wave breaking of ocean waters with high biological activity can contain sea salts associated with organic material, with smaller particles containing a larger mass fraction of organics than larger particles. This likely indicates a link between phytoplankton productivity in oceans and particulate organic material in marine air. Once aerosolized, particles with significant amount of organic material can affect cloud activation and formation of ice crystals, among other atmospheric processes, thus influencing climate. This is significant for clouds and climate particularly over nutrient rich polar seas, in which concentrations of biological organisms can reach up to 109 cells per ml during spring phytoplankton blooms. Here we present results of bubble bursting aerosol production from a seawater mesocosm containing artificial seawater, natural seawater and unialgal cultures of three representative phytoplankton species. These phytoplankton (Thalassiosira pseudonana, Emilianaia huxleyi, and Nannochloris atomus), possessed siliceous frustules, calcareous frustules and no frustules, respectively. Bubbles were generated employing recirculating impinging water jets or glass frits. Dry and humidified aerosol size distributions and bulk aerosol organic composition were measured as a function of phytoplankton growth, and chlorophyll composition and particulate and dissolved organic carbon in the water were determined. Finally, particles were collected on substrates for ice nucleation and water uptake experiments, their elemental compositions were determined using computer controlled scanning electron microscopy and energy dispersive analysis of X-rays (CCSEMEDAX), and their carbon speciation was determined using scanning transmission X-ray microscopy and near-edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS). Particle size distributions exposed to dry and humidified air employing

16. Mass analysis of charged aerosol particles in NLC and PMSE during the ECOMA/MASS campaign

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S. Robertson

2009-03-01

Full Text Available MASS (Mesospheric Aerosol Sampling Spectrometer is a multichannel mass spectrometer for charged aerosol particles, which was flown from the Andøya Rocket Range, Norway, through NLC and PMSE on 3 August 2007 and through PMSE on 6 August 2007. The eight-channel analyzers provided for the first time simultaneous measurements of the charge density residing on aerosol particles in four mass ranges, corresponding to ice particles with radii <0.5 nm (including ions, 0.5–1 nm, 1–2 nm, and >3 nm (approximately. Positive and negative particles were recorded on separate channels. Faraday rotation measurements provided electron density and a means of checking charge density measurements made by the spectrometer. Additional complementary measurements were made by rocket-borne dust impact detectors, electric field booms, a photometer and ground-based radar and lidar. The MASS data from the first flight showed negative charge number densities of 1500–3000 cm−3 for particles with radii >3 nm from 83–88 km approximately coincident with PMSE observed by the ALWIN radar and NLC observed by the ALOMAR lidar. For particles in the 1–2 nm range, number densities of positive and negative charge were similar in magnitude (~2000 cm−3 and for smaller particles, 0.5–1 nm in radius, positive charge was dominant. The occurrence of positive charge on the aerosol particles of the smallest size and predominately negative charge on the particles of largest size suggests that nucleation occurs on positive condensation nuclei and is followed by collection of negative charge during subsequent growth to larger size. Faraday rotation measurements show a bite-out in electron density that increases the time for positive aerosol particles to be neutralized and charged negatively. The larger particles (>3 nm are observed throughout the NLC region, 83–88 km, and the smaller particles are observed primarily at the high end of the range, 86–88 km

17. Aerosol measurements during COPE: composition, size, and sources of CCN and INPs at the interface between marine and terrestrial influences

Science.gov (United States)

Taylor, Jonathan W.; Choularton, Thomas W.; Blyth, Alan M.; Flynn, Michael J.; Williams, Paul I.; Young, Gillian; Bower, Keith N.; Crosier, Jonathan; Gallagher, Martin W.; Dorsey, James R.; Liu, Zixia; Rosenberg, Philip D.

2016-09-01

Heavy rainfall from convective clouds can lead to devastating flash flooding, and observations of aerosols and clouds are required to improve cloud parameterisations used in precipitation forecasts. We present measurements of boundary layer aerosol concentration, size, and composition from a series of research flights performed over the southwest peninsula of the UK during the COnvective Precipitation Experiment (COPE) of summer 2013. We place emphasis on periods of southwesterly winds, which locally are most conducive to convective cloud formation, when marine air from the Atlantic reached the peninsula. Accumulation-mode aerosol mass loadings were typically 2-3 µg m-3 (corrected to standard cubic metres at 1013.25 hPa and 273.15 K), the majority of which was sulfuric acid over the sea, or ammonium sulfate inland, as terrestrial ammonia sources neutralised the aerosol. The cloud condensation nuclei (CCN) concentrations in these conditions were ˜ 150-280 cm-3 at 0.1 % and 400-500 cm-3 at 0.9 % supersaturation (SST), which are in good agreement with previous Atlantic measurements, and the cloud drop concentrations at cloud base ranged from 100 to 500 cm-3. The concentration of CCN at 0.1 % SST was well correlated with non-sea-salt sulfate, meaning marine sulfate formation was likely the main source of CCN. Marine organic aerosol (OA) had a similar mass spectrum to previous measurements of sea spray OA and was poorly correlated with CCN. In one case study that was significantly different to the rest, polluted anthropogenic emissions from the southern and central UK advected to the peninsula, with significant enhancements of OA, ammonium nitrate and sulfate, and black carbon. The CCN concentrations here were around 6 times higher than in the clean cases, and the cloud drop number concentrations were 3-4 times higher. Sources of ice-nucleating particles (INPs) were assessed by comparing different parameterisations used to predict INP concentrations, using measured

18. Development and characterization of a single particle laser ablation mass spectrometer (SPLAM for organic aerosol studies

Directory of Open Access Journals (Sweden)

F. Gaie-Levrel

2012-01-01

Full Text Available A single particle instrument was developed for real-time analysis of organic aerosol. This instrument, named Single Particle Laser Ablation Mass Spectrometry (SPLAM, samples particles using an aerodynamic lens system for which the theoretical performances were calculated. At the outlet of this system, particle detection and sizing are realized by using two continuous diode lasers operating at λ = 403 nm. Polystyrene Latex (PSL, sodium chloride (NaCl and dioctylphtalate (DOP particles were used to characterize and calibrate optical detection of SPLAM. The optical detection limit (DL and detection efficiency (DE were determined using size-selected DOP particles. The DE ranges from 0.1 to 90% for 100 and 350 nm DOP particles respectively and the SPLAM instrument is able to detect and size-resolve particles as small as 110–120 nm. During optical detection, particle scattered light from the two diode lasers, is detected by two photomultipliers and the detected signals are used to trigger UV excimer laser (λ = 248 nm used for one-step laser desorption ionization (LDI of individual aerosol particles. The formed ions are analyzed by a 1 m linear time-of-flight mass spectrometer in order to access to the chemical composition of individual particles. The TOF-MS detection limit for gaseous aromatic compounds was determined to be 0.85 × 10−15 kg (∼4 × 103 molecules. DOP particles were also used to test the overall operation of the instrument. The analysis of a secondary organic aerosol, formed in a smog chamber by the ozonolysis of indene, is presented as a first application of the instrument. Single particle mass spectra were obtained with an effective hit rate of 8%. Some of these mass spectra were found to be very different from one particle to another possibly reflecting chemical differences within the investigated indene SOA particles. Our study shows that an exhaustive statistical analysis, over hundreds of particles

19. Aqueous organic chemistry in the atmosphere: sources and chemical processing of organic aerosols.

Science.gov (United States)

McNeill, V Faye

2015-02-03

Over the past decade, it has become clear that aqueous chemical processes occurring in cloud droplets and wet atmospheric particles are an important source of organic atmospheric particulate matter. Reactions of water-soluble volatile (or semivolatile) organic gases (VOCs or SVOCs) in these aqueous media lead to the formation of highly oxidized organic particulate matter (secondary organic aerosol; SOA) and key tracer species, such as organosulfates. These processes are often driven by a combination of anthropogenic and biogenic emissions, and therefore their accurate representation in models is important for effective air quality management. Despite considerable progress, mechanistic understanding of some key aqueous processes is still lacking, and these pathways are incompletely represented in 3D atmospheric chemistry and air quality models. In this article, the concepts, historical context, and current state of the science of aqueous pathways of SOA formation are discussed.

20. Measurements of airborne influenza virus in aerosol particles from human coughs.

Directory of Open Access Journals (Sweden)

William G Lindsley

Full Text Available Influenza is thought to be communicated from person to person by multiple pathways. However, the relative importance of different routes of influenza transmission is unclear. To better understand the potential for the airborne spread of influenza, we measured the amount and size of aerosol particles containing influenza virus that were produced by coughing. Subjects were recruited from patients presenting at a student health clinic with influenza-like symptoms. Nasopharyngeal swabs were collected from the volunteers and they were asked to cough three times into a spirometer. After each cough, the cough-generated aerosol was collected using a NIOSH two-stage bioaerosol cyclone sampler or an SKC BioSampler. The amount of influenza viral RNA contained in the samplers was analyzed using quantitative real-time reverse-transcription PCR (qPCR targeting the matrix gene M1. For half of the subjects, viral plaque assays were performed on the nasopharyngeal swabs and cough aerosol samples to determine if viable virus was present. Fifty-eight subjects were tested, of whom 47 were positive for influenza virus by qPCR. Influenza viral RNA was detected in coughs from 38 of these subjects (81%. Thirty-five percent of the influenza RNA was contained in particles>4 µm in aerodynamic diameter, while 23% was in particles 1 to 4 µm and 42% in particles<1 µm. Viable influenza virus was detected in the cough aerosols from 2 of 21 subjects with influenza. These results show that coughing by influenza patients emits aerosol particles containing influenza virus and that much of the viral RNA is contained within particles in the respirable size range. The results support the idea that the airborne route may be a pathway for influenza transmission, especially in the immediate vicinity of an influenza patient. Further research is needed on the viability of airborne influenza viruses and the risk of transmission.

1. The effect of phase partitioning of semivolatile compounds on the measured CCN activity of aerosol particles

Directory of Open Access Journals (Sweden)

S. Romakkaniemi

2013-09-01

Full Text Available The effect of inorganic semivolatile aerosol compounds on the CCN activity of aerosol particles was studied by using a computational model for a DMT-CCN counter, a cloud parcel model for condensation kinetics and experiments to quantify the modelled results. Concentrations of water vapour and semivolatiles as well as aerosol trajectories in the CCN column were calculated by a computational fluid dynamics model. These trajectories and vapour concentrations were then used as an input for the cloud parcel model to simulate mass transfer kinetics of water and semivolatiles between aerosol particles and the gas phase. Two different questions were studied: (1 how big fraction of semivolatiles is evaporated from particles before activation in the CCN counter? (2 How much the CCN activity can be increased due to condensation of semivolatiles prior to the maximum water supersaturation in the case of high semivolatile concentration in the gas phase? The results show that, to increase the CCN activity of aerosol particles, a very high gas phase concentration (as compared to typical ambient conditions is needed. We used nitric acid as a test compound. A concentration of several ppb or higher is needed for measurable effect. In the case of particle evaporation, we used ammonium nitrate as a test compound and found that it partially evaporates before maximum supersaturation is reached in the CCN counter, thus causing an underestimation of CCN activity. The effect of evaporation is clearly visible in all supersaturations, leading to an underestimation of the critical dry diameter by 10 to 15 nanometres in the case of ammonium nitrate particles in different supersaturations. This result was also confirmed by measurements in supersaturations between 0.1 and 0.7%.

2. Aerosol black carbon quantification in the central Indo-Gangetic Plain: Seasonal heterogeneity and source apportionment

Science.gov (United States)

Vaishya, Aditya; Singh, Prayagraj; Rastogi, Shantanu; Babu, S. Suresh

2017-03-01

Two years of aerosol spectral light absorption measurements, using filter based technique, from the central Indo-Gangetic plain (IGP), Gorakhpur (26.75°N, 83.38°E, 85 m amsl), are analyzed to study their seasonal behavior and to quantify their magnitude in terms of absorbing aerosols loading and source speciation. Spectral absorption analysis reveals a four-fold enhancement in absorption in winter (W) and post-monsoon (PoM) seasons at UV wavelengths as compared to IR wavelengths on account of increased biomass burning aerosol contribution to total absorbing aerosol load. Aerosols from the biomass sources contribute 28% during W and PoM seasons as against 16% in pre-monsoon (PM) and monsoon (M) seasons to the total absorbing aerosol content. A Mode shift in the distribution of the Absorption Ångström exponent (α) from 1.3 to 1.6 from PM-M seasons to PoM-W seasons signifies change in source type of absorbing aerosols from fossil fuel to biomass burning and their relative source strength. Due to near stagnant wind conditions combined with shallow boundary layer height, where air masses travelling to the central IGP are confined to a smaller volume, in W and PoM seasons, local sources assume more prominence rather than long-range transport of aerosols. Long-term measurements of aerosols physicochemical and radiative properties from this measurement location will enhance our understanding of the complex aerosol system over the IGP and its climatic implications.

3. Aerosol number size distributions over a coastal semi urban location: Seasonal changes and ultrafine particle bursts

Energy Technology Data Exchange (ETDEWEB)

Babu, S. Suresh, E-mail: s_sureshbabu@vssc.gov.in [Space Physics Laboratory, Vikram Sarabhai Space Centre, Thiruvananthapuram 695022 (India); Kompalli, Sobhan Kumar [Space Physics Laboratory, Vikram Sarabhai Space Centre, Thiruvananthapuram 695022 (India); Moorthy, K. Krishna [Centre for Atmospheric and Oceanic Sciences, Indian Institute of Science, Bangalore 560 012 (India)

2016-09-01

Number-size distribution is one of the important microphysical properties of atmospheric aerosols that influence aerosol life cycle, aerosol-radiation interaction as well as aerosol-cloud interactions. Making use of one-yearlong measurements of aerosol particle number-size distributions (PNSD) over a broad size spectrum (~ 15–15,000 nm) from a tropical coastal semi-urban location-Trivandrum (Thiruvananthapuram), the size characteristics, their seasonality and response to mesoscale and synoptic scale meteorology are examined. While the accumulation mode contributed mostly to the annual mean concentration, ultrafine particles (having diameter < 100 nm) contributed as much as 45% to the total concentration, and thus constitute a strong reservoir, that would add to the larger particles through size transformation. The size distributions were, in general, bimodal with well-defined modes in the accumulation and coarse regimes, with mode diameters lying in the range 141 to 167 nm and 1150 to 1760 nm respectively, in different seasons. Despite the contribution of the coarse sized particles to the total number concentration being meager, they contributed significantly to the surface area and volume, especially during transport of marine air mass highlighting the role of synoptic air mass changes. Significant diurnal variation occurred in the number concentrations, geometric mean diameters, which is mostly attributed to the dynamics of the local coastal atmospheric boundary layer and the effect of mesoscale land/sea breeze circulation. Bursts of ultrafine particles (UFP) occurred quite frequently, apparently during periods of land-sea breeze transitions, caused by the strong mixing of precursor-rich urban air mass with the cleaner marine air mass; the resulting turbulence along with boundary layer dynamics aiding the nucleation. These ex-situ particles were observed at the surface due to the transport associated with boundary layer dynamics. The particle growth rates from

4. COLLABORATIVE RESEARCH: Study of Aerosol Sources and Processing at the GVAX Pantnagar Supersite

Energy Technology Data Exchange (ETDEWEB)

Worsnop, Douglas R. [Principal Investigator

2014-07-28

This project funded the participation of scientists from seven research groups, running more than thirty instruments, in the Winter Intensive Operating Period (January-February 2012) of the Clean Air for London (ClearfLo) campaign at a rural site in Detling, UK, 45 km southeast of central London. The primary science questions for the ClearfLo Winter IOP were, 1) what is the urban increment of particulate matter (PM) and other pollutants in the greater London area, and, 2) what is the contribution of solid fuel use for home heating to wintertime PM? An additional motivation for the Detling measurements was the question of whether coatings on black carbon particles enhance absorption. The following four key accomplishments have been identified so far: 1) Chemical, physical and optical characterization of PM from local and regional sources (Figures 2, 4, 5 and 6). 2) Measurement of urban increment in particulate matter and gases in London (Figure 3). 3) Measurement of optical properties and chemical composition of coatings on black carbon containing particles indicates absorption enhancement. 4) First deployment of chemical ionization instrument (MOVI-CI-TOFMS) to measure both particle-phase and gas-phase organic acids. (See final report from Joel Thornton, University of Washington, for details.) Analysis of the large dataset acquired in Detling is ongoing and will yield further key accomplishments. These measurements of urban and rural aerosol properties will contribute to improved modeling of regional aerosol emissions, and of atmospheric aging and removal. The measurement of absorption enhancement by coatings on black carbon will contribute to improved modeling of the direct radiative properties of PM.

5. Simulating Deposition of Aerosol Particles on Single Fiber Surface

Institute of Scientific and Technical Information of China (English)

FU Hai-ming; ZHU Hui

2009-01-01

The stochastic simulation method, based on the concept of control window and the numerical solution of the Langevin equation, is applied to solve the deposition problem of particles from the flowing suspensions onto a fiber collector. Using the Kuwabara model to characterize the flow field, the effects of Stokes number, interception parameter, packing density, particle size distribution on the collection efficiency, and the deposition morphology of particles onto a collector areexamined. The morphology of deposit obtained in the simulated results agrees well with experimental observations. The estimation of the initial collection efficiency through the simulations considers that the deposited particles are in good agreement with published experimental data. In addition, the collection efficiency of particles increases in a wider particle size distribution region.

6. Fine and Ultrafine Particles from Combustion Sources - Investigations with in-situ techniques

Energy Technology Data Exchange (ETDEWEB)

Pagels, Joakim

2005-04-01

Fine airborne particles are associated with adverse health effects in the human population. The aim of this research was to develop and evaluate methods for in-situ characterisation of fine and ultrafine particles and to determine their deposition in the human airways. The aim was also to increase knowledge about health and environmentally relevant properties of aerosols from biomass combustion and selected indoor sources. The methods include instrumental techniques such as Scanning Mobility Particle Sizer (SMPS), Electrical Low-Pressure Impactor (ELPI), Aerodynamic Particle Sizer (APS) and Tandem Differential Mobility Analysers (TDMA) based on volatility and hygroscopic growth. Filter samplers and impactors were used for collecting particles on substrates for subsequent chemical analysis. Emissions from local district heating plants (0.5-12 MW), based on moving grate combustion of woody fuels, were sampled with a dilution system and characterised. Particles from the indoor sources of cigarettes, incense and candles were examined in the laboratory by using an airtight 22 m{sup 3} stainless steel chamber. A set-up to determine respiratory deposition in humans was constructed. It was automatised and uses an electrical mobility spectrometer with an improved inversion algorithm to perform fast measurements of particles of different sizes in the inhaled and exhaled air. It was evaluated on human test-persons. The investigated biomass combustion sources emit high concentrations of fine and ultrafine particles. The chemical composition is dominated by KCl and K{sub 2}SO{sub 4}; Zn, Cd and Pb were also quantified. Elemental carbon was identified in particles larger than 150 nm during periods of incomplete combustion. The particle concentration depends on the fuel ash content and the combustion efficiency. The aerosol is essentially internally mixed with hygroscopic growth factors significantly higher than reported for diesel exhaust and environmental tobacco smoke. The

7. Quantitative evaluation of emission control of primary and secondary organic aerosol sources during Beijing 2008 Olympics

Science.gov (United States)

Guo, S.; Hu, M.; Guo, Q.; Zhang, X.; Schauer, J. J.; Zhang, R.

2012-12-01

To explore the primary and secondary sources of fine organic particles after the aggressive implementation of air pollution controls during 2008 Beijing Olympic Games, 12-h PM2.5 concentrations were measured at one urban and one upwind rural site during the CAREBeijing-2008 (Campaigns of Air quality REsearch in Beijing and surrounding region) summer field campaign. The PM2.5 concentrations were 72.5±43.6μg m3 and 64.3±36.2μg m-3 at the urban site and rural site, respectively, which were the lowest in recent years due to the implementation of drastic control measures and favorable weather conditions. Five primary and four secondary fine organic particle sources were quantified using a CMB (chemical mass balance) model and tracer-yield method. Compared with previous studies in Beijing, the contribution of vehicle emission increased, with diesel engines contributing 16.2±5.9% and 14.5±4.1% to the total organic carbon (OC) concentrations and gasoline vehicles accounting for 10.3±8.7% and 7.9±6.2% of the OC concentrations at two sites. Due to the implementation of emission control measures, the OC concentrations from important primary sources have been reduced, and secondary formation has become an important contributor to fine organic aerosols. Compared with the non-controlled period, primary vehicle contributions were reduced by 30% and 24% in the urban and regional area, and reductions in the contribution from coal combustion were 57% and 7%, respectively. These results demonstrate the emission control measures significantly alleviated the primary organic particle pollution in and around Beijing. However, the control effectiveness of secondary organic particles was not significant.

8. Adsorption of NO{sub 2} on carbon aerosols particles at the low ppb-level

Energy Technology Data Exchange (ETDEWEB)

Kalberer, M.; Ammann, M.; Baltensperger, U.; Gaeggeler, H.W. [Paul Scherrer Inst. (PSI), Villigen (Switzerland)

1997-09-01

The adsorption of NO{sub 2} at the low ppb-level (3-40 ppb) on carbon aerosol particles was investigated. A sticking coefficient of about 2.10{sup -4} was found, similar to that in previous studies using radioactively labeled {sup 13}NO{sub 2}. (author) 2 figs., 2 refs.

9. MISR Dark Water aerosol retrievals: operational algorithm sensitivity to particle non-sphericity

Directory of Open Access Journals (Sweden)

O. V. Kalashnikova

2013-02-01

Full Text Available The aim of this study is to theoretically investigate the sensitivity of the Multi-angle Imaging SpectroRadiometer (MISR operational (Version 22 Dark Water retrieval algorithm to aerosol non-sphericity over the global oceans under actual observing conditions, accounting for current algorithm assumptions. Non-spherical (dust aerosol models, which were introduced in Version 16 of the MISR aerosol product, improved the quality and coverage of retrievals in dusty regions. Due to the sensitivity of the retrieval to the presence of non-spherical aerosols, the MISR aerosol product has been successfully used to track the location and evolution of mineral dust plumes from the Sahara across the Atlantic, for example. However, the MISR global non-spherical aerosol optical depth (AOD fraction product has been found to have several climatological artifacts superimposed on valid detections of mineral dust, including high non-spherical fraction in the Southern Ocean and seasonally variable bands of high non-sphericity. In this paper we introduce a formal approach to examine the ability of the operational MISR Dark Water algorithm to distinguish among various spherical and non-spherical particles as a function of the variable MISR viewing geometry. We demonstrate that under the criteria currently implemented: (1 Dark Water retrieval sensitivity to particle non-sphericity decreases for AOD below about 0.1 primarily due to an unnecessarily large lower bound imposed on the uncertainty in MISR observations at low light levels, and improves when this lower bound is removed; (2 Dark Water retrievals are able to distinguish between the spherical and non-spherical particles currently used for all MISR viewing geometries when the AOD exceeds 0.1; (3 the sensitivity of the MISR retrievals to aerosol non-sphericity varies in a complex way that depends on the sampling of the scattering phase function and the contribution from multiple scattering; and (4 non

10. MISR Dark Water aerosol retrievals: operational algorithm sensitivity to particle non-sphericity

Directory of Open Access Journals (Sweden)

O. V. Kalashnikova

2013-08-01

Full Text Available The aim of this study is to theoretically investigate the sensitivity of the Multi-angle Imaging SpectroRadiometer (MISR operational (version 22 Dark Water retrieval algorithm to aerosol non-sphericity over the global oceans under actual observing conditions, accounting for current algorithm assumptions. Non-spherical (dust aerosol models, which were introduced in version 16 of the MISR aerosol product, improved the quality and coverage of retrievals in dusty regions. Due to the sensitivity of the retrieval to the presence of non-spherical aerosols, the MISR aerosol product has been successfully used to track the location and evolution of mineral dust plumes from the Sahara across the Atlantic, for example. However, the MISR global non-spherical aerosol optical depth (AOD fraction product has been found to have several climatological artifacts superimposed on valid detections of mineral dust, including high non-spherical fraction in the Southern Ocean and seasonally variable bands of high non-sphericity. In this paper we introduce a formal approach to examine the ability of the operational MISR Dark Water algorithm to distinguish among various spherical and non-spherical particles as a function of the variable MISR viewing geometry. We demonstrate the following under the criteria currently implemented: (1 Dark Water retrieval sensitivity to particle non-sphericity decreases for AOD below about 0.1 primarily due to an unnecessarily large lower bound imposed on the uncertainty in MISR observations at low light levels, and improves when this lower bound is removed; (2 Dark Water retrievals are able to distinguish between the spherical and non-spherical particles currently used for all MISR viewing geometries when the AOD exceeds 0.1; (3 the sensitivity of the MISR retrievals to aerosol non-sphericity varies in a complex way that depends on the sampling of the scattering phase function and the contribution from multiple scattering; and (4 non

11. Characteristics, sources and evolution of fine aerosol (PM1) at urban, coastal and forest background sites in Lithuania

Science.gov (United States)

Masalaite, A.; Holzinger, R.; Remeikis, V.; Röckmann, T.; Dusek, U.

2017-01-01

The chemical and isotopic composition of organic aerosol (OA) samples collected on PM1 filters was determined as a function of desorption temperature to investigate the main sources of organic carbon and the effects of photochemical processing on atmospheric aerosol. The filter samples were collected at an urban (54°38‧ N, 25°18‧ E), coastal (55°55‧ N, 21°00‧ E) and forest (55°27‧ N, 26°00' E) site in Lithuania in March 2013. They can be interpreted as winter-time samples because the monthly averaged temperature was -4 °C. The detailed chemical composition of organic compounds was analysed with a thermal desorption PTR-MS. The mass concentration of organic aerosol at the forest site was roughly by a factor of 30 lower than at the urban and coastal site. This fact could be an indication that in this cold month the biogenic secondary organic aerosol (SOA) formation was very low. Moreover, the organic aerosol collected at the forest site was more refractory and contained a larger fraction of heavy molecules with m/z > 200. The isotopic composition of the aerosol was used to differentiate the two main sources of organic aerosol in winter, i.e. biomass burning (BB) and fossil fuel (FF) combustion. Organic aerosol from biomass burning is enriched in 13C compared to OA from fossil fuel emissions. δ13COC values of the OA samples showed a positive correlation with the mass fraction of several individual organic compounds. Most of these organic compounds contained nitrogen indicating that organic nitrogen compounds formed during the combustion of biomass may be indicative of BB. Other compounds that showed negative correlations with δ13COC were possibly indicative of FF. These compounds included heavy hydrocarbons and were on the average less oxidized than the bulk organic carbon. The correlation of δ13COC and the O/C ratio was positive at low but negative at high desorption temperatures at the forest site. We propose that this might be due to

12. A Novel Aerosol Method for the Production of Hydrogel Particles

Directory of Open Access Journals (Sweden)

Diana Guzman-Villanueva

2011-01-01

Full Text Available A novel method of generating hydrogel particles for various applications including drug delivery purposes was developed. This method is based on the production of hydrogel particles from sprayed polymeric nano/microdroplets obtained by a nebulization process that is immediately followed by gelation in a crosslinking fluid. In this study, particle synthesis parameters such as type of nebulizer, type of crosslinker, air pressure, and polymer concentration were investigated for their impact on the mean particle size, swelling behavior, and morphology of the developed particles. Spherical alginate-based hydrogel particles with a mean particle size in the range from 842 to 886 nm were obtained. Using statistical analysis of the factorial design of experiment it was found that the main factors influencing the size and swelling values of the particles are the alginate concentration and the air pressure. Thus, it was demonstrated that the method described in the current study is promising for the generation of hydrogel particles and it constitutes a relatively simple and low-cost system.

13. Ice Formation by Sulfate and Sulfuric Acid Aerosol Particles under Upper-Tropospheric Conditions.

Science.gov (United States)

Chen, Yalei; Demott, Paul J.; Kreidenweis, Sonia M.; Rogers, David C.; Eli Sherman, D.

2000-11-01

Ice formation in ammoniated sulfate and sulfuric acid aerosol particles under upper-tropospheric conditions was studied using a continuous flow thermal diffusion chamber. This technique allowed for particle exposure to controlled temperatures and relative humidities for known residence times. The phase states of (NH4)2SO4 and NH4HSO4 particles were found to have important impacts on their ice formation capabilities. Dry (NH4)2SO4 particles nucleated ice only at high relative humidity (RH 94%) with respect to water at temperatures between 40° and 60°C. This result suggested either an impedance or finite time dependence to deliquescence and subsequent homogeneous freezing nucleation. Ammonium sulfate particles that entered the diffusion chamber in a liquid state froze homogeneously at relative humidities that were 10% lower than where ice nucleated on initially dry particles. Likewise, crystalline or partially crystallized (as letovicite) NH4HSO4 particles required higher relative humidities for ice nucleation than did initially liquid bisulfate particles. Liquid particles of size 0.2 m composed of either ammonium sulfate or bisulfate froze at lower relative humidity at upper-tropospheric temperatures than did 0.05-m sulfuric acid aerosol particles. Comparison of calculated homogeneous freezing point depressions suggest that size effects on freezing may be more important than the degree of ammoniation of the sulfate compound.

14. Arctic Sea Salt Aerosol from Blowing Snow and Sea Ice Surfaces - a Missing Natural Source in Winter

Science.gov (United States)

Frey, M. M.; Norris, S. J.; Brooks, I. M.; Nishimura, K.; Jones, A. E.

2015-12-01

Atmospheric particles in the polar regions consist mostly of sea salt aerosol (SSA). SSA plays an important role in regional climate change through influencing the surface energy balance either directly or indirectly via cloud formation. SSA irradiated by sunlight also releases very reactive halogen radicals, which control concentrations of ozone, a pollutant and greenhouse gas. However, models under-predict SSA concentrations in the Arctic during winter pointing to a missing source. It has been recently suggested that salty blowing snow above sea ice, which is evaporating, to be that source as it may produce more SSA than equivalent areas of open ocean. Participation in the 'Norwegian Young Sea Ice Cruise (N-ICE 2015)' on board the research vessel Lance' allowed to test this hypothesis in the Arctic sea ice zone during winter. Measurements were carried out from the ship frozen into the pack ice North of 80º N during February to March 2015. Observations at ground level (0.1-2 m) and from the ship's crows nest (30 m) included number concentrations and size spectra of SSA (diameter range 0.3-10 μm) as well as snow particles (diameter range 50-500 μm). During and after blowing snow events significant SSA production was observed. In the aerosol and snow phase sulfate is fractionated with respect to sea water, which confirms sea ice surfaces and salty snow, and not the open ocean, to be the dominant source of airborne SSA. Aerosol shows depletion in bromide with respect to sea water, especially after sunrise, indicating photochemically driven release of bromine. We discuss the SSA source strength from blowing snow in light of environmental conditions (wind speed, atmospheric turbulence, temperature and snow salinity) and recommend improved model parameterisations to estimate regional aerosol production. N-ICE 2015 results are then compared to a similar study carried out previously in the Weddell Sea during the Antarctic winter.

15. Online Aerosol Mass Spectrometry of Single Micrometer-Sized Particles Containing Poly(ethylene glycol)

Energy Technology Data Exchange (ETDEWEB)

Bogan, M J; Patton, E; Srivastava, A; Martin, S; Fergenson, D; Steele, P; Tobias, H; Gard, E; Frank, M

2006-10-25

Analysis of poly(ethylene glycol)(PEG)-containing particles by online single particle aerosol mass spectrometers equipped with laser desorption ionization (LDI) is reported. We demonstrate that PEG-containing particles are useful in the development of aerosol mass spectrometers because of their ease of preparation, low cost, and inherently recognizable mass spectra. Solutions containing millimolar quantities of PEGs were nebulized and, after drying, the resultant micrometer-sized PEG containing particles were sampled. LDI (266 nm) of particles containing NaCl and PEG molecules of average molecular weight <500 generated mass spectra reminiscent of mass spectra of PEG collected by other MS schemes including the characteristic distribution of positive ions (Na{sup +} adducts) separated by the 44 Da of the ethylene oxide units separating each degree of polymerization. PEGs of average molecular weight >500 were detected from particles that also contained t the tripeptide tyrosine-tyrosine-tyrosine or 2,5-dihydroxybenzoic acid, which were added to nebulized solutions to act as matrices to assist LDI using pulsed 266 nm and 355 nm lasers, respectively. Experiments were performed on two aerosol mass spectrometers, one reflectron and one linear, that each utilize two time-of-flight mass analyzers to detect positive and negative ions created from a single particle. PEG-containing particles are currently being employed in the optimization of our bioaerosol mass spectrometers for the application of measurements of complex biological samples, including human effluents, and we recommend that the same strategies will be of great utility to the development of any online aerosol LDI mass spectrometer platform.

16. Interaction of aerosol particles composed of protein and saltswith water vapor: hygroscopic growth and microstructural rearrangement

OpenAIRE

Mikhailov, E.; Vlasenko, S.; Niessner, R.; U. Pöschl

2004-01-01

The interaction of aerosol particles composed of the protein bovine serum albumin (BSA) and the inorganic salts sodium chloride and ammonium nitrate with water vapor has been investigated by hygroscopicity tandem differential mobility analyzer (H-TDMA) experiments complemented by transmission electron microscopy (TEM) and Köhler theory calculations (100-300nm particle size range, 298K, 960hPa). BSA was chosen as a well-defined model substance for proteins and other macromolecular compoun...

17. Fullerene Soot in Eastern China Air: Results from Soot Particle-Aerosol Mass Spectrometer

Science.gov (United States)

Wang, J.; Ge, X.; Chen, M.; Zhang, Q.; Yu, H.; Sun, Y.; Worsnop, D. R.; Collier, S.

2015-12-01

In this work, we present for the first time, the observation and quantification of fullerenes in ambient airborne particulate using an Aerodyne Soot Particle - Aerosol Mass Spectrometer (SP-AMS) deployed during 2015 winter in suburban Nanjing, a megacity in eastern China. The laser desorption and electron impact ionization techniques employed by the SP-AMS allow us to differentiate various fullerenes from other aerosol components. Mass spectrum of the identified fullerene soot is consisted by a series of high molecular weight carbon clusters (up to m/z of 2000 in this study), almost identical to the spectral features of commercially available fullerene soot, both with C70 and C60 clusters as the first and second most abundant species. This type of soot was observed throughout the entire study period, with an average mass loading of 0.18 μg/m3, accounting for 6.4% of the black carbon mass, 1.2% of the total organic mass. Temporal variation and diurnal pattern of fullerene soot are overall similar to those of black carbon, but are clearly different in some periods. Combining the positive matrix factorization, back-trajectory and analyses of the meteorological parameters, we identified the petrochemical industrial plants situating upwind from the sampling site, as the major source of fullerene soot. In this regard, our findings imply the ubiquitous presence of fullerene soot in ambient air of industry-influenced area, especially the oil and gas production regions. This study also offers new insights into the characterization of fullerenes from other environmental samples via the advanced SP-AMS technique.

18. EXACERBATION OF ATHEROSCLEROSIS FOLLOWING EXPOSURE TO VARIOUS COMBUSTION SOURCE PARTICLES

Science.gov (United States)

Exposure of ApoE knockout (ApoE-/-) mice to concentrated ambient particles (CAPs) has been shown to increase arterial plaque area and size. CAPs are a complex aerosol mixture consisting of wind-blown dust, emissions from the combustion of fossil fuels, and secondary tr...

19. Resonant fiber based aerosol particle sensor and method

DEFF Research Database (Denmark)

2013-01-01

in resonance frequency due to depositing of nano-sized particles is correlated with the mass deposited on the elongate member and the vibration frequency of the elongate member is determined by a detector. The read-out from the detector is transformed into a mass deposited on the elongate member. Particles...

20. Mass Concentration and Mineralogical Characteristics Aerosol Particles Collected at Dunhuang During ACE-Asia

Institute of Scientific and Technical Information of China (English)

2006-01-01

Measurements were performed in spring 2001 and 2002 to determine the characteristics of soil dust in the Chinese desert region of Dunhuang, one of the ground sites of the Asia-Pacific Regional Aerosol Characterization Experiment (ACE-Asia). The mean mass concentrations of total suspended particle matter during the spring of 2001 and 2002 were 317 μg m-3 and 307 μg m-3, respectively. Eleven dust storm events were observed with a mean aerosol concentration of 1095 μg m-3, while the non-dusty days with calm or weak wind speed had a background aerosol loading of 196 μg m-3 on average in the springtime.The main minerals detected in the aerosol samples by X-ray diffraction were illite, kaolinite, chlorite, quartz,feldspar, calcite and dolomite. Gypsum, halite and amphibole were also detected in a few samples. The mineralogical data also show that Asian dust is characterized by a kaolinite to chlorite (K/C) ratio lower than 1 whereas Saharan dust exhibits a K/C ratio larger than 2. Air mass back-trajectory analysis show that three families of pathways are associated with the aerosol particle transport to Dunhuang, but these have similar K/C ratios, which further demonstrates that the mineralogical characteristics of Asian dust are different from African dust.

1. Aerosol Optical Properties Measured Onboard the Ronald H. Brown During ACE Asia as a Function of Aerosol Chemical Composition and Source Region

Science.gov (United States)

Quinn, P. K.; Coffman, D. J.; Bates, T. S.; Welton, E. J.; Covert, D. S.; Miller, T. L.; Johnson, J. E.; Maria, S.; Russell, L.; Arimoto, R.

2004-01-01

During the ACE Asia intensive field campaign conducted in the spring of 2001 aerosol properties were measured onboard the R/V Ronald H. Brown to study the effects of the Asian aerosol on atmospheric chemistry and climate in downwind regions. Aerosol properties measured in the marine boundary layer included chemical composition; number size distribution; and light scattering, hemispheric backscattering, and absorption coefficients. In addition, optical depth and vertical profiles of aerosol 180 deg backscatter were measured. Aerosol within the ACE Asia study region was found to be a complex mixture resulting from marine, pollution, volcanic, and dust sources. Presented here as a function of air mass source region are the mass fractions of the dominant aerosol chemical components, the fraction of the scattering measured at the surface due to each component, mass scattering efficiencies of the individual components, aerosol scattering and absorption coefficients, single scattering albedo, Angstrom exponents, optical depth, and vertical profiles of aerosol extinction. All results except aerosol optical depth and the vertical profiles of aerosol extinction are reported at a relative humidity of 55 +/- 5%. An over-determined data set was collected so that measured and calculated aerosol properties could be compared, internal consistency in the data set could be assessed, and sources of uncertainty could be identified. By taking into account non-sphericity of the dust aerosol, calculated and measured aerosol mass and scattering coefficients agreed within overall experimental uncertainties. Differences between measured and calculated aerosol absorption coefficients were not within reasonable uncertainty limits, however, and may indicate the inability of Mie theory and the assumption of internally mixed homogeneous spheres to predict absorption by the ACE Asia aerosol. Mass scattering efficiencies of non-sea salt sulfate aerosol, sea salt, submicron particulate organic

2. LMFBR source term experiments in the Fuel Aerosol Simulant Test (FAST) facility

Energy Technology Data Exchange (ETDEWEB)

Petrykowski, J.C.; Longest, A.W.

1985-01-01

The transport of uranium dioxide (UO/sub 2/) aerosol through liquid sodium was studied in a series of ten experiments in the Fuel Aerosol Simulant Test (FAST) facility at Oak Ridge National Laboratory (ORNL). The experiments were designed to provide a mechanistic basis for evaluating the radiological source term associated with a postulated, energetic core disruptive accident (CDA) in a liquid metal fast breeder reactor (LMFBR). Aerosol was generated by capacitor discharge vaporization of UO/sub 2/ pellets which were submerged in a sodium pool under an argon cover gas. Measurements of the pool and cover gas pressures were used to study the transport of aerosol contained by vapor bubbles within the pool. Samples of cover gas were filtered to determine the quantity of aerosol released from the pool. The depth at which the aerosol was generated was found to be the most critical parameter affecting release. The largest release was observed in the baseline experiment where the sample was vaporized above the sodium pool. In the nine ''undersodium'' experiments aerosol was generated beneath the surface of the pool at depths varying from 30 to 1060 mm. The mass of aerosol released from the pool was found to be a very small fraction of the original specimen. It appears that the bulk of aerosol was contained by bubbles which collapsed within the pool. 18 refs., 11 figs., 4 tabs.

3. In-canopy gradients, composition, and sources of optically active aerosols over the Amazon forest

Science.gov (United States)

Guyon, P.; Graham, B.; Roberts, G. C.; Mayol-Bracero, O. L.; Andreae, M. O.; Artaxo, P.; Maenhaut, W.

2003-04-01

As part of the European contribution to the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA-EUSTACH), size-fractionated aerosol samples were collected at a primary rainforest site in the Brazilian Amazon during the wet and dry seasons. Daytime-nighttime segregated sampling was carried out at three different heights (above, within and below canopy level) on a 54 m meteorological tower. The samples were analyzed for up to 19 trace elements, equivalent black carbon (BCe) and mass concentrations. Additionally, measurements of scattering and absorption coefficients were performed. Absolute principal component analysis revealed that the wet and dry season aerosols contained the same three main aerosol components, namely a natural biogenic, a pyrogenic, and a soil dust component, but that these were present in different (absolute and relative) amounts. The elements related to biomass burning and soil dust generally exhibited highest concentrations above the canopy and during daytime, whilst forest-derived aerosol was more concentrated underneath the canopy and during nighttime. These variations can be largely attributed to daytime convective mixing and the formation of a shallow nocturnal boundary layer, along with the possibility of enhanced nighttime release of biogenic aerosol particles. All three components contributed significantly to light extinction, suggesting that, in addition to pyrogenic particles, biogenic and soil dust aerosols must be taken into account when modeling the physical and optical properties of aerosols in forested regions such the Amazon Basin.

4. Black carbon aerosol characterization in a coastal city in South China using a single particle soot photometer

Science.gov (United States)

Huang, Xiao-Feng; Sun, Tian-Le; Zeng, Li-Wu; Yu, Guang-He; Luan, Sheng-Ji

2012-05-01

Black carbon (BC) is the dominant light-absorbing aerosol component in the atmosphere and plays an important role in atmospheric pollution and climate change. The light-absorbing properties of BC rely on particle size, shape, composition, as well as the BC mixing state with other aerosol components, thus more thorough exploration of BC aerosol characteristics is critical in understanding its atmospheric sources and effects. In this study, a newly-developed Single Particle Soot Photometer (SP2) was deployed in Shenzhen, China, for continuous BC measurements to obtain the important information about size distribution and mixing state of BC under severe air pollution conditions of China. The mean BC mass concentrations were found to be 6.0 and 4.1 μg m-3 at an urban site (UT) in the fall and winter, respectively, while it is much lower (2.6 μg m-3) at a rural site (BG) in the fall. The mass size distributions of BC in volume equivalent diameter (VED) at the three sites showed a similar lognormal pattern, with the peak diameter at BG (222 nm) slightly larger than at the UT (210 nm) site. As to mixing state, the average percentage of internally mixed BC at the UT site was detected to be 40% and 46% in the fall and winter, respectively, while that at the BG site in the fall was only a slightly higher (47%), which implies that fresh local fossil fuel combustions were still significant at this rural site. The analysis of extremely high BC concentrations (>20 μg m-3) at UT indicates that they were a complex of comparable contributions from both local fresh emissions and regional transport under unfavorable meteorology. Other characteristics of BC aerosol and their influencing factors in Shenzhen were also discussed.

5. Particle growth by acid-catalyzed heterogeneous reactions of organic carbonyls on preexisting aerosols.

Science.gov (United States)

Jang, Myoseon; Carroll, Brian; Chandramouli, Bharadwaj; Kamens, Richard M

2003-09-01

Aerosol growth by the heterogeneous reactions of different aliphatic and alpha,beta-unsaturated carbonyls in the presence/absence of acidified seed aerosols was studied in a 2 m long flow reactor (2.5 cm i.d.) and a 0.5-m3 Teflon film bag under darkness. For the flow reactor experiments, 2,4-hexadienal, 5-methyl-3-hexen-2-one, 2-cyclohexenone, 3-methyl-2-cyclopentenone, 3-methyl-2-cyclohexenone, and octanal were studied. The carbonyls were selected based on their reactivity for acid-catalyzed reactions, their proton affinity, and their similarity to the ring-opening products from the atmospheric oxidation of aromatics. To facilitate acid-catalyzed heterogeneous hemiacetal/acetal formation, glycerol was injected along with inorganic seed aerosols into the flow reactor system. Carbonyl heterogeneous reactions were accelerated in the presence of acid catalysts (H2SO4), leading to higher aerosol yields than in their absence. Aldehydes were more reactive than ketones for acid-catalyzed reactions. The conjugated functionality also resulted in higher organic aerosol yieldsthan saturated aliphatic carbonyls because conjugation with the olefinic bond increases the basicity of the carbonyl leading to increased stability of the protonated carbonyl. Aerosol population was measured from a series of sampling ports along the length of the flow reactor using a scanning mobility particle sizer. Fourier transform infrared spectrometry of either an impacted liquid aerosol layer or direct reaction of carbonyls as a thin liquid layer on a zinc selenide FTIR disk was employed to demonstrate the direct transformation of chemical functional groups via the acid-catalyzed reactions. These results strongly indicate that atmospheric multifunctional organic carbonyls, which are created by atmospheric photooxidation reactions, can contribute significantly to secondary organic aerosol formation through acid-catalyzed heterogeneous reactions. Exploratory studies in 25- and 190-m3 outdoor chambers

6. Particle water and pH in the eastern Mediterranean: source variability and implications for nutrient availability

Science.gov (United States)

Bougiatioti, Aikaterini; Nikolaou, Panayiota; Stavroulas, Iasonas; Kouvarakis, Giorgos; Weber, Rodney; Nenes, Athanasios; Kanakidou, Maria; Mihalopoulos, Nikolaos

2016-04-01

Particle water (liquid water content, LWC) and aerosol pH are important parameters of the aerosol phase, affecting heterogeneous chemistry and bioavailability of nutrients that profoundly impact cloud formation, atmospheric composition, and atmospheric fluxes of nutrients to ecosystems. Few measurements of in situ LWC and pH, however, exist in the published literature. Using concurrent measurements of aerosol chemical composition, cloud condensation nuclei activity, and tandem light scattering coefficients, the particle water mass concentrations associated with the aerosol inorganic (Winorg) and organic (Worg) components are determined for measurements conducted at the Finokalia atmospheric observation station in the eastern Mediterranean between June and November 2012. These data are interpreted using the ISORROPIA-II thermodynamic model to predict the pH of aerosols originating from the various sources that influence air quality in the region. On average, closure between predicted aerosol water and that determined by comparison of ambient with dry light scattering coefficients was achieved to within 8 % (slope = 0.92, R2 = 0.8, n = 5201 points). Based on the scattering measurements, a parameterization is also derived, capable of reproducing the hygroscopic growth factor (f(RH)) within 15 % of the measured values. The highest aerosol water concentrations are observed during nighttime, when relative humidity is highest and the collapse of the boundary layer increases the aerosol concentration. A significant diurnal variability is found for Worg with morning and afternoon average mass concentrations being 10-15 times lower than nighttime concentrations, thus rendering Winorg the main form of particle water during daytime. The average value of total aerosol water was 2.19 ± 1.75 µg m-3, contributing on average up to 33 % of the total submicron mass concentration. Average aerosol water associated with organics, Worg, was equal to 0.56 ± 0.37 µg m-3; thus, organics

7. Impact of wild forest fires in Eastern Europe on aerosol composition and particle optical properties

Directory of Open Access Journals (Sweden)

Tymon Zielinski

2016-01-01

Full Text Available In this paper the authors discuss the changes of aerosol optical depth (AOD in the region of eastern Europe and the Baltic Sea due to wild fire episodes which occurred in the area of Belarus and Ukraine in 2002. The authors discuss how the biomass burning aerosols were advected over the Baltic area and changed the composition of aerosol ensemble for a period of several summer weeks. The air pressure situation and slow wind speeds also facilitated the development of such conditions. As a consequence very high AOD levels were recorded, by an order of 3–4 higher versus normal conditions and they significantly increased the annual averages. On particular days of August 2002 the AOD values reached a level of over 0.7. On these days fine particles fully dominated the entire ensemble of aerosol particles. They were either sulfates or smoke particles. Such situation was unique over a period of many years and it had its serious consequences for the region and especially for the Baltic Sea.

8. Characterization of new particle and secondary aerosol formation during summertime in Beijing, China

Science.gov (United States)

Zhang, Y. M.; Zhang, X. Y.; Sun, J. Y.; Lin, W. L.; Gong, S. L.; Shen, X. J.; Yang, S.

2011-07-01

Size-resolved aerosol number and mass concentrations and the mixing ratios of O3 and various trace gases were continuously measured at an urban station before and during the Beijing Olympic and Paralympic Games (5 June to 22 September, 2008). 23 new particle formation (NPF) events were identified; these usually were associated with changes in wind direction and/or rising concentrations of gas-phase precursors or after precipitation events. Most of the NPF events started in the morning and continued to noon as particles in the nucleation mode grew into the Aitken mode. From noon to midnight, the aerosols grew into the accumulation mode through condensation and coagulation. Ozone showed a gradual rise starting around 10:00 local time, reached its peak around 15:00 and then declined as the organics increased. The dominant new particle species were organics (40-75% of PM1) and sulphate; nitrate and ammonium were more minor contributors.

9. Characterization of new particle and secondary aerosol formation during summertime in Beijing, China

Energy Technology Data Exchange (ETDEWEB)

Zhang, Y. M. (Key Laboratory for Atmospheric Chemistry, Centre for Atmosphere Watch and Services, Chinese Academy of Meteorological Sciences, China Meteorological Administration, Beijing (China); Graduate Univ. of Chinese Academy of Sciences, Beijing (China)); Zhang, X. Y.; Sun, J. Y.; Lin, W. L.; Shen, X. J. (Key Laboratory for Atmospheric Chemistry, Centre for Atmosphere Watch and Services, Chinese Academy of Meteorological Sciences, China Meteorological Administration, Beijing (China)), e-mail: xiaoye@cams.cma.gov.cn; Gong, S. L. (Air Quality Research Div., Science and Technology Branch, Environment Canada, Toronto (Canada)); Yang, S. (State Key Laboratory of Numerical Modeling for Atmospheric Sciences and Geophysical Fluid Dynamics, Inst. of Atmospheric Physics, CAS, Beijing (China))

2011-07-15

Size-resolved aerosol number and mass concentrations and the mixing ratios of O{sub 3} and various trace gases were continuously measured at an urban station before and during the Beijing Olympic and Paralympic Games (5 June to 22 September, 2008). 23 new particle formation (NPF) events were identified; these usually were associated with changes in wind direction and/or rising concentrations of gas-phase precursors or after precipitation events. Most of the NPF events started in the morning and continued to noon as particles in the nucleation mode grew into the Aitken mode. From noon to midnight, the aerosols grew into the accumulation mode through condensation and coagulation. Ozone showed a gradual rise starting around 10:00 local time, reached its peak around 15:00 and then declined as the organics increased. The dominant new particle species were organics (40-75% of PM{sub 1}) and sulphate; nitrate and ammonium were more minor contributors

10. Kinetic analysis of competition between aerosol particle removal and generation by ionization air purifiers.

Science.gov (United States)

Alshawa, Ahmad; Russell, Ashley R; Nizkorodov, Sergey A

2007-04-01

Ionization air purifiers are increasingly used to remove aerosol particles from indoor air. However, certain ionization air purifiers also emit ozone. Reactions between the emitted ozone and unsaturated volatile organic compounds (VOC) commonly found in indoor air produce additional respirable aerosol particles in the ultrafine (air purifiers under conditions of a typical residential building. This model predicts that certain widely used ionization air purifiers may actually increase the mass concentration of fine and ultrafine particulates in the presence of common unsaturated VOC, such as limonene contained in many household cleaning products. This prediction is supported by an explicit observation of ultrafine particle nucleation events caused by the addition of D-limonene to a ventilated office room equipped with a common ionization air purifier.

11. In-situ observations of interstitial aerosol particles and cloud residues found in contrails

Energy Technology Data Exchange (ETDEWEB)

Stroem, J. [Stockholm Univ. (Sweden). Dept. of Meteorology

1997-12-31

In spring 1994 a series of flights were conducted in cirrus clouds and contrails over southern Germany. One of the aims of this campaign was to study the phase partitioning of aerosols and water in these clouds. To achieve this separation of particles two complementary sampling probes were mounted on the research aircraft Falcon. These are the Counterflow Virtual Impactor (CVI) or super-micrometer inlet, and the interstitial inlet or submicrometer inlet. The CVI is a device that inertially separates cloud elements larger than a certain aerodynamic size from the surrounding atmosphere into a warm, dry and particle free air. Assuming that each cloud element leaves behind only one residue particle, these measurements yield an equivalent number concentration for cloud particles having an aerodynamic diameter larger than the lower cut size of the CVI. The size distribution of the sampled aerosol and residual particles between 0.1 to 3.5 {mu}m diameter was measured by a PMS PCASP (Passive Cavity Aerosol Spectrometer) working alternatively on both inlets. The gas-phase water vapor content was measured by a cryogenic frost point mirror. (R.P.) 4 refs.

12. Transition metal associations with primary biological particles in sea spray aerosol generated in a wave channel.

Science.gov (United States)

Guasco, Timothy L; Cuadra-Rodriguez, Luis A; Pedler, Byron E; Ault, Andrew P; Collins, Douglas B; Zhao, Defeng; Kim, Michelle J; Ruppel, Matthew J; Wilson, Scott C; Pomeroy, Robert S; Grassian, Vicki H; Azam, Farooq; Bertram, Timothy H; Prather, Kimberly A

2014-01-21

In the ocean, breaking waves generate air bubbles which burst at the surface and eject sea spray aerosol (SSA), consisting of sea salt, biogenic organic species, and primary biological aerosol particles (PBAP). Our overall understanding of atmospheric biological particles of marine origin remains poor. Here, we perform a control experiment, using an aerosol time-of-flight mass spectrometer to measure the mass spectral signatures of individual particles generated by bubbling a salt solution before and after addition of heterotrophic marine bacteria. Upon addition of bacteria, an immediate increase occurs in the fraction of individual particle mass spectra containing magnesium, organic nitrogen, and phosphate marker ions. These biological signatures are consistent with 21% of the supermicrometer SSA particles generated in a previous study using breaking waves in an ocean-atmosphere wave channel. Interestingly, the wave flume mass spectral signatures also contain metal ions including silver, iron, and chromium. The nascent SSA bioparticles produced in the wave channel are hypothesized to be as follows: (1) whole or fragmented bacterial cells which bioaccumulated metals and/or (2) bacteria-derived colloids or biofilms which adhered to the metals. This study highlights the potential for transition metals, in combination with specific biomarkers, to serve as unique indicators for the presence of marine PBAP, especially in metal-impacted coastal regions.

13. The relationship between aerosol particles chemical composition and optical properties to identify the biomass burning contribution to fine particles concentration: a case study for São Paulo city, Brazil.

Science.gov (United States)

de Miranda, Regina Maura; Lopes, Fabio; do Rosário, Nilton Évora; Yamasoe, Marcia Akemi; Landulfo, Eduardo; de Fatima Andrade, Maria

2016-12-01

The air quality in the Metropolitan Area of São Paulo (MASP) is primarily determined by the local pollution source contribution, mainly the vehicular fleet, but there is a concern about the role of remote sources to the fine mode particles (PM2.5) concentration and composition. One of the most important remote sources of atmospheric aerosol is the biomass burning emissions from São Paulo state's inland and from the central and north portions of Brazil. This study presents a synergy of different measurements of atmospheric aerosol chemistry and optical properties in the MASP in order to show how they can be used as a tool to identify particles from local and remote sources. For the clear identification of the local and remote source contribution, aerosol properties measurements at surface level were combined with vertical profiles information. Over 15 days in the austral winter of 2012, particulate matter (PM) was collected using a cascade impactor and a Partisol sampler in São Paulo City. Mass concentrations were determined by gravimetry, black carbon concentrations by reflectance, and trace element concentrations by X-ray fluorescence. Aerosol optical properties were studied using a multifilter rotating shadowband radiometer (MFRSR), a Lidar system and satellite data. Optical properties, concentrations, size distributions, and elemental composition of atmospheric particles were strongly related and varied according to meteorological conditions. During the sampling period, PM mean mass concentrations were 17.4 ± 10.1 and 15.3 ± 6.9 μg/m(3) for the fine and coarse fractions, respectively. The mean aerosol optical depths at 415 nm and Ångström exponent (AE) over the whole period were 0.29 ± 0.14 and 1.35 ± 0.11, respectively. Lidar ratios reached values of 75 sr. The analyses of the impacts of an event of biomass burning smoke transport to the São Paulo city revealed significant changing on local aerosol concentrations and optical parameters

14. Sulfur Isotopic Compositions of Individual Aerosol Particles from Below and Within Stratocumulus Clouds over the Southeast Pacific Ocean During VOCALS

Science.gov (United States)

Bose, M.; Anderson, J. R.; Twohy, C. H.; Williams, P.

2012-12-01

The VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-Rex) was a large multi-national field experiment that collected data and samples from a region of the southeast Pacific with the world's largest stratocumulus cloud systems. Samples examined here are residues of cloud droplets and ambient particles from below the clouds collected during flights of the NCAR C-130 off the coast of Chile. Selected samples were studied using scanning electron microscopy (SEM) and secondary ion mass spectrometry (SIMS) in order to contribute to the understanding of the source of non-sea-salt sulfate in this region. Particles in the size range from 0.2 to 1μm diameter on holey and lacey carbon were characterized by SEM combined with energy dispersive spectrometry (EDS), thus identifying sulfur-containing particles. Subsequently, sulfur ion imaging of identified sea salt, ammonium sulfate and sodium sulfate particles was done with the Cameca Ametek NanoSIMS 50L at Arizona State University. A electrons were collected simultaneously at high mass resolution (m/Δm>10000). Each measurement typically consists of 5 to 8 frames (~5.4 min/frame). NIST barium sulfate and ammonium sulfate particles were used as isotopic standards. Preliminary analyses on a small pool of VOCALS individual particles show a wide range in sulfur isotopic compositions (δ34S = -56 to +41‰). In addition, the in-cloud particles are enriched in 32S, while the ambient particles exhibit 34S excesses. Isotopic data on a large inventory of particles is being currently acquired, which will be presented at the meeting. Data will be used to investigate sulfur sources (marine vs. continental) and the processing of aerosols through sulfate formation.

15. Differences in physical chemistry and dissolution rate of solid particle aerosols from solution pressurised inhalers.

Science.gov (United States)

Buttini, Francesca; Miozzi, Michele; Balducci, Anna Giulia; Royall, Paul G; Brambilla, Gaetano; Colombo, Paolo; Bettini, Ruggero; Forbes, Ben

2014-04-25

Solution composition alters the dynamics of beclomethasone diproprionate (BDP) particle formation from droplets emitted by pressurised metered dose inhalers (pMDIs). The hypothesis that differences in inhaler solutions result in different solid particle physical chemistry was tested using a suite of complementary calorimetric techniques. The atomisation of BDP-ethanol solutions from commercial HFA-pMDI produced aerodynamically-equivalent solid particle aerosols. However, differences in particle physico-chemistry (morphology and solvate/clathrate formation) were detected by differential scanning calorimetry (DSC), thermogravimetric analysis (TGA) and supported by hot stage microscopy (HSM). Increasing the ethanol content of the formulation from 8 to 12% (w/w), which retards the evaporation of propellant and slows the increase in droplet surface viscosity, enhanced the likelihood of particles drying with a smooth surface. The dissolution rate of BDP from the 12% (w/w) ethanol formulation-derived particles (63% dissolved over 120 min) was reduced compared to the 8% (w/w) ethanol formulation-derived particles (86% dissolved over 120 min). The addition of 0.01% (w/w) formoterol fumarate or 1.3% (w/w) glycerol to the inhaler solution modified the particles and reduced the BDP dissolution rate further to 34% and 16% dissolved in 120 min, respectively. These data provide evidence that therapeutic aerosols from apparently similar inhaler products, including those with similar aerodynamic performance, may behave non-equivalently after deposition in the lungs.

16. Impacts of new particle formation on aerosol cloud condensation nuclei (CCN activity in Shanghai: case study

Directory of Open Access Journals (Sweden)

C. Leng

2014-07-01

Full Text Available New particle formation (NPF events and their impacts on cloud condensation nuclei (CCN were investigated using continuous measurements collected in urban Shanghai from 1 to 30 April 2012. During the campaign, NPF occurred in 8 out of the 30 days and enhanced CCN number concentration (NCCN by a actor of 1.2–1.8, depending on supersaturation (SS. The NPF event on 3 April 2012 was chosen as an example to investigate the NPF influence on CCN activity. In this NPF event, secondary aerosols were produced continuously and increased PM2.5 mass concentration at a~rate of 4.33 μg cm−3 h−1, and the growth rate (GR and formation rate (FR were on average 5 nm h−1 and 0.36 cm−3 s−1, respectively. The newly formed particles grew quickly from nucleation mode (10–20 nm into CCN size range. NCCN increased rapidly at SS of 0.4–1.0% but weakly at SS of 0.2%. Correspondingly, aerosol CCN activities (fractions of activated aerosol particles in total aerosols, NCCN / NCN were significantly enhanced from 0.24–0.60 to 0.30–0.91 at SS of 0.2–1.0% due to the NPF. On the basis of the κ-Köhler theory, aerosol size distributions and chemical composition measured simultaneously were used to predict NCCN. There was a good agreement between the predicted and measured NCCN (R2 = 0.96, Npredicted / Nmeasured = 1.04. This study reveals that NPF exerts large impacts on aerosol particle abundance and size spectra, thus significantly promotes NCCN and aerosol CCN activity in this urban environment. The GR of NPF is the key factor controlling the newly formed particles to become CCN at all SS levels, whereas the FR is an effective factor only under high SS (e.g. 1.0% conditions.

17. PD-FiTE - an efficient method for calculating gas / liquid equilibria in atmospheric aerosol particles

Science.gov (United States)

Topping, D.; Lowe, D.; McFiggans, G.; Barley, M.

2009-04-01

Assessing the impact of atmospheric aerosol particles on the environment requires adequate representation of appropriate key processes within large scale models. In the absence of primary particulate material, interactions between the atmospheric gaseous components and particles means that the chemical nature of the particles is largely determined by the availability of condensable gaseous material, such as sulphuric and nitric acids, and by the ambient environmental conditions. Gas to particle mass transfer of semi-volatile components,driven by a difference in equilibrium and actual partial pressures above an aerosol particle, is an important factor in determining the evolving chemical composition of the particle and is necessary for predicting aerosol loading and composition. The design of an appropriate framework required for parameterizations of key variables is challenging. These thermodynamic frameworks are often numerically very complex, resulting in significant computational expense. Three dimensional chemical and aerosol transport models demand that computational expense be kept at a minimum,resulting in a trade-off between accuracy and efficiency. To calculate the equilibrium vapour pressure above a solution requires treatment of solution nonideality. This is manifest through activity coefficients of components pertinent to each condensing specie. However, activity coefficients are complex functions of the solution composition. Parameterisation of activity coefficients provides the main focus of this work largely because reducing the numerical complexity whilst retaining a good level of accuracy is very challenging. The approach presented here, the hybrid Partial Derivative Fitted Taylor Expansion (PDFiTE) (Topping et al 2008), builds on previously reported work, with an aim to derive parameters for an accurate and computationally efficient framework through coupling with a complex thermodynamic model. Such a reduction in complexity is important as it is

18. Biological aerosol particle concentrations and size distributions measured in pristine tropical rainforest air during AMAZE-08

OpenAIRE

J. A. Huffman; Sinha, B.; R. M. Garland; A. Snee-Pollmann; Gunthe, S. S.; Artaxo, P.; S. T. Martin; Andreae, M. O.; U. Pöschl

2012-01-01

As a part of the AMAZE-08 campaign during the wet season in the rainforest of Central Amazonia, an ultraviolet aerodynamic particle sizer (UV-APS) was operated for continuous measurements of fluorescent biological aerosol particles (FBAP). In the coarse particle size range (> 1 μm) the campaign median and quartiles of FBAP number and mass concentration were 7.3 × 104 m−3 (4.0–13.2 × 104 m&m...

19. Lung cancer mortality and exposure to atmospheric aerosol particles in Guangzhou, China

Science.gov (United States)

Tie, Xuexi; Wu, Dui; Brasseur, Guy

In recent years, China and other emerging countries have been experiencing severe air pollution problems with high concentrations of atmospheric aerosol particles. Satellite measurements indicate that the aerosol loading of the atmosphere in highly populated regions of China is about 10 times higher than, for example, in Europe and in the Eastern United States. The exposure to extremely high aerosol concentrations might lead to important human health effects, including respiratory and cardiovascular diseases as well as lung cancers. Here, we analyze 52-year historical surface measurements of haze data in the Chinese city of Guangzhou, and show that the dramatic increase in the occurrence of air pollution events between 1954 and 2006 has been followed by a large enhancement in the incidence of lung cancer.

20. Early growth dynamical implications for the steerability of stratospheric solar radiation management via sulfur aerosol particles

Science.gov (United States)

Benduhn, François; Schallock, Jennifer; Lawrence, Mark G.

2016-09-01

Aerosol growth dynamics may have implications for the steerability of stratospheric solar radiation management via sulfur particles. This paper derives a set of critical initial growth conditions that are analyzed as a function of two key parameters: the initial concentration of the injected sulfuric acid and its dilution rate with the surrounding air. Based upon this analysis, early aerosol growth dynamical regimes may be defined and classified in terms of their likelihood to serve as candidates for the controlled generation of a radiatively effective aerosol. Our results indicate that the regime that fulfills all critical conditions would require that airplane turbines be used to provide sufficient turbulence. The regime's parameter space is narrow and related to steep gradients, thus pointing to potential fine tuning requirements. More research, development, and testing would be required to refine our findings and determine their global-scale implications.

1. INTEGRAL COLLISION KERNEL FOR THE GROWTH OF AEROSOL PARTICLES

Institute of Scientific and Technical Information of China (English)

Hongyong Xie

2005-01-01

Integral collision kernel is elucidated using experimental results for titania, silica and alumina nanoparticles synthesized by FCVD process, and titania submicron particles synthesized in a tube furnace reactor. The integral collision kernel was obtained from a particle number balance equation by the integration of collision rates from the kinetic theory of dilute gases for the free-molecule regime, from the Smoluchowski theory for the continuum regime, and by a semi-empirical interpolation for the transition regime between the two limiting regimes. Comparisons have been made on particle size and the integral collision kernel, showing that the predicted integral collision kernel agreed well with the experimental results in Knudsen number range from about 1.5 to 20.

2. Simulating the evolution of soot mixing state with a particle-resolved aerosol model

CERN Document Server

Riemer, N; Zaveri, R A; Easter, R C

2008-01-01

The mixing state of soot particles in the atmosphere is of crucial importance for assessing their climatic impact, since it governs their chemical reactivity, cloud condensation nuclei activity and radiative properties. To improve the mixing state representation in models, we present a new approach, the stochastic particle-resolved model PartMC-MOSAIC, which explicitly resolves the composition of individual particles in a given population of different types of aerosol particles. This approach accurately tracks the evolution of the mixing state of particles due to emission, dilution, condensation and coagulation. To make this direct stochastic particle-based method practical, we implemented a new multiscale stochastic coagulation method. With this method we achieved optimal efficiency for applications when the coagulation kernel is highly non-uniform, as is the case for many realistic applications. PartMC-MOSAIC was applied to an idealized urban plume case representative of a large urban area to simulate the e...

3. The effect of atmospheric aerosol particles and clouds on net ecosystem exchange in the Amazon

Science.gov (United States)

Cirino, G. G.; Souza, R. A. F.; Adams, D. K.; Artaxo, P.

2014-07-01

Carbon cycling in the Amazon is closely linked to atmospheric processes and climate in the region as a consequence of the strong coupling between the atmosphere and biosphere. This work examines the effects of changes in net radiation due to atmospheric aerosol particles and clouds on the net ecosystem exchange (NEE) of CO2 in the Amazon region. Some of the major environmental factors affecting the photosynthetic activity of plants, such as air temperature and relative humidity, were also examined. An algorithm for clear-sky irradiance was developed and used to determine the relative irradiance, f, which quantifies the percentage of solar radiation absorbed and scattered due to atmospheric aerosol particles and clouds. Aerosol optical depth (AOD) was calculated from irradiances measured with the MODIS (Moderate Resolution Imaging Spectroradiometer) sensor, onboard the Terra and Aqua satellites, and was validated with ground-based AOD measurements from AERONET (Aerosol Robotic Network) sun photometers. Carbon fluxes were measured using eddy covariance technique at the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA) flux towers. Two sites were studied: the Jaru Biological Reserve (RBJ), located in Rondonia, and the Cuieiras Biological Reserve at the K34 LBA tower (located in a preserved region in the central Amazon). Analysis was performed continuously from 1999 to 2009 at K34 and from 1999 to 2002 at RBJ, and includes wet, dry and transition seasons. In the Jaru Biological Reserve, a 29% increase in carbon uptake (NEE) was observed when the AOD ranged from 0.10 to 1.5 at 550 nm. In the Cuieiras Biological Reserve, the aerosol effect on NEE was smaller, accounting for an approximate 20% increase in NEE. High aerosol loading (AOD above 3 at 550 nm) or high cloud cover leads to reductions in solar flux and strong decreases in photosynthesis up to the point where NEE approaches zero. The observed increase in NEE is attributed to an enhancement (~50%) in

4. In-situ studies on volatile jet exhaust particle emissions - impacts of fuel sulfur content and environmental conditions on nuclei-mode aerosols

Energy Technology Data Exchange (ETDEWEB)

Schroeder, F.; Baumann, R.; Petzold, A.; Busen, R.; Schulte, P.; Fiebig, M. [DLR Deutsches Zentrum fuer Luft- und Raumfahrt e.V., Wessling (Germany). Inst. fuer Physik der Atmosphaere; Brock, C.A. [Denver Univ., CO (United States). Dept. of Engineering

2000-02-01

In-situ measurements of ultrafine aerosol particle emissions were performed at cruise altitudes behind the DLR ATTAS research jet (RR M45H M501 engines) and a B737-300 aircraft (CFM56-3B1 engines). Measurements were made 0.15-20 seconds after emission as the source aircraft burned fuel with sulfur contents (FSC) of 2.6, 56 or 118 mg kg{sup -1}. Particle size distributions of from 3 to 60 nm diameter were determined using CN-counters with varying lower size detection limits. Volatile particle concentrations in the aircraft plumes strongly increased as diameter decreased toward the sizes of large molecular clusters, illustrating that apparent particle emissions are extremely sensitive to the smallest particle size detectable by the instrument used. Environmental conditions and plume age alone could influence the number of detected ultrafine (volatile) aerosols within an order of magnitude, as well. The observed volatile particle emissions decreased nonlinearly as FSC decreased to 60 mg kg{sup -1}, reaching minimum values of about 2 x 10{sup 17} kg{sup -1} and 2 x 10{sup 16} kg{sup -1} for particles >3 nm and >5 nm, respectively. Volatile particle emissions did not change significantly as FSCs were further reduced below 60 mg kg{sup -1}. Volatile particle emissions did not differ significantly between the two studied engine types. In contrast, soot particle emissions from the modern CFM56-3B1 engines were 4-5 times less (4 x 10{sup 14} kg{sup -1}) than from the older RR M45H M501 engines (1.8 x 10{sup 15} kg{sup -1}). Contrail processing has been identified as an efficient sink/quenching parameter for ultrafine particles and reduces the remaining interstitial aerosol by factors 2-10 depending on particle size.

5. Sensitivity of aerosol properties to new particle formation mechanism and to primary emissions in a continental-scale chemical transport model

Energy Technology Data Exchange (ETDEWEB)

Chang,L.S.; Schwartz, S.E.; McGraw, R.; Lewis, E.R.

2009-04-02

Four theoretical formulations of new particle formation (NPF) and one empirical formulation are used to examine the sensitivity of observable aerosol properties to NPF formulation and to properties of emitted particles in a continental-scale model for the United States over a 1-month simulation (July 2004). For each formulation the dominant source of Aitken mode particles is NPF with only a minor contribution from primary emissions, whereas for the accumulation mode both emissions and transfer of particles from the Aitken mode are important. The dominant sink of Aitken mode number is coagulation, whereas the dominant sink of accumulation mode number is wet deposition (including cloud processing), with a minor contribution from coagulation. The aerosol mass concentration, which is primarily in the accumulation mode, is relatively insensitive to NPF formulation despite order-of-magnitude differences in the Aitken mode number concentration among the different parameterizations. The dominant sensitivity of accumulation mode number concentration is to the number of emitted particles (for constant mass emission rate). Comparison of modeled aerosol properties with aircraft measurements shows, as expected, better agreement in aerosol mass concentration than in aerosol number concentration for all NPF formulations considered. These comparisons yield instances of rather accurate simulations in the planetary boundary layer, with poor model performance in the free troposphere attributed mainly to lack of representation of biomass burning and/or to long-range transport of particles from outside the model domain. Agreement between model results and measurements is improved by using smaller grid cells (12 km versus 60 km).

6. 单颗粒气溶胶质谱仪研究进展%Progress in Research of Single Particle Aerosol Mass Spectrometer

Institute of Scientific and Technical Information of China (English)

黄正旭; 李梅; 李磊; 高伟; 粘慧青; 傅忠; 董俊国; 周振

2011-01-01

大气气溶胶因其对气候和公众健康的影响而成为当今环境研究领域的中心课题.单颗粒分析是目前国际上大气气溶胶研究的一个前沿领域,该方法具有高的时间和空间分辨率,能够提供全颗粒物分析所无法提供的大量信息.利用自主研制的单颗粒气溶胶质谱仪(single particle aerosol mass spectrometer,SPAMS),对广东鹤山地区气溶胶进行在线分析.重点分析含金属颗粒的相关性、数浓度和可能的来源,并简单介绍该仪器的产业化情况.%Atmospheric aerosol has become a key issue in environmental research due to its impact on climate and public health. In atmospheric aerosol research, single particle analysis has high temporal and spatial resolution, and is a leading-edge approach. It can provide far more information beyond the capacity of bulk particle analysis. Aerosol particles in Heshan City, Guangdong, are characterized online using a self-made single particle aerosol mass spectrometer ( SPAMS). Correlation, number concentration and possible sources of the particles that contain metallic substances are analyzed. Commercialization prospect of SPAMS is briefly discussed.

7. Characterization of PM2.5 particles originating from a modern waste incineration plant by factor analysis of chemical data, mass and black carbon in ambient aerosol

DEFF Research Database (Denmark)

Aboh, Innocent Joy Kwame; Henrikson, Dag; Laursen, Jens

contribute to PM2.5 in urban air. Thus, the general problem is to characterise and identify the particle pollution, which can be attributed to gases and/or particles emitted by the waste incineration plant. For this reason aerosol samples, PM2.5, were collected and analyzed for concentrations of twenty...... are subject to restrictions are well below the allowed limits as stated by Swedish and European standards. The aim of the present work is to study the particle pollutants with emphasis on PM2.5 in the ambient air and to identify the specific contribution from the new incineration plant. Many different sources...

8. Size-resolved aerosol and cloud condensation nuclei (CCN) properties in the remote marine South China Sea - Part 1: Observations and source classification

Science.gov (United States)

Atwood, Samuel A.; Reid, Jeffrey S.; Kreidenweis, Sonia M.; Blake, Donald R.; Jonsson, Haflidi H.; Lagrosas, Nofel D.; Xian, Peng; Reid, Elizabeth A.; Sessions, Walter R.; Simpas, James B.

2017-01-01

Ship-based measurements of aerosol and cloud condensation nuclei (CCN) properties are presented for 2 weeks of observations in remote marine regions of the South China Sea/East Sea during the southwestern monsoon (SWM) season. Smoke from extensive biomass burning throughout the Maritime Continent advected into this region during the SWM, where it was mixed with anthropogenic continental pollution and emissions from heavy shipping activities. Eight aerosol types were identified using a k-means cluster analysis with data from a size-resolved CCN characterization system. Interpretation of the clusters was supplemented by additional onboard aerosol and meteorological measurements, satellite, and model products for the region. A typical bimodal marine boundary layer background aerosol population was identified and observed mixing with accumulation mode aerosol from other sources, primarily smoke from fires in Borneo and Sumatra. Hygroscopicity was assessed using the κ parameter and was found to average 0.40 for samples dominated by aged accumulation mode smoke; 0.65 for accumulation mode marine aerosol; 0.60 in an anthropogenic aerosol plume; and 0.22 during a short period that was characterized by elevated levels of volatile organic compounds not associated with biomass burning impacts. As a special subset of the background marine aerosol, clean air masses substantially scrubbed of particles were observed following heavy precipitation or the passage of squall lines, with changes in observed aerosol properties occurring on the order of minutes. Average CN number concentrations, size distributions, and κ values are reported for each population type, along with CCN number concentrations for particles that activated at supersaturations between 0.14 and 0.85 %.

9. Transmission Electron Microscopy Analysis of Submicronic Aerosol Particles Sampled at Jungfraujoch, Switzerland (CLACE-4)

Science.gov (United States)

Grobéty, B.; Lorenzo, R.

2007-05-01

Submicronic aerosol particles were collected in two sampling campaigns during CLACE-4 and -5 ("the Cloud and Aerosol Characterisation Experiment in the Free Troposphere") at the high alpine research station on top of Jungfraujoch (altitude: 3580 m.a.s.l.). The particles were deposited directly on transmission electron microscopy (TEM) grids placed in a home-made, calibrated thermophoretic sampling device. The samples were taken during periods of clear skies and temperatures below 0°C. Average sampling time was two days. The primary state of the particles was either solid, mixed solid-liquid or completely liquid. EDS spectra of solid particles without visible traces of a liquid coating contain only carbon and oxygen peaks. Mixed solid-fluid particles, however, have either carbon (C), mixed carbon-silicate (CS) or silicate (S) (probably SiO2) nuclei. The condensates remaining after evaporation of the liquid components contain sulfate (sulfur and oxygen peaks in EDS spectra), but no nitrate was found. The fraction > 500 nm is dominated by C and CS particles, the silicate particles have a narrow size distribution around 100 nm and contain, if at all, only faint sulfur peaks in their EDS spectra. The results are qualitatively consistent with analyses of samples collected during the same campaign (Weinbruch et al., 2005), but during mixed cloud events. There seem to be, however a differrence in the amount of particles with sulfate coatings, which is higher for samples taken under clear sky conditions. Weinbruch, S., Ebert, S., Worringen, A., and Brenker (2005), Identification of the ice forming fraction of the atmospheric aerosol in mixed-phase clouds by environmental scanning electron microscopy. Activity report 2005, International Foundation HFSJG.

10. Hygroscopic behaviour of aerosol particles emitted from biomass fired grate boilers

Energy Technology Data Exchange (ETDEWEB)

Rissler, Jenny; Swietlicki, Erik [Lund Univ. (Sweden). Div. of Nuclear Physics; Pagels, Joakim; Wierzbicka, Aneta; Bohgard, Mats [Lund Univ. (Sweden). Div. of Ergonomics and Aerosol Technology; Strand, Michael; Lillieblad, Lena; Sanati, Mehri [Vaexjoe Univ. (Sweden). Bioenergy Technology

2005-02-01

This study focuses on the hygroscopic properties of sub-micrometer aerosol particles emitted from two small-scale district heating combustion plants (1 and 1.5 MW) burning two types of biomass fuels (moist forest residue and pellets). The hygroscopic particle diameter growth was measured when taken from a dehydrated to a humidified state for particle diameters between 30-350 nm (dry size) using a Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA). Particles of a certain dry size all showed similar hygroscopic growth and the average diameter growth at RH=90% for 110/100 nm particles was 1.68 in the 1 MW boiler, and 1.52 in the 1.5 MW boiler. These growth factors are considerably higher in comparison to other combustion aerosol particles such as diesel exhaust, and are the result of the efficient combustion and the high concentration of alkali species in the fuel. The observed water uptake could be explained using the Zdanovskii-Stokes-Robinson (ZSR) mixing rule and a chemical composition of only potassium salts, taken from an Ion Chromatography analysis of filter sample (KCl, K{sub 2}SO{sub 4}, and K{sub 2}CO{sub 3}). Agglomerated particles collapsed and became more spherical when initially exposed to a moderately high relative humidity. When diluting with hot particle-free air, the fractal-like structures remained intact until humidified in the HTDMA. A method is presented to by which to estimate the fractal dimension of the agglomerated combustion aerosol and correct the measured mobility diameter hygroscopic growth to the more useful pro
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