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Nontoxic quantum dot research improves solar cells
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Solar cells made with low-cost, nontoxic copper-based quantum dots can achieve ... LOS ALAMOS, N.M., Dec. 10, 2013-Solar cells made with low-cost, nontoxic copper-based ...
Pulsed laser deposition of Mn doped CdSe quantum dots for improved...
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Pulsed laser deposition of Mn doped CdSe quantum dots for improved solar cell performance Citation Details In-Document Search Title: Pulsed laser deposition of Mn doped CdSe ...
'Giant' Nanocrystal Quantum Dots
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Energy Frontier Research Centers: Solid-State Lighting Science Center for Frontiers of ... 'Giant' Nanocrystal Quantum Dots HomeEnergy ResearchEFRCsSolid-State Lighting Science ...
Pulsed laser deposition of Mn doped CdSe quantum dots for improved solar cell performance
Dai, Qilin; Wang, Wenyong E-mail: email@example.com; Tang, Jinke E-mail: email@example.com; Sabio, Erwin M.
In this work, we demonstrate (1) a facile method to prepare Mn doped CdSe quantum dots (QDs) on Zn{sub 2}SnO{sub 4} photoanodes by pulsed laser deposition and (2) improved device performance of quantum dot sensitized solar cells of the Mn doped QDs (CdSe:Mn) compared to the undoped QDs (CdSe). The band diagram of photoanode Zn{sub 2}SnO{sub 4} and sensitizer CdSe:Mn QD is proposed based on the incident-photon-to-electron conversion efficiency (IPCE) data. Mn-modified band structure leads to absorption at longer wavelengths than the undoped CdSe QDs, which is due to the exchange splitting of the CdSe:Mn conduction band by the Mn dopant. Three-fold increase in the IPCE efficiency has also been observed for the Mn doped samples.
Vukmirovic, Nenad; Wang, Lin-Wang
This review covers the description of the methodologies typically used for the calculation of the electronic structure of self-assembled and colloidal quantum dots. These are illustrated by the results of their application to a selected set of physical effects in quantum dots.
Surface treatment of nanocrystal quantum dots after film deposition
Sykora, Milan; Koposov, Alexey; Fuke, Nobuhiro
Provided are methods of surface treatment of nanocrystal quantum dots after film deposition so as to exchange the native ligands of the quantum dots for exchange ligands that result in improvement in charge extraction from the nanocrystals.
'Giant' Nanocrystal Quantum Dots
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'Giant' Nanocrystal Quantum Dots - Sandia Energy Energy Search Icon Sandia Home Locations Contact Us Employee Locator Energy & Climate Secure & Sustainable Energy Future Stationary Power Energy Conversion Efficiency Solar Energy Wind Energy Water Power Supercritical CO2 Geothermal Natural Gas Safety, Security & Resilience of the Energy Infrastructure Energy Storage Nuclear Power & Engineering Grid Modernization Battery Testing Nuclear Energy Defense Waste Management Programs
TiO2 Nanotubes with a ZnO Thin Energy Barrier for Improved Current Efficiency of CdSe Quantum-Dot-Sensitized Solar Cells
Lee, W.; Kang, S. H.; Kim, J. Y.; Kolekar, G. B.; Sung, Y. E.; Han, S. H.
This paper reports the formation of a thin ZnO energy barrier between a CdSe quantum dot (Q dots) sensitizer and TiO{sub 2} nanotubes (TONTs) for improved current efficiency of Q dot-sensitized solar cells. The formation of a ZnO barrier between TONTs and the Q dot sensitizer increased the short-circuit current under illumination and also reduced the dark current in a dark environment. The power conversion efficiency of Q dot-sensitized TONT solar cells increased by 25.9% in the presence of the ZnO thin layer due to improved charge-collecting efficiency and reduced recombination.
Hybrid quantum dot-tin disulfide field-effect transistors with improved photocurrent and spectral responsivity
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Cotlet, Mircea; Huang, Yuan Zang; Chen, Jia -Shiang; Huidong Zang; Sutter, Eli A.; Sutter, Peter W.; Nam, Chang -Yong
We report an improved photosensitivity in few-layer tin disulfide (SnS2) field-effect transistors(FETs) following doping with CdSe/ZnS core/shell quantum dots(QDs). The hybrid QD-SnS2 FET devices achieve more than 500% increase in the photocurrent response compared with the starting SnS2-only FET device and a spectral responsivity reaching over 650 A/W at 400 nm wavelength. The negligible electrical conductance in a control QD-only FET device suggests that the energy transfer between QDs and SnS2 is the main mechanism responsible for the sensitization effect, which is consistent with the strong spectral overlap between QDphotoluminescence and SnS2 optical absorption as well as the large nominalmore » donor-acceptor interspacing between QD core and SnS2. Furthermore, we also find enhanced charge carrier mobility in hybrid QD-SnS2 FETs which we attribute to a reduced contact Schottky barrier width due to an elevated background charge carrier density.« less
Few Electron Quantum Dot coupling ...
Office of Scientific and Technical Information (OSTI)
Electron Quantum Dot coupling to Donor Implanted Electron Spins Martin Rudolph1. P. Harvey-Collard12, E. Nielson1, J.K. Gamble1, R. Muller1, T. Jacobson1, G. Ten-Eyck1, J. ...
Improvement of the quality of graphene-capped InAs/GaAs quantum dots
Othmen, Riadh Rezgui, Kamel; Ajlani, Hosni; Oueslati, Meherzi; Cavanna, Antonella; Madouri, Ali
In this paper, we study the transfer of graphene onto InAs/GaAs quantum dots (QDs). The graphene is first grown on Cu foils by chemical vapor deposition and then polymer Polymethyl Methacrylate (PMMA) is deposited on the top of graphene/Cu. High quality graphene sheet has been obtained by lowering the dissolving rate of PMMA using vapor processing. Uncapped as well as capped graphene InAs/GaAs QDs have been studied using optical microscopy, scanning electron microscopy, and Raman spectroscopy. We gather from this that the average shifts ?? of QDs Raman peaks are reduced compared to those previously observed in graphene and GaAs capped QDs. The encapsulation by graphene makes the indium atomic concentration intact in the QDs by the reduction of the strain effect of graphene on QDs and the migration of In atoms towards the surface. This gives us a new hetero-structure graphene�InAs/GaAs QDs wherein the graphene plays a key role as a cap layer.
NREL and Partners Demonstrate Quantum Dots that Assemble Themselves - News
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Releases | NREL and Partners Demonstrate Quantum Dots that Assemble Themselves Surprising breakthrough could bolster quantum photonics, solar cell efficiency February 8, 2013 Scientists from the U.S. Department of Energy's National Renewable Energy Laboratory and other labs have demonstrated a process whereby quantum dots can self-assemble at optimal locations in nanowires, a breakthrough that could improve solar cells, quantum computing, and lighting devices. A paper on the new technology,
Quantitative multiplexed quantum dot immunohistochemistry
Sweeney, E.; Ward, T.H.; Gray, N.; Womack, C.; Jayson, G.; Hughes, A.; Dive, C.; Byers, R.
Quantum dots are photostable fluorescent semiconductor nanocrystals possessing wide excitation and bright narrow, symmetrical, emission spectra. These characteristics have engendered considerable interest in their application in multiplex immunohistochemistry for biomarker quantification and co-localisation in clinical samples. Robust quantitation allows biomarker validation, and there is growing need for multiplex staining due to limited quantity of clinical samples. Most reported multiplexed quantum dot staining used sequential methods that are laborious and impractical in a high-throughput setting. Problems associated with sequential multiplex staining have been investigated and a method developed using QDs conjugated to biotinylated primary antibodies, enabling simultaneous multiplex staining with three antibodies. CD34, Cytokeratin 18 and cleaved Caspase 3 were triplexed in tonsillar tissue using an 8 h protocol, each localised to separate cellular compartments. This demonstrates utility of the method for biomarker measurement enabling rapid measurement of multiple co-localised biomarkers on single paraffin tissue sections, of importance for clinical trial studies.
Quantum Dot Light Emitting Diode
Keith Kahen
The project objective is to create low cost coatable inorganic light emitting diodes, composed of quantum dot emitters and inorganic nanoparticles, which have the potential for efficiencies equivalent to that of LEDs and OLEDs and lifetime, brightness, and environmental stability between that of LEDs and OLEDs. At the end of the project the Recipient shall gain an understanding of the device physics and properties of Quantum-Dot LEDs (QD-LEDs), have reliable and accurate nanocrystal synthesis routines, and have formed green-yellow emitting QD-LEDs with a device efficiency greater than 3 lumens/W, a brightness greater than 400 cd/m2, and a device operational lifetime of more than 1000 hours. Thus the aim of the project is to break the current cost-efficiency paradigm by creating novel low cost inorganic LEDs composed of inorganic nanoparticles.
Quantum Dot Light Emitting Diode
Kahen, Keith
The project objective is to create low cost coatable inorganic light emitting diodes, composed of quantum dot emitters and inorganic nanoparticles, which have the potential for efficiencies equivalent to that of LEDs and OLEDs and lifetime, brightness, and environmental stability between that of LEDs and OLEDs. At the end of the project the Recipient shall gain an understanding of the device physics and properties of Quantum-Dot LEDs (QD-LEDs), have reliable and accurate nanocrystal synthesis routines, and have formed green-yellow emitting QD-LEDs with a device efficiency greater than 3 lumens/W, a brightness greater than 400 cd/m{sup 2}, and a device operational lifetime of more than 1000 hours. Thus the aim of the project is to break the current cost-efficiency paradigm by creating novel low cost inorganic LEDs composed of inorganic nanoparticles.
Modeling of the quantum dot filling and the dark current of quantum dot infrared photodetectors
Ameen, Tarek A.; El-Batawy, Yasser M.; Abouelsaood, A. A.
A generalized drift-diffusion model for the calculation of both the quantum dot filling profile and the dark current of quantum dot infrared photodetectors is proposed. The confined electrons inside the quantum dots produce a space-charge potential barrier between the two contacts, which controls the quantum dot filling and limits the dark current in the device. The results of the model reasonably agree with a published experimental work. It is found that increasing either the doping level or the temperature results in an exponential increase of the dark current. The quantum dot filling turns out to be nonuniform, with a dot near the contacts containing more electrons than one in the middle of the device where the dot occupation approximately equals the number of doping atoms per dot, which means that quantum dots away from contacts will be nearly unoccupied if the active region is undoped.
Controlling thermal conductance through quantum dot roughening...
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Journal Article: Controlling thermal conductance through quantum dot roughening at interfaces. Citation Details ... Publication Date: 2011-01-01 OSTI Identifier: 1110382 Report ...
Promising future of quantum dots explored in conference
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Promising future of quantum dots explored Promising future of quantum dots explored in conference Researchers are gathering to reflect on two decades of quantum dot research at a special topical conference, "20 Years of Quantum Dots at Los Alamos" April 13, 2015 Quantum dot LSC devices under ultraviolet illumination. Quantum dot LSC devices under ultraviolet illumination. Contact Los Alamos National Laboratory Nancy Ambrosiano Communications Office (505) 667-0471 Email "This
Generation of even harmonics in coupled quantum dots (Journal...
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Generation of even harmonics in coupled quantum dots Citation Details In-Document Search Title: Generation of even harmonics in coupled quantum dots Using the spatial-temporal...
Thick-shell nanocrystal quantum dots
Hollingsworth, Jennifer A.; Chen, Yongfen; Klimov, Victor I.; Htoon, Han; Vela, Javier
Colloidal nanocrystal quantum dots comprising an inner core having an average diameter of at least 1.5 nm and an outer shell, where said outer shell comprises multiple monolayers, wherein at least 30% of the quantum dots have an on-time fraction of 0.80 or greater under continuous excitation conditions for a period of time of at least 10 minutes.
Shiny quantum dots brighten future of solar cells
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Shiny quantum dots brighten future of solar cells Shiny quantum dots brighten future of solar cells The project demonstrates that superior light-emitting properties of quantum dots can be applied in solar energy by helping more efficiently harvest sunlight. April 14, 2014 Quantum dot LSC devices under ultraviolet illumination. Quantum dot LSC devices under ultraviolet illumination. Contact Nancy Ambrosiano Communications Office (505) 667-0471 Email "The key accomplishment is the
Comparison of quantum confinement effects between quantum wires and dots
Li, Jingbo; Wang, Lin-Wang
Dimensionality is an important factor to govern the electronic structures of semiconductor nanocrystals. The quantum confinement energies in one-dimensional quantum wires and zero-dimensional quantum dots are quite different. Using large-scale first-principles calculations, we systematically study the electronic structures of semiconductor (including group IV, III-V, and II-VI) surface-passivated quantum wires and dots. The band-gap energies of quantum wires and dots have the same scaling with diameter for a given material. The ratio of band-gap-increases between quantum wires and dots is material-dependent, and slightly deviates from 0.586 predicted by effective-mass approximation. Highly linear polarization of photoluminescence in quantum wires is found. The degree of polarization decreases with the increasing temperature and size.
Theory Of Alkyl Terminated Silicon Quantum Dots
Reboredo, F; Galli, G
We have carried out a series of ab-initio calculations to investigate changes in the optical properties of Si quantum dots as a function of surface passivation. In particular, we have compared hydrogen passivated dots with those having alkyl groups at the surface. We find that, while on clusters with reconstructed surfaces a complete alkyl passivation is possible, steric repulsion prevents full passivation of Si dots with unreconstructed surfaces. In addition, our calculations show that steric repulsion may have a dominant effect in determining the surface structure, and eventually the stability of alkyl passivated clusters, with results dependent on the length of the carbon chain. Alkyl passivation weakly affects optical gaps of silicon quantum dots, while it substantially decreases ionization potentials and electron affinities and affect their excited state properties. On the basis of our results we propose that alkyl terminated quantum dots may be size selected taking advantage of the change in ionization potential as a function of the cluster size.
What the Blank Makes Quantum Dots Blink?
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if scientists can stop them blinking. (Photo by Antipoff, CC BY-SA 3.0) Quantum dots are nanoparticles of semiconductor that can be tuned to glow in a rainbow of colors. ...
Electron Spin Dynamics in Semiconductor Quantum Dots
Marie, X.; Belhadj, T.; Urbaszek, B.; Amand, T.; Krebs, O.; Lemaitre, A.; Voisin, P.
An electron spin confined to a semiconductor quantum dot is not subject to the classical spin relaxation mechanisms known for free carriers but it strongly interacts with the nuclear spin system via the hyperfine interaction. We show in time resolved photoluminescence spectroscopy experiments on ensembles of self assembled InAs quantum dots in GaAs that this interaction leads to strong electron spin dephasing.
First principle thousand atom quantum dot calculations
Wang, Lin-Wang; Li, Jingbo
A charge patching method and an idealized surface passivation are used to calculate the single electronic states of IV-IV, III-V, II-VI semiconductor quantum dots up to a thousand atoms. This approach scales linearly and has a 1000 fold speed-up compared to direct first principle methods with a cost of eigen energy error of about 20 meV. The calculated quantum dot band gaps are parametrized for future references.
Nonradiative Recombination Pathways in Noncarcinogenic Quantum Dot
Broader source: Energy.gov (indexed) [DOE]
Composites | Department of Energy Lead Performer: UbiQD, LLC - Los Alamos, NM DOE Total Funding: $150,000 Project Term: February 22, 2016 - November 21, 2016 Funding Type: SBIR PROJECT OBJECTIVE Quantum dots composed of I-III-VI materials such as CuInS2 offer a compelling alternative to typical semiconductor quantum-dot systems, because they have no known toxicity and can be manufactured at a much lower cost. The project proposes to evaluate the commercial viability of CuInS2/ZnS quantum
Promising future of quantum dots explored in conference
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... Los Alamos Quantum Dots for Solar, Display Technology 2:55 Los Alamos Quantum Dots for Solar, Display Technology Two for the price of one An important breakthrough reported by the ...
Nanoscale engineering boosts performance of quantum dot light...
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Quantum dots are nano-sized semiconductor particles whose emission color can be tuned by ... Quantum dots are nano-sized semiconductor particles whose emission color can be tuned by ...
Next-Generation "Giant" Quantum Dots: Performance-Engineered...
This project seeks to develop quantum-dot downconverters to be used in LED lighting. The focus will be on synthesizing red-emitting quantum dots, revealing their failure ...
Scalable quantum computer architecture with coupled donor-quantum dot qubits
Schenkel, Thomas; Lo, Cheuk Chi; Weis, Christoph; Lyon, Stephen; Tyryshkin, Alexei; Bokor, Jeffrey
A quantum bit computing architecture includes a plurality of single spin memory donor atoms embedded in a semiconductor layer, a plurality of quantum dots arranged with the semiconductor layer and aligned with the donor atoms, wherein a first voltage applied across at least one pair of the aligned quantum dot and donor atom controls a donor-quantum dot coupling. A method of performing quantum computing in a scalable architecture quantum computing apparatus includes arranging a pattern of single spin memory donor atoms in a semiconductor layer, forming a plurality of quantum dots arranged with the semiconductor layer and aligned with the donor atoms, applying a first voltage across at least one aligned pair of a quantum dot and donor atom to control a donor-quantum dot coupling, and applying a second voltage between one or more quantum dots to control a Heisenberg exchange J coupling between quantum dots and to cause transport of a single spin polarized electron between quantum dots.
Quantum Dot Tracers for Use in Engineered Geothermal
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Quantum Dot Tracers for Use in Engineered Geothermal presentation at the April 2013 peer review meeting held in Denver, Colorado.
Quantum Dot-Based Cell Motility Assay
Gu, Weiwei; Pellegrino, Teresa; Parak Wolfgang J; Boudreau,Rosanne; Le Gros, Mark A.; Gerion, Daniele; Alivisatos, A. Paul; Larabell, Carolyn A.
Because of their favorable physical and photochemical properties, colloidal CdSe/ZnS-semiconductor nanocrystals (commonly known as quantum dots) have enormous potential for use in biological imaging. In this report, we present an assay that uses quantum dots as markers to quantify cell motility. Cells that are seeded onto a homogeneous layer of quantum dots engulf and absorb the nanocrystals and, as a consequence, leave behind a fluorescence-free trail. By subsequently determining the ratio of cell area to fluorescence-free track area, we show that it is possible to differentiate between invasive and noninvasive cancer cells. Because this assay uses simple fluorescence detection, requires no significant data processing, and can be used in live-cell studies, it has the potential to be a powerful new tool for discriminating between invasive and noninvasive cancer cell lines or for studying cell signaling events involved in migration.
Exciton binding energy in semiconductor quantum dots
Pokutnii, S. I.
In the adiabatic approximation in the context of the modified effective mass approach, in which the reduced exciton effective mass {mu} = {mu}(a) is a function of the radius a of the semiconductor quantum dot, an expression for the exciton binding energy E{sub ex}(a) in the quantum dot is derived. It is found that, in the CdSe and CdS quantum dots with the radii a comparable to the Bohr exciton radii a{sub ex}, the exciton binding energy E{sub ex}(a) is substantially (respectively, 7.4 and 4.5 times) higher than the exciton binding energy in the CdSe and CdS single crystals.
Spin filtering in a double quantum dot device: Numerical renormalizati...
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Country of Publication: United States Language: English Subject: 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; MATHEMATICAL MODELS; MATHEMATICAL SOLUTIONS; QUANTUM DOTS; ...
Bilayer graphene quantum dot defined by topgates
Müller, André; Kaestner, Bernd; Hohls, Frank; Weimann, Thomas; Pierz, Klaus; Schumacher, Hans W.
We investigate the application of nanoscale topgates on exfoliated bilayer graphene to define quantum dot devices. At temperatures below 500 mK, the conductance underneath the grounded gates is suppressed, which we attribute to nearest neighbour hopping and strain-induced piezoelectric fields. The gate-layout can thus be used to define resistive regions by tuning into the corresponding temperature range. We use this method to define a quantum dot structure in bilayer graphene showing Coulomb blockade oscillations consistent with the gate layout.
Synthesis of CdSe quantum dots for quantum dot sensitized solar cell
Singh, Neetu Kapoor, Avinashi; Kumar, Vinod; Mehra, R. M.
CdSe Quantum Dots (QDs) of size 0.85 nm were synthesized using chemical route. ZnO based Quantum Dot Sensitized Solar Cell (QDSSC) was fabricated using CdSe QDs as sensitizer. The Pre-synthesized QDs were found to be successfully adsorbed on front ZnO electrode and had potential to replace organic dyes in Dye Sensitized Solar Cells (DSSCs). The efficiency of QDSSC was obtained to be 2.06 % at AM 1.5.
Single-dot optical emission from ultralow density well-isolated InP quantum dots
Ugur, A.; Hatami, F.; Masselink, W. T.; Vamivakas, A. N.; Lombez, L.; Atatuere, M.
We demonstrate a straightforward way to obtain single well-isolated quantum dots emitting in the visible part of the spectrum and characterize the optical emission from single quantum dots using this method. Self-assembled InP quantum dots are grown using gas-source molecular-beam epitaxy over a wide range of InP deposition rates, using an ultralow growth rate of about 0.01 atomic monolayers/s, a quantum-dot density of 1 dot/{mu}m{sup 2} is realized. The resulting isolated InP quantum dots embedded in an InGaP matrix are individually characterized without the need for lithographical patterning and masks on the substrate. Such low-density quantum dots show excitonic emission at around 670 nm with a linewidth limited by instrument resolution. This system is applicable as a single-photon source for applications such as quantum cryptography.
GaAsSb/GaAsN short-period superlattices as a capping layer for improved InAs quantum dot-based optoelectronics
Utrilla, A. D.; Ulloa, J. M. Guzman, A.; Hierro, A.
The application of a GaAsSb/GaAsN short-period superlattice capping layer (CL) on InAs/GaAs quantum dots (QDs) is shown to be an option for providing improved luminescence properties to this system. Separating both GaAsSb and GaAsN ternaries during the growth in 2 monolayer-thick phases solves the GaAsSbN immiscibility-related problems. Strong fluctuations in the CL composition and strain field as well as in the QD size distribution are significantly reduced, and a more regular CL interface is also obtained. Room-temperature (RT) photoluminescence (PL) is obtained for overall N contents as high as 3%, yielding PL peak wavelengths beyond 1.4 μm in samples with a type-II band alignment. High external quantum efficiency electroluminescence and photocurrent from the QD ground state are also demonstrated at RT in a single QD-layer p-i-n device. Thus, it becomes possible to combine and transfer the complementary benefits of Sb- and N-containing GaAs alloys to InAs QD-based optoelectronics.
Improving PbS Quantum Dot Solar Cell Power Conversion Efficiency to an NREL-Certified 4.4% (Fact Sheet)
Not Available
Transition metal oxide improves overall efficiency and maintains performance with inexpensive metals. A research team at the National Renewable Energy Laboratory (NREL) has demonstrated that inserting a transition metal oxide (TMO) between the lead sulfide (PbS) quantum dot (QD) layer and the metal electrode eliminates the Schottky barrier that impedes efficient hole extraction and thereby improves the overall conversion efficiency. This allows for inexpensive metals such as Al to be employed without loss of performance. n-type TMOs consisting of molybdenum oxide (MoO{sub x}) and vanadium oxide (V{sub 2}O{sub x}) were used as an efficient hole extraction layer (HEL) in heterojunction ZnO/PbS QD solar cells. A 4.4% NREL-certified device was reported based on the MoO{sub x} HEL with Al as the back contact material, representing a more than 65% efficiency improvement compared with the case of Au contacting the PbS QD layer directly. The team finds the acting mechanism of the HEL to be a dipole formed at the MoO{sub x} and PbS interface, which enhances band bending to allow efficient hole extraction from the valence band of the PbS layer by MoO{sub x}. The carrier transport to the metal anode is likely enhanced through shallow gap states in the MoO{sub x} layer.
Geometric spin manipulation in semiconductor quantum dots
Prabhakar, Sanjay Melnik, Roderick; Inomata, Akira
We propose a method to flip the spin completely by an adiabatic transport of quantum dots. We show that it is possible to flip the spin by inducing a geometric phase on the spin state of a quantum dot. We estimate the geometric spin flip time (approximately 2 ps) which turned out to be much shorter than the experimentally reported decoherence time (approximately 100 ns) that would provide an alternative means of fliping the spin before reaching decoherence. It is important that both the Rashba coupling and the Dresselhaus coupling are present for inducing a phase necessary for spin flip. If one of them is absent, the induced phase is trivial and irrelevant for spin-flip.
Research Challenge 2: Quantum Dots and Phosphors
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2: Quantum Dots and Phosphors - Sandia Energy Energy Search Icon Sandia Home Locations Contact Us Employee Locator Energy & Climate Secure & Sustainable Energy Future Stationary Power Energy Conversion Efficiency Solar Energy Wind Energy Water Power Supercritical CO2 Geothermal Natural Gas Safety, Security & Resilience of the Energy Infrastructure Energy Storage Nuclear Power & Engineering Grid Modernization Battery Testing Nuclear Energy Defense Waste Management Programs
Relaxation dynamics in correlated quantum dots
Andergassen, S.; Schuricht, D.; Pletyukhov, M.; Schoeller, H.
We study quantum many-body effects on the real-time evolution of the current through quantum dots. By using a non-equilibrium renormalization group approach, we provide analytic results for the relaxation dynamics into the stationary state and identify the microscopic cutoff scales that determine the transport rates. We find rich non-equilibrium physics induced by the interplay of the different energy scales. While the short-time limit is governed by universal dynamics, the long-time behavior features characteristic oscillations as well as an interplay of exponential and power-law decay.
Nanoscale engineering boosts performance of quantum dot light emitting
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diodes Quantum dot light emitting diodes Nanoscale engineering boosts performance of quantum dot light emitting diodes Quantum dots are nano-sized semiconductor particles whose emission color can be tuned by simply changing their dimensions. October 25, 2013 Postdoctoral researcher Young-Shin Park characterizing emission spectra of LEDs in the Los Alamos National Laboratory optical laboratory. Postdoctoral researcher Young-Shin Park characterizing emission spectra of LEDs in the Los Alamos
Co-sensitization of ZnO by CdS quantum dots in natural dye-sensitized solar cells with polymeric electrolytes to improve the cell stability
Junhom, W.; Magaraphan, R.
The CdS quantum dots (QDs) were deposited on ZnO layer by chemical bath deposition method to absorb light in the shorter wavelength region and used as photoanode in the dye sensitized solar cell (DSSCs) with natural dye extracted from Noni leaves. Microstructures of CdS-ZnO from various dipping time were characterized by XRD, FE-SEM and EDX. The results showed that the CdS is hexagonal structure and the amount of CdS increases when the dipping time increases. The maximal conversion efficiency of 0.292% was achieved by the DSSCs based on CdS QDs-sensitized ZnO film obtained from 9 min-dipping time. Furthermore, the stability of DSSCs was improved by using polymeric electrolyte. Poly (acrylic acid) (PAA) and Polyacrylamide (PAM) were introduced to CdS QDs-sensitized ZnO film from 9 min-dipping time. Each polymeric electrolyte was prepared by swelling from 0.1-2.0 %w in H2O. The maximal conversion efficiency of 0.207% was achieved for DSSCs based on CdS QDs-sensitized ZnO film with PAM 1.0% and the conversion efficiency was decreased 25% when it was left for1 hr.
Tuning Into the Right Wavelength: Quantum Dot Rainbow Increases...
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Tuning Into the Right Wavelength: Quantum Dot Rainbow Increases Solar Cell Efficiency Basic Energy Sciences (BES) BES Home About Research Facilities Science Highlights Benefits of ...
Quantum Dot Tracers for Use in Engineered Geothermal Systems...
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Project objective: To develop and demonstrate a new class of tracerssemiconductor nanoparticles(quantum dots)that offer great promise for use in characterizing fracture ...
Few Electron Quantum Dot coupling to Donor Implanted Electron...
Office of Scientific and Technical Information (OSTI)
Title: Few Electron Quantum Dot coupling to Donor Implanted Electron Spins. Abstract not provided. Authors: Rudolph, Martin ; Patrick Harvey-Collard ; Nielsen, Erik ; Gamble, John ...
Controlling quantum dot energies using submonolayer bandstructure engineering
Yu, L.; Law, S.; Wasserman, D.; Jung, D.; Lee, M. L.; Shen, J.; Cha, J. J.
We demonstrate control of energy states in epitaxially-grown quantum dot structures formed by stacked submonolayer InAs depositions via engineering of the internal bandstructure of the dots. Transmission electron microscopy of the stacked sub-monolayer regions shows compositional inhomogeneity, indicative of the presence of quantum dots. The quantum dot ground state is manipulated not only by the number of deposited InAs layers, but also by control of the thickness and material composition of the spacing layers between submonolayer InAs depositions. In this manner, we demonstrate the ability to shift the quantum dot ground state energy at 77?K from 1.38?eV to 1.88?eV. The results presented offer a potential avenue towards enhanced control of dot energies for a variety of optoelectronic applications.
Numerical simulation of optical feedback on a quantum dot lasers
Al-Khursan, Amin H.; Ghalib, Basim Abdullattif; Al-Obaidi, Sabri J.
We use multi-population rate equations model to study feedback oscillations in the quantum dot laser. This model takes into account all peculiar characteristics in the quantum dots such as inhomogeneous broadening of the gain spectrum, the presence of the excited states on the quantum dot and the non-confined states due to the presence of wetting layer and the barrier. The contribution of quantum dot groups, which cannot follow by other models, is simulated. The results obtained from this model show the feedback oscillations, the periodic oscillations which evolves to chaos at higher injection current of higher feedback levels. The frequency fluctuation is attributed mainly to wetting layer with a considerable contribution from excited states. The simulation shows that is must be not using simple rate equation models to express quantum dots working at excited state transition.
Electron states in semiconductor quantum dots
Dhayal, Suman S.; Ramaniah, Lavanya M.; Ruda, Harry E.; Nair, Selvakumar V.
In this work, the electronic structures of quantum dots (QDs) of nine direct band gap semiconductor materials belonging to the group II-VI and III-V families are investigated, within the empirical tight-binding framework, in the effective bond orbital model. This methodology is shown to accurately describe these systems, yielding, at the same time, qualitative insights into their electronic properties. Various features of the bulk band structure such as band-gaps, band curvature, and band widths around symmetry points affect the quantum confinement of electrons and holes. These effects are identified and quantified. A comparison with experimental data yields good agreement with the calculations. These theoretical results would help quantify the optical response of QDs of these materials and provide useful input for applications.
Competing interactions in semiconductor quantum dots
van den Berg, R.; Brandino, G. P.; El Araby, O.; Konik, R. M.; Gritsev, V.; Caux, J. -S.
In this study, we introduce an integrability-based method enabling the study of semiconductor quantum dot models incorporating both the full hyperfine interaction as well as a mean-field treatment of dipole-dipole interactions in the nuclear spin bath. By performing free induction decay and spin echo simulations we characterize the combined effect of both types of interactions on the decoherence of the electron spin, for external fields ranging from low to high values. We show that for spin echo simulations the hyperfine interaction is the dominant source of decoherence at short times for low fields, and competes with the dipole-dipole interactions at longer times. On the contrary, at high fields the main source of decay is due to the dipole-dipole interactions. In the latter regime an asymmetry in the echo is observed. Furthermore, the non-decaying fraction previously observed for zero field free induction decay simulations in quantum dots with only hyperfine interactions, is destroyed for longer times by the mean-field treatment of the dipolar interactions.
Competing interactions in semiconductor quantum dots
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
van den Berg, R.; Brandino, G. P.; El Araby, O.; Konik, R. M.; Gritsev, V.; Caux, J. -S.
In this study, we introduce an integrability-based method enabling the study of semiconductor quantum dot models incorporating both the full hyperfine interaction as well as a mean-field treatment of dipole-dipole interactions in the nuclear spin bath. By performing free induction decay and spin echo simulations we characterize the combined effect of both types of interactions on the decoherence of the electron spin, for external fields ranging from low to high values. We show that for spin echo simulations the hyperfine interaction is the dominant source of decoherence at short times for low fields, and competes with the dipole-dipole interactions atmore » longer times. On the contrary, at high fields the main source of decay is due to the dipole-dipole interactions. In the latter regime an asymmetry in the echo is observed. Furthermore, the non-decaying fraction previously observed for zero field free induction decay simulations in quantum dots with only hyperfine interactions, is destroyed for longer times by the mean-field treatment of the dipolar interactions.« less
RKKY interaction in a chirally coupled double quantum dot system
Heine, A. W.; Tutuc, D.; Haug, R. J.; Zwicknagl, G.; Schuh, D.; Wegscheider, W.
The competition between the Kondo effect and the Ruderman-Kittel-Kasuya-Yoshida (RKKY) interaction is investigated in a double quantum dots system, coupled via a central open conducting region. A perpendicular magnetic field induces the formation of Landau Levels which in turn give rise to the so-called Kondo chessboard pattern in the transport through the quantum dots. The two quantum dots become therefore chirally coupled via the edge channels formed in the open conducting area. In regions where both quantum dots exhibit Kondo transport the presence of the RKKY exchange interaction is probed by an analysis of the temperature dependence. The thus obtained Kondo temperature of one dot shows an abrupt increase at the onset of Kondo transport in the other, independent of the magnetic field polarity, i.e. edge state chirality in the central region.
Kondo and mixed-valence regimes in multilevel quantum dots
Chudnovskiy, A. L.; Ulloa, S. E.
We investigate the dependence of the ground state of a multilevel quantum dot on the coupling to an external fermionic system and on the interactions in the dot. As the coupling to the external system increases, the rearrangement of the effective energy levels in the dot signals the transition from the Kondo regime to a mixed-valence (MV) regime. The MV regime in a two-level dot is characterized by an intrinsic mixing of the levels in the dot, resulting in nonperturbative subtunneling and supertunneling phenomena that strongly influence the Kondo effect.
Photocurrent extraction efficiency in colloidal quantum dot photovoltaics
Kemp, K. W.; Wong, C. T. O.; Hoogland, S. H.; Sargent, E. H.
The efficiency of photocurrent extraction was studied directly inside operating Colloidal Quantum Dot (CQD) photovoltaic devices. A model was derived from first principles for a thin film p-n junction with a linearly spatially dependent electric field. Using this model, we were able to clarify the origins of recent improvement in CQD solar cell performance. From current-voltage diode characteristics under 1 sun conditions, we extracted transport lengths ranging from 39 nm to 86 nm for these materials. Characterization of the intensity dependence of photocurrent extraction revealed that the dominant loss mechanism limiting the transport length is trap-mediated recombination.
A triple quantum dot based nano-electromechanical memory device
Pozner, R.; Lifshitz, E.; Peskin, U.
Colloidal quantum dots (CQDs) are free-standing nano-structures with chemically tunable electronic properties. This tunability offers intriguing possibilities for nano-electromechanical devices. In this work, we consider a nano-electromechanical nonvolatile memory (NVM) device incorporating a triple quantum dot (TQD) cluster. The device operation is based on a bias induced motion of a floating quantum dot (FQD) located between two bound quantum dots (BQDs). The mechanical motion is used for switching between two stable states, "ON" and "OFF" states, where ligand-mediated effective interdot forces between the BQDs and the FQD serve to hold the FQD in each stable position under zero bias. Considering realistic microscopic parameters, our quantum-classical theoretical treatment of the TQD reveals the characteristics of the NVM.
Quantum dot conjugates in a sub-micrometer fluidic channel
Stavis, Samuel M.; Edel, Joshua B.; Samiee, Kevan T.; Craighead, Harold G.
A nanofluidic channel fabricated in fused silica with an approximately 500 nm square cross section was used to isolate, detect and identify individual quantum dot conjugates. The channel enables the rapid detection of every fluorescent entity in solution. A laser of selected wavelength was used to excite multiple species of quantum dots and organic molecules, and the emission spectra were resolved without significant signal rejection. Quantum dots were then conjugated with organic molecules and detected to demonstrate efficient multicolor detection. PCH was used to analyze coincident detection and to characterize the degree of binding. The use of a small fluidic channel to detect quantum dots as fluorescent labels was shown to be an efficient technique for multiplexed single molecule studies. Detection of single molecule binding events has a variety of applications including high throughput immunoassays.
Quantum dot conjugates in a sub-micrometer fluidic channel
Stavis, Samuel M.; Edel, Joshua B.; Samiee, Kevan T.; Craighead, Harold G.
A nanofluidic channel fabricated in fused silica with an approximately 500 nm square cross section was used to isolate, detect and identify individual quantum dot conjugates. The channel enables the rapid detection of every fluorescent entity in solution. A laser of selected wavelength was used to excite multiple species of quantum dots and organic molecules, and the emission spectra were resolved without significant signal rejection. Quantum dots were then conjugated with organic molecules and detected to demonstrate efficient multicolor detection. PCH was used to analyze coincident detection and to characterize the degree of binding. The use of a small fluidic channel to detect quantum dots as fluorescent labels was shown to be an efficient technique for multiplexed single molecule studies. Detection of single molecule binding events has a variety of applications including high throughput immunoassays.
Synthesis of Non-blinking Semiconductor Quantum Dots Emitting...
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Our previous work demonstrates that Quasi-Type II CdSeCdS core-shell quantum dots with ... synthesized to reduce cadmium exposure for applications in the biological environment. ...
Los Alamos researchers unravel the mystery of quantum dot blinking
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Researchers unravel the mystery of quantum dot blinking Los Alamos researchers unravel the mystery of quantum dot blinking Most exciting is that the Los Alamos researchers have shown that blinking can be controlled and even completely suppressed electrochemically. November 9, 2011 Los Alamos National Laboratory sits on top of a once-remote mesa in northern New Mexico with the Jemez mountains as a backdrop to research and innovation covering multi-disciplines from bioscience, sustainable energy
Deformation potentials of CdSe quantum dots
Li, Jingbo; Wang, Lin-Wang
The size dependent deformation potentials of CdSe quantum dots are studied by first principle and semi-empirical pseudopotentials calculations. They find that the amplitude of the quantum dot deformation potential is only slightly larger than the bulk value, and this increase is mostly caused by the off {Lambda} point deformation potentials in the bulk, which are larger in amplitude than the {Lambda} point deformation potential.
Los Alamos Quantum Dots for Solar, Display Technology
Klimov, Victor
Quantum dots are ultra-small bits of semiconductor matter that can be synthesized with nearly atomic precision via modern methods of colloidal chemistry. Their emission color can be tuned by simply varying their dimensions. Color tunability is combined with high emission efficiencies approaching 100 percent. These properties have recently become the basis of a new technology – quantum dot displays – employed, for example, in the newest generation of e-readers and video monitors.
On-chip generation and guiding of quantum light from a site-controlled quantum dot
Jamil, Ayesha; Farrer, Ian; Griffiths, Jonathan P.; Jones, Geb A. C.; Ritchie, David A.; Skiba-Szymanska, Joanna; Kalliakos, Sokratis; Ward, Martin B.; Ellis, David J. P.; Shields, Andrew J.; Schwagmann, Andre; Brody, Yarden; Cambridge Research Laboratory, Toshiba Research Europe Limited, 208 Science Park, Milton Road, Cambridge, CB4 0GZ
We demonstrate the emission and routing of single photons along a semiconductor chip originating from carrier recombination in an actively positioned InAs quantum dot. Device�scale arrays of quantum dots are formed by a two�step regrowth process. We precisely locate the propagating region of a unidirectional photonic crystal waveguide with respect to the quantum dot nucleation site. Under pulsed optical excitation, the multiphoton emission probability from the waveguide's exit is 12%?�?5% before any background correction. Our results are a major step towards the deterministic integration of a quantum emitter with the waveguiding components of photonic quantum circuits.
Zeno-logic applications of semiconductor quantum dots
Schneebeli, L.; Peyghambarian, N.; Feldtmann, T.; Kira, M.; Koch, S. W.
Microscopic calculations show that CdSe-based semiconductor quantum dots with confined exciton and biexciton states are suitable candidates for Zeno-logic applications. The frequencies of the control and signal fields are chosen to guarantee very high transmission of the individual beams. If both fields are present simultaneously, they are strongly absorbed due to efficient ground-state-to-biexciton transitions. The optical Bloch equations for a three-level quantum-dot model with self-consistent light-matter coupling are solved numerically. The influence of dephasing and/or inhomogeneous dot distributions is analyzed and the conditions for satisfactory device operation are identified.
Surface Induced Magnetism in Quantum Dots
Meulenberg, R W; Lee, J I
The study of nanometer sized semiconductor crystallites, also known as quantum dots (QDs), has seen rapid advancements in recent years in scientific disciplines ranging from chemistry, physics, biology, materials science, and engineering. QD materials of CdSe, ZnSe, InP, as well as many others, can be prepared in the size range of 1-10 nm producing uniform, nearly monodisperse materials that are typically coated with organic molecules [1-3]. The strength of charge carrier confinement, which dictates the size-dependent properties, in these QDs depends on the nature of the material and can be correlated to the Bohr radius for the system of interest. For instance, the Bohr radius for CdSe is {approx} 5 nm, while in the more covalent structure of InP, the Bohr radius approaches {approx} 10 nm. The study of CdSe QDs has been particularly extensive during the last decade because they exhibit unique and tunable optical properties and are readily synthesized with high-crystallinity and narrow size dispersions. Although the core electronic properties of CdSe are explained in terms of the quantum confinement model, experimental efforts to elucidate the surface structure of these materials have been limited. Typically, colloidal CdSe QDs are coated with an organic surfactant, which typically consists of an organo-phosphine, -thiol, or -amine, that has the function of energetically relaxing defect states via coordination to partially coordinated surface atoms. The organic surfactant also acts to enhance carrier confinement and prevent agglomeration of the particles. Chemically, it has been shown that the bonding of the surfactant to the CdSe QD occurs through Cd atoms resulting cleavage of the Se atoms and formation of a Cd-rich (i.e. non-stoichiometric) particle [5].
Effect of carrier dynamics and temperature on two-state lasing in semiconductor quantum dot lasers
Korenev, V. V. Savelyev, A. V.; Zhukov, A. E.; Omelchenko, A. V.; Maximov, M. V.
It is analytically shown that the both the charge carrier dynamics in quantum dots and their capture into the quantum dots from the matrix material have a significant effect on two-state lasing phenomenon in quantum dot lasers. In particular, the consideration of desynchronization in electron and hole capture into quantum dots allows one to describe the quenching of ground-state lasing observed at high injection currents both qualitatevely and quantitatively. At the same time, an analysis of the charge carrier dynamics in a single quantum dot allowed us to describe the temperature dependences of the emission power via the ground- and excited-state optical transitions of quantum dots.
Analysis of the efficiency of intermediate band solar cells based on quantum dot supercrystals
Heshmati, S; Golmohammadi, S; Abedi, K; Taleb, H
We have studied the influence of the quantum-dot (QD) width and the quantum-dot conduction band (QD-CB) offset on the efficiency of quantum-dot intermediate band solar cells (QD-IBSCs). Simulation results demonstrate that with increasing QD-CB offset and decreasing QD width, the maximum efficiency is achieved. (laser applications and other topics in quantum electronics)
Mid-Infrared Quantum-Dot Quantum Cascade Laser: A Theoretical Feasibility Study
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Michael, Stephan; Chow, Weng; Schneider, Hans
In the framework of a microscopic model for intersubband gain from electrically pumped quantum-dot structures we investigate electrically pumped quantum-dots as active material for a mid-infrared quantum cascade laser. Our previous calculations have indicated that these structures could operate with reduced threshold current densities while also achieving a modal gain comparable to that of quantum well active materials. We study the influence of two important quantum-dot material parameters, here, namely inhomogeneous broadening and quantum-dot sheet density, on the performance of a proposed quantum cascade laser design. In terms of achieving a positive modal net gain, a high quantum-dot density canmore » compensate for moderately high inhomogeneous broadening, but at a cost of increased threshold current density. By minimizing quantum-dot density with presently achievable inhomogeneous broadening and total losses, significantly lower threshold densities than those reported in quantum-well quantum-cascade lasers are predicted by our theory.« less
Quantum Hall effect in semiconductor systems with quantum dots and antidots
Beltukov, Ya. M.; Greshnov, A. A.
The integer quantum Hall effect in systems of semiconductor quantum dots and antidots is studied theoretically as a factor of temperature. It is established that the conditions for carrier localization in quantum-dot systems favor the observation of the quantum Hall effect at higher temperatures than in quantum-well systems. The obtained numerical results show that the fundamental plateau corresponding to the transition between the ground and first excited Landau levels can be retained up to a temperature of T ∼ 50 K, which is an order of magnitude higher than in the case of quantum wells. Implementation of the quantum Hall effect at such temperatures requires quantum-dot systems with controllable characteristics, including the optimal size and concentration and moderate geometrical and composition fluctuations. In addition, ordered arrangement is desirable, hence quantum antidots are preferable.
Intermediate-band photosensitive device with quantum dots having tunneling barrier embedded in organic matrix
Forrest, Stephen R.
A plurality of quantum dots each have a shell. The quantum dots are embedded in an organic matrix. At least the quantum dots and the organic matrix are photoconductive semiconductors. The shell of each quantum dot is arranged as a tunneling barrier to require a charge carrier (an electron or a hole) at a base of the tunneling barrier in the organic matrix to perform quantum mechanical tunneling to reach the respective quantum dot. A first quantum state in each quantum dot is between a lowest unoccupied molecular orbital (LUMO) and a highest occupied molecular orbital (HOMO) of the organic matrix. Wave functions of the first quantum state of the plurality of quantum dots may overlap to form an intermediate band.
Thick-shell nanocrystal quantum dots (Patent) | SciTech Connect
Office of Scientific and Technical Information (OSTI)
Title: Thick-shell nanocrystal quantum dots Colloidal nanocrystal quantum dots comprising an inner core having an average diameter of at least 1.5 nm and an outer shell, where said ...
R&D Magazine: Windows into Solar Power Sources with Quantum Dots
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R&D Magazine: Windows into Solar Power Sources with Quantum Dots R&D Magazine: Windows into Solar Power Sources with Quantum Dots A luminescent solar concentrator is an emerging ...
Kondo effect in coupled quantum dots under magnetic fields
Aono, Tomosuke; Eto, Mikio
The Kondo effect in coupled quantum dots is investigated theoretically under magnetic fields. We show that the magnetoconductance (MC) illustrates the peak structures of Kondo resonant spectra. When the dot-dot tunneling coupling V{sub C} is smaller than the dot-lead coupling {Delta} (level broadening), Kondo resonant levels appear at the Fermi level (E{sub F}). The Zeeman splitting of the levels weakens the Kondo effect, which results in a negative MC. When V{sub C} is larger than {Delta}, the Kondo resonances form bonding and antibonding levels, located below and above E{sub F}, respectively. We observe a positive MC since the Zeeman splitting increases the overlap between the levels at E{sub F}. In the presence of antiferromagnetic spin coupling between the dots, the sign of the MC can change as a function of the gate voltage.
Generation of even harmonics in coupled quantum dots
Guo Shifang; Duan Suqing; Yang Ning; Chu Weidong; Zhang Wei
Using the spatial-temporal symmetry principle we developed recently, we propose an effective scheme for even-harmonics generation in coupled quantum dots. The relative intensity of odd and even harmonic components in the emission spectrum can be controlled by tuning the dipole couplings among the dots, which can be realized in experiments by careful design of the nanostructures. In particular, pure 2nth harmonics and (2n+1)th harmonics (where n is an integer) can be generated simultaneously with polarizations in two mutual perpendicular directions in our systems. An experimental design of the coupled dots system is presented.
A prototype silicon double quantum dot with dispersive microwave readout
Schmidt, A. R. Henry, E.; Namaan, O.; Siddiqi, I.; Lo, C. C.; Wang, Y.-T.; Bokor, J.; Yablonovitch, E.; Li, H.; Greenman, L.; Whaley, K. B.; Schenkel, T.
We present a unique design and fabrication process for a lateral, gate-confined double quantum dot in an accumulation mode metal-oxide-semiconductor (MOS) structure coupled to an integrated microwave resonator. All electrostatic gates for the double quantum dot are contained in a single metal layer, and use of the MOS structure allows for control of the location of the two-dimensional electron gas via the location of the accumulation gates. Numerical simulations of the electrostatic confinement potential are performed along with an estimate of the coupling of the double quantum dot to the microwave resonator. Prototype devices are fabricated and characterized by transport measurements of electron confinement and reflectometry measurements of the microwave resonator.
QCAD simulation and optimization of semiconductor double quantum dots
Nielsen, Erik; Gao, Xujiao; Kalashnikova, Irina; Muller, Richard Partain; Salinger, Andrew Gerhard; Young, Ralph Watson
We present the Quantum Computer Aided Design (QCAD) simulator that targets modeling quantum devices, particularly silicon double quantum dots (DQDs) developed for quantum qubits. The simulator has three di erentiating features: (i) its core contains nonlinear Poisson, e ective mass Schrodinger, and Con guration Interaction solvers that have massively parallel capability for high simulation throughput, and can be run individually or combined self-consistently for 1D/2D/3D quantum devices; (ii) the core solvers show superior convergence even at near-zero-Kelvin temperatures, which is critical for modeling quantum computing devices; (iii) it couples with an optimization engine Dakota that enables optimization of gate voltages in DQDs for multiple desired targets. The Poisson solver includes Maxwell- Boltzmann and Fermi-Dirac statistics, supports Dirichlet, Neumann, interface charge, and Robin boundary conditions, and includes the e ect of dopant incomplete ionization. The solver has shown robust nonlinear convergence even in the milli-Kelvin temperature range, and has been extensively used to quickly obtain the semiclassical electrostatic potential in DQD devices. The self-consistent Schrodinger-Poisson solver has achieved robust and monotonic convergence behavior for 1D/2D/3D quantum devices at very low temperatures by using a predictor-correct iteration scheme. The QCAD simulator enables the calculation of dot-to-gate capacitances, and comparison with experiment and between solvers. It is observed that computed capacitances are in the right ballpark when compared to experiment, and quantum con nement increases capacitance when the number of electrons is xed in a quantum dot. In addition, the coupling of QCAD with Dakota allows to rapidly identify which device layouts are more likely leading to few-electron quantum dots. Very efficient QCAD simulations on a large number of fabricated and proposed Si DQDs have made it possible to provide fast feedback for design
Self-organized formation of quantum dots of a material on a substrate
Zhang, Zhenyu; Wendelken, John F.; Chang, Ming-Che; Pai, Woei Wu
Systems and methods are described for fabricating arrays of quantum dots. A method for making a quantum dot device, includes: forming clusters of atoms on a substrate; and charging the clusters of atoms such that the clusters of atoms repel one another. The systems and methods provide advantages because the quantum dots can be ordered with regard to spacing and/or size.
Optical control of the emission direction of a quantum dot
Luxmoore, I. J.; Wasley, N. A.; Fox, A. M.; Skolnick, M. S.; Ramsay, A. J.; Thijssen, A. C. T.; Oulton, R.; Hugues, M.; CNRS-CRHEA, rue Bernard Gr�gory, 06560 Valbonne
Using the helicity of a non-resonant excitation laser, control over the emission direction of an InAs/GaAs quantum dot is demonstrated. The quantum dot is located off-center in a crossed-waveguide structure, such that photons of opposite circular polarization are emitted into opposite waveguide directions. By preferentially exciting spin-polarized excitons, the direction of emission can therefore be controlled. The directional control is quantified by using the ratio of the intensity of the light coupled into the two waveguides, which reaches a maximum of �35%.
Quantum-dot based nanothermometry in optical plasmonic recording media
Maestro, Laura Martinez; Zhang, Qiming; Li, Xiangping; Gu, Min; Jaque, Daniel
We report on the direct experimental determination of the temperature increment caused by laser irradiation in a optical recording media constituted by a polymeric film in which gold nanorods have been incorporated. The incorporation of CdSe quantum dots in the recording media allowed for single beam thermal reading of the on-focus temperature from a simple analysis of the two-photon excited fluorescence of quantum dots. Experimental results have been compared with numerical simulations revealing an excellent agreement and opening a promising avenue for further understanding and optimization of optical writing processes and media.
Statistical theory of Coulomb blockade oscillations: Quantum chaos in quantum dots
Jalabert, R.A.; Stone, A.D.; Alhassid, Y. (Center for Theoretical Physics, Sloane Physics Laboratory, Yale University, New Haven, Connecticut 06511 (United States))
We develop a statistical theory of the amplitude of Coulomb blockade oscillations in semiconductor quantum dots based on the hypothesis that chaotic dynamics in the dot potential leads to behavior described by random-matrix theory. Breaking time-reversal symmetry is predicted to cause an experimentally observable change in the distribution of amplitudes. The theory is tested numerically and good agreement is found.
Out-of-Equilibrium Kondo Effect in Double Quantum Dots
Aguado, Ramon; Langreth, David C.
The out-of-equilibrium transport properties of a double quantum dot system in the Kondo regime are studied theoretically by means of a two-impurity Anderson Hamiltonian with interimpurity hopping. The Hamiltonian is solved by means of a nonequilibrium generalization of the slave-boson mean-field theory. It is demonstrated that measurements of the differential conductance dI/dV , for appropriate values of voltages and tunneling couplings, can give a direct observation of the coherent superposition between the many-body Kondo states of each dot. For large voltages and arbitrarily large interdot tunneling, there is a critical voltage above which the physical behavior of the system again resembles that of two decoupled quantum dots. (c) 2000 The American Physical Society.
Suppression of low-frequency charge noise in gates-defined GaAs quantum dots
You, Jie; Li, Hai-Ou E-mail: email@example.com; Wang, Ke; Cao, Gang; Song, Xiang-Xiang; Xiao, Ming; Guo, Guo-Ping E-mail: email@example.com
To reduce the charge noise of a modulation-doped GaAs/AlGaAs quantum dot, we have fabricated shallow-etched GaAs/AlGaAs quantum dots using the wet-etching method to study the effects of two-dimensional electron gas (2DEG) underneath the metallic gates. The low-frequency 1/f noise in the Coulomb blockade region of the shallow-etched quantum dot is compared with a non-etched quantum dot on the same wafer. The average values of the gate noise are approximately 0.5 μeV in the shallow-etched quantum dot and 3 μeV in the regular quantum dot. Our results show the quantum dot low-frequency charge noise can be suppressed by the removal of the 2DEG underneath the metallic gates, which provides an architecture for noise reduction.
High Efficiency Colloidal Quantum Dot Phosphors
Kahen, Keith
The project showed that non-Cd containing, InP-based nanocrystals (semiconductor materials with dimensions of ~6 nm) have high potential for enabling next-generation, nanocrystal-based, on chip phosphors for solid state lighting. Typical nanocrystals fall short of the requirements for on chip phosphors due to their loss of quantum efficiency under the operating conditions of LEDs, such as, high temperature (up to 150 �C) and high optical flux (up to 200 W/cm2). The InP-based nanocrystals invented during this project maintain high quantum efficiency (>80%) in polymer-based films under these operating conditions for emission wavelengths ranging from ~530 to 620 nm. These nanocrystals also show other desirable attributes, such as, lack of blinking (a common problem with nanocrystals which limits their performance) and no increase in the emission spectral width from room to 150 �C (emitters with narrower spectral widths enable higher efficiency LEDs). Prior to these nanocrystals, no nanocrystal system (regardless of nanocrystal type) showed this collection of properties; in fact, other nanocrystal systems are typically limited to showing only one desirable trait (such as high temperature stability) but being deficient in other properties (such as high flux stability). The project showed that one can reproducibly obtain these properties by generating a novel compositional structure inside of the nanomaterials; in addition, the project formulated an initial theoretical framework linking the compositional structure to the list of high performance optical properties. Over the course of the project, the synthetic methodology for producing the novel composition was evolved to enable the synthesis of these nanomaterials at a cost approximately equal to that required for forming typical conventional nanocrystals. Given the above results, the last major remaining step prior to scale up of the nanomaterials is to limit the oxidation of these materials during the tens of
The emission wavelength dependent photoluminescence lifetime of the N-doped graphene quantum dots
Deng, Xingxia; Sun, Jing; Yang, Siwei; Ding, Guqiao; Shen, Hao; Zhou, Wei; Lu, Jian; Wang, Zhongyang
Aromatic nitrogen doped graphene quantum dots were investigated by steady-state and time-resolved photoluminescence (PL) techniques. The PL lifetime was found to be dependent on the emission wavelength and coincident with the PL spectrum, which is different from most semiconductor quantum dots and fluorescent dyes. This result shows the synergy and competition between the quantum confinement effect and edge functional groups, which may have the potential to guide the synthesis and expand the applications of graphene quantum dots.
NREL Certifies First All-Quantum-Dot Photovoltaic Cell; Demonstrates Stability, Performance (Fact Sheet)
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Researchers at the National Renewable Energy Laboratory (NREL) have certified the first all-quantum-dot photovoltaic cell, which was based on lead sulfide and demonstrated reasonable quantum dot solar cell performance for an initial efficiency measurement along with good stability. The certified open-circuit voltage of the quantum dot cell is greater than that possible from bulk lead sulfide because of quantum confinement.
Approaches to Future Generation Photovoltaics and Solar Fuels: Quantum Dots, Arrays, and Quantum Dot Solar Cells
Semonin, O.; Luther, J.; Beard, M.; Johnson, J.; Gao, J.; Nozik, A.
One potential, long-term approach to more efficient and lower cost future generation solar cells for solar electricity and solar fuels is to utilize the unique properties of quantum dots (QDs) to control the relaxation pathways of excited states to enhance multiple exciton generation (MEG). We have studied MEG in close-packed PbSe QD arrays where the QDs are electronically coupled in the films and thus exhibit good transport while still maintaining quantization and MEG. We have developed simple, all-inorganic solution-processable QD solar cells that produce large short-circuit photocurrents and power conversion efficiencies above 5% via nanocrystalline p-n junctions. These solar cells show QYs for photocurrent that exceed 100% in the photon energy regions where MEG is possible; the photocurrent MEG QYs as a function of photon energy match those determined via time-resolved spectroscopy Recent analyses of the major effect of MEG combined with solar concentration on the conversion efficiency of solar cells will also be discussed.
Fluorescence resonance energy transfer measured by spatial photon migration in CdSe-ZnS quantum dots colloidal systems as a function of concentration
Azevedo, G.; Monte, A. F. G.; Reis, A. F.; Messias, D. N.
The study of the spatial photon migration as a function of the concentration brings into attention the problem of the energy transfer in quantum dot embedded systems. By measuring the photon propagation and its spatial dependence, it is possible to understand the whole dynamics in a quantum dot system, and also improve their concentration dependence to maximize energy propagation due to radiative and non-radiative processes. In this work, a confocal microscope was adapted to scan the spatial distribution of photoluminescence from CdSe-ZnS core-shell quantum dots in colloidal solutions. The energy migration between the quantum dots was monitored by the direct measurement of the photon diffusion length, according to the diffusion theory. We observed that the photon migration length decreases by increasing the quantum dot concentration, this kind of behavior has been regarded as a signature of F�rster resonance energy transfer in the system.
Quasi-periodic quantum dot arrays produced by electrochemical synthesis
Bandyopadhyay, S.; Miller, A.E.; Yue, D.F.; Banerjee, G.; Ricker, R.E.; Jones, S.; Eastman, J.A.; Baugher, E.; Chandrasekhar, M.
We discuss a ``gentle`` electrochemical technique for fabricating quasi-periodic quantum dot arrays. The technique exploits a self-organizing phenomenon to produce quasi-periodic arrangement of dots and provides excellent control over dot size and interdot spacing. Unlike conventional nanolithography, it does not cause radiation damage to the structures during exposure to pattern delineating beams (e-beam, ion-beam or x-ray). Moreover, it does not require harsh processing steps like reactive ion etching, offers a minimum feature size of {approximately}40 {angstrom}, allows the fabrication of structures on nonplanar surfaces (e.g. spherical or cylindrical substrates), is amenable to mass production (millions of wafers can be processed simultaneously) and is potentially orders of magnitude cheaper than conventional nanofabrication. In this paper, we describe our initial results and show the promise of this technique for low-cost and high-yield nanosynthesis.
Observation of the Kondo effect in a spin-3/2 hole quantum dot (Journal
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Article) | SciTech Connect Observation of the Kondo effect in a spin-3/2 hole quantum dot Citation Details In-Document Search Title: Observation of the Kondo effect in a spin-3/2 hole quantum dot We report the observation of the Kondo effect in a spin-3/2 hole quantum dot formed near pinch-off in a GaAs quantum wire. We clearly observe two distinctive hallmarks of quantum dot Kondo physics. First, the zero-bias peak in the differential conductance splits an in-plane magnetic field and the
Charging dynamics of a floating gate transistor with site-controlled quantum dots
Maier, P. Hartmann, F.; Emmerling, M.; Schneider, C.; H�fling, S.; Kamp, M.; Worschech, L.
A quantum dot memory based on a GaAs/AlGaAs quantum wire with site-controlled InAs quantum dots was realized by means of molecular beam epitaxy and etching techniques. By sampling of different gate voltage sweeps for the determination of charging and discharging thresholds, it was found that discharging takes place at short time scales of ?s, whereas several seconds of waiting times within a distinct negative gate voltage range were needed to charge the quantum dots. Such quantum dot structures have thus the potential to implement logic functions comprising charge and time dependent ingredients such as counting of signals or learning rules.
Simulation of quantum dots size and spacing effect for intermediate band solar cell application based on InAs quantum dots arrangement in GaAs
Hendra, P. I. B. Rahayu, F. Darma, Y.
Intermediate band solar cell (IBSC) has become a promising technology in increasing solar cell efficiency. In this work we compare absorption coefficient profile between InAs quantum dots with GaAs bulk. We calculate the efficiency of GaAs bulk and GaAs doped with 2, 5, and 10 nm InAs quantum dot. Effective distances in quantum dot arrangement based on electron tunneling consideration were also calculated. We presented a simple calculation method with low computing power demand. Results showed that arrangement of quantum dot InAs in GaAs can increase solar cell efficiency from 23.9 % initially up to 60.4%. The effective distance between two quantum dots was found 2 nm in order to give adequate distance to prevent electron tunneling and wave functions overlap.
Induced spin-accumulation and spin-polarization in a quantum-dot ring by using magnetic quantum dots and Rashba spin-orbit effect
Eslami, L., E-mail: firstname.lastname@example.com; Faizabadi, E. [School of Physics, Iran University of Science and Technology, Tehran 16846 (Iran, Islamic Republic of)
The effect of magnetic contacts on spin-dependent electron transport and spin-accumulation in a quantum ring, which is threaded by a magnetic flux, is studied. The quantum ring is made up of four quantum dots, where two of them possess magnetic structure and other ones are subjected to the Rashba spin-orbit coupling. The magnetic quantum dots, referred to as magnetic quantum contacts, are connected to two external leads. Two different configurations of magnetic moments of the quantum contacts are considered; the parallel and the anti-parallel ones. When the magnetic moments are parallel, the degeneracy between the transmission coefficients of spin-up and spin-down electrons is lifted and the system can be adjusted to operate as a spin-filter. In addition, the accumulation of spin-up and spin-down electrons in non-magnetic quantum dots are different in the case of parallel magnetic moments. When the intra-dot Coulomb interaction is taken into account, we find that the electron interactions participate in separation between the accumulations of electrons with different spin directions in non-magnetic quantum dots. Furthermore, the spin-accumulation in non-magnetic quantum dots can be tuned in the both parallel and anti-parallel magnetic moments by adjusting the Rashba spin-orbit strength and the magnetic flux. Thus, the quantum ring with magnetic quantum contacts could be utilized to create tunable local magnetic moments which can be used in designing optimized nanodevices.
Resonant scattering of surface plasmon polaritons by dressed quantum dots
Huang, Danhong; Cardimona, Dave; Easter, Michelle; Gumbs, Godfrey; Maradudin, A. A.; Lin, Shawn-Yu; Zhang, Xiang
The resonant scattering of surface plasmon-polariton waves (SPP) by embedded semiconductor quantum dots above the dielectric/metal interface is explored in the strong-coupling regime. In contrast to non-resonant scattering by a localized dielectric surface defect, a strong resonant peak in the spectrum of the scattered field is predicted that is accompanied by two side valleys. The peak height depends nonlinearly on the amplitude of SPP waves, reflecting the feedback dynamics from a photon-dressed electron-hole plasma inside the quantum dots. This unique behavior in the scattered field peak strength is correlated with the occurrence of a resonant dip in the absorption spectrum of SPP waves due to the interband photon-dressing effect. Our result on the scattering of SPP waves may be experimentally observable and applied to spatially selective illumination and imaging of individual molecules.
Facile synthesis and photoluminescence mechanism of graphene quantum dots
Yang, Ping; Zhou, Ligang; Zhang, Shenli; Pan, Wei Shen, Wenzhong; Wan, Neng
We report a facile hydrothermal synthesis of intrinsic fluorescent graphene quantum dots (GQDs) with two-dimensional morphology. This synthesis uses glucose, concentrate sulfuric acid, and deionized water as reagents. Concentrated sulfuric acid is found to play a key role in controlling the transformation of as-prepared hydrothermal products from amorphous carbon nanodots to well-crystallized GQDs. These GQDs show typical absorption characteristic for graphene, and have nearly excitation-independent ultraviolet and blue intrinsic emissions. Temperature-dependent PL measurements have demonstrated strong electron-electron scattering and electron-phonon interactions, suggesting a similar temperature behavior of GQDs to inorganic semiconductor quantum dots. According to optical studies, the ultraviolet emission is found to originate from the recombination of electron-hole pairs localized in the C=C bonds, while the blue emission is from the electron transition of sp{sup 2} domains.
Final LDRD report : infrared detection and power generation using self-assembled quantum dots.
Cederberg, Jeffrey George; Ellis, Robert; Shaner, Eric Arthur
Alternative solutions are desired for mid-wavelength and long-wavelength infrared radiation detection and imaging arrays. We have investigated quantum dot infrared photodetectors (QDIPs) as a possible solution for long-wavelength infrared (8 to 12 {mu}m) radiation sensing. This document provides a summary for work done under the LDRD 'Infrared Detection and Power Generation Using Self-Assembled Quantum Dots'. Under this LDRD, we have developed QDIP sensors and made efforts to improve these devices. While the sensors fabricated show good responsivity at 80 K, their detectivity is limited by high noise current. Following efforts concentrated on how to reduce or eliminate this problem, but with no clear path was identified to the desired performance improvements.
Carbon quantum dots coated BiVO{sub 4} inverse opals for enhanced photoelectrochemical hydrogen generation
Nan, Feng; Shen, Mingrong; Fang, Liang E-mail: firstname.lastname@example.com; Kang, Zhenhui E-mail: email@example.com; Wang, Junling
Carbon quantum dots (CQDs) coated BiVO{sub 4} inverse opal (io-BiVO{sub 4}) structure that shows dramatic improvement of photoelectrochemical hydrogen generation has been fabricated using electrodeposition with a template. The io-BiVO{sub 4} maximizes photon trapping through slow light effect, while maintaining adequate surface area for effective redox reactions. CQDs are then incorporated to the io-BiVO{sub 4} to further improve the photoconversion efficiency. Due to the strong visible light absorption property of CQDs and enhanced separation of the photoexcited electrons, the CQDs coated io-BiVO{sub 4} exhibit a maximum photo-to-hydrogen conversion efficiency of 0.35%, which is 6 times higher than that of the pure BiVO{sub 4} thin films. This work is a good example of designing composite photoelectrode by combining quantum dots and photonic crystal.
Exploring Competing Kinetic Processes in Quantum Dots Linked to Electrode
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Surfaces | MIT-Harvard Center for Excitonics Competing Kinetic Processes in Quantum Dots Linked to Electrode Surfaces March 14, 2012 at 2:30pm/4-349 Mark Hybertsen Brookhaven National Laboratory, Columbia University Mark_Hybertsen001_000 Abstract: Exploiting the unique properties of nanostructured chromophores for light harvesting applications relies on the balance between competing kinetic processes including energy transfer, carrier relaxation and carrier tunneling. In the first part of
Quantum Dot Tracers for Use in Engineered Geothermal
Office of Energy Efficiency and Renewable Energy (EERE) Indexed Site
Quantum Dot Tracers for Use in Engineered Geothermal Systems DE-EE0002768 Peter Rose, EGI/University of Utah Michael Bartl, Department of Chemistry at the University of Utah Paul Reimus, Los Alamos National Lab Project Officer: Lauren Boyd Total Project Funding: $1,238,499 April 23, 2013 This presentation does not contain any proprietary confidential, or otherwise restricted information. 2 | US DOE Geothermal Office eere.energy.gov Relevance/Impact of Research The objective of this project is to
Computational models for the berry phase in semiconductor quantum dots
Prabhakar, S. Melnik, R. V. N.; Sebetci, A.
By developing a new model and its finite element implementation, we analyze the Berry phase low-dimensional semiconductor nanostructures, focusing on quantum dots (QDs). In particular, we solve the Schr�dinger equation and investigate the evolution of the spin dynamics during the adiabatic transport of the QDs in the 2D plane along circular trajectory. Based on this study, we reveal that the Berry phase is highly sensitive to the Rashba and Dresselhaus spin-orbit lengths.
Optical, electronic, and structural properties of uncoupled and close-packed arrays of InP quantum dots
Micic, O.I.; Jones, K.M.; Cahill, A.; Nozik, A.J.
Solid films consisting of close-packed arrays of InP quantum dots have been prepared by slowly evaporating colloidal solutions of InP quantum dots. The diameters of the quantum dots were controlled to be between about 30 to 60 {angstrom}; size-selective precipitation yielded a size distribution of about 10% about the mean diameter. The arrays show regions of hexagonal order, as well as disordered regions. Oxide layers can form irreversibly on the quantum dot surface and limit the effectiveness of the size-selective precipitation. Photoluminescence spectra obtained from close-packed films of InP quantum dots formed from quantum dots with a single mean diameter and from a mixture of two quantum dot sizes show that energy transfer occurs from the photoexcited smaller quantum dots to the larger quantum dots. The efficiency of this energy transfer process is high.
GaAs quantum dot solar cell under concentrated radiation
Sablon, K.; Little, J. W.; Hier, H.; Li, Y.; Mitin, V.; Vagidov, N.; Sergeev, A.
Effects of concentrated solar radiation on photovoltaic performance are investigated in well-developed GaAs quantum dot (QD) solar cells with 1-Sun efficiencies of 18%–19%. In these devices, the conversion processes are enhanced by nanoscale potential barriers and/or AlGaAs atomically thin barriers around QDs, which prevent photoelectron capture to QDs. Under concentrated radiation, the short circuit current increases proportionally to the concentration and the open circuit voltage shows the logarithmic increase. In the range up to hundred Suns, the contributions of QDs to the photocurrent are proportional to the light concentration. The ideality factors of 1.1–1.3 found from the V{sub OC}-Sun characteristics demonstrate effective suppression of recombination processes in barrier-separated QDs. The conversion efficiency shows the wide maximum in the range of 40–90 Suns and reaches 21.6%. Detailed analysis of I-V-Sun characteristics shows that at low intensities, the series resistance decreases inversely proportional to the concentration and, at ∼40 Suns, reaches the plateau determined mainly by the front contact resistance. Improvement of contact resistance would increase efficiency to above 24% at thousand Suns.
Density functional calculation of the structural and electronic properties of germanium quantum dots
Anas, M. M.; Gopir, G.
We apply first principles density functional computational methods to study the structures, densities of states (DOS), and higher occupied molecular orbital (HOMO) � lowest unoccupied molecular orbital (LUMO) gaps of selected free-standing Ge semiconductor quantum dots up to 1.8nm. Our calculations are performed using numerical atomic orbital approach where linear combination of atomic orbital was applied. The surfaces of the quantum dots was passivized by hydrogen atoms. We find that surface passivation does affect the electronic properties associated with the changes of surface state, electron localization, and the energy gaps of germanium nanocrystals as well as the confinement of electrons inside the quantum dots (QDs). Our study shows that the energy gaps of germanium quantum dots decreases with the increasing dot diameter. The size-dependent variations of the computed HOMO-LUMO gaps in our quantum dots model were found to be consistent with the effects of quantum confinement reported in others theoretical and experimental calculation.
Increased InAs quantum dot size and density using bismuth as a surfactant
Dasika, Vaishno D.; Krivoy, E. M.; Nair, H. P.; Maddox, S. J.; Park, K. W.; Yu, E. T.; Bank, S. R.; Jung, D.; Lee, M. L.
We have investigated the growth of self-assembled InAs quantum dots using bismuth as a surfactant to control the dot size and density. We find that the bismuth surfactant increases the quantum dot density, size, and uniformity, enabling the extension of the emission wavelength with increasing InAs deposition without a concomitant reduction in dot density. We show that these effects are due to bismuth acting as a reactive surfactant to kinetically suppress the surface adatom mobility. This mechanism for controlling quantum dot density and size has the potential to extend the operating wavelength and enhance the performance of various optoelectronic devices.
Magneto-optical absorption in semiconducting spherical quantum dots: Influence of the dot-size, confining potential, and magnetic field
Kushwaha, Manvir S.
Semiconducting quantum dots – more fancifully dubbed artificial atoms – are quasi-zero dimensional, tiny, man-made systems with charge carriers completely confined in all three dimensions. The scientific quest behind the synthesis of quantum dots is to create and control future electronic and optical nanostructures engineered through tailoring size, shape, and composition. The complete confinement – or the lack of any degree of freedom for the electrons (and/or holes) – in quantum dots limits the exploration of spatially localized elementary excitations such as plasmons to direct rather than reciprocal space. Here we embark on a thorough investigation of the magneto-optical absorption in semiconducting spherical quantum dots characterized by a confining harmonic potential and an applied magnetic field in the symmetric gauge. This is done within the framework of Bohm-Pines' random-phase approximation that enables us to derive and discuss the full Dyson equation that takes proper account of the Coulomb interactions. As an application of our theoretical strategy, we compute various single-particle and many-particle phenomena such as the Fock-Darwin spectrum; Fermi energy; magneto-optical transitions; probability distribution; and the magneto-optical absorption in the quantum dots. It is observed that the role of an applied magnetic field on the absorption spectrum is comparable to that of a confining potential. Increasing (decreasing) the strength of the magnetic field or the confining potential is found to be analogous to shrinking (expanding) the size of the quantum dots: resulting into a blue (red) shift in the absorption spectrum. The Fermi energy diminishes with both increasing magnetic-field and dot-size; and exhibits saw-tooth-like oscillations at large values of field or dot-size. Unlike laterally confined quantum dots, both (upper and lower) magneto-optical transitions survive even in the extreme instances. However, the intra-Landau level
Formation of long-range ordered quantum dots arrays in amorphous matrix by ion beam irradiation
Buljan, M.; Bogdanovic-Radovic, I.; Karlusic, M.; Desnica, U. V.; Radic, N.; Dubcek, P.; Drazic, G.; Salamon, K.; Bernstorff, S.; Holy, V.
We demonstrate the production of a well ordered three-dimensional array of Ge quantum dots in amorphous silica matrix. The ordering is achieved by ion beam irradiation and annealing of a multilayer film. Structural analysis shows that quantum dots nucleate along the direction of the ion beam used for irradiation, while the mutual distance of the quantum dots is determined by the diffusion properties of the multilayer material rather than the distances between traces of ions that are used for irradiation.
R&D Magazine: Windows into Solar Power Sources with Quantum Dots
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R&D Magazine: Windows into Solar Power Sources with Quantum Dots A luminescent solar concentrator is an emerging sunlight harvesting technology that has the potential to disrupt ...
Giant Nanocrystal Quantum Dots as Stable and Efficient Down-Conversion...
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Technical Report: Giant Nanocrystal Quantum Dots as Stable and Efficient Down-Conversion Phosphor for LED based Solid State Lighting Citation Details In-Document Search Title: ...
Excited-state spectroscopy of InP quantum dots
Bertram, D.; Micic, O.I.; Nozik, A.J.
We have measured low-temperature size-selective photoluminescence excitation spectra of high-quality InP quantum dots prepared by collodial chemistry. A set of samples with mean emission energies in the range from 1.9 to 2.2 eV was investigated. All samples have a size distribution of about 10{percent}, resulting in an inhomogeneously broadened photoluminescence lineshape. Due to the finite size distribution, spectra were collected at different detection wavelengths to reveal the energies of the excited excitonic states. The size dependence of the quantization energies of InP nanoparticles was determined by measuring photoluminescence excitation at different detection energies within one sample. Up to eight excited-state transitions in a set of seven samples were observed, as the estimated quantum dot size was scanned from 1.8 to 4.0 nm. A comparison of the observed peaks with a six-band {bold k}{center_dot}{bold p} calculation is given. In contrast to the successful interpretation in the case of CdSe, no agreement between the calculated and the observed excited-state energies is achieved. {copyright} {ital 1998} {ital The American Physical Society}
Excited-State Relaxation in PbSe Quantum Dots
An, J. M.; Califano, M.; Franceschetti, A.; Zunger, A.
In solids the phonon-assisted, nonradiative decay from high-energy electronic excited states to low-energy electronic excited states is picosecond fast. It was hoped that electron and hole relaxation could be slowed down in quantum dots, due to the unavailability of phonons energy matched to the large energy-level spacings ('phonon-bottleneck'). However, excited-state relaxation was observed to be rather fast ({le}1 ps) in InP, CdSe, and ZnO dots, and explained by an efficient Auger mechanism, whereby the excess energy of electrons is nonradiatively transferred to holes, which can then rapidly decay by phonon emission, by virtue of the densely spaced valence-band levels. The recent emergence of PbSe as a novel quantum-dot material has rekindled the hope for a slow down of excited-state relaxation because hole relaxation was deemed to be ineffective on account of the widely spaced hole levels. The assumption of sparse hole energy levels in PbSe was based on an effective-mass argument based on the light effective mass of the hole. Surprisingly, fast intraband relaxation times of 1-7 ps were observed in PbSe quantum dots and have been considered contradictory with the Auger cooling mechanism because of the assumed sparsity of the hole energy levels. Our pseudopotential calculations, however, do not support the scenario of sparse hole levels in PbSe: Because of the existence of three valence-band maxima in the bulk PbSe band structure, hole energy levels are densely spaced, in contradiction with simple effective-mass models. The remaining question is whether the Auger decay channel is sufficiently fast to account for the fast intraband relaxation. Using the atomistic pseudopotential wave functions of Pb{sub 2046}Se{sub 2117} and Pb{sub 260}Se{sub 249} quantum dots, we explicitly calculated the electron-hole Coulomb integrals and the P {yields} S electron Auger relaxation rate. We find that the Auger mechanism can explain the experimentally observed P {yields} S
Quantum Dot Solar Cells with Multiple Exciton Generation
Hanna, M. C.; Beard, M. C.; Johnson, J. C.; Murphy, J.; Ellingson, R. J.; Nozik, A. J.
We have measured the quantum yield of the multiple exciton generation (MEG) process in quantum dots (QDs) of the lead-salt semiconductor family (PbSe, PbTe, and PbS) using fs pump-probe transient absorption measurements. Very high quantum yields (up to 300%) for charge carrier generation from MEG have been measured in all of the Pb-VI QDs. We have calculated the potential maximum performance of various MEG QD solar cells in the detailed balance limit. We examined a two-cell tandem PV device with singlet fission (SF), QD, and normal dye (N) absorbers in the nine possible series-connected combinations to compare the tandem combinations and identify the combinations with the highest theoretical efficiency. We also calculated the maximum efficiency of an idealized single-gap MEG QD solar cell with M multiplications and its performance under solar concentration.
Sandia Develops a Synthesis of Quantum Dots that Increases the Quantum
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Yield to 95.5% Develops a Synthesis of Quantum Dots that Increases the Quantum Yield to 95.5% - Sandia Energy Energy Search Icon Sandia Home Locations Contact Us Employee Locator Energy & Climate Secure & Sustainable Energy Future Stationary Power Energy Conversion Efficiency Solar Energy Wind Energy Water Power Supercritical CO2 Geothermal Natural Gas Safety, Security & Resilience of the Energy Infrastructure Energy Storage Nuclear Power & Engineering Grid Modernization
Probing the size and environment induced phase transformation in CdSe quantum dots
Karakoti, Ajay S.; Sanghavi, Shail P.; Nachimuthu, Ponnusamy; Yang, Ping; Thevuthasan, Suntharampillai
The structural and electronic properties of CdSe quantum dots in toluene and drop-casted on Si wafer were investigated by in-situ micro X-ray diffraction, X-ray photoelectron spectroscopy and UV-Vis absorption and emission spectroscopy. The in-situ micro diffraction data show that the CdSe quantum dots capped with TOPO or hexadecylamine (HDA) in toluene exhibit predominantly wurtzite crystal structure, which undergoes a phase transformation to zinc blende crystal structure following drop casting on Si and this phase transition increases with decreasing the size of the CdSe quantum dots. Decreasing the size of quantum dots also increases the Se vacancies that facilitate the phase transformation. The X-ray photoelectron spectra show a systematic increase in the core level binding energies of Cd 3d and Se 3d, the band gap and the Cd/Se ratio as the size of the quantum dots decreases from 6.6nm to 2.1nm. This is attributed to the quantum confinement of CdSe crystallites by the capping ligands in toluene which increases with decreasing the size of the quantum dots. However, drop-casting quantum dots on Si alter the density and arrangement of capping ligands and solvent molecules on the quantum dots which causes significant phase transformation.
Grazing-incidence small-angle X-ray scattering: application to the study of quantum dot lattices
Buljan, Maja Radi?, Nikola; Bernstorff, Sigrid; Dra�i?, Goran; Bogdanovi?-Radovi?, Iva; Hol�, V�clav
The modelling of grazing-incidence small-angle X-ray scattering (GISAXS) from three-dimensional quantum dot lattices is described. The ordering of quantum dots in three-dimensional quantum dot lattices is investigated by grazing-incidence small-angle X-ray scattering (GISAXS). Theoretical models describing GISAXS intensity distributions for three general classes of lattices of quantum dots are proposed. The classes differ in the type of disorder of the positions of the quantum dots. The models enable full structure determination, including lattice type, lattice parameters, the type and degree of disorder in the quantum dot positions and the distributions of the quantum dot sizes. Applications of the developed models are demonstrated using experimentally measured data from several types of quantum dot lattices formed by a self-assembly process.
Computational modeling of electrophotonics nanomaterials: Tunneling in double quantum dots
Vlahovic, Branislav Filikhin, Igor
Single electron localization and tunneling in double quantum dots (DQD) and rings (DQR) and in particular the localized-delocalized states and their spectral distributions are considered in dependence on the geometry of the DQDs (DQRs). The effect of violation of symmetry of DQDs geometry on the tunneling is studied in details. The cases of regular and chaotic geometries are considered. It will be shown that a small violation of symmetry drastically affects localization of electron and that anti-crossing of the levels is the mechanism of tunneling between the localized and delocalized states in DQRs.
Photoluminescence-enhanced biocompatible quantum dots by phospholipid functionalization
Shi Yunfeng; He Peng Zhu Xinyuan
A simple two-step strategy using phospholipid (PPL) to functionalize core/shell CdSe/ZnS quantum dots (QDs) has been described. The experimental data show that the use of S-H terminated PPL results not only in the high colloidal stability of core/shell CdSe/ZnS QDs in the aqueous phase, but also in the significant enhancement of photoluminescence. The degree of the enhancement is a function of the PPL-CdSe/ZnS QDs sample concentration. These results might be promising for future biological platform in new devices ranging from photovoltaic cells to biosensors and other devices.
Electronic structure of nanocrystal quantum-dot quantumwells
Schrier, Joshua; Wang, Lin-Wang
The electronic states of CdS/CdSe/CdS colloidal nanocrystalquantum-dot quantum wells are studied by large-scale pseudopotentiallocal density approximation (LDA) calculations. Using this approach, wedetermine the effects of CdS core size, CdSe well thickness, and CdSshell thickness on the band-edge wave functions, band-gap, andelectron-hole Coulomb interactions. We find the conduction-band wavefunction to be less confined to the CdSe well layer than predicted by kcdot p effective-mass theory, which accounts for the previous underestimation of the electron g factor.
Activation of molecular catalysts using semiconductor quantum dots
Meyer, Thomas J.; Sykora, Milan; Klimov, Victor I.
Photocatalytic materials based on coupling of semiconductor nanocrystalline quantum dots (NQD) and molecular catalysts. These materials have capability to drive or catalyze non-spontaneous chemical reactions in the presence of visible radiation, ultraviolet radiation, or both. The NQD functions in these materials as a light absorber and charge generator. Following light absorption, the NQD activates a molecular catalyst adsorbed on the surface of the NQD via transfer of one or more charges (either electrons or electron-holes) from the NQD to the molecular catalyst. The activated molecular catalyst can then drive a chemical reaction. A photoelectrolytic device that includes such photocatalytic materials is also described.
Water-soluble luminescent quantum dots and biomolecular conjugates thereof and related compositions and method of use
Nie, Shuming; Chan, Warren C. W.; Emory, Steven R.
The present invention provides a water-soluble luminescent quantum dot, a biomolecular conjugate thereof and a composition comprising such a quantum dot or conjugate. Additionally, the present invention provides a method of obtaining a luminescent quantum dot, a method of making a biomolecular conjugate thereof, and methods of using a biomolecular conjugate for ultrasensitive nonisotopic detection in vitro and in vivo.
Water-soluble luminescent quantum dots and biomolecular conjugates thereof and related compositions and methods of use
Nie, Shuming; Chan, Warren C. W.; Emory, Stephen
The present invention provides a water-soluble luminescent quantum dot, a biomolecular conjugate thereof and a composition comprising such a quantum dot or conjugate. Additionally, the present invention provides a method of obtaining a luminescent quantum dot, a method of making a biomolecular conjugate thereof, and methods of using a biomolecular conjugate for ultrasensitive nonisotopic detection in vitro and in vivo.
Intermediate-band photosensitive device with quantum dots embedded in energy fence barrier
Forrest, Stephen R.; Wei, Guodan
A plurality of layers of a first semiconductor material and a plurality of dots-in-a-fence barriers disposed in a stack between a first electrode and a second electrode. Each dots-in-a-fence barrier consists essentially of a plurality of quantum dots of a second semiconductor material embedded between and in direct contact with two layers of a third semiconductor material. Wave functions of the quantum dots overlap as at least one intermediate band. The layers of the third semiconductor material are arranged as tunneling barriers to require a first electron and/or a first hole in a layer of the first material to perform quantum mechanical tunneling to reach the second material within a respective quantum dot, and to require a second electron and/or a second hole in a layer of the first semiconductor material to perform quantum mechanical tunneling to reach another layer of the first semiconductor material.
Charge-transfer dynamics in multilayered PbS and PbSe quantum dot architectures
Xu, F.; Ma, X.; Haughn, C. R.; Doty, M. F.; Cloutier, S. G.
We demonstrate control of the charge transfer process in PbS and PbSe quantum dot assemblies. We first demonstrate efficient charge transfer from donor quantum dots to acceptor quantum dots in a multi-layer PbSe cascade structure. Then, we assemble type-I and type-II heterostructures using both PbS and PbSe quantum dots via careful control of the band alignment. In type-I structures, photo-generated carriers are transferred and localized in the smaller bandgap (acceptor) quantum dots, resulting in a significant luminescence enhancement. In contrast, a significant luminescence quenching and shorter emission lifetime confirms an efficient separation of photo-generated carriers in the type-II architecture.
Applicability of the {bold k}{center_dot}{bold p} method to the electronic structure of quantum dots
Fu, H.; Wang, L.; Zunger, A.
The {bold k}{center_dot}{bold p} method has become the {open_quotes}standard model{close_quotes} for describing the electronic structure of nanometer-size quantum dots. In this paper we perform parallel {bold k}{center_dot}{bold p} (6{times}6 and 8{times}8) and direct-diagonalization pseudopotential studies on spherical quantum dots of an ionic material{emdash}CdSe, and a covalent material{emdash}InP. By using an equivalent input in both approaches, i.e., starting from a given atomic pseudopotential and deriving from it the Luttinger parameters in {bold k}{center_dot}{bold p} calculation, we investigate the effect of the different underlying wave-function representations used in {bold k}{center_dot}{bold p} and in the more exact pseudopotential direct diagonalization. We find that (i) the 6{times}6{bold k}{center_dot}{bold p} envelope function has a distinct (odd or even) parity, while atomistic wave function is parity-mixed. The 6{times}6{bold k}{center_dot}{bold p} approach produces an incorrect order of the highest valence states for both InP and CdSe dots: the p-like level is above the s-like level. (ii) It fails to reveal that the second conduction state in small InP dots is folded from the L point in the Brillouin zone. Instead, all states in {bold k}{center_dot}{bold p} are described as {Gamma}-like. (iii) The {bold k}{center_dot}{bold p} overestimates the confinement energies of both valence states and conduction states. A wave-function projection analysis shows that the principal reasons for these {bold k}{center_dot}{bold p} errors in dots are (a) use of restricted basis set, and (b) incorrect {ital bulk} dispersion relation. Error (a) can be reduced only by increasing the number of basis functions. Error (b) can be reduced by altering the {bold k}{center_dot}{bold p} implementation so as to bend upwards the second lowest bulk band, and to couple the conduction band into the s-like dot valence state. Our direct diagonalization approach provides an
Colloidal quantum dot solar cells on curved and flexible substrates
Kramer, Illan J.; Moreno-Bautista, Gabriel; Minor, James C.; Kopilovic, Damir; Sargent, Edward H.
Colloidal quantum dots (CQDs) are semiconductor nanocrystals synthesized with, processed in, and deposited from the solution phase, potentially enabling low-cost, facile manufacture of solar cells. Unfortunately, CQD solar cell reports, until now, have only explored batch-processing methods—such as spin-coating—that offer limited capacity for scaling. Spray-coating could offer a means of producing uniform colloidal quantum dot films that yield high-quality devices. Here, we explore the versatility of the spray-coating method by producing CQD solar cells in a variety of previously unexplored substrate arrangements. The potential transferability of the spray-coating method to a roll-to-roll manufacturing process was tested by spray-coating the CQD active layer onto six substrates mounted on a rapidly rotating drum, yielding devices with an average power conversion efficiency of 6.7%. We further tested the manufacturability of the process by endeavoring to spray onto flexible substrates, only to find that spraying while the substrate was flexed was crucial to achieving champion performance of 7.2% without compromise to open-circuit voltage. Having deposited onto a substrate with one axis of curvature, we then built our CQD solar cells onto a spherical lens substrate having two axes of curvature resulting in a 5% efficient device. These results show that CQDs deposited using our spraying method can be integrated to large-area manufacturing processes and can be used to make solar cells on unconventional shapes.
Metallic nanoparticle shape and size effects on aluminum oxide-induced enhancement of exciton-plasmon coupling and quantum dot emission
Wing, Waylin J.; Sadeghi, Seyed M. Gutha, Rithvik R.; Campbell, Quinn; Mao, Chuanbin
We investigate the shape and size effects of gold metallic nanoparticles on the enhancement of exciton-plasmon coupling and emission of semiconductor quantum dots induced via the simultaneous impact of metal-oxide and plasmonic effects. This enhancement occurs when metallic nanoparticle arrays are separated from the quantum dots by a layered thin film consisting of a high index dielectric material (silicon) and aluminum oxide. Our results show that adding the aluminum oxide layer can increase the degree of polarization of quantum dot emission induced by metallic nanorods by nearly two times, when these nanorods have large aspect ratios. We show when the aspect ratio of these nanorods is reduced to half, the aluminum oxide loses its impact, leading to no improvement in the degree of polarization. These results suggest that a silicon/aluminum oxide layer can significantly enhance exciton-plasmon coupling when quantum dots are in the vicinity of metallic nanoantennas with high aspect ratios.
Engineering the hole confinement for CdTe-based quantum dot molecules
Kłopotowski, Ł. Wojnar, P.; Kret, S.; Fronc, K.; Wojtowicz, T.; Karczewski, G.
We demonstrate an efficient method to engineer the quantum confinement in a system of two quantum dots grown in a vertical stack. We achieve this by using materials with a different lattice constant for the growth of the outer and inner barriers. We monitor the resulting dot morphology with transmission electron microscopy studies and correlate the results with ensemble quantum dot photoluminescence. Furthermore, we embed the double quantum dots into diode structures and study photoluminescence as a function of bias voltage. We show that in properly engineered structures, it is possible to achieve a resonance of the hole states by tuning the energy levels with electric field. At the resonance, we observe signatures of a formation of a molecular state, hybridized over the two dots.
Effect of swift heavy ion irradiation on bare and coated ZnS quantum dots
Chowdhury, S. Hussain, A.M.P.; Ahmed, G.A.; Singh, F.; Avasthi, D.K.; Choudhury, A.
The present study compares structural and optical modifications of bare and silica (SiO{sub 2}) coated ZnS quantum dots under swift heavy ion (SHI) irradiation. Bare and silica coated ZnS quantum dots were prepared following an inexpensive chemical route using polyvinyl alcohol (PVA) as the dielectric host matrix. X-ray diffraction (XRD) and transmission electron microscopy (TEM) study of the samples show the formation of almost spherical ZnS quantum dots. The UV-Vis absorption spectra reveal blue shift relative to bulk material in absorption energy while photoluminescence (PL) spectra suggests that surface state and near band edge emissions are dominating in case of bare and coated samples, respectively. Swift heavy ion irradiation of the samples was carried out with 160 MeV Ni{sup 12+} ion beam with fluences 10{sup 12} to 10{sup 13} ions/cm{sup 2}. Size enhancement of bare quantum dots after irradiation has been indicated in XRD and TEM analysis of the samples which has also been supported by optical absorption spectra. However similar investigations on irradiated coated quantum dots revealed little change in quantum dot size and emission. The present study thus shows that the coated ZnS quantum dots are stable upon SHI irradiation compared to the bare one.
Tuning the properties of Ge-quantum dots superlattices in amorphous silica matrix through deposition conditions
Pinto, S. R. C.; Ramos, M. M. D.; Gomes, M. J. M.; Buljan, M.; Chahboun, A.; Roldan, M. A.; Molina, S. I.; Bernstorff, S.; Varela, M.; Pennycook, S. J.; Barradas, N. P.; Alves, E.
In this work, we investigate the structural properties of Ge quantum dot lattices in amorphous silica matrix, prepared by low-temperature magnetron sputtering deposition of (Ge+SiO{sub 2})/SiO{sub 2} multilayers. The dependence of quantum dot shape, size, separation, and arrangement type on the Ge-rich (Ge + SiO{sub 2}) layer thickness is studied. We show that the quantum dots are elongated along the growth direction, perpendicular to the multilayer surface. The size of the quantum dots and their separation along the growth direction can be tuned by changing the Ge-rich layer thickness. The average value of the quantum dots size along the lateral (in-plane) direction along with their lateral separation is not affected by the thickness of the Ge-rich layer. However, the thickness of the Ge-rich layer significantly affects the quantum dot ordering. In addition, we investigate the dependence of the multilayer average atomic composition and also the quantum dot crystalline quality on the deposition parameters.
White-blue electroluminescence from a Si quantum dot hybrid light-emitting diode
Xin, Yunzi; Nishio, Kazuyuki; Saitow, Ken-ichi
A silicon (Si) quantum dot (QD)-based hybrid inorganic/organic light-emitting diode (LED) was fabricated via solution processing. This device exhibited white-blue electroluminescence at a low applied voltage of 6?V, with 78% of the effective emission obtained from the Si QDs. This hybrid LED produced current and optical power densities 280 and 350 times greater than those previously reported for such device. The superior performance of this hybrid device was obtained by both the prepared Si QDs and the optimized layer structure and thereby improving carrier migration through the hybrid LED and carrier recombination in the homogeneous Si QD layer.
High performance continuous wave 1.3 μm quantum dot lasers on silicon
Liu, Alan Y. Norman, Justin; Zhang, Chong; Snyder, Andrew; Lubyshev, Dmitri; Fastenau, Joel M.; Liu, Amy W. K.; Gossard, Arthur C.; Bowers, John E.
We demonstrate record performance 1.3 μm InAs quantum dot lasers grown on silicon by molecular beam epitaxy. Ridge waveguide lasers fabricated from the as-grown material achieve room temperature continuous wave thresholds as low as 16 mA, output powers exceeding 176 mW, and lasing up to 119 °C. P-modulation doping of the active region improves T{sub 0} to the range of 100–200 K while maintaining low thresholds and high output powers. Device yield is presented showing repeatable performance across different dies and wafers.
An oleic acid-capped CdSe quantum-dot sensitized solar cell
Chen Jing; Song, J. L.; Deng, W. Q.; Sun, X. W.; Jiang, C. Y.; Lei, W.; Huang, J. H.; Liu, R. S.
In this letter, we report an oleic acid (OA)-capped CdSe quantum-dot sensitized solar cell (QDSSC) with an improved performance. The TiO{sub 2}/OA-CdSe photoanode in a two-electrode device exhibited a photon-to-current conversion efficiency of 17.5% at 400 nm. At AM1.5G irradiation with 100 mW/cm{sup 2} light intensity, the QDSSCs based on OA-capped CdSe showed a power conversion efficiency of about 1%. The function of OA was to increase QD loading, extend the absorption range and possibly suppress the surface recombination.
Three dimensional time-gated tracking of non-blinking quantum dots in live cells
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
DeVore, Matthew S.; Werner, James H.; Goodwin, Peter M.; Keller, Aaron M.; Hollingsworth, Jennifer A.; Wilson, Bridget S.; Cleyrat, Cedric; Lidke, Diane S.; Ghosh, Yagnaseni; Stewart, Michael H.; et al
Single particle tracking has provided a wealth of information about biophysical processes such as motor protein transport and diffusion in cell membranes. However, motion out of the plane of the microscope or blinking of the fluorescent probe used as a label generally limits observation times to several seconds. Here, we overcome these limitations by using novel non-blinking quantum dots as probes and employing a custom 3D tracking microscope to actively follow motion in three dimensions (3D) in live cells. As a result, signal-to-noise is improved in the cellular milieu through the use of pulsed excitation and time-gated detection.
Approaches to Future Generation Photovoltaics and Solar Fuels: Multiple Exciton Generation in Quantum Dots, Quantum Dot Arrays, Molecular Singlet Fission, and Quantum Dot Solar Cells
Nozik, A. J.; Beard, M. C.; Johnson, J. C.; Hanna, M. C.; Luther, J. M.; Midgett, A.; Semonin, O.; Michel, J.
One potential, long-term approach to more efficient future generation solar cells is to utilize the unique properties of quantum dots (QDs) and unique molecular chromophores to control the relaxation pathways of excited states to produce enhanced conversion efficiency through efficient multiple electron-hole pair generation from single photons . We have observed efficient multiple exciton generation (MEG) in PbSe, PbS, PbTe, and Si QDs and efficient singlet fission (SF) in molecules that satisfy specific requirements for their excited state energy level structure to achieve carrier multiplication. We have studied MEG in close-packed QD arrays where the QDs are electronically coupled in the films and thus exhibit good transport while still maintaining quantization and MEG. We have developed simple, all-inorganic QD solar cells that produce large short-circuit photocurrents and power conversion efficiencies in the 3-5% range via both nanocrystalline Schottky junctions and nanocrystalline p-n junctions. These solar cells also show QYs for photocurrent that exceed 100% in the photon energy regions where MEG is possible; the photocurrent MEG QYs as a function of photon energy match those determined via time-resolved spectroscopy. We have also observed very efficient SF in thin films of molecular crystals of 1,3 diphenylisobenzofuran with quantum yields of 200% at the optimum SF threshold of 2Eg (HOMO-LUMO for S{sub 0}-S{sub 1}), reflecting the creation of two excited triplet states from the first excited singlet state. Various possible configurations for novel solar cells based on MEG in QDs and SF in molecules that could produce high conversion efficiencies will be presented, along with progress in developing such new types of solar cells. Recent analyses of the effect of MEG or SF combined with solar concentration on the conversion efficiency of solar cells will be discussed.
Red light-emitting diodes based on InP/GaP quantum dots
Hatami, F.; Lordi, V.; Harris, J.S.; Kostial, H.; Masselink, W.T.
The growth, fabrication, and device characterization of InP quantum-dot light-emitting diodes based on GaP are described and discussed. The diode structures are grown on gallium phosphide substrates using gas-source molecular-beam epitaxy and the active region of the diode consists of self-assembled InP quantum dots embedded in a GaP matrix. Red electroluminescence originating from direct band-gap emission from the InP quantum dots is observed at low temperatures.With increasing temperature, however, the emission line shifts to the longer wavelength. The emission light is measured to above room temperature.
R&D Magazine: Windows into Solar Power Sources with Quantum Dots
Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)
R&D Magazine: Windows into Solar Power Sources with Quantum Dots R&D Magazine: Windows into Solar Power Sources with Quantum Dots A luminescent solar concentrator is an emerging sunlight harvesting technology that has the potential to disrupt the way we think about energy: It could turn any window into a daytime power source. August 30, 2015 R&D Magazine: Windows into Solar Power Sources with Quantum Dots A luminescent solar concentrator is an emerging sunlight harvesting technology
Direct Observation of Energy-Gap Scaling Law in CdSe Quantum Dots with Positrons
Denison, Arthur Blanchard; Weber, M. H.; Lynn, K. G.; Barbiellini, B.; Sterne, P. A.
CdSe quantum dot samples with sizes in the range of 1.8�~6 nm in diameter were examined by positron annihilation spectroscopy. The results were compared to data obtained for single-crystal bulk CdSe. Evidence is provided that the positrons annihilate within the nanospheres. The annihilation line shape shows a smearing at the boundary of the Jones zone proportional to the widening of the band gap due to a reduction in the size of the quantum dots. The data confirm that the change in the band gap is inversely proportional to the square of the quantum dot diameter.
The use of bulk states to accelerate the band edge statecalculation of a semiconductor quantum dot
Vomel, Christof; Tomov, Stanimire Z.; Wang, Lin-Wang; Marques,Osni A.; Dongarra, Jack J.
We present a new technique to accelerate the convergence of the folded spectrum method in empirical pseudopotential band edge state calculations for colloidal quantum dots. We use bulk band states of the materials constituent of the quantum dot to construct initial vectors and a preconditioner. We apply these to accelerate the convergence of the folded spectrum method for the interior states at the top of the valence and the bottom of the conduction band. For large CdSe quantum dots, the number of iteration steps until convergence decreases by about a factor of 4 compared to previous calculations.
Far off-resonant coupling between photonic crystal microcavity and single quantum dot with resonant excitation
Banihashemi, Mehdi; Ahmadi, Vahid, E-mail: firstname.lastname@example.com [Department of Electrical and Computer Engineering, Tarbiat Modares University, Tehran, P.O. Box 14115-194 (Iran, Islamic Republic of)] [Department of Electrical and Computer Engineering, Tarbiat Modares University, Tehran, P.O. Box 14115-194 (Iran, Islamic Republic of); Nakamura, Tatsuya; Kojima, Takanori; Kojima, Kazunobu; Noda, Susumu [Department of Electronic Science and Engineering, Kyoto University, Katsura, Nishikyo-ku, Kyoto 615-8510 (Japan)] [Department of Electronic Science and Engineering, Kyoto University, Katsura, Nishikyo-ku, Kyoto 615-8510 (Japan)
In this paper, we experimentally demonstrate that with sub-nanowatt coherent s-shell excitation of a single InAs quantum dot, off-resonant coupling of 4.1?nm is possible between L3 photonic crystal microcavity and the quantum dot at 50?K. This resonant excitation reduces strongly the effect of surrounding charges to quantum dot, multiexciton complexes and pure dephasing. It seems that this far off-resonant coupling is the result of increased number of acoustical phonons due to high operating temperature of 50?K. The 4.1?nm detuning is the largest amount for this kind of coupling.
R&D Magazine: Windows into Solar Power Sources with Quantum Dots
Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)
R&D Magazine: Windows into Solar Power Sources with Quantum Dots August 30, 2015 R&D Magazine: Windows into Solar Power Sources with Quantum Dots A luminescent solar concentrator is an emerging sunlight harvesting technology that has the potential to disrupt the way we think about energy: It could turn any window into a daytime power source. "In these devices, a fraction of light transmitted through the window is absorbed by nano-sized particles (semiconductor quantum dots)
Nontoxic quantum dot research improves solar cells
Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)
Nonproliferation Policy Challenge: Address evolving threats/challenges to the nonproliferation and arms control regimes. Solution: Develop programs and strategies to address emerging nonproliferation and arms control challenges and opportunities. Learn More 10 CFR Part 810 Related Topics international security international security policy NIS nuclear controls safeguards safeguards and security verification Related News Nuclear Verification International Nuclear Safeguards Nonproliferation and
Profiling the local carrier concentration across a semiconductor quantum dot
Walrath, J. C.; Lin, Yen-Hsiang; Huang, S.; Goldman, R. S.
We profile the local carrier concentration, n, across epitaxial InAs/GaAs quantum dots (QDs) consisting of 3D islands on top of a 2D alloy layer. We use scanning thermoelectric microscopy to measure a profile of the temperature gradient-induced voltage, which is converted to a profile of the local Seebeck coefficient, S. The S profile is then converted to a conduction band-edge profile and compared with Poisson-Schrodinger band-edge simulations. Our combined computational-experimental approach suggests a reduced carrier concentration in the QD center in comparison to that of the 2D alloy layer. The relative roles of free carrier trapping and/or dopant expulsion are discussed.
Interaction of graphene quantum dots with bulk semiconductor surfaces
Mohapatra, P. K.; Singh, B. P.; Kushavah, Dushyant; Mohapatra, J.
Highly luminescent graphene quantum dots (GQDs) are synthesized through thermolysis of glucose. The average lateral size of the synthesized GQDs is found to be ?5 nm. The occurrence of D and G band at 1345 and 1580 cm{sup ?1} in Raman spectrum confirms the presence of graphene layers. GQDs are mostly consisting of 3 to 4 graphene layers as confirmed from the AFM measurements. Photoluminescence (PL) measurement shows a distinct broadening of the spectrum when GQDs are on the semiconducting bulk surface compared to GQDs in water. The time resolved PL measurement shows a significant shortening in PL lifetime due to the substrate interaction on GQDs compared to the GQDs in solution phase.
Location deterministic biosensing from quantum-dot-nanowire assemblies
Liu, Chao; Kim, Kwanoh; Fan, D. L.
Semiconductor quantum dots (QDs) with high fluorescent brightness, stability, and tunable sizes, have received considerable interest for imaging, sensing, and delivery of biomolecules. In this research, we demonstrate location deterministic biochemical detection from arrays of QD-nanowire hybrid assemblies. QDs with diameters less than 10 nm are manipulated and precisely positioned on the tips of the assembled Gold (Au) nanowires. The manipulation mechanisms are quantitatively understood as the synergetic effects of dielectrophoretic (DEP) and alternating current electroosmosis (ACEO) due to AC electric fields. The QD-nanowire hybrid sensors operate uniquely by concentrating bioanalytes to QDs on the tips of nanowires before detection, offering much enhanced efficiency and sensitivity, in addition to the position-predictable rationality. This research could result in advances in QD-based biomedical detection and inspires an innovative approach for fabricating various QD-based nanodevices.
Quantum Dots Promise to Significantly Boost Solar Cell Efficiencies (Fact Sheet)
Not Available
In the search for a third generation of solar-cell technologies, a leading candidate is the use of 'quantum dots' -- tiny spheres of semiconductor material measuring only about 2-10 billionths of a meter in diameter. Quantum dots have the potential to dramatically increase the efficiency of converting sunlight into energy -- perhaps even doubling it in some devices -- because of their ability to generate more than one bound electron-hole pair, or exciton, per incoming photon. NREL has produced quantum dots using colloidal suspensions; then, using molecular self-assembly, they have been fabricated into the first-ever quantum-dot solar cells. While these devices operate with only 4.4% efficiency, they demonstrate the capability for low-cost manufacturing.
Observation of the Kondo effect in a spin-3/2 hole quantum dot...
Office of Scientific and Technical Information (OSTI)
Citation Details In-Document Search Title: Observation of the Kondo effect in a spin-32 hole quantum dot We report the ... OSTI Identifier: 22261852 Resource Type: Journal Article ...
Quantum Dot Solar Cells: High Efficiency through Multiple Exciton Generation
Hanna, M. C.; Ellingson, R. J.; Beard, M.; Yu, P.; Micic, O. I.; Nozik, A. J.; c.
Impact ionization is a process in which absorbed photons in semiconductors that are at least twice the bandgap can produce multiple electron-hole pairs. For single-bandgap photovoltaic devices, this effect produces greatly enhanced theoretical thermodynamic conversion efficiencies that range from 45-85%, depending upon solar concentration, the cell temperature, and the number of electron-hole pairs produced per photon. For quantum dots (QDs), electron-hole pairs exist as excitons. We have observed astoundingly efficient multiple exciton generation (MEG) in QDs of PbSe (bulk Eg = 0.28 eV), ranging in diameter from 3.9 to 5.7nm (Eg = 0.73, 0.82, and 0.91 eV, respectively). The effective masses of electron and holes are about equal in PbSe, and the onset for efficient MEG occurs at about three times the QD HOMO-LUMO transition (its ''bandgap''). The quantum yield rises quickly after the onset and reaches 300% at 4 x Eg (3.64 eV) for the smallest QD; this means that every QD in the sample produces three electron-hole pairs/photon.
Evaluating charge noise acting on semiconductor quantum dots in the circuit quantum electrodynamics architecture
Basset, J.; Stockklauser, A.; Jarausch, D.-D.; Frey, T.; Reichl, C.; Wegscheider, W.; Wallraff, A.; Ensslin, K.; Ihn, T.
We evaluate the charge noise acting on a GaAs/GaAlAs based semiconductor double quantum dot dipole-coupled to the voltage oscillations of a superconducting transmission line resonator. The in-phase (I) and the quadrature (Q) components of the microwave tone transmitted through the resonator are sensitive to charging events in the surrounding environment of the double dot with an optimum sensitivity of 8.5�10{sup ?5}?e/?(Hz). A low frequency 1/f type noise spectrum combined with a white noise level of 6.6�10{sup ?6} e{sup 2}/Hz above 1?Hz is extracted, consistent with previous results obtained with quantum point contact charge detectors on similar heterostructures. The slope of the 1/f noise allows to extract a lower bound for the double-dot charge qubit dephasing rate which we compare to the one extracted from a Jaynes-Cummings Hamiltonian approach. The two rates are found to be similar emphasizing that charge noise is the main source of dephasing in our system.
The effect of Coulomb interactions on thermoelectric properties of quantum dots
Zimbovskaya, Natalya A.
Thermoelectric effects in a quantum dot coupled to the source and drain charge reservoirs are explored using a nonequilibrium Green's functions formalism beyond the Hartree-Fock approximation. Thermal transport is analyzed within a linear response regime. A transition from Coulomb blockade regime to Kondo regime in thermoelectric transport through a single-level quantum dot is traced using unified approximations for the relevant Green's functions.
Quantum Dot�Bridge�Fullerene Heterodimers with Controlled Photoinduced Electron Transfer
Cotlet, M.; Xu, Z.
A series of donor-bridge-acceptor systems in the form of core/shell CdSe/ZnS quantum dot-bridge-fullerene heterodimers (see picture) with varying bridge length and varying quantum dot size were self-assembled by a surface-based stepwise method to demonstrate control of the rate and of the magnitude of fluctuations of photoinduced electron transfer at the single-molecule level.
Final Progress Report for Project Entitled: Quantum Dot Tracers for Use in Engineered Geothermal Systems
Rose, Peter; Bartl, Michael; Reimus, Paul; Williams, Mark; Mella, Mike
The objective of this project was to develop and demonstrate a new class of tracers that offer great promise for use in characterizing fracture networks in EGS reservoirs. From laboratory synthesis and testing through numerical modeling and field demonstrations, we have demonstrated the amazing versatility and applicability of quantum dot tracers. This report summarizes the results of four years of research into the design, synthesis, and characterization of semiconductor nanocrystals (quantum dots) for use as geothermal tracers.
SUNY/Buffalo Developing High-Efficiency Colloidal Quantum Dot Phosphors
Office of Energy Efficiency and Renewable Energy (EERE)
The State University of New York at Buffalo is working to reduce the cost and increase the performance of LEDs for general illumination by developing high-efficiency colloidal quantum dot phosphors to replace conventional phosphors (i.e., those placed directly on the chip). Colloidal quantum dot phosphors are nanocrystal emitters and contain no rare-earth elements. What's more, it's possible to tune the emission wavelength merely by changing their size.
Giant Nanocrystal Quantum Dots as Stable and Efficient Down-Conversion
Office of Scientific and Technical Information (OSTI)
Phosphor for LED based Solid State Lighting (Technical Report) | SciTech Connect Technical Report: Giant Nanocrystal Quantum Dots as Stable and Efficient Down-Conversion Phosphor for LED based Solid State Lighting Citation Details In-Document Search Title: Giant Nanocrystal Quantum Dots as Stable and Efficient Down-Conversion Phosphor for LED based Solid State Lighting Authors: Kundu, Janardan [1] ; Ghosh, Yagnaseni [1] ; Dennis, Allison M. [1] ; Htoon, Han [1] ; Hollingsworth, Jennifer A
Multi-stacked InAs/GaAs quantum dots grown with different growth modes for quantum dot solar cells
Kim, Yeongho; Ban, Keun-Yong Honsberg, Christiana B.
We have studied the material properties and device performance of InAs/GaAs quantum dot solar cells (QDSCs) made using three different QD growth modes: Stranski-Krastanov (S-K), quasi-monolayer (QML), and sub-monolayer (SML) growth modes. All QDSCs show an extended external quantum efficiency (EQE) at near infrared wavelengths of 950�1070?nm from the QD absorption. Compared to the S-K and SML QDSCs, the QML QDSC with a higher strain exhibits a poor EQE response in the wavelength region of 300�880?nm due to increased non-radiative recombination. The conversion efficiency of the S-K and SML QDSCs exceeds that of the reference cell (13.4%) without QDs due to an enhanced photocurrent (>16% increase) produced by the silicon doped QD stacks. However, as expected from the EQE of the QML QDSC, the increase of strain-induced crystalline defects greatly degrades the photocurrent and open-circuit voltage, leading to the lowest conversion efficiency (8.9%)
Enhancing efficiency and power of quantum-dots resonant tunneling thermoelectrics in three-terminal geometry by cooperative effects
Jiang, Jian-Hua
We propose a scheme of multilayer thermoelectric engine where one electric current is coupled to two temperature gradients in three-terminal geometry. This is realized by resonant tunneling through quantum dots embedded in two thermal and electrical resisting polymer matrix layers between highly conducting semiconductor layers. There are two thermoelectric effects, one of which is pertaining to inelastic transport processes (if energies of quantum dots in the two layers are different), while the other exists also for elastic transport processes. These two correspond to the transverse and longitudinal thermoelectric effects, respectively, and are associated with different temperature gradients. We show that cooperation between the two thermoelectric effects leads to markedly improved figure of merit and power factor, which is confirmed by numerical calculation using material parameters. Such enhancement is robust against phonon heat conduction and energy level broadening. Therefore, we demonstrated cooperative effect as an additional way to effectively improve performance of thermoelectrics in three-terminal geometry.
Tunnel-injection GaN quantum dot ultraviolet light-emitting diodes
Verma, Jai; Kandaswamy, Prem Kumar; Protasenko, Vladimir; Verma, Amit; Grace Xing, Huili; Jena, Debdeep
We demonstrate a GaN quantum dot ultraviolet light-emitting diode that uses tunnel injection of carriers through AlN barriers into the active region. The quantum dot heterostructure is grown by molecular beam epitaxy on AlN templates. The large lattice mismatch between GaN and AlN favors the formation of GaN quantum dots in the Stranski-Krastanov growth mode. Carrier injection by tunneling can mitigate losses incurred in hot-carrier injection in light emitting heterostructures. To achieve tunnel injection, relatively low composition AlGaN is used for n- and p-type layers to simultaneously take advantage of effective band alignment and efficient doping. The small height of the quantum dots results in short-wavelength emission and are simultaneously an effective tool to fight the reduction of oscillator strength from quantum-confined Stark effect due to polarization fields. The strong quantum confinement results in room-temperature electroluminescence peaks at 261 and 340 nm, well above the 365 nm bandgap of bulk GaN. The demonstration opens the doorway to exploit many varied features of quantum dot physics to realize high-efficiency short-wavelength light sources.
Pseudopotential study of electron-hole excitations in colloidal free-standing InAs quantum dots
Williamson, A. J.; Zunger, Alex
Excitonic spectra are calculated for free-standing, surface passivated, InAs quantum dots using atomic pseudopotentials for the single-particle states and screened Coulomb interactions for the two-body terms. We present an analysis of the single particle states involved in each excitation in terms of their angular momenta and Bloch-wave parentage. We find that (i) in agreement with other pseudopotential studies of CdSe and InP quantum dots, but in contrast to k{center_dot}p calculations, the dot wave functions exhibit strong odd-even angular momentum envelope function mixing (e.g., s with p) and large valence-conduction coupling. (ii) While the pseudopotential approach produced very good agreement with experiment for free-standing, colloidal CdSe and InP dots, and for self-assembled (GaAs-embedded) InAs dots, here the predicted spectrum does not agree well with the measured (ensemble average over dot sizes) spectra. (1) Our calculated excitonic gap is larger than the photoluminescence measured one, and (2) while the spacing between the lowest excitons is reproduced, the spacings between higher excitons is not fit well. Discrepancy (1) could result from surface state emission. As for (2), agreement is improved when account is taken of the finite-size distribution in the experimental data. (iii) We find that the single-particle gap scales as R{sup -1.01} (not R{sup -2}), that the screened (unscreened) electron-hole Coulomb interaction scales as R{sup -1.79} (R{sup -0.7}), and that the excitonic gap scales as R{sup -0.9}. These scaling laws are different from those expected from simple models. (c) 2000 The American Physical Society.
NREL Researchers Demonstrate External Quantum Efficiency Surpassing 100% in a Quantum Dot Solar Cell (Fact Sheet)
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A new device that produces and collects multiple electrons per photon could yield inexpensive, high-efficiency photovoltaics. A new device developed through research at the National Renewable Energy Laboratory (NREL) reduces conventional losses in photovoltaic (PV) solar cells, potentially increasing the power conversion efficiency-but not the cost-of the solar cells. Solar cells convert optical energy from the sun into usable electricity; however, almost 50% of the incident energy is lost as heat with present-day technologies. High-efficiency, multi-junction cells reduce this heat loss, but their cost is significantly higher. NREL's new device uses excess energy in solar photons to create extra charges rather than heat. This was achieved using 5-nanometer-diameter quantum dots of lead selenide (PbSe) tightly packed into a film. The researchers chemically treated the film, and then fabricated a device that yielded an external quantum efficiency (number of electrons produced per incident photon) exceeding 100%, a value beyond that of all current solar cells for any incident photon. Quantum dots are known to efficiently generate multiple excitons (a bound electron-hole pair) per absorbed high-energy photon, and this device definitively demonstrates the collection of multiple electrons per photon in a PV cell. The internal quantum efficiency corrects for photons that are not absorbed in the photoactive layer and shows that the PbSe film generates 30% to 40% more electrons in the high-energy spectral region than is possible with a conventional solar cell. While the unoptimized overall power conversion efficiency is still low (less than 5%), the results have important implications for PV because such high quantum efficiency can lead to more electrical current produced than possible using present technologies. Furthermore, this fabrication is also amenable to inexpensive, high-throughput roll-to-roll manufacturing.
Magnetic field induced quantum dot brightening in liquid crystal synergized magnetic and semiconducting nanoparticle composite assemblies
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Amaral, Jose Jussi; Wan, Jacky; Rodarte, Andrea L.; Ferri, Christopher; Quint, Makiko T.; Pandolfi, Ronald J.; Scheibner, Michael; Hirst, Linda S.; Ghosh, Sayantani
The design and development of multifunctional composite materials from artificial nano-constituents is one of the most compelling current research areas. This drive to improve over nature and produce 'meta-materials' has met with some success, but results have proven limited with regards to both the demonstration of synergistic functionalities and in the ability to manipulate the material properties post-fabrication and in situ. Here, magnetic nanoparticles (MNPs) and semiconducting quantum dots (QDs) are co-assembled in a nematic liquid crystalline (LC) matrix, forming composite structures in which the emission intensity of the quantum dots is systematically and reversibly controlled with a small appliedmore » magnetic field (<100 mT). This magnetic field-driven brightening, ranging between a two- to three-fold peak intensity increase, is a truly cooperative effect: the LC phase transition creates the co-assemblies, the clustering of the MNPs produces LC re-orientation at atypical low external field, and this re-arrangement produces compaction of the clusters, resulting in the detection of increased QD emission. These results demonstrate a synergistic, reversible, and an all-optical process to detect magnetic fields and additionally, as the clusters are self-assembled in a fluid medium, they offer the possibility for these sensors to be used in broad ranging fluid-based applications.« less
Magnetic field induced quantum dot brightening in liquid crystal synergized magnetic and semiconducting nanoparticle composite assemblies
Amaral, Jose Jussi; Wan, Jacky; Rodarte, Andrea L.; Ferri, Christopher; Quint, Makiko T.; Pandolfi, Ronald J.; Scheibner, Michael; Hirst, Linda S.; Ghosh, Sayantani
The design and development of multifunctional composite materials from artificial nano-constituents is one of the most compelling current research areas. This drive to improve over nature and produce �meta-materials� has met with some success, but results have proven limited with regards to both the demonstration of synergistic functionalities and in the ability to manipulate the material properties post-fabrication and in situ. Here, magnetic nanoparticles (MNPs) and semiconducting quantum dots (QDs) are co-assembled in a nematic liquid crystalline (LC) matrix, forming composite structures in which the emission intensity of the quantum dots is systematically and reversibly controlled with a small applied magnetic field (<100 mT). This magnetic field-driven brightening, ranging between a two- to three-fold peak intensity increase, is a truly cooperative effect: the LC phase transition creates the co-assemblies, the clustering of the MNPs produces LC re-orientation at atypical low external field, and this re-arrangement produces compaction of the clusters, resulting in the detection of increased QD emission. These results demonstrate a synergistic, reversible, and an all-optical process to detect magnetic fields and additionally, as the clusters are self-assembled in a fluid medium, they offer the possibility for these sensors to be used in broad ranging fluid-based applications.
Revolutionary Method for Increasing the Efficiency of White Light Quantum Dot LEDs
Duty, Chad E [ORNL; Bennett, Charlee J C [ORNL; Sabau, Adrian S [ORNL; Jellison Jr, Gerald Earle [ORNL; Boudreaux, Philip R [ORNL; Walker, Steven C [ORNL; Ott, Ronald D [ORNL
Covering a light-emitting diode (LED) with quantum dots (QDs) can produce a broad spectrum of white light. However, current techniques for applying QDs to LEDs suffer from a high density of defects and a non-uniform distribution of QDs, which respec-tively diminish the efficiency and quality of emitted light. Oak Ridge National Laboratory (ORNL) has the unique capability to thermally anneal QD structures at extremely high power densities for very short durations. This process, called pulse thermal proc-essing (PTP), reduces the number of point defects while main-taining the size and shape of the original QD nanostructure. Therefore, the efficiency of the QD wavelength conversion layer is improved without altering the emission spectrum defined by the size distribution of the quantum dot nanoparticles. The cur-rent research uses a thermal model to predict annealing tempera-tures during PTP and demonstrates up to a 300% increase in pho-toluminescence for QDs on passive substrates
Cavity-enhanced single photon emission from site-controlled In(Ga)As quantum dots fabricated using nanoimprint lithography
Tommila, J.; Hakkarainen, T. V.; Schramm, A. Guina, M.; Belykh, V. V.; Sibeldin, N. N.; Heinonen, E.
We report on the emission dynamics of single In(Ga)As quantum dots formed in etched GaAs pits and integrated into micropillar cavities. The site-controlled quantum dots were fabricated by molecular beam epitaxy on nanoimprint lithography patterned GaAs(001) surfaces. Triggered single photon emission confirmed by photon autocorrelation measurements is demonstrated. Time-resolved photoluminescence experiments clearly show an effect of the cavity on the spontaneous emission rate of the quantum dot.
Ground state energy of an exciton in a spherical quantum dot in the presence of an external magnetic field
Jahan K, Luhluh Boda, Aalu; Chatterjee, Ashok
The problem of an exciton trapped in a three dimensional Gaussian quantum dot is studied in the presence of an external magnetic field. A variational method is employed to obtain the ground state energy of the exciton as a function of the quantum dot size, the confinement strength and the magnetic field. It is also shown that the variation of the size of the exciton with the radius of the quantum dot.
Quantum-Dots Based Electrochemical Immunoassay of Interleukin-1?
Wu, Hong; Liu, Guodong; Wang, Jun; Lin, Yuehe
We describe a quantum-dot (QD, CdSe@ZnS)-based electrochemical immunoassay to detect a protein biomarker, interleukin-1? (IL-1?). QD conjugated with anti-IL-1? antibody was used as a label in an immunorecognition event. After a complete sandwich immunoreaction among the primary IL-1? antibody (immobilized on the avidin-modified magnetic beads), IL-1?, and the QD-labeled secondary antibody, QD labels were attached to the magnetic-bead surface through the antibody-antigen immunocomplex. Electrochemical stripping analysis of the captured QDs was used to quantify the concentration of IL-1? after an acid-dissolution step. The streptavidin-modified magnetic beads and the magnetic separation platform were used to integrate a facile antibody immobilization (through a biotin/streptavidin interaction) with immunoreactions and the isolation of immunocomplexes from reaction solutions in the assay. The voltammetric response is highly linear over the range of 0.5 to 50 ng mL-1 IL 1?, and the limit of detection is estimated to be 0.3 ng mL-1 (18 pM). This QD-based electrochemical immunoassay shows great promise for rapid, simple, and cost-effective analysis of protein biomarkers.
Electrically driven single photon emission from a CdSe/ZnSSe single quantum dot at 200?K
Quitsch, Wolf; K�mmell, Tilmar; Bacher, Gerd; Gust, Arne; Kruse, Carsten; Hommel, Detlef
High temperature operation of an electrically driven single photon emitter based on a single epitaxial quantum dot is reported. CdSe/ZnSSe/MgS quantum dots are embedded into a p-i-n diode architecture providing almost background free excitonic and biexcitonic electroluminescence from individual quantum dots through apertures in the top contacts. Clear antibunching with g{sup 2}(??=?0)?=?0.28?�?0.20 can be tracked up to T?=?200?K, representing the highest temperature for electrically triggered single photon emission from a single quantum dot device.
Photo-modulated thin film transistor based on dynamic charge transfer within quantum-dots-InGaZnO interface
Liu, Xiang; Yang, Xiaoxia; Liu, Mingju; Tao, Zhi; Wei, Lei Li, Chi Zhang, Xiaobing; Wang, Baoping; Dai, Qing; Nathan, Arokia
The temporal development of next-generation photo-induced transistor across semiconductor quantum dots and Zn-related oxide thin film is reported in this paper. Through the dynamic charge transfer in the interface between these two key components, the responsibility of photocurrent can be amplified for scales of times (?10{sup 4}?A/W 450?nm) by the electron injection from excited quantum dots to InGaZnO thin film. And this photo-transistor has a broader waveband (from ultraviolet to visible light) optical sensitivity compared with other Zn-related oxide photoelectric device. Moreover, persistent photoconductivity effect can be diminished in visible waveband which lead to a significant improvement in the device's relaxation time from visible illuminated to dark state due to the ultrafast quenching of quantum dots. With other inherent properties such as integrated circuit compatible, low off-state current and high external quantum efficiency resolution, it has a great potential in the photoelectric device application, such as photodetector, phototransistor, and sensor array.
Observation of the Kondo effect in a spin-3/2 hole quantum dot
Klochan, O.; Micolich, A. P.; Hamilton, A. R.; Trunov, K.; Reuter, D.; Wieck, A. D.
We report the observation of the Kondo effect in a spin-3/2 hole quantum dot formed near pinch-off in a GaAs quantum wire. We clearly observe two distinctive hallmarks of quantum dot Kondo physics. First, the zero-bias peak in the differential conductance splits an in-plane magnetic field and the splitting is independent of gate voltage. Second, the splitting rate is twice as large as that for the lowest one-dimensional subband. We show that the Zeeman splitting of the zero-bias peak is highly anisotropic and attribute this to the strong spin-orbit interaction for holes in GaAs.
g-factor anisotropy in nanowire-based InAs quantum dots
D'Hollosy, Samuel; Fábián, Gábor; Baumgartner, Andreas; Schönenberger, Christian; Nygård, Jesper
The determination and control of the electron g-factor in semiconductor quantum dots (QDs) are fundamental prerequisites in modern concepts of spintronics and spin-based quantum computation. We study the dependence of the g-factor on the orientation of an external magnetic field in quantum dots (QDs) formed between two metallic contacts on stacking fault free InAs nanowires. We extract the g-factor from the splitting of Kondo resonances and find that it varies continuously in the range between |g*| = 5 and 15.
Extraction of inhomogeneous broadening and nonradiative losses in InAs quantum-dot lasers
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Chow, Weng W.; Liu, Alan Y.; Gossard, Arthur C.; Bowers, John E.
We present a method to quantify inhomogeneous broadening and nonradiative losses in quantum dot lasers by comparing the gain and spontaneous emission results of a microscopic laser theory with measurements made on 1.3 μm InAs quantum-dot lasers. Calculated spontaneous-emission spectra are first matched to those measured experimentally to determine the inhomogeneous broadening in the experimental samples. This is possible because treatment of carrier scattering at the level of quantum kinetic equations provides the homogeneously broadened spectra without use of free parameters, such as the dephasing rate. Thus we then extract the nonradiative recombination current associated with the quantum-dot active regionmore » from a comparison of measured and calculated gain versus current relations.« less
Prediction of a strain-induced conduction-band minimum in embedded quantum dots
Williamson, A.J.; Zunger, A.; Canning, A.
Free-standing InP quantum dots have previously been theoretically and experimentally shown to have a direct band gap across a large range of experimentally accessible sizes. We demonstrated that when these dots are embedded coherently within a GaP barrier material, the effects of quantum confinement in conjunction with coherent strain suggest there will be a critical diameter of dot ({approx}60 {Angstrom}), above which the dot is direct, type I, and below which it is indirect, type II. However, the strain in the system acts to produce another conduction state with an even lower energy, in which electrons are localized in small pockets at the interface between the InP dot and the GaP barrier. Since this conduction state is GaP X{sub 1c} derived and the highest occupied valence state is InP, {Gamma} derived, the fundamental transition is predicted to be indirect in both real and reciprocal space ({open_quotes}type II{close_quotes}) for all dot sizes. This effect is peculiar to the strained dot, and is absent in the freestanding dot. {copyright} {ital 1998} {ital The American Physical Society}
Semiconductor Quantum Dots and Quantum Dot Arrays and Applications of Multiple Exciton Generation to Third-Generation Photovoltaic Solar Cells
Nozik, Arthur J.; Beard, Matthew C.; Luther, Joseph M.; Law, Matt; Ellingson, Randy J.; Johnson, Justin C.
Here, we will first briefly summarize the general principles of QD synthesis using our previous work on InP as an example. Then we will focus on QDs of the IV-VI Pb chalcogenides (PbSe, PbS, and PbTe) and Si QDs because these were among the first QDs that were reported to produce multiple excitons upon absorbing single photons of appropriate energy (a process we call multiple exciton generation (MEG)). We note that in addition to Si and the Pb-VI QDs, two other semiconductor systems (III-V InP QDs(56) and II-VI core-shell CdTe/CdSe QDs(57)) were very recently reported to also produce MEG. Then we will discuss photogenerated carrier dynamics in QDs, including the issues and controversies related to the cooling of hot carriers and the magnitude and significance of MEG in QDs. Finally, we will discuss applications of QDs and QD arrays in novel quantum dot PV cells, where multiple exciton generation from single photons could yield significantly higher PV conversion efficiencies.
Quantum Dot Materials Can Reduce Heat, Boost Electrical Output...
Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)
Golden, Colo. - Researchers at the U.S. Department of Energy's National Renewable Energy ... dots," produce as many as three electrons from one high energy photon of sunlight. ...
Photoluminescence properties of cadmium-selenide quantum dots embedded in a liquid-crystal polymer matrix
Tselikov, G. I. Timoshenko, V. Yu.; Plenge, J.; Ruehl, E.; Shatalova, A. M.; Shandryuk, G. A.; Merekalov, A. S.; Tal'roze, R. V.
The photoluminescence properties of cadmium-selenide (CdSe) quantum dots with an average size of {approx}3 nm, embedded in a liquid-crystal polymer matrix are studied. It was found that an increase in the quantum-dot concentration results in modification of the intrinsic (exciton) photoluminescence spectrum in the range 500-600 nm and a nonmonotonic change in its intensity. Time-resolved measurements show the biexponential decay of the photoluminescence intensity with various ratios of fast and slow components depending on the quantum-dot concentration. In this case, the characteristic lifetimes of exciton photoluminescence are 5-10 and 35-50 ns for the fast and slow components, respectively, which is much shorter than the times for colloidal CdSe quantum dots of the same size. The observed features of the photoluminescence spectra and kinetics are explained by the effects of light reabsorption, energy transfer from quantum dots to the liquid-crystal polymer matrix, and the effect of the electronic states at the CdSe/(liquid crystal) interface.
Inhibition of plasmonically enhanced interdot energy transfer in quantum dot solids via photo-oxidation
Sadeghi, S. M.; Nejat, A.; West, R. G.
We studied the impact of photophysical and photochemical processes on the interdot Forster energy transfer in monodisperse CdSe/ZnS quantum dot solids. For this, we investigated emission spectra of CdSe/ZnS quantum dot solids in the vicinity of gold metallic nanoparticles coated with chromium oxide. The metallic nanoparticles were used to enhance the rate of the energy transfer between the quantum dots, while the chromium oxide coating led to significant increase of their photo-oxidation rates. Our results showed that irradiation of such solids with a laser beam can lead to unique spectral changes, including narrowing and blue shift. We investigate these effects in terms of inhibition of the plasmonically enhanced interdot energy transfer between quantum dots via the chromium-oxide accelerated photo-oxidation process. We demonstrate this considering energy-dependent rate of the interdot energy transfer process, plasmonic effects, and the way photo-oxidation enhances non-radiative decay rates of quantum dots with different sizes.
Energy levels of double triangular graphene quantum dots
Liang, F. X.; Jiang, Z. T. Zhang, H. Y.; Li, S.; Lv, Z. T.
We investigate theoretically the energy levels of the coupled double triangular graphene quantum dots (GQDs) based on the tight-binding Hamiltonian model. The double GQDs including the ZZ-type, ZA-type, and AA-type GQDs with the two GQDs having the zigzag or armchair boundaries can be coupled together via different interdot connections, such as the direct coupling, the chains of benzene rings, and those of carbon atoms. It is shown that the energy spectrum of the coupled double GQDs is the amalgamation of those spectra of the corresponding two isolated GQDs with the modification triggered by the interdot connections. The interdot connection is inclined to lift up the degeneracies of the energy levels in different degree, and as the connection changes from the direct coupling to the long chains, the removal of energy degeneracies is suppressed in ZZ-type and AA-type double GQDs, which indicates that the two coupled GQDs are inclined to become decoupled. Then we consider the influences on the spectra of the coupled double GQDs induced by the electric fields applied on the GQDs or the connection, which manifests as the global spectrum redistribution or the local energy level shift. Finally, we study the symmetrical and asymmetrical energy spectra of the double GQDs caused by the substrates supporting the two GQDs, clearly demonstrating how the substrates affect the double GQDs' spectrum. This research elucidates the energy spectra of the coupled double GQDs, as well as the mechanics of manipulating them by the electric field and the substrates, which would be a significant reference for designing GQD-based devices.
Seeding of InP islands on InAs quantum dot templates
Medeiros-Ribeiro, G.; Maltez, R. L.; Bernussi, A. A.; Ugarte, D.; de Carvalho, W.
The ability of stacking layers of islands and their corresponding alignment have prompted a number of studies. The main focus so far has been on stacking self-assembled quantum dot (QD) layers of the same material and composition. Our goal is to create systems of coupled QDs of different electronic properties, aiming at hybridization of their different electronic levels. In this work, we investigate the early stages of the coupling of alternate InAs{endash}InP QD layers through a GaAs spacer layer. We have found that by using an InAs layer containing QDs as seeds, we can control the size, shape and density of InP islands by varying the spacer thickness. We have observed a significant improvement of the InP island size uniformity, as well as an induced size reduction, thus providing an extra degree of tunability previously available only through growth kinetics. {copyright} 2001 American Institute of Physics.
Advanced method for increasing the efficiency of white light quantum dot LEDs
Duty, Chad E [ORNL; Bennett, Charlee J C [ORNL; Sabau, Adrian S [ORNL; Jellison Jr, Gerald Earle [ORNL; Boudreaux, Philip R [ORNL; Walker, Steven C [ORNL; Ott, Ronald D [ORNL
Covering a light-emitting diode (LED) with quantum dots (QDs) can produce a broad spectrum of white light. However, current techniques for applying QDs to LEDs suffer from a high density of defects and a non-uniform distribution of QDs, which, respectively, diminish the efficiency and quality of emitted light. Oak Ridge National Laboratory (ORNL) has the unique capability to thermally anneal QD structures at extremely high power densities for very short durations. This process, called pulse thermal processing (PTP), reduces the number of point defects while maintaining the size and shape of the original QD nanostructure. Therefore, the efficiency of the QD wavelength conversion layer is improved without altering the emission spectrum defined by the size distribution of theQD nanoparticles. The current research uses a thermal model to predict annealing temperatures during PTP and demonstrates up to a 300% increase in photoluminescence for QDs on passive substrates.
Luminescence of CdSe/ZnS quantum dots infiltrated into an opal matrix
Gruzintsev, A. N. Emelchenko, G. A.; Masalov, V. M.; Yakimov, E. E.; Barthou, C.; Maitre, A.
The effect of the photonic band gap in the photonic crystal, the synthesized SiO{sub 2} opal with embedded CdSe/ZnS quantum dots, on its luminescence in the visible spectral region is studied. It is shown that the position of the photonic band gap in the luminescence and reflectance spectra for the infiltrated opal depends on the diameter of the constituent nanospheres and on the angle of recording the signal. The optimal conditions for embedding the CdSe/ZnS quantum dots from the solution into the opal matrix are determined. It is found that, for the opal-CdSe/ZnS nanocomposites, the emission intensity decreases and the luminescence decay time increases in the spatial directions, in which the spectral positions of the photonic band gap and the luminescence peak of the quantum dots coincide.
Carrier multiplication detected through transient photocurrent in device-grade films of lead selenide quantum dots
Gao, Jianbo; Fidler, Andrew F.; Klimov, Victor I.
In carrier multiplication, the absorption of a single photon results in two or more electron–hole pairs. Quantum dots are promising materials for implementing carrier multiplication principles in real-life technologies. So far, however, most of research in this area has focused on optical studies of solution samples with yet to be proven relevance to practical devices. We report ultra-fast electro-optical studies of device-grade films of electronically coupled quantum dots that allow us to observe multiplication directly in the photocurrent. Our studies help rationalize previous results from both optical spectroscopy and steady-state photocurrent measurements and also provide new insights into effects of electric field and ligand treatments on multiexciton yields. Importantly, we demonstrate that using appropriate chemical treatments of the films, extra charges produced by carrier multiplication can be extracted from the quantum dots before they are lost to Auger recombination and hence can contribute to photocurrent of practical devices.
Determination of carrier lifetime and mobility in colloidal quantum dot films via impedance spectroscopy
Rath, Arup K.; Lasanta, Tania; Bernechea, Maria; Diedenhofen, Silke L.; Konstantatos, Gerasimos
Impedance Spectroscopy (IS) proves to be a powerful tool for the determination of carrier lifetime and majority carrier mobility in colloidal quantum dot films. We employ IS to determine the carrier lifetime in PbS quantum dot Schottky solar cells with Al and we verify the validity of the technique via transient photovoltage. We also present a simple approach based on an RC model that allows the determination of carrier mobility in PbS quantum dot films and we corroborate the results via comparison with space charge limited measurements. In summary, we demonstrate the potential of IS to characterize key-to-photovoltaics optoelectronic properties, carrier lifetime, and mobility, in a facile way.
Design of quantum dot lattices in amorphous matrices by ion beam irradiation
Buljan, M.; Bogdanovic-Radovic, I.; Karlusic, M.; Desnica, U. V.; Radic, N.; Jaksic, M.; Salamon, K.; Drazic, G.; Bernstorff, S.; Holy, V.
We report on the highly controllable self-assembly of semiconductor quantum dots and metallic nanoparticles in a solid amorphous matrix, induced by ion beam irradiation of an amorphous multilayer. We demonstrate experimentally and theoretically a possibility to tune the basic structural properties of the quantum dots in a wide range. Furthermore, the sizes, distances, and arrangement type of the quantum dots follow simple equations dependent on the irradiation and the multilayer properties. We present a Monte Carlo model for the simulation and prediction of the structural properties of the materials formed by this method. The presented results enable engineering and simple production of functional materials or simple devices interesting for applications in nanotechnology.
Enhanced spontaneous emission of CdSe quantum dots in monolithic II-VI pillar microcavities
Lohmeyer, H.; Kruse, C.; Sebald, K.; Gutowski, J.; Hommel, D.
The emission properties of CdSe/ZnSe quantum dots in ZnSe-based pillar microcavities are studied. All-epitaxial cavities made of ZnSSe and MgS/ZnCdSe superlattices with a single quantum-dot sheet embedded have been grown by molecular beam epitaxy. Pillar structures with diameters down to 500 nm have been realized by focused-ion-beam etching. A pronounced enhancement of the spontaneous emission rate of quantum dots coupling to the fundamental mode of the cavities is found as evidence for the Purcell effect. The enhancement by a factor of up to 3.8 depends systematically on the pillar diameter and thus on the Purcell factor of the individual pillars.
Microscopic model for intersubband gain from electrically pumped quantum-dot structures
Michael, Stephan; Chow, Weng Wah; Schneider, Han Christian
We study theoretically the performance of electrically pumped self-organized quantum dots as a gain material in the mid-infrared range at room temperature. We analyze an AlGaAs/InGaAs based structure composed of dots-in-a-well sandwiched between two quantum wells. We numerically analyze a comprehensive model by combining a many-particle approach for electronic dynamics with a realistic modeling of the electronic states in the whole structure. We investigate the gain both for quasi-equilibrium conditions and current injection. We find, comparing different structures, that steady-state gain can only be realized by an efficient extraction process, which prevents an accumulation of electrons in continuum states, that make the available scattering pathways through the quantum-dot active region too fast to sustain inversion.
Determination of shape anisotropy in embedded low contrast submonolayer quantum dot structures
Dhomkar, S.; Ji, H.; Kuskovsky, I. L.; Vaxelaire, N.; Noyan, I. C.; Shuvayev, V.; Tamargo, M. C.
We describe a procedure for the morphological characterization of hard-to-image submonolayer quantum dot structures. This procedure employs high resolution x-ray diffraction based reciprocal space mapping, accompanied by rigorous diffraction modeling for precise determination of the morphology of submonolayer quantum dots. Our modelling results and experimental data clearly show that the investigated quantum dots are anisotropically elongated along the [110] orientation. Complementary polarization dependent photoluminescence measurements, combined with our previously reported magneto-photoluminescence data, confirm this conclusion. Our formalism enables direct extraction of structural information of complex embedded three-dimensional structures, which, due to their low electron density contrast with respect to the surrounding host matrix, cannot be readily investigated by traditional electron diffraction techniques.
Microscopic model for intersubband gain from electrically pumped quantum-dot structures
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Michael, Stephan; Chow, Weng Wah; Schneider, Han Christian
We study theoretically the performance of electrically pumped self-organized quantum dots as a gain material in the mid-infrared range at room temperature. We analyze an AlGaAs/InGaAs based structure composed of dots-in-a-well sandwiched between two quantum wells. We numerically analyze a comprehensive model by combining a many-particle approach for electronic dynamics with a realistic modeling of the electronic states in the whole structure. We investigate the gain both for quasi-equilibrium conditions and current injection. We find, comparing different structures, that steady-state gain can only be realized by an efficient extraction process, which prevents an accumulation of electrons in continuum states, thatmore » make the available scattering pathways through the quantum-dot active region too fast to sustain inversion.« less
Blue and green electroluminescence from CdSe nanocrystal quantum-dot-quantum-wells
Lu, Y. F.; Cao, X. A.
CdS/CdSe/ZnS quantum dot quantum well (QDQW) nanocrystals were synthesized using the successive ion layer adsorption and reaction technique, and their optical properties were tuned by bandgap and strain engineering. 3-monolayer (ML) CdSe QWs emitted blue photoluminescence at 467 nm with a spectral full-width-at-half-maximum of ∼30 nm. With a 3 ML ZnS cladding layer, which also acts as a passivating and strain-compensating layer, the QDQWs acquired a ∼35% quantum yield of the QW emission. Blue and green electroluminescence (EL) was obtained from QDQW light-emitting devices with 3–4.5 ML CdSe QWs. It was found that as the peak blueshifted, the overall EL was increasingly dominated by defect state emission due to poor hole injection into the QDQWs. The weak EL was also attributed to strong field-induced charge separation resulting from the unique QDQW geometry, weakening the oscillator strength of optical transitions.
The impact of disorder on charge transport in three dimensional quantum dot resonant tunneling structures
Puthen-Veettil, B. Patterson, R.; K�nig, D.; Conibeer, G.; Green, M. A.
Efficient iso-entropic energy filtering of electronic waves can be realized through nanostructures with three dimensional confinement, such as quantum dot resonant tunneling structures. Large-area deployment of such structures is useful for energy selective contacts but such configuration is susceptible to structural disorders. In this work, the transport properties of quantum-dot-based wide-area resonant tunneling structures, subject to realistic disorder mechanisms, are studied. Positional variations of the quantum dots are shown to reduce the resonant transmission peaks while size variations in the device are shown to reduce as well as broaden the peaks. Increased quantum dot size distribution also results in a peak shift to lower energy which is attributed to large dots dominating transmission. A decrease in barrier thickness reduces the relative peak height while the overall transmission increases dramatically due to lower �series resistance.� While any shift away from ideality can be intuitively expected to reduce the resonance peak, quantification allows better understanding of the tolerances required for fabricating structures based on resonant tunneling phenomena/.
Single InAs quantum dot coupled to different 'environments' in one wafer for quantum photonics
Yu, Ying; Shang, Xiang-Jun; Li, Mi-Feng; Zha, Guo-Wei; Xu, Jian-Xing; Wang, Li-Juan; Wang, Guo-Wei; Ni, Hai-Qiao; Dou, Xiuming; Sun, Baoquan; Niu, Zhi-Chuan
Self assembled small InAs quantum dots (SQDs) were formed in various densities and environments using gradient InAs deposition on a non-rotating GaAs substrate. Two SQD environments (SQD I and SQD II) were characterized. SQD I featured SQDs surrounded by large QDs, and SQD II featured individual SQDs in the wetting layer (WL). Micro-photoluminescence of single QDs embedded in a cavity under various excitation powers and electric fields gave insight into carrier transport processes. Potential fluctuations of the WL in SQD II, induced by charge redistribution, show promise for charge-tunable QD devices; SQD I shows higher luminescence intensity as a single-photon source.
Temperature dependency of the emission properties from positioned In(Ga)As/GaAs quantum dots
Braun, T.; Schneider, C.; Maier, S.; Forchel, A.; Höfling, S.; Kamp, M.; Igusa, R.; Iwamoto, S.; Arakawa, Y.
In this letter we study the influence of temperature and excitation power on the emission linewidth from site-controlled InGaAs/GaAs quantum dots grown on nanoholes defined by electron beam lithography and wet chemical etching. We identify thermal electron activation as well as direct exciton loss as the dominant intensity quenching channels. Additionally, we carefully analyze the effects of optical and acoustic phonons as well as close-by defects on the emission linewidth by means of temperature and power dependent micro-photoluminescence on single quantum dots with large pitches.
All-optical depletion of dark excitons from a semiconductor quantum dot
Schmidgall, E. R.; Schwartz, I.; Cogan, D.; Gershoni, D.; Gantz, L.; Heindel, T.; Reitzenstein, S.
Semiconductor quantum dots are considered to be the leading venue for fabricating on-demand sources of single photons. However, the generation of long-lived dark excitons imposes significant limits on the efficiency of these sources. We demonstrate a technique that optically pumps the dark exciton population and converts it to a bright exciton population, using intermediate excited biexciton states. We show experimentally that our method considerably reduces the dark exciton population while doubling the triggered bright exciton emission, approaching thereby near-unit fidelity of quantum dot depletion.
Simulation of a broadband nano-biosensor based on an onion-like quantum dot-quantum well structure
Absalan, H; SalmanOgli, A; Rostami, R
The fluorescence resonance energy transfer is studied between modified quantum-dots and quantum-wells used as a donor and an acceptor. Because of the unique properties of quantum dots, including diverse surface modification flexibility, bio-compatibility, high quantum yields and wide absorption, their use as nano-biosensors and bio-markers used in diagnosis of cancer is suggested. The fluorescence resonance energy transfer is simulated in a quantum dot-quantum well system, where the energy can flow from donor to acceptor. If the energy transfer can be either turned on or off by a specific interaction, such as interaction with any dyes, a molecular binding event or a cleavage reaction, a sensor can be designed (under assumption that the healthy cells have a known effect or unyielding effect on output parameters while cancerous cells, due to their pandemic optical properties, can impact the fluorescence resonance energy transfer parameters). The developed nano-biosensor can operate in a wide range of wavelengths (310 - 760 nm). (laser applications in biology and medicine)
InP quantum dots: Electronic structure, surface effects, and the redshifted emission
Fu, H.; Zunger, A.
We present pseudopotential plane-wave electronic-structure calculations on InP quantum dots in an effort to understand quantum confinement and surface effects and to identify the origin of the long-lived and redshifted luminescence. We find that (i) unlike the case in small GaAs dots, the lowest unoccupied state of InP dots is the {Gamma}{sub 1c}-derived direct state rather than the X{sub 1c}-derived indirect state and (ii) unlike the prediction of {bold k}{center_dot}{bold p} models, the highest occupied state in InP dots has a 1sd-type envelope function rather than a (dipole-forbidden) 1pf envelope function. Thus explanations (i) and (ii) to the long-lived redshifted emission in terms of an orbitally forbidden character can be excluded. Furthermore, (iii) fully passivated InP dots have no surface states in the gap. However, (iv) removal of the anion-site passivation leads to a P dangling bond (DB) state just above the valence band, which will act as a trap for photogenerated holes. Similarly, (v) removal of the cation-site passivation leads to an In dangling-bond state below the conduction band. While the energy of the In DB state depends only weakly on quantum size, its radiative lifetime increases with quantum size. The calculated {approximately}300-meV redshift and the {approximately}18 times longer radiative lifetime relative to the dot-interior transition for the 26-{Angstrom} dot with an In DB are in good agreement with the observations of full-luminescence experiments for unetched InP dots. Yet, (vi) this type of redshift due to surface defect is inconsistent with that measured in {ital selective} excitation for HF-etched InP dots. (vii) The latter type of ({open_quotes}resonant{close_quotes}) redshift is compatible with the calculated {ital screened} singlet-triplet splitting in InP dots, suggesting that the slow emitting state seen in selective excitation could be a triplet state. {copyright} {ital 1997} {ital The American Physical Society}
Interference with a quantum dot single-photon source and a laser at telecom wavelength
Felle, M.; Huwer, J. Stevenson, R. M.; Skiba-Szymanska, J.; Ward, M. B.; Shields, A. J.; Farrer, I.; Ritchie, D. A.; Penty, R. V.
The interference of photons emitted by dissimilar sources is an essential requirement for a wide range of photonic quantum information applications. Many of these applications are in quantum communications and need to operate at standard telecommunication wavelengths to minimize the impact of photon losses and be compatible with existing infrastructure. Here, we demonstrate for the first time the quantum interference of telecom-wavelength photons from an InAs/GaAs quantum dot single-photon source and a laser; an important step towards such applications. The results are in good agreement with a theoretical model, indicating a high degree of indistinguishability for the interfering photons.
InGaAs/GaAs (110) quantum dot formation via step meandering
Diez-Merino, Laura; Tejedor, Paloma
InGaAs (110) semiconductor quantum dots (QDs) offer very promising prospects as a material base for a new generation of high-speed spintronic devices, such as single electron transistors for quantum computing. However, the spontaneous formation of InGaAs QDs is prevented by two-dimensional (2D) layer-by-layer growth on singular GaAs (110) substrates. In this work we have studied, by using atomic force microscopy and photoluminescence spectroscopy (PL), the growth of InGaAs/GaAs QDs on GaAs (110) stepped substrates by molecular beam epitaxy (MBE), and the modification of the adatom incorporation kinetics to surface steps in the presence of chemisorbed atomic hydrogen. The as-grown QDs exhibit lateral dimensions below 100 nm and emission peaks in the 1.35-1.37 eV range. It has been found that a step meandering instability derived from the preferential attachment of In adatoms to [110]-step edges relative to [11n]-type steps plays a key role in the destabilization of 2D growth that leads to 3D mound formation on both conventional and H-terminated vicinal substrates. In the latter case, the driving force for 3D growth via step meandering is enhanced by H-induced upward mass transport in addition to the lower energy cost associated with island formation on H-terminated substrates, which results in a high density array of InGaAs/GaAs dots selectively nucleated on the terrace apices with reduced lateral dimensions and improved PL efficiency relative to those of conventional MBE-grown samples.
Full counting statistics as a probe of quantum coherence in a side-coupled double quantum dot system
Xue, Hai-Bin
We study theoretically the full counting statistics of electron transport through side-coupled double quantum dot (QD) based on an efficient particle-number-resolved master equation. It is demonstrated that the high-order cumulants of transport current are more sensitive to the quantum coherence than the average current, which can be used to probe the quantum coherence of the considered double QD system. Especially, quantum coherence plays a crucial role in determining whether the super-Poissonian noise occurs in the weak inter-dot hopping coupling regime depending on the corresponding QD-lead coupling, and the corresponding values of super-Poissonian noise can be relatively enhanced when considering the spins of conduction electrons. Moreover, this super-Poissonian noise bias range depends on the singly-occupied eigenstates of the system, which thus suggests a tunable super-Poissonian noise device. The occurrence-mechanism of super-Poissonian noise can be understood in terms of the interplay of quantum coherence and effective competition between fast-and-slow transport channels. -- Highlights: �The FCS can be used to probe the quantum coherence of side-coupled double QD system. �Probing quantum coherence using FCS may permit experimental tests in the near future. �The current noise characteristics depend on the quantum coherence of this QD system. �The super-Poissonian noise can be enhanced when considering conduction electron spin. �The side-coupled double QD system suggests a tunable super-Poissonian noise device.
Effect of matrix on InAs self-organized quantum dots on InP substrate
Ustinov, V.M.; Weber, E.R.; Ruvimov, S.; Liliental-Weber, Z.; Zhukov, A.E.; Egorov, A.Y.; Kovsh, A.R.; Tsatsulnikov, A.F.; Kopev, P.S.
InAs self-organized quantum dots in In{sub 0.53}Ga{sub 0.47}As and In{sub 0.52}Al{sub 0.48}As matrices have been grown on InP substrates by molecular beam epitaxy. The dot size in InGaAs has been found to be 3{endash}4 times larger, but the areal density about an order of magnitude smaller than that in InAlAs. Low-temperature photoluminescence (PL) of the InAs/InGaAs quantum dots is characterized by a narrow (35 meV) PL line as compared to that of InAs/InAlAs quantum dots (170 meV). Quantum dot formation increases the carrier localization energy as compared to quantum well structures with the same InAs thickness in a similar manner for both InAs/InGaAs and InAs/InAlAs structures. The effect of the barrier band gap on the optical transition energy is qualitatively the same for quantum well and quantum dot structures. The results demonstrate a possibility of controlling the quantum dot emission wavelength by varying the matrix composition. {copyright} {ital 1998 American Institute of Physics.}
CdSe Quantum-Dot-Sensitized Solar Cell with ~100% Internal Quantum Efficiency
Fuke, Nobuhiro; Hoch, Laura B.; Koposov, Alexey Y.; Manner, Virginia W.; Werder, Donald J.; Fukui, Atsushi; Koide, Naoki; Katayama, Hiroyuki; Sykora, Milan
We have constructed and studied photoelectrochemical solar cells (PECs) consisting of a photoanode prepared by direct deposition of independently synthesized CdSe nanocrystal quantum dots (NQDs) onto a nanocrystalline TiO2 film (NQD/TiO2), aqueous Na2S or Li2S electrolyte, and a Pt counter electrode. We show that light harvesting efficiency (LHE) of the NQD/TiO2 photoanode is significantly enhanced when the NQD surface passivation is changed from tri-n-octylphosphine oxide (TOPO) to 4-butylamine (BA). In the PEC the use of NQDs with a shorter passivating ligand, BA, leads to a significant enhancement in both the electron injection efficiency at the NQD/TiO2 interface and charge collection efficiency at the NQD/electrolyte interface, with the latter attributed mostly to a more efficient diffusion of the electrolyte through the pores of the photoanode. We show that by utilizing BA-capped NQDs and aqueous Li2S as an electrolyte, it is possible to achieve ~100% internal quantum efficiency of photon-to-electron conversion, matching the performance of dye-sensitized solar cells.
Background limited mid-infrared photodetection with photovoltaic HgTe colloidal quantum dots
Guyot-Sionnest, Philippe Roberts, John Andris
The photovoltaic response of thin films of HgTe colloidal quantum dots in the 3–5 μm range is observed. With no applied bias, internal quantum efficiency exceeding 40%, specific detectivity above 10{sup 10} Jones and microseconds response times are obtained at 140 K. The cooled devices detect the ambient thermal radiation. A detector with 5.25 μm cut-off achieves Background Limited Infrared Photodetection at 90 K.
Exciton dissociation and interdot transport in CdSe quantum-dot molecules
Franceschetti, Alberto; Zunger, Alex
One of the most important parameters that determine the transport properties of a quantum dot array is the exciton dissociation energy, i.e., the energy {Delta}E required to dissociate an exciton into an electron and a hole localized in different dots. We show that a pseudopotential calculation for a dot molecule, coupled with a basic configuration interaction calculation of the exciton energy levels, provides directly the exciton dissociation energy, including the effects of wave function overlap, screened Coulomb attraction between the electron and the hole in different dots, and polarization effects. We find that {Delta}E decreases as the interdot distance decreases and as the dielectric constant of the medium increases.
Deep-level transient spectroscopy of InAs/GaAs quantum dot superlattices
Sobolev, M. M.; Nevedomskii, V. N.; Zolotareva, R. V.; Vasil'ev, A. P.; Ustinov, V. M.
Deep level transient spectroscopy (DLTS) has been applied to study the carrier emission from states of a 10-layer system of tunnel-coupled vertically correlated quantum dots (VCQDs) in p-n InAs/GaAs heterostructures with different widths of GaAs spacers under varied reverse bias (U{sub r}) and filling voltage pulse U{sub f}.
Ligand-Mediated Modification of the Electronic Structure of CdSe Quantum Dots
Lee, Jonathan R.; Whitley, Heather D.; Meulenberg, Robert W.; Wolcott, Abraham; Zhang, Jin Z.; Prendergast, Peter; Lovingood, Derek D.; Strouse, Geoffrey F.; Ogitsu, Tadashi; Schwegler, Eric; Terminello, Louis J.; Van Buuren, Tony W.
X-ray absorption spectroscopy and ab initio modeling of the experimental spectra have been used to investigate the effects of surface passivation on the unoccupied electronic states of CdSe quantum dots (QDs). Significant differences are observed in the unoccupied electronic structure of the CdSe QDs, which are shown to arise from variations in specific ligand-surface bonding interactions.
Red, green, and blue lasing enabled by single-exciton gain in colloidal quantum dot films
Nurmikko, Arto V.; Dang, Cuong
The methods and materials described herein contemplate the use films of colloidal quantum dots as a gain medium in a vertical-cavity surface-emitting laser. The present disclosure demonstrates a laser with single-exciton gain in the red, green, and blue wavelengths. Leveraging this nanocomposite gain, the results realize a significant step toward full-color single-material lasers.
Synthesis and optical properties of cadmium selenide quantum dots for white light-emitting diode application
Xu, Xianmei; Wang, Yilin; Gule, Teri; Luo, Qiang [School of Chemistry and Chemical Engineering, Guangxi University, Nanning 53000 (China); Zhou, Liya, E-mail: firstname.lastname@example.com [School of Chemistry and Chemical Engineering, Guangxi University, Nanning 53000 (China); Gong, Fuzhong [School of Chemistry and Chemical Engineering, Guangxi University, Nanning 53000 (China)
Highlights: ? Stable CdSe QDs were synthesized by the one-step and two-level process respectively. ? The fabricated white LEDs show good white balance. ? CdSe QDs present well green to yellow band luminescence. ? CdSe QDs displayed a broad excitation band. - Abstract: Yellow light-emitting cadmium selenide quantum dots were synthesized using one-step and two-step methods in an aqueous medium. The structural luminescent properties of these quantum dots were investigated. The obtained cadmium selenide quantum dots displayed a broad excitation band suitable for blue or near-ultraviolet light-emitting diode applications. White light-emitting diodes were fabricated by coating the cadmium selenide samples onto a 460 nm-emitting indium gallium nitrite chip. Both samples exhibited good white balance. Under a 20 mA working current, the white light-emitting diode fabricated via the one-step and two-step methods showed Commission Internationale de l��clairage coordinates at (0.27, 0.23) and (0.27, 0.33), respectively, and a color rendering index equal to 41 and 37, respectively. The one-step approach was simpler, greener, and more effective than the two-step approach. The one-step approach can be enhanced by combining cadmium selenide quantum dots with proper phosphors.
Theoretical performance of solar cell based on mini-bands quantum dots
Aly, Abou El-Maaty M. E-mail: email@example.com; Nasr, A. E-mail: email@example.com
The tremendous amount of research in solar energy is directed toward intermediate band solar cell for its advantages compared with the conventional solar cell. The latter has lower efficiency because the photons have lower energy than the bandgap energy and cannot excite mobile carriers from the valence band to the conduction band. On the other hand, if mini intermediate band is introduced between the valence and conduction bands, then the smaller energy photons can be used to promote charge carriers transfer to the conduction band and thereby the total current increases while maintaining a large open circuit voltage. In this article, the influence of the new band on the power conversion efficiency for structure of quantum dots intermediate band solar cell is theoretically investigated and studied. The time-independent Schr�dinger equation is used to determine the optimum width and location of the intermediate band. Accordingly, achievement of a maximum efficiency by changing the width of quantum dots and barrier distances is studied. Theoretical determination of the power conversion efficiency under the two different ranges of QD width is presented. From the obtained results, the maximum power conversion efficiency is about 70.42%. It is carried out for simple cubic quantum dot crystal under fully concentrated light. It is strongly dependent on the width of quantum dots and barrier distances.
Determining the exact number of dye molecules attached to colloidal CdSe/ZnS quantum dots in F�rster resonant energy transfer assemblies
Kaiser, Uwe; Jimenez de Aberasturi, Dorleta; V�zquez-Gonz�lez, Margarita; Carrillo-Carrion, Carolina; Niebling, Tobias; Parak, Wofgang J.; Heimbrodt, Wolfram
Semiconductor quantum dots functionalized with organic dye molecules are important tools for biological sensor applications. Energy transfer between the quantum dot and the attached dyes can be utilized for sensing. Though important, the determination of the real number of dye molecules attached per quantum dot is rather difficult. In this work, a method will be presented to determine the number of ATTO-590 dye molecules attached to CdSe/ZnS quantum dots based on time resolved spectral analysis. The energy transfer from the excited quantum dot to the attached ATTO-590 dye leads to a reduced lifetime of the quantum dot's excitons. The higher the concentration of dye molecules, the shorter the excitonic lifetime becomes. However, the number of dye molecules attached per quantum dot will vary. Therefore, for correctly explaining the decay of the luminescence upon photoexcitation of the quantum dot, it is necessary to take into account the distribution of the number of dyes attached per quantum dot. A Poisson distribution of the ATTO-590 dye molecules not only leads to excellent agreement between experimental and theoretical decay curves but also additionally yields the average number of dye molecules attached per quantum dot. In this way, the number of dyes per quantum dot can be conveniently determined.
Toxicological studies of semiconductor quantum dots on immune cells.
Ricken, James Bryce; Rios, Lynette; Poschet, Jens Fredrich; Bachand, Marlene; Bachand, George David; Greene, Adrienne Celeste; Carroll-Portillo, Amanda
Nanoengineered materials hold a vast promise of enabling revolutionary technologies, but also pose an emerging and potentially serious threat to human and environmental health. While there is increasing knowledge concerning the risks posed by engineered nanomaterials, significant inconsistencies exist within the current data based on the high degree of variability in the materials (e.g., synthesis method, coatings, etc) and biological test systems (e.g., cell lines, whole organism, etc). In this project, we evaluated the uptake and response of two immune cell lines (RAW macrophage and RBL mast cells) to nanocrystal quantum dots (Qdots) with different sizes and surface chemistries, and at different concentrations. The basic experimental design followed a 2 x 2 x 3 factorial model: two Qdot sizes (Qdot 520 and 620), two surface chemistries (amine 'NH{sub 2}' and carboxylic acid 'COOH'), and three concentrations (0, 1 nM, and 1 {micro}M). Based on this design, the following Qdots from Evident Technologies were used for all experiments: Qdot 520-COOH, Qdot 520-NH{sub 2}, Qdot 620-COOH, and Qdot 620-NH{sub 2}. Fluorescence and confocal imaging demonstrated that Qdot 620-COOH and Qdot 620-NH{sub 2} nanoparticles had a greater level of internalization and cell membrane association in RAW and RBL cells, respectively. From these data, a two-way interaction between Qdot size and concentration was observed in relation to the level of cellular uptake in RAW cells, and association with RBL cell membranes. Toxicity of both RBL and RAW cells was also significantly dependent on the interaction of Qdot size and concentration; the 1 {micro}M concentrations of the larger, Qdot 620 nanoparticles induced a greater toxic effect on both cell lines. The RBL data also demonstrate that Qdot exposure can induce significant toxicity independent of cellular uptake. A significant increase in TNF-{alpha} and decrease in IL-10 release was observed in RAW cells, and suggested that Qdot exposure
Suppression of dark current through barrier engineer for solution-processed colloidal quantum-dots infrared photodetectors
Jiang, Zhenyu E-mail: email@example.com; Liu, Yan; Mo, Chen; Wang, Li; Atalla, Mahmoud R. M.; Liu, Jie; Kurhade, Kandhar K.; Xu, Jian E-mail: firstname.lastname@example.com; Hu, Wenjia; Zhang, Wenjun; You, Guanjun; Zhang, Yu
In an attempt to suppress the dark current, the barrier layer engineer for solution-processed PbSe colloidal quantum-dot (CQD) photodetectors has been investigated in the present study. It was found that the dark current can be significantly suppressed by implementing two types of carrier blocking layers, namely, hole blocking layer and electron blocking layer, sandwiched in between two active PbSe CQD layers. Meanwhile no adverse impact has been observed for the photo current. Our study suggests that this improvement resides on the transport pathway created via carrier recombination at intermediate layer, which provides wide implications for the suppression of dark current for infrared photodetectors.
The use of bulk states to accelerate the band edge state calculation of a semiconductor quantum dot
Voemel, Christof . E-mail: firstname.lastname@example.com; Tomov, Stanimire Z. . E-mail: email@example.com; Wang, Lin-Wang . E-mail: email@example.com; Marques, Osni A. . E-mail: email@example.com; Dongarra, Jack J. . E-mail: email@example.com
We present a new technique to accelerate the convergence of the folded spectrum method in empirical pseudopotential band edge state calculations for colloidal quantum dots. We use bulk band states of the materials constituent of the quantum dot to construct initial vectors and a preconditioner. We apply these to accelerate the convergence of the folded spectrum method for the interior states at the top of the valence and the bottom of the conduction band. For large CdSe quantum dots, the number of iteration steps until convergence decreases by about a factor of 4 compared to previous calculations.
Tunable Quantum Dot Solids: Impact of Interparticle Interactions on Bulk Properties
Sinclair, Michael B.; Fan, Hongyou; Brener, Igal; Liu, Sheng; Luk, Ting S.; Li, Binsong
QD-solids comprising self-assembled semiconductor nanocrystals such as CdSe are currently under investigation for use in a wide array of applications including light emitting diodes, solar cells, field effect transistors, photodetectors, and biosensors. The goal of this LDRD project was develop a fundamental understanding of the relationship between nanoparticle interactions and the different regimes of charge and energy transport in semiconductor quantum dot (QD) solids. Interparticle spacing was tuned through the application of hydrostatic pressure in a diamond anvil cell, and the impact on interparticle interactions was probed using x-ray scattering and a variety of static and transient optical spectroscopies. During the course of this LDRD, we discovered a new, previously unknown, route to synthesize semiconductor quantum wires using high pressure sintering of self-assembled quantum dot crystals. We believe that this new, pressure driven synthesis approach holds great potential as a new tool for nanomaterials synthesis and engineering.
Sandia Develops a Synthesis of Quantum Dots that Increases the...
Broader source: All U.S. Department of Energy (DOE) Office Webpages (Extended Search)
Energy Frontier Research Centers: Solid-State Lighting Science Center for Frontiers of ... Research & Capabilities, Solid-State LightingSandia Develops a Synthesis of Quantum ...
Effect of parameter variations on the static and dynamic behaviour of a self-assembled quantum-dot laser using circuit-level modelling
Razm-Pa, M; Emami, F
We report a new circuit model for a self-assembled quantum-dot (SAQD) laser made of InGaAs/GaAs structures. The model is based on the excited state and standard rate equations, improves the previously suggested circuit models and also provides and investigates the performance of this kind of laser. The carrier dynamic effects on static and dynamic characteristics of a SAQD laser are analysed. The phonon bottleneck problem is simulated. Quantum-dot lasers are shown to be quite sensitive to the crystal quality outside and inside quantum dots. The effects of QD coverage factor, inhomogeneous broadening, the physical source of which is the size fluctuation of quantum dots formed by self-assembly of atoms, and cavity length on the SAQD laser characteristics are analysed. The results of simulation show that an increase in the cavity length and in the QD coverage factor results in the growth of the output power. On the other hand, an increase in the coverage factor and a degradation of inhomogeneous broadening lead to an increase in the modulation bandwidth. The effect of the QD height (cylindrical shape) and stripe width of the laser cavity on QD laser modulation is also analysed. (lasers)
Photo-induced conductance fluctuations in mesoscopic Ge/Si systems with quantum dots
Stepina, N. P.; Dvurechenskii, A. V.; Nikiforov, A. I.; Moers, J.; Gruetzmacher, D.
We study the evolution of electron transport in strongly localized mesoscopic system with quantum dots under small photon flux. Exploring devices with narrow transport channels lead to the observation of giant fluctuations of the photoconductance, which is attributed to the strong dependence of hopping current on the filling of dots by holes. In our experiments, single-photon mode operation is indicated by the linear dependence of the frequency of photo-induced fluctuations on the light intensity and the step-like response of conductance on the pulse excitation. The effect of the light wavelength, measurement temperature, size of the conductive channel on the device efficiency are considered.
Temperature dependent photoluminescence and micromapping of multiple stacks InAs quantum dots
Xu, Ming Jaffré, Alexandre Alvarez, José Kleider, Jean-Paul Boutchich, Mohamed; Jittrong, Apichat; Chokamnuai, Thitipong; Panyakeow, Somsak; Kanjanachuchai, Songphol
We utilized temperature dependent photoluminescence (PL) techniques to investigate 1, 3 and 5 stack InGaAs quantum dots (QDs) grown on cross-hatch patterns. PL mapping can well reproduce the QDs distribution as AFM and position dependency of QD growth. It is possible to observe crystallographic dependent PL. The temperature dependent spectra exhibit the QDs energy distribution which reflects the size and shape. The inter-dot carrier coupling effect is observed and translated as a red shift of 120mV on the [1–10] direction peak is observed at 30K on 1 stack with regards to 3 stacks samples, which is assigned to lateral coupling.
Superconducting transport in single and parallel double InAs quantum dot Josephson junctions with Nb-based superconducting electrodes
Baba, Shoji Sailer, Juergen; Deacon, Russell S.; Oiwa, Akira; Shibata, Kenji; Hirakawa, Kazuhiko; Tarucha, Seigo
We report conductance and supercurrent measurements for InAs single and parallel double quantum dot Josephson junctions contacted with Nb or NbTiN superconducting electrodes. Large superconducting gap energy, high critical field, and large switching current are observed, all reflecting the features of Nb-based electrodes. For the parallel double dots, we observe an enhanced supercurrent when both dots are on resonance, which may reflect split Cooper pair tunneling.
Probing the structural dependency of photoinduced properties of colloidal quantum dots using metal-oxide photo-active substrates
Patty, Kira; Campbell, Quinn; Hamilton, Nathan; West, Robert G.; Sadeghi, Seyed M.; Mao, Chuanbin
We used photoactive substrates consisting of about 1 nm coating of a metal oxide on glass substrates to investigate the impact of the structures of colloidal quantum dots on their photophysical and photochemical properties. We showed during irradiation these substrates can interact uniquely with such quantum dots, inducing distinct forms of photo-induced processes when they have different cores, shells, or ligands. In particular, our results showed that for certain types of core-shell quantum dot structures an ultrathin layer of a metal oxide can reduce suppression of quantum efficiency of the quantum dots happening when they undergo extensive photo-oxidation. This suggests the possibility of shrinking the sizes of quantum dots without significant enhancement of their non-radiative decay rates. We show that such quantum dots are not influenced significantly by Coulomb blockade or photoionization, while those without a shell can undergo a large amount of photo-induced fluorescence enhancement via such blockade when they are in touch with the metal oxide.
Ultrafast spin tunneling and injection in coupled nanostructures of InGaAs quantum dots and quantum well
Yang, Xiao-Jie Kiba, Takayuki; Yamamura, Takafumi; Takayama, Junichi; Subagyo, Agus; Sueoka, Kazuhisa; Murayama, Akihiro
We investigate the electron-spin injection dynamics via tunneling from an In{sub 0.1}Ga{sub 0.9}As quantum well (QW) to In{sub 0.5}Ga{sub 0.5}As quantum dots (QDs) in coupled QW-QDs nanostructures. These coupled nanostructures demonstrate ultrafast (5 to 20 ps) spin injection into the QDs. The degree of spin polarization up to 45% is obtained in the QDs after the injection, essentially depending on the injection time. The spin injection and conservation are enhanced with thinner barriers due to the stronger electronic coupling between the QW and QDs.
Enhanced photorefractive performance in CdSe quantum-dot-dispersed poly(styrene-co-acrylonitrile) polymers
Li Xiangping; Embden, Joel van; Chon, James W. M.; Gu Min; Evans, Richard A.
This paper reports on the enhanced photorefractive behavior of a CdSe quantum-dot-dispersed less expensive polymer of poly(styrene-co-acrylonitrile). The capability of CdSe quantum dots used as photosensitizers and the associated photorefractive performance are characterized through a photocurrent experiment and a two-beam coupling experiment, respectively. An enhanced two-beam coupling gain coefficient of 12.2 cm{sup -1} at 46 V/mum was observed owning to the reduced potential barrier. The photorefractive performance per CdSe quantum dot is three orders of magnitude higher than that in the sample sensitized by trinitrofluorenone in poly(styrene-co-acrylonitrile), and almost ten times higher than that in the CdSe quantum-dot-sensitized poly(N-vinylcarbazole) polymers.
Radiative lifetimes of zincblende CdSe/CdS quantum dots
Gong, Ke; Martin, James E.; Shea-Rohwer, Lauren E.; Lu, Ping; Kelley, David F.
Recent synthetic advances have made available very monodisperse zincblende CdSe/CdS quantum dots having near-unity photoluminescence quantum yields. Because of the absence of nonradiative decay pathways, accurate values of the radiative lifetimes can be obtained from time-resolved PL measurements. Radiative lifetimes can also be obtained from the Einstein relations, using the static absorption spectra and the relative thermal populations in the angular momentum sublevels. We found that one of the inputs into these calculations is the shell thickness, and it is useful to be able to determine shell thickness from spectroscopic measurements. We use an empirically corrected effective mass model to produce a "map" of exciton wavelength as a function of core size and shell thickness. These calculations use an elastic continuum model and the known lattice and elastic constants to include the effect of lattice strain on the band gap energy. The map is in agreement with the known CdSe sizing curve and with the shell thicknesses of zincblende core/shell particles obtained from TEM images. Furthermore, if selenium–sulfur diffusion is included and lattice strain is omitted from the calculation then the resulting map is appropriate for wurtzite CdSe/CdS quantum dots synthesized at high temperatures, and this map is very similar to one previously reported (J. Am. Chem. Soc. 2009, 131, 14299). Radiative lifetimes determined from time-resolved measurements are compared to values obtained from the Einstein relations, and found to be in excellent agreement. For a specific core size (2.64 nm diameter, in the present case), radiative lifetimes are found to decrease with increasing shell thickness. Thus, this is similar to the size dependence of one-component CdSe quantum dots and in contrast to the size dependence in type-II quantum dots.
Radiative lifetimes of zincblende CdSe/CdS quantum dots
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Gong, Ke; Martin, James E.; Shea-Rohwer, Lauren E.; Lu, Ping; Kelley, David F.
Recent synthetic advances have made available very monodisperse zincblende CdSe/CdS quantum dots having near-unity photoluminescence quantum yields. Because of the absence of nonradiative decay pathways, accurate values of the radiative lifetimes can be obtained from time-resolved PL measurements. Radiative lifetimes can also be obtained from the Einstein relations, using the static absorption spectra and the relative thermal populations in the angular momentum sublevels. We found that one of the inputs into these calculations is the shell thickness, and it is useful to be able to determine shell thickness from spectroscopic measurements. We use an empirically corrected effective mass model tomore » produce a "map" of exciton wavelength as a function of core size and shell thickness. These calculations use an elastic continuum model and the known lattice and elastic constants to include the effect of lattice strain on the band gap energy. The map is in agreement with the known CdSe sizing curve and with the shell thicknesses of zincblende core/shell particles obtained from TEM images. Furthermore, if selenium–sulfur diffusion is included and lattice strain is omitted from the calculation then the resulting map is appropriate for wurtzite CdSe/CdS quantum dots synthesized at high temperatures, and this map is very similar to one previously reported (J. Am. Chem. Soc. 2009, 131, 14299). Radiative lifetimes determined from time-resolved measurements are compared to values obtained from the Einstein relations, and found to be in excellent agreement. For a specific core size (2.64 nm diameter, in the present case), radiative lifetimes are found to decrease with increasing shell thickness. Thus, this is similar to the size dependence of one-component CdSe quantum dots and in contrast to the size dependence in type-II quantum dots.« less
Spectral Barcoding of Quantum Dots: Deciphering Structural Motifs from the Excitonic Spectra
Mlinar, V.; Zunger, A.
Self-assembled semiconductor quantum dots (QDs) show in high-resolution single-dot spectra a multitude of sharp lines, resembling a barcode, due to various neutral and charged exciton complexes. Here we propose the 'spectral barcoding' method that deciphers structural motifs of dots by using such barcode as input to an artificial-intelligence learning system. Thus, we invert the common practice of deducing spectra from structure by deducing structure from spectra. This approach (i) lays the foundation for building a much needed structure-spectra understanding for large nanostructures and (ii) can guide future design of desired optical features of QDs by controlling during growth only those structural motifs that decide given optical features.
Tunnel magnetoresistance and linear conductance of double quantum dots strongly coupled to ferromagnetic leads
Weymann, Ireneusz
We analyze the spin-dependent linear-response transport properties of double quantum dots strongly coupled to external ferromagnetic leads. By using the numerical renormalization group method, we determine the dependence of the linear conductance and tunnel magnetoresistance on the degree of spin polarization of the leads and the position of the double dot levels. We focus on the transport regime where the system exhibits the SU(4) Kondo effect. It is shown that the presence of ferromagnets generally leads the suppression of the linear conductance due to the presence of an exchange field. Moreover, the exchange field gives rise to a transition from the SU(4) to the orbital SU(2) Kondo effect. We also analyze the dependence of the tunnel magnetoresistance on the double dot levels' positions and show that it exhibits a very nontrivial behavior.
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Carrier transfer from InAs quantum dots to ErAs metal nanoparticles
Haughn, C. R.; Chen, E. Y.; Zide, J. M. O.; Doty, M. F.; Steenbergen, E. H.; Bissell, L. J.; Eyink, K. G.
Erbium arsenide (ErAs) is a semi-metallic material that self-assembles into nanoparticles when grown in GaAs via molecular beam epitaxy. We use steady-state and time-resolved photoluminescence to examine the mechanism of carrier transfer between indium arsenide (InAs) quantum dots and ErAs nanoparticles in a GaAs host. We probe the electronic structure of the ErAs metal nanoparticles (MNPs) and the optoelectronic properties of the nanocomposite and show that the carrier transfer rates are independent of pump intensity. This result suggests that the ErAs MNPs have a continuous density of states and effectively act as traps. The absence of a temperature dependence tells us that carrier transfer from the InAs quantum dots to ErAs MNPs is not phonon assisted. We show that the measured photoluminescence decay rates are consistent with a carrier tunneling model.
Low-temperature transport in ac-driven quantum dots in the Kondo regime
Lopez, Rosa; Aguado, Ramon; Platero, Gloria; Tejedor, Carlos
We present a fully nonequilibrium calculation of the low-temperature transport properties of a quantum dot in the Kondo regime when an ac potential is applied to the gate. We solve a time-dependent Anderson model with finite on-site Coulomb interaction. The interaction self-energy is calculated up to second order in perturbation theory in the on-site interaction, in the context of the Keldysh nonequilibrium technique, and the effect of the ac voltage is taken into account exactly for all ranges of ac frequencies and ac intensities. The obtained linear conductance and time-averaged density of states of the quantum dot evolve in a nontrivial way as a function of the ac frequency and ac intensity of the harmonic modulation.
Ultrafast dynamics of type-II GaSb/GaAs quantum dots
Komolibus, K.; Piwonski, T.; Gradkowski, K.; Reyner, C. J.; Liang, B.; Huffaker, D. L.; Huyet, G.; Houlihan, J.
In this paper, room temperature two-colour pump-probe spectroscopy is employed to study ultrafast carrier dynamics in type-II GaSb/GaAs quantum dots. Our results demonstrate a strong dependency of carrier capture/escape processes on applied reverse bias voltage, probing wavelength and number of injected carriers. The extracted timescales as a function of both forward and reverse bias may provide important information for the design of efficient solar cells and quantum dot memories based on this material. The first few picoseconds of the dynamics reveal a complex behaviour with an interesting feature, which does not appear in devices based on type-I materials, and hence is linked to the unique carrier capture/escape processes possible in type-II structures.
Intermediate band solar cell simulation use InAs quantum dot in GaAs
Hendra P, I. B. Rahayu, F.; Sahdan, M. F.; Darma, Y.
Intermediate band solar cell (IBSC) has become a new approach in increasing solar cell efficiency significantly. One way to create intermediate band is by proposing quantum dots (QD) technology. One of the important aspects in utilizing IBSC is the absorption of light. In this work we simulated the influence of QD arrangement in order to increase absorption coefficient and solar cell efficiency. We also simulated the influence of QD size to capture a wider light spectrum. We present a simple calculation method with low computing power demand. Results show that the increasing in quantum dot size can increase in capturing wider spectrum of light. Arrangement InAs QD in bulk material GaAs can capture wider spectrum of light and increase the absorption coefficient. The arrangement InAs QD 2 nm in GaAs bulk can increase solar cell efficiency up to 49.68%.
Second harmonic generation from direct band gap quantum dots pumped by femtosecond laser pulses
Liu, Liwei Wang, Yue; Hu, Siyi; Ren, Yu; Huang, Chen
We report on nonlinear optical experiments performed on Cu{sub 2}S quantum dots (QDs) pumped by femtosecond laser pulses. We conduct a theoretical simulation and experiments to determine their second harmonic generation characteristics. Furthermore, we demonstrate that the QDs have a second harmonic generation conversion efficiency of up to 76%. Our studies suggest that these Cu{sub 2}S QDs can be used for solar cells, bioimaging, biosensing, and electric detection.
(In,Ga)As/GaP electrical injection quantum dot laser
Heidemann, M. Höfling, S.; Kamp, M.
The paper reports on the realization of multilayer (In,Ga)As/GaP quantum dot (QD) lasers grown by gas source molecular beam epitaxy. The QDs have been embedded in (Al,Ga)P/GaP waveguide structures. Laser operation at 710 nm is obtained for broad area laser devices with a threshold current density of 4.4 kA/cm{sup 2} at a heat-sink temperature of 80 K.
Tuning photoluminescence of reduced graphene oxide quantum dots from blue to purple
Liu, Fuchi; Tang, Tao; Feng, Qian; Li, Ming; Liu, Yuan; Tang, Nujiang Zhong, Wei; Du, Youwei
Reduced graphene oxide quantum dots (rGOQDs) were synthesized by annealing GOQDs in H{sub 2} atmosphere. The photoluminescence (PL) properties of GOQDs and the rGOQDs samples were investigated. The results showed that compared to GOQDs, a blue to purple tunable PL of rGOQDs can be obtained by regulating the annealing temperature. The increase fraction of the newly formed isolated sp{sup 2} clusters may be responsible for the observed tunable PL.
Solution-Processed Solar Cells using Colloidal Quantum Dots | MIT-Harvard
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Center for Excitonics Solution-Processed Solar Cells using Colloidal Quantum Dots September 27, 2012 at 3pm/36-428 Ted Sargent Department of Electrical and Computer Engineering - Canada Research Chair in Nanotechnology, University of Toronto, Canada sargent001_000 Abstract: Solution-processed photovoltaics offer a cost-effective path to harvesting the abundant resource that is solar energy. The organic and polymer semiconductors at the heart of these devices generally absorb visible light;
Group-V intermixing in InAs/InP quantum dots
Chia, C.K.; Chua, S.J.; Tripathy, S.; Dong, J.R.
Postgrowth intermixing in InAs/InP quantum dot (QD) structures have been investigated by rapid thermal annealing and laser irradiation techniques. In both cases, room-temperature photoluminescence (PL) measured from the QD structures after intermixing shows a substantial blueshift accompanied by an improvement in PL intensity and a reduction in linewidth. In the case of impurity free vacancy disordering, an energy shift of up to 350 meV has been achieved. The maximum differential energy shift for samples capped with SiO{sub 2} and SiN{sub x} dielectrics was found to be 90 meV. On the other hand, laser-induced intermixing allows differential energy shifts of more than 250 meV in this material system. Micro-Raman measurement shows the appearance of InAs-type and InP-type optical phonon peaks from laser-annealed InAs/InP QDs due to the exchange of As and P at the QD interfaces.
Integrated semiconductor quantum dot scintillation detector: Ultimate limit for speed and light yield
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Oktyabrsky, Serge; Yakimov, Michael; Tokranov, Vadim; Murat, Pavel
Here, a picosecond-range timing of charged particles and photons is a long-standing challenge for many high-energy physics, biophysics, medical and security applications. We present a design, technological pathway and challenges, and some properties important for realization of an ultrafast high-efficient room-temperature semiconductor scintillator based on self-assembled InAs quantum dots (QD) embedded in a GaAs matrix. Low QD density (<; 1015 cm-3), fast (~5 ps) electron capture, luminescence peak redshifted by 0.2-0.3 eV from GaAs absorption edge with fast decay time (0.5-1 ns) along with the efficient energy transfer in the GaAs matrix (4.2 eV/pair) allows for fabrication of a semiconductormore » scintillator with the unsurpassed performance parameters. The major technological challenge is fabrication of a large volume (> 1 cm3 ) of epitaxial QD medium. This requires multiple film separation and bonding, likely using separate epitaxial films as waveguides for improved light coupling. Compared to traditional inorganic scintillators, the semiconductor-QD based scintillators could have about 5x higher light yield and 20x faster decay time, opening a way to gamma detectors with the energy resolution better than 1% and sustaining counting rates MHz. Picosecond-scale timing requires segmented low-capacitance photodiodes integrated with the scintillator. For photons, the proposed detector inherently provides the depth-of-interaction information.« less
Layered insulator hexagonal boron nitride for surface passivation in quantum dot solar cell
Shanmugam, Mariyappan; Jain, Nikhil; Jacobs-Gedrim, Robin; Yu, Bin; Xu, Yang
Single crystalline, two dimensional (2D) layered insulator hexagonal boron nitride (h-BN), is demonstrated as an emerging material candidate for surface passivation on mesoporous TiO{sub 2}. Cadmium selenide (CdSe) quantum dot based bulk heterojunction (BHJ) solar cell employed h-BN passivated TiO{sub 2} as an electron acceptor exhibits photoconversion efficiency ?46% more than BHJ employed unpassivated TiO{sub 2}. Dominant interfacial recombination pathways such as electron capture by TiO{sub 2} surface states and recombination with hole at valence band of CdSe are efficiently controlled by h-BN enabled surface passivation, leading to improved photovoltaic performance. Highly crystalline, confirmed by transmission electron microscopy, dangling bond-free 2D layered h-BN with self-terminated atomic planes, achieved by chemical exfoliation, enables efficient passivation on TiO{sub 2}, allowing electronic transport at TiO{sub 2}/h-BN/CdSe interface with much lower recombination rate compared to an unpassivated TiO{sub 2}/CdSe interface.
Effect of graphene on photoluminescence properties of graphene/GeSi quantum dot hybrid structures
Chen, Y. L.; Ma, Y. J.; Wang, W. Q.; Ding, K.; Wu, Q.; Fan, Y. L.; Yang, X. J.; Zhong, Z. Y.; Jiang, Z. M., E-mail: firstname.lastname@example.com [State Key Laboratory of Surface Physics, Key Laboratory of Micro and Nano Photonic Structures (Ministry of Education) and Department of Physics, Fudan University, Shanghai 200433 (China); Chen, D. D.; Xu, F. [SHU-SolarE R and D Lab, Department of Physics, College of Science, Shanghai University, Shanghai 200444 (China)
Graphene has been discovered to have two effects on the photoluminescence (PL) properties of graphene/GeSi quantum dot (QD) hybrid structures, which were formed by covering monolayer graphene sheet on the multilayer ordered GeSi QDs sample surfaces. At the excitation of 488?nm laser line, the hybrid structure had a reduced PL intensity, while at the excitation of 325?nm, it had an enhanced PL intensity. The attenuation in PL intensity can be attributed to the transferring of electrons from the conducting band of GeSi QDs to the graphene sheet. The electron transfer mechanism was confirmed by the time resolved PL measurements. For the PL enhancement, a mechanism called surface-plasmon-polariton (SPP) enhanced absorption mechanism is proposed, in which the excitation of SPP in the graphene is suggested. Due to the resonant excitation of SPP by incident light, the absorption of incident light is much enhanced at the surface region, thus leading to more exciton generation and a PL enhancement in the region. The results may be helpful to provide us a way to improve optical properties of low dimensional surface structures.
Identification of luminescent surface defect in SiC quantum dots
Dai, Dejian; Guo, Xiaoxiao; Fan, Jiyang
The surface defect that results in the usually observed blue luminescence in the SiC quantum dots (QDs) remains unclear. We experimentally identify that the surface defect C=O (in COO) is responsible for this constant blue luminescence. The HO���C=O [n{sub (OH)} ? ?*{sub (CO)}] interaction between the hydroxyl and carbonyl groups changes the energy levels of C=O and makes the light absorption/emission arise at around 326/438?nm. Another surface defect (Si�Si) is identified and its light absorption contributes to both C=O-related luminescence and quantum-confinement luminescence of the SiC QDs.
An intentionally positioned (In,Ga)As quantum dot in a micron sized light emitting diode
Mehta, M.; Michaelis de Vasconcellos, S.; Zrenner, A.; Meier, C. [Department of Physics and Center for Optoelectronics and Photonics Paderborn (CeOPP), University of Paderborn, Warburger Street 100, 33098 Paderborn (Germany); Reuter, D.; Wieck, A. D. [Applied Solid State Physics, Ruhr-University of Bochum, Universitaetsstr. 150, 44780 Bochum (Germany)
We have integrated individual (In,Ga)As quantum dots (QDs) using site-controlled molecular beam epitaxial growth into the intrinsic region of a p-i-n junction diode. This is achieved using an in situ combination of focused ion beam prepatterning, annealing, and overgrowth, resulting in arrays of individually electrically addressable (In,Ga)As QDs with full control on the lateral position. Using microelectroluminescence spectroscopy we demonstrate that these QDs have the same optical quality as optically pumped Stranski-Krastanov QDs with random nucleation located in proximity to a doped interface. The results suggest that this technique is scalable and highly interesting for different applications in quantum devices.
Ab Initio Simulation of Charge Transfer at the Semiconductor Quantum Dot/TiO 2 Interface in Quantum Dot-Sensitized Solar Cells
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Xin, Xukai; Li, Bo; Jung, Jaehan; Yoon, Young Jun; Biswas, Rana; Lin, Zhiqun
Quantum dot-sensitized solar cells (QDSSCs) have emerged as a promising solar architecture for next-generation solar cells. The QDSSCs exhibit a remarkably fast electron transfer from the quantum dot (QD) donor to the TiO2 acceptor with size quantization properties of QDs that allows for the modulation of band energies to control photoresponse and photoconversion efficiency of solar cells. In order to understand the mechanisms that underpin this rapid charge transfer, the electronic properties of CdSe and PbSe QDs with different sizes on the TiO2 substrate are simulated using a rigorous ab initio density functional method. Our method capitalizes on localized orbitalmore » basis set, which is computationally less intensive. Quite intriguingly, a remarkable set of electron bridging states between QDs and TiO2 occurring via the strong bonding between the conduction bands of QDs and TiO2 is revealed. Such bridging states account for the fast adiabatic charge transfer from the QD donor to the TiO2 acceptor, and may be a general feature for strongly coupled donor/acceptor systems. All the QDs/TiO2 systems exhibit type II band alignments, with conduction band offsets that increase with the decrease in QD size. This facilitates the charge transfer from QDs donors to TiO2 acceptors and explains the dependence of the increased charge transfer rate with the decreased QD size.« less
Enhancement of photoluminescence in ZnS/ZnO quantum dots interfacial heterostructures
Rajalakshmi, M.; Sohila, S.; Ramesh, R.; Bhalerao, G.M.
Highlights: ? ZnS/ZnO quantum dots (QDs) were synthesized by controlled oxidation of ZnS nanoparticles. ? Interfacial heterostructure formation of ZnS/ZnO QDs is seen in HRTEM. ? Enormous enhancement of UV emission (?10 times) in ZnS/ZnO QDs heterostructure is observed. ? Phonon confinement effect is seen in the Raman spectrum. -- Abstract: ZnS/ZnO quantum dots (QDs) were synthesized by controlled oxidation of ZnS nanoparticles. HRTEM image showed small nanocrystals of size 4 nm and the magnified image of single quantum dot shows interfacial heterostructure formation. The optical absorption spectrum shows a blue shift of 0.19 and 0.23 eV for ZnO and ZnS QDs, respectively. This is due to the confinement of charge carries within the nanostructures. Enormous enhancement in UV emission (10 times) is reported which is attributed to interfacial heterostructure formation. Raman spectrum shows phonons of wurtzite ZnS and ZnO. Phonon confinement effect is seen in the Raman spectrum wherein LO phonon peaks of ZnS and ZnO are shifted towards lower wavenumber side and are broadened.
Visualization of Current and Mapping of Elements in Quantum Dot Solar Cells
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Niezgoda, J. Scott; Ng, Amy; Poplawsky, Jonathan D.; McBride, James R.; Pennycook, Stephen J.; Rosenthal, Sandra J.
The delicate influence of properties such as high surface state density and organic-inorganic boundaries on the individual quantum dot electronic structure complicates pursuits toward forming quantitative models of quantum dot thin films ab initio. Our report describes the application of electron beam-induced current (EBIC) microscopy to depleted-heterojunction colloidal quantum dot photovoltaics (DH-CQD PVs), a technique which affords one a map of current production within the active layer of a PV device. The effects of QD sample size polydispersity as well as layer thickness in CQD active layers as they pertain to current production within these PVs are imaged and explained.more » The results from these experiments compare well with previous estimations, and confirm the ability of EBIC to function as a valuable empirical tool for the design and betterment of DH-CQD PVs. Lastly, extensive and unexpected PbS QD penetration into the mesoporous TiO2 layer is observed through imaging of device cross sections by energy-dispersive X-ray spectroscopy combined with scanning transmission electron microscopy. Finally, the effects of this finding are discussed and corroborated with the EBIC studies on similar devices.« less
Carrier multiplication detected through transient photocurrent in device-grade films of lead selenide quantum dots
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Gao, Jianbo; Fidler, Andrew F.; Klimov, Victor I.
In carrier multiplication, the absorption of a single photon results in two or more electron–hole pairs. Quantum dots are promising materials for implementing carrier multiplication principles in real-life technologies. So far, however, most of research in this area has focused on optical studies of solution samples with yet to be proven relevance to practical devices. We report ultra-fast electro-optical studies of device-grade films of electronically coupled quantum dots that allow us to observe multiplication directly in the photocurrent. Our studies help rationalize previous results from both optical spectroscopy and steady-state photocurrent measurements and also provide new insights into effects ofmore » electric field and ligand treatments on multiexciton yields. Importantly, we demonstrate that using appropriate chemical treatments of the films, extra charges produced by carrier multiplication can be extracted from the quantum dots before they are lost to Auger recombination and hence can contribute to photocurrent of practical devices.« less
Investigation of size dependent structural and optical properties of thin films of CdSe quantum dots
Sharma, Madhulika; Department of Metallurgical Engineering and Materials Science, Indian Institute of Technology, Bombay, Powai, Mumbai 400076 ; Sharma, A.B.; Mishra, N.; Pandey, R.K.
Research highlights: {yields} CdSe q-dots have been synthesized using simple chemical synthesis route. {yields} Thin film of CdSe quantum dots exhibited self-organized growth. {yields} Size dependent blue shift observed in the absorption edge of CdSe nanocrystallites. {yields} PL emission band corresponds to band edge luminescence and defect luminescence. {yields} Organized growth led to enhancement in luminescence yield of smaller size Q-dots. -- Abstract: Cadmium selenide (CdSe) quantum dots were grown on indium tin oxide substrate using wet chemical technique for possible application as light emitting devices. The structural, morphological and luminescence properties of the as deposited thin films of CdSe Q-dot have been investigated, using X-ray diffraction, transmission electron microscopy, atomic force microscopy and optical and luminescence spectroscopy. The quantum dots have been shown to deposit in an organized array on ITO/glass substrate. The as grown Q-dots exhibited size dependent blue shift in the absorption edge. The effect of quantum confinement also manifested as a blue shift of photoluminescence emission. It is shown that the nanocrystalline CdSe exhibits intense photoluminescence as compared to the large grained polycrystalline CdSe films.
Effect of Bi isovalent dopants on the formation of homogeneous coherently strained InAs quantum dots in GaAs matrices
Peleshchak, R. M.; Guba, S. K.; Kuzyk, O. V.; Kurilo, I. V.; Dankiv, O. O.
The distribution of hydrostatic strains in Bi{sup 3+}-doped InAs quantum dots embedded in a GaAs matrix are calculated in the context of the deformation-potential model. The dependences of strains in the material of spherical InAs quantum dots with substitutional (Bi {yields} As) and interstitial (Bi) impurities on the quantum-dot size are derived. The qualitative correlation of the model with the experiment is discussed. The data on the effect of doping on the morphology of self-assembled InAs:Bi quantum dots in a GaAs matrix are obtained.
Improvement in carrier transport properties by mild thermal annealing...
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quantum dot solar cells Citation Details In-Document Search Title: Improvement in carrier transport properties by mild thermal annealing of PbS quantum dot solar cells Authors: ...
Emission spectra of a laser based on an In(Ga)As/GaAs quantum-dot superlattice
Sobolev, M. M. Buyalo, M. S.; Nevedomskiy, V. N.; Zadiranov, Yu. M.; Zolotareva, R. V.; Vasil'ev, A. P.; Ustinov, V. M.; Portnoi, E. L.
The spectral characteristics of a laser with an active region based on a ten-layer system of In(Ga)As/GaAs vertically correlated quantum dots with 4.5-nm GaAs spacer layers between InAs quantum dots are studied under the conditions of spontaneous and stimulated emission, depending on the current and the duration of pump pulses. Data obtained by transmission electron microscopy and electroluminescence and absorption polarization anisotropy measurements make it possible to demonstrate that the investigated system of tunnel-coupled InAs quantum dots separated by thin GaAs barriers represents a quantum-dot superlattice. With an increase in the laser pump current, the electroluminescence intensity increases linearly and the spectral position of the electroluminescence maximum shifts to higher energies, which is caused by the dependence of the miniband density-of-states distribution on the pump current. Upon exceeding the threshold current, multimode lasing via the miniband ground state is observed. One of the lasing modes can be attributed to the zero-phonon line, and the other is determined by the longitudinal-optical phonon replica of quantum-dot emission. The results obtained give evidence that, under conditions of the laser pumping of an In(Ga)As/GaAs quantum-dot superlattice, strong coupling between the discrete electron states in the miniband and optical phonons takes place. This leads to the formation of quantum-dot polarons, resulting from the resonant mixing of electronic states whose energy separation is comparable to the optical-phonon energy.
Near-Infrared Localized Surface Plasmon Resonances Arising from Free Carriers in Doped Quantum Dots
Jain, Prashant K.; Luther, Joey; Ewers, Trevor; Alivisatos, A. Paul
Quantum confinement of electronic wavefunctions in semiconductor quantum dots (QDs) yields discrete atom-like and tunable electronic levels, thereby allowing the engineering of excitation and emission spectra. Metal nanoparticles, on the other hand, display strong resonant interactions with light from localized surface plasmon resonance (LSPR) oscillations of free carriers, resulting in enhanced and geometrically tunable absorption and scattering resonances. The complementary attributes of these nanostructures lends strong interest toward integration into hybrid nanostructures to explore enhanced properties or the emergence of unique attributes arising from their interaction. However, the physicochemical interface between the two components can be limiting for energy transfer and synergistic coupling within such a hybrid nanostructure. Therefore, it is advantageous to realize both attributes, i.e., LSPRs and quantum confinement within the same nanostructure. Here, we describe well-defined LSPRs arising from p-type carriers in vacancy-doped semiconductor quantum dots. This opens up possibilities for light harvesting, non-linear optics, optical sensing and manipulation of solid-state processes in single nanocrystals.
Carrier dynamics in inhomogeneously broadened InAs/AlGaInAs/InP quantum-dot semiconductor optical amplifiers
Karni, O. Mikhelashvili, V.; Eisenstein, G.; Kuchar, K. J.; Capua, A.; Sęk, G.; Misiewicz, J.; Ivanov, V.; Reithmaier, J. P.
We report on a characterization of fundamental gain dynamics in recently developed InAs/InP quantum-dot semiconductor optical amplifiers. Multi-wavelength pump-probe measurements were used to determine gain recovery rates, following a powerful optical pump pulse, at various wavelengths for different bias levels and pump excitation powers. The recovery was dominated by coupling between the electronic states in the quantum-dots and the high energy carrier reservoir via capture and escape mechanisms. These processes determine also the wavelength dependencies of gain saturation depth and the asymptotic gain recovery level. Unlike quantum-dash amplifiers, these quantum-dots exhibit no instantaneous gain response, confirming their quasi zero-dimensional nature.
A theoretical analysis of the optical absorption properties in one-dimensional InAs/GaAs quantum dot superlattices
Kotani, Teruhisa; Birner, Stefan; Lugli, Paolo; Hamaguchi, Chihiro
We present theoretical investigations of miniband structures and optical properties of InAs/GaAs one-dimensional quantum dot superlattices (1D-QDSLs). The calculation is based on the multi-band k�p theory, including the conduction and valence band mixing effects, the strain effect, and the piezoelectric effect; all three effects have periodic boundary conditions. We find that both the electronic and optical properties of the 1D-QDSLs show unique states which are different from those of well known single quantum dots (QDs) or quantum wires. We predict that the optical absorption spectra of the 1D-QDSLs strongly depend on the inter-dot spacing because of the inter-dot carrier coupling and changing strain states, which strongly influence the conduction and valence band potentials. The inter-miniband transitions form the absorption bands. Those absorption bands can be tuned from almost continuous (closely stacked QD case) to spike-like shape (almost isolated QD case) by changing the inter-dot spacing. The polarization of the lowest absorption peak for the 1D-QDSLs changes from being parallel to the stacking direction to being perpendicular to the stacking direction as the inter-dot spacing increases. In the case of closely stacked QDs, in-plane anisotropy, especially [110] and [11{sup �}0] directions also depend on the inter-dot spacing. Our findings and predictions will provide an additional degree of freedom for the design of QD-based optoelectronic devices.
Interdot Coulomb correlation effects and spin-orbit coupling in two carbon nanotube quantum dots
Wang, Zhen-Hua; Kuang, Xiao-Yu Zhong, Ming-Min; Shao, Peng; Li, Hui
Transport properties of the two-level Kondo effect involving spin, orbital, and pseudospin degrees of freedom are examined in a parallel carbon nanotube double quantum dot with a sufficient interdot Coulomb interaction and small interdot tunneling. The interdot Coulomb correlation effects are taken into account, and it plays an important role in forming bonding and antibonding states. Attached to ferromagnetic leads, the Kondo effect is observed at the interdot Coulomb blockade region with degeneracy of spin, orbital, and pseudospin degrees of freedom. A crossover from a two-level Kondo state involving the fivefold degeneracy of the double quantum dots to an SU(4) spin-orbit Kondo state and to an SU(2) spin-Kondo effect is demonstrated. At finite magnetic field, the splitting of the spin, orbital, and pseudospin Kondo resonance can be restored. For finite intradot Coulomb interaction U, there is a competition between the single-dot Kondo effect and the antiferromagnetic exchange coupling J{sub AFM}, resulting in the suppression of the Kondo resonance. Moreover, both the J{sub AFM} and the Zeeman interactions compete, leading to need a much higher value of the magnetic field to compensate for the Kondo splitting.
III-nitride quantum dots for ultra-efficient solid-state lighting: III-nitride quantum dots for ultra-efficient solid-state lighting
DOE Public Access Gateway for Energy & Science Beta (PAGES Beta)
Wierer, Jonathan J.; Tansu, Nelson; Fischer, Arthur J.; Tsao, Jeffrey Y.
III-nitride light-emitting diodes (LEDs) and laser diodes (LDs) are ultimately limited in performance due to parasitic Auger recombination. For LEDs, the consequences are poor efficiencies at high current densities; for LDs, the consequences are high thresholds and limited efficiencies. Here, we present arguments for III-nitride quantum dots (QDs) as active regions for both LEDs and LDs, to circumvent Auger recombination and achieve efficiencies at higher current densities that are not possible with quantum wells. QD-based LDs achieve gain and thresholds at lower carrier densities before Auger recombination becomes appreciable. QD-based LEDs achieve higher efficiencies at higher currents because of highermore » spontaneous emission rates and reduced Auger recombination. The technical challenge is to control the size distribution and volume of the QDs to realize these benefits. If constructed properly, III-nitride light-emitting devices with QD active regions have the potential to outperform quantum well light-emitting devices, and enable an era of ultra-efficient solidstate lighting.« less
On-chip electrically controlled routing of photons from a single quantum dot
Bentham, C.; Coles, R. J.; Royall, B.; O'Hara, J.; Prtljaga, N.; Fox, A. M.; Skolnick, M. S.; Wilson, L. R.; Itskevich, I. E.; Clarke, E.
Electrical control of on-chip routing of photons emitted by a single InAs/GaAs self-assembled quantum dot (SAQD) is demonstrated in a photonic crystal cavity-waveguide system. The SAQD is located inside an H1 cavity, which is coupled to two photonic crystal waveguides. The SAQD emission wavelength is electrically tunable by the quantum-confined Stark effect. When the SAQD emission is brought into resonance with one of two H1 cavity modes, it is preferentially routed to the waveguide to which that mode is selectively coupled. This proof of concept provides the basis for scalable, low-power, high-speed operation of single-photon routers for use in integrated quantum photonic circuits.
Metal Halide Surface Treatment of Quantum Dots - Energy Innovation...
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The method developed produces solar cells that perform well even at film thicknesses approaching a micron, indicating improved carrier transportation in the QD films. The best QD ...