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Mobility-Classified Mass Spectrometry Reveals a Complete Picture of the Electrospray Outcome.

Electrospray ionization mass spectrometry supported by mobility classification (ESI-DMA-MS) is a strong tool for the comprehensive analysis of organic and inorganic clusters and small nanoparticles. In-depth understanding and optimization of the electrospray process is the key for unlocking new fields of application and for extension of the accessible range of data. We show that the combination of mobility-classified mass spectrometry (DMA-MS) with an electrospray operated in well-defined cone jet mode is capable to provide a full picture of the outcome of an electrospray process including the evaporation residues of the parent drops. Based on ESI-DMA-MS measurements of lysozyme we find that clusters up to almost 1MDa (around 60 lysozyme molecules per cluster) formed as evaporation residues of the parent drops can be detected. The escape probability of lysozyme molecules from the parent drops is polarity-dependent. A quantitative analysis of clusters is possible at analyte concentrations where the likeliness of finding more than a single molecule in generated drop is low. At higher concentrations one can, however, quantify the analyte concentration from the detected size of the drop evaporation residues. The approach works is widely applicable for organic and inorganic nanostructures. The results allow clear statements on the conditions under which mixtures of larger molecules, clusters and nanoparticles are accessible to quantitative analysis by mass spectrometry.