Size-resolved sea spray aerosol particles studied by vibrational sum frequency generation

TitleSize-resolved sea spray aerosol particles studied by vibrational sum frequency generation
Publication TypeJournal Article
Year of Publication2013
AuthorsEbben CJ, Ault AP, Ruppel MJ, Ryder OS, Bertram TH, Grassian VH, Prather KA, Geiger FM
JournalJournal of Physical Chemistry A
Volume117
Pagination6589-6601
Date Published2013/08
Type of ArticleArticle
ISBN Number1089-5639
Accession NumberWOS:000322807300018
Keywords2nd-harmonic generation; chain; chemistry; fused silica/aqueous interfaces; interfaces; liquid; multiphase; salt particles; simple ionic surfactants; spectroscopy; tropospheric chemistry; water
Abstract

We present vibrational sum frequency generation (SFG) spectra of the external surfaces and the internal interfaces of size-selected sea spray aerosol (SSA) particles generated at the wave flume of the Scripps Hydraulics Laboratory. Our findings support SSA particle models that invoke the presence of surfactants in the topmost particle layer and indicate that the alkyl chains of surfactant-rich SSA particles are likely to be disordered. Specifically, the SFG spectra suggest that across the range of sizes studied, surfactant-rich SSA particles contain CH oscillators that are subject to molecular orientation distributions that are broader than the narrow molecular distribution functions associated with well-ordered and well-aligned alkyl chains. This result is consistent with the interpretation that the permeability of organic layers at SSA particle surfaces to small reactive and nonreactive molecules may be substantial, allowing for much more exchange between reactive and nonreactive species in the gas or the condensed phase than previously thought. The SFG data also suggest that a one-component model is likely to be insufficient for describing the SFG responses of the SSA particles. Finally, the similarity of the SFG spectra obtained from the wave flume microlayer and 150 nm-sized SSA particles suggests that the SFG active CH oscillators in the topmost layer of the wave flume and the particle accumulation mode may be in similar chemical environments. Needs for additional research activities are discussed in the context of the results presented.

DOI10.1021/jp401957k
Short TitleJ. Phys. Chem. A
Integrated Research Themes: 
Student Publication: 
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