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Aqueous multiphase chemistry in the atmosphere can lead to rapidtransformation of organic compounds, forming highly oxidized, low-volatilityorganic aerosol and, in some cases, light-absorbing (brown) carbon. Becauseliquid water is globally abundant, this chemistry could substantially impactclimate, air quality, and health. Gas-phase precursors released from biogenicand anthropogenic sources are oxidized and fragmented, forming water-solublegases that can undergo reactions in the aqueous phase (in clouds, fogs, andwet aerosols), leading to the formation of secondary organic aerosol(SOAAQ). Recent studies have highlighted the role of certainprecursors like glyoxal, methylglyoxal, glycolaldehyde, acetic acid, acetone,and epoxides in the formation of SOAAQ. The goal of this work is toidentify additional precursors and products that may be atmosphericallyimportant. In this study, ambient mixtures of water-soluble gases werescrubbed from the atmosphere into water at Brent, Alabama, during the 2013Southern Oxidant and Aerosol Study (SOAS). Hydroxyl (OH⚫) radicaloxidation experiments were conducted with the aqueous mixtures collected fromSOAS to better understand the formation of SOA through gas-phase followed byaqueous-phase chemistry. Total aqueous-phase organic carbon concentrationsfor these mixtures ranged from 92 to 179 µM-C, relevant for cloud andfog waters. Aqueous OH-reactive compounds were primarily observed as odd ionsin the positive ion mode by electrospray ionization mass spectrometry(ESI-MS). Ultra high-resolution Fourier-transform ion cyclotron resonancemass spectrometry (FT-ICR-MS) spectra and tandem MS (MS–MS) fragmentation ofthese ions were consistent with the presence of carbonyls and tetrols.Products were observed in the negative ion mode and included pyruvate andoxalate, which were confirmed by ion chromatography. Pyruvate and oxalatehave been found in the particle phase in many locations (as salts andcomplexes). Thus, formation of pyruvate/oxalate suggests the potential foraqueous processing of these ambient mixtures to form SOAAQ

Identifying precursors and aqueous organic aerosol formation pathways during the SOAS campaign