In Situ Observation of Multiphase Oxidation-Driven Secondary Organic Aerosol Formation during Cloud Processing at a Mountain Site in Southern China

Secondary organic aerosols (SOAs) account for a large fraction of atmospheric fine particles, but the mechanisms of their formation and evolution processes remain unclear. In this study, a ground-based counterflow virtual impactor was used in combination with an online time-of-flight aerosol chemical speciation monitor to investigate the multiphase (gaseous and aqueous) oxidation processes and the SOA influencing factors during cloud events at a mountain site in southern China. Our results showed that the clouds promoted the formation of low-oxidized oxygenated organic aerosol (LO-OOA) and more-oxidized oxygenated organic aerosol (MO-OOA). At night, ozone (O3) and nitrate radicals (NO3•) oxidized volatile organic compounds (VOCs, mostly biogenic VOCs) to the precursors of LO-OOA and were absorbed in the cloud droplets to form LO-OOA, while the hydroxyl radical (•OH) was the main oxidant for LO-OOA during daytime. In the cloud droplets, LO-OOA was further oxidized by •OH to form MO-OOA. We propose that isoprene can be oxidized to form products in the gas phase and then absorbed by acidic cloud droplets to form 2-methylglyceric acid (2-MG), 2-MG-organosulfate, and 2-MG-organonitrate. This study improves our understanding of SOA formation, driven by multiphase oxidation during cloud events.