Aqueous processing of water-soluble organic compounds in the eastern United States during winter

Abstract

Aqueous multi-phase processes are significant contributors to organic aerosol (OA) mass in the atmosphere. This study characterizes the formation of water-soluble organic matter during the winter in the eastern United States through simultaneous measurements of water-soluble organic carbon in the gas and particle phases (WSOC_g and WSOC_p, respectively). The formation of secondary WSOC_p occurred primarily through two pathways: (1) absorptive partitioning of oxygenated organics to the bulk OA and (2) aqueous phase processes. WSOC_p formation through the former pathway was evident through the relationship between the fraction of total WSOC in the particle phase (F_p) and the total OA concentration. Conversely, evidence for nighttime aqueous WSOC_p formation was based upon the strong enhancement in F_p with increasing relative humidity, indicating the uptake of WSOC_g to aerosol liquid water (ALW). The F_p–RH relationship was only observed for temperatures between 0–10 °C, suggesting conditions for aqueous multi-phase processes were enhanced during these times. Temperature exhibited an inverse relationship with ALW and a proportional relationship with aerosol potassium. ALW and biomass burning precursors were both abundant in the 0–10 °C temperature range, facilitating aqueous WSOC_p formation. To assess the impact of particle drying on the WSOC_p concentrations, the particle measurements alternated between ambient and dried channels. No change was observed in the concentration of particles before and after drying, indicating that the WSOC_p formed through the uptake of WSOC_g into OA and ALW remained in the condensed phase upon particle drying at all temperature ranges. This work contributes to our understanding of sources, pathways, and factors affecting aqueous aerosol formation in the winter.