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We present a new volatility basis set (VBS) representation of aromatic secondary organic aerosol (SOA) for atmospheric chemistry models by fitting a statistical oxidation model with aerosol microphysics (SOM-TOMAS) to results from laboratory chamber experiments. The resulting SOM-VBS scheme also including previous work on SOA formation from semi- and intermediate volatile organic compounds (S/IVOCs) is implemented in the GEOS-Chem chemical transport model and applied to simulation of observations from the Korea-United States Air Quality Study (KORUS-AQ) field campaign over South Korea in May–June 2016. Our SOM-VBS scheme can simulate the KORUS-AQ organic aerosol (OA) observations from aircraft and surface sites better than the default schemes used in GEOS-Chem including for vertical profiles, diurnal cycle, and partitioning between hydrocarbon-like OA and oxidized OA. Our results confirm the important contributions of oxidized primary OA and aromatic SOA found in previous analyses of the KORUS-AQ data and further show a large contribution from S/IVOCs. Model source attribution of OA in surface air over South Korea indicates one third from domestic anthropogenic emissions, with a large contribution from toluene and xylenes, one third from external anthropogenic emissions, and one third from natural emissions. © 2023. American Geophysical Union. All Rights Reserved.

Geostationary satellite measurements of aerosol optical depth (AOD) over East Asia from the Geostationary Ocean Color Imager (GOCI) and Advanced Himawari Imager (AHI) instruments can augment surface monitoring of fine particulate matter (PM2.5) air quality, but this requires better understanding of the AOD–PM2.5 relationship. Here we use the GEOS-Chem chemical transport model to analyze the critical variables determining the AOD–PM2.5 relationship over East Asia by simulation of observations from satellite, aircraft, and ground-based datasets. This includes the detailed vertical aerosol profiling over South Korea from the KORUS-AQ aircraft campaign (May–June 2016) with concurrent ground-based PM2.5 composition, PM10, and AERONET AOD measurements. The KORUS-AQ data show that 550 nm AOD is mainly contributed by sulfate–nitrate–ammonium (SNA) and organic aerosols in the planetary boundary layer (PBL), despite large dust concentrations in the free troposphere, reflecting the optically effective size and high hygroscopicity of the PBL aerosols. We updated SNA and organic aerosol size distributions in GEOS-Chem to represent aerosol optical properties over East Asia by using in situ measurements of particle size distributions from KORUS-AQ. We find that SNA and organic aerosols over East Asia have larger size (number median radius of 0.11 µm with geometric standard deviation of 1.4) and 20 % larger mass extinction efficiency as compared to aerosols over North America (default setting in GEOS-Chem). Although GEOS-Chem is successful in reproducing the KORUS-AQ vertical profiles of aerosol mass, its ability to link AOD to PM2.5 is limited by under-accounting of coarse PM and by a large overestimate of nighttime PM2.5 nitrate. The GOCI–AHI AOD data over East Asia in different seasons show agreement with AERONET AODs and a spatial distribution consistent with surface PM2.5 network data. The AOD observations over North China show a summer maximum and winter minimum, opposite in