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Abstract 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. 

Abstract The Arctic is warming at almost four times the global rate. An estimated sixty percent of greenhouse‐gas‐induced Arctic warming has been offset by anthropogenic aerosols, but the contribution of aerosols to radiative forcing (RF) represents the largest uncertainty in estimating total RF, largely due to unknown preindustrial aerosol abundance. Here, sulfur isotope measurements in a Greenland ice core show that passive volcanic degassing contributes up to 66 ± 10% of preindustrial ice core sulfate in years without major eruptions. A state‐of‐the‐art model indicates passive volcanic sulfur emissions influencing the Arctic are underestimated by up to a factor of three, possibly because many volcanic inventories do not include hydrogen sulfide emissions. Higher preindustrial volcanic sulfur emissions reduce modeled anthropogenic Arctic aerosol cooling by up to a factor of two (+0.11 to +0.29 W m⁻²), suggesting that underestimating passive volcanic sulfur emissions has significant implications for anthropogenic‐induced Arctic climate change.