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Organic aerosol (OA) simulations using the volatility basis-set approachwere made for East Asia and its outflow region. Model simulations wereevaluated through comparisons with OA measured by aerosol mass spectrometersin and around Tokyo (at Komaba and Kisai in summer 2003 and 2004) and overthe outflow region in East Asia (at Fukue and Hedo in spring 2009). Thesimulations with aging processes of organic vaporsreproduced the mass concentrations, temporal variations, and formationefficiencies of observed OA at all of the sites reasonably well. As OA mass was severelyunderestimated in the simulations without the aging processes, theoxidations of organic vapors are essential for reasonable OA simulationsover East Asia. By considering the aging processes, simulated OAconcentrations increased from 0.24 to 1.28 μg m<sup>−3</sup> in theboundary layer over the whole of East Asia. OA formed from the interactionof anthropogenic and biogenic sources was also enhanced by the agingprocesses. The fraction of controllable OA was estimated to be 87% oftotal OA over the whole of East Asia, which indicated that most of the OA inour simulations were formed anthropogenically (from controllable combustionsources). A large portion of biogenic secondary OA (78% of biogenicsecondary OA) was formed through the influence of anthropogenic sources.These fractions were higher than the fraction of anthropogenic emissions. Animportant reason for these higher controllable fractions was higher oxidantconcentrations and the resulting faster oxidation rates of OA precursors byconsidering anthropogenic sources. Both the amounts (from 0.18 to 1.12 μg m<sup>−3</sup>) and the fraction (from 75 to 87%) ofcontrollable OA were increased by aging processes of organic vapors overEast Asia

atmospheric chemistry and physics

Volatility basis-set approach simulation of organic aerosol formation in East Asia: implications for anthropogenic–biogenic interaction and controllable amounts