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Title: The effect of dry and wet deposition of condensable vapors on secondary organic aerosols concentrations over the continental US

The effect of dry and wet deposition of semi-volatile organic compounds (SVOC) in the gas-phase on the concentrations of secondary organic aerosol (SOA) is reassessed using recently derived water solubility information. The water solubility of SVOCs was implemented as a function of their volatility distribution within the regional chemistry transport model WRF-Chem, and simulations were carried out over the continental United States for the year 2010. Results show that including dry and wet removal of gas-phase SVOCs reduces annual average surface concentrations of anthropogenic and biogenic SOA by 48% and 63% respectively over the continental US Dry deposition of gas-phase SVOCs is found to be more effective than wet deposition in reducing SOA concentrations (−40% vs. −8% for anthropogenics, −52% vs. −11% for biogenics). Reductions for biogenic SOA are found to be higher due to the higher water solubility of biogenic SVOCs. The majority of the total mass of SVOC + SOA is actually deposited via the gas-phase (61% for anthropogenics, 76% for biogenics). A number of sensitivity studies shows that this is a robust feature of the modeling system. Other models that do not consider dry and wet removal of gas-phase SVOCs would hence overestimate SOA concentrations by roughlymore » 50%. Assumptions about the water solubility of SVOCs made in some current modeling systems (H* = 105 M atm−1; H* = H* (HNO3)) still lead to an overestimation of 25% / 10% compared to our best estimate. A saturation effect is observed for Henry's law constants above 108 M atm−1, suggesting an upper bound of reductions in surface level SOA concentrations by 60% through removal of gas-phase SVOCs. Considering reactivity of gas-phase SVOCs in the dry deposition scheme was found to be negligible. Further sensitivity studies where we reduce the volatility of organic matter show that consideration of gas-phase SVOC removal still reduces average SOA concentrations by 31% on average. We consider this a lower bound for the effect of gas-phase SVOC removal on SOA concentrations.« less
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Atmospheric Chemistry and Physics Discussions (Online)
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Journal Name: Atmospheric Chemistry and Physics Discussions (Online); Journal Volume: 14; Journal Issue: 9; Journal ID: ISSN 1680-7375
European Geosciences Union
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