Sensitivity of Simulated PM2.5 Concentrations over Northeast Asia to Different Secondary Organic Aerosol Modules during the KORUS-AQ Campaign

Abstract

A numerical sensitivity study on secondary organic aerosol formation has been carried out by employing the WRF-Chem (Weather Research and Forecasting model coupled with Chemistry). Two secondary organic aerosol formation modules, the Modal Aerosol Dynamics model for Europe/Volatility Basis Set (MADE/VBS) and the Modal Aerosol Dynamics model for Europe/Secondary Organic Aerosol Model (MADE/SORGAM) were employed in the WRF-Chem model, and surface PM2.5 (particulate matter less than 2.5 mu m in size) mass concentration and the composition of its relevant chemical sources, i.e., SO42-, NO3-, NH4+, and organic carbon (OC) were simulated during the Korea-United States Air Quality (KORUS-AQ) campaign period (1 May to 12 June 2016). We classified the KORUS-AQ period into two cases, the stagnant period (16-21 May) which was dominated by local emission and the long-range transport period (25-31 May) which was affected by transport from the leeward direction, and focused on the differences in OC secondary aerosol formation between two modules over Northeast Asia. The simulated surface PM2.5 chemical components via the two modules showed the largest systematic biases in surface OC, with a mean bias of 4.5 mu g m(-3), and the second largest in SO42- abundance of 2.2 mu g m(-3) over Seoul. Compared with surface observations at two ground sites located near the western coastal Korean Peninsula, MADE/VBS exhibited the overpredictions in OC by 170-180%, whereas MADE/SORGAM showed underpredictions by 49-65%. OC and sulfate via MADE/VBS were simulated to be much higher than that simulated by MADE/SORGAM by a factor of 2.8-3.5 and 1.5-1.9, respectively. Model verification against KORUS-AQ aircraft measurements also showed large discrepancies in simulated non-surface OC between the two modules by a factor of five, with higher OC by MADE/VBS and lower IC by MADE/SORGAM, whereas much closer MADE/VBS simulations to the KORUS-AQ aircraft measurements were found. On the basis of the aircraft measurements, the aggregated bias (sum of four components) for PM2.5 mass concentrations from the MADE/VBS module indicated that the simulation was much closer to the measurements, nevertheless more elaborate analysis on the surface OC simulation performance would be needed to improve the ground results. Our findings show that significant inconsistencies are present in the secondary organic aerosol formation simulations, suggesting that PM2.5 forecasts should be considered with great caution, as well as in the context of policymaking in the Northeast Asia region.