A new chemistry option in WRF/Chem v. 3.4 for the simulation of direct and indirect aerosol effects using VBS: evaluation against IMPACT-EUCAARI data

Abstract

Abstract. A parameterization for secondary organic aerosol (SOA) production based on the volatility basis set (VBS) approach has been coupled with microphysics and radiative scheme in WRF/Chem model. The new chemistry option called "RACM/MADE/VBS" was evaluated on a cloud resolving scale against ground-based and aircraft measurements collected during the IMPACT-EUCAARI campaign, and complemented with satellite data from MODIS. The day-to-day variability and the diurnal cycle of ozone (O3) and nitrogen oxides (NOx) at the surface is captured by the model. Surface aerosol mass of sulphate (SO4), nitrate (NO3), ammonium (NH4), and organic matter (OM) is simulated with a correlation larger than 0.55. WRF/Chem captures the vertical profile of the aerosol mass in both the planetary boundary layer (PBL) and free troposphere (FT) as a function of the synoptic condition, but the model does not capture the full range of the measured concentrations. Predicted OM concentration is at the lower end of the observed mass. The bias may be attributable to the missing aqueous chemistry processes of organic compounds, the uncertainties in meteorological fields, the assumption on the deposition velocity of condensable organic vapours, and the uncertainties in the anthropogenic emissions of primary organic carbon. Aerosol particle number concentration (condensation nuclei, CN) is overestimated by a factor 1.4 and 1.7 within PBL and FT, respectively. Model bias is most likely attributable to the uncertainties of primary particle emissions (mostly in the PBL) and to the nucleation rate. The overestimation of simulated cloud condensation nuclei (CCN) is more contained with respect to that of CN. The CCN efficiency, which is a measure of the ability of aerosol particles to nucleate cloud droplets, is underestimated by a factor of 1.5 and 3.8 in the PBL and FT, respectively. The comparison with MODIS data shows that the model overestimates the aerosol optical thickness (AOT). The domain averages (for one day) are 0.38 ± 0.12 and 0.42 ± 0.10 for MODIS and WRF/Chem data, respectively. Cloud water path (CWP) is overestimated on average by a factor of 1.7, whereas modelled cloud optical thickness (COT) agrees with observations within 10%. In a sensitivity test where the SOA was not included, simulated CWP is reduced by 40%, and its distribution function shifts toward lower values with respect to the reference run with SOA. The sensitivity test exhibits also 10% more optically thin clouds (COT < 40) and an average COT roughly halved. Moreover, the run with SOA shows convective clouds with an enhanced content of liquid and frozen hydrometers, and stronger updrafts and downdrafts. Considering that the previous version of WRF/Chem coupled with a modal aerosol module predicted very low SOA content (SORGAM mechanism) the new proposed option may lead to a better characterization of aerosol–cloud feedbacks.