Modeling the meteorological and chemical effects of secondary organic aerosols during an EUCAARI campaign

摘要

A volatility basis set (VBS) approach for the simulation of secondary organic aerosol (SOA) formation is incorporated in the online coupled atmospheric model system COSMO-ART and applied over Europe during the EUCAARI May 2008 campaign. Organic aerosol performance is improved when compared to the default SOA module of COSMO-ART (SORGAM) against high temporal resolution aerosol mass spectrometer ground measurements. The impact of SOA on the overall radiative budget was investigated. The mean direct surface radiative cooling averaged over Europe is ?1.2 W m?2, representing approximately 20% of the total effect of aerosols on the radiative budget. However, responses are not spatially correlated with the radiative forcing, due to the nonlinear interactions among changes in particle chemical composition, water content, size distribution and cloud cover. These interactions initiated~by the effect of SOA on radiation are found to result even in a positive forcing in specific areas. Further model experiments showed that the availability of nitrogen oxides slightly affects SOA production, but that the aging rate constant used in the VBS approximation and boundary concentrations assumed in the model should be carefully selected. The aging of SOA is found to reduce hourly nitrate levels by up to 30%, while the condensation of inorganic species upon pre-existing, SOA-rich particles results in a monthly average increase of 5% in sulfate and ammonium formation in the accumulation mode.