1Laboratory for Air Pollution/Env. Technology, Empa Materials and Science, Duebendorf, Switzerland
2C2SM Center for Climate Systems Modeling, ETH, Zurich, Switzerland
*now at: Atmospheric Chemistry Division, National Center for Atmospheric Research, Boulder, CO, USA
Received: 12 Aug 2012 – Published in Atmos. Chem. Phys. Discuss.: 05 Oct 2012
Abstract. Clouds are reaction chambers for atmospheric trace gases and aerosols, and the associated precipitation is a major sink for atmospheric constituents. The regional chemistry-climate model COSMO-ART has been lacking a description of wet scavenging of gases and aqueous-phase chemistry. In this work we present a coupling of COSMO-ART with a wet scavenging and aqueous-phase chemistry scheme. The coupling is made consistent with the cloud microphysics scheme of the underlying meteorological model COSMO. While the choice of the aqueous-chemistry mechanism is flexible, the effects of a simple sulfur oxidation scheme are shown in the application of the coupled system in this work. We give details explaining the coupling and extensions made, then present results from idealized flow-over-hill experiments in a 2-D model setup and finally results from a full 3-D simulation. Comparison against measurement data shows that the scheme efficiently reduces SO2 trace gas concentrations by 0.3 ppbv (−30%) on average, while leaving O3 and NOx unchanged. PM10 aerosol mass was increased by 10% on average. While total PM2.5 changes only little, chemical composition is improved notably. Overestimations of nitrate aerosols are reduced by typically 0.5–1 μg m−3 (up to −2 μg m−3 in the Po Valley) while sulfate mass is increased by 1–1.5 μg m−3 on average (up to 2.5 μg m−3 in Eastern Europe). The effect of cloud processing of aerosols on its size distribution, i.e. a shift towards larger diameters, is observed. Compared against wet deposition measurements the system tends to underestimate the total wet deposited mass for the simulated case study.
Revised: 25 Jan 2013 – Accepted: 29 Jan 2013 – Published: 01 Feb 2013
Citation: Knote, C. and Brunner, D.: An advanced scheme for wet scavenging and liquid-phase chemistry in a regional online-coupled chemistry transport model, Atmos. Chem. Phys., 13, 1177-1192, doi:10.5194/acp-13-1177-2013, 2013.