An advanced scheme for wet scavenging and liquid-phase chemistry in a regional online-coupled chemistry transport model

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...

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Main Authors: C. Knote, D. Brunner
Format: Article
Language:English
Published: Copernicus Publications 2013-02-01
Series:Atmospheric Chemistry and Physics
Online Access:http://www.atmos-chem-phys.net/13/1177/2013/acp-13-1177-2013.pdf
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spelling doaj-8b9911625a8447269873c909f9fa3b0c2020-11-24T23:13:15ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242013-02-011331177119210.5194/acp-13-1177-2013An advanced scheme for wet scavenging and liquid-phase chemistry in a regional online-coupled chemistry transport modelC. KnoteD. BrunnerClouds 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 SO<sub>2</sub> trace gas concentrations by 0.3 ppbv (−30%) on average, while leaving O<sub>3</sub> and NO<sub>x</sub> unchanged. PM<sub>10</sub> aerosol mass was increased by 10% on average. While total PM<sub>2.5</sub> changes only little, chemical composition is improved notably. Overestimations of nitrate aerosols are reduced by typically 0.5–1 μg m<sup>−3</sup> (up to −2 μg m<sup>−3</sup> in the Po Valley) while sulfate mass is increased by 1–1.5 μg m<sup>−3</sup> on average (up to 2.5 μg m<sup>−3</sup> 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.http://www.atmos-chem-phys.net/13/1177/2013/acp-13-1177-2013.pdf
collection DOAJ
language English
format Article
sources DOAJ
author C. Knote
D. Brunner
spellingShingle C. Knote
D. Brunner
An advanced scheme for wet scavenging and liquid-phase chemistry in a regional online-coupled chemistry transport model
Atmospheric Chemistry and Physics
author_facet C. Knote
D. Brunner
author_sort C. Knote
title An advanced scheme for wet scavenging and liquid-phase chemistry in a regional online-coupled chemistry transport model
title_short An advanced scheme for wet scavenging and liquid-phase chemistry in a regional online-coupled chemistry transport model
title_full An advanced scheme for wet scavenging and liquid-phase chemistry in a regional online-coupled chemistry transport model
title_fullStr An advanced scheme for wet scavenging and liquid-phase chemistry in a regional online-coupled chemistry transport model
title_full_unstemmed An advanced scheme for wet scavenging and liquid-phase chemistry in a regional online-coupled chemistry transport model
title_sort advanced scheme for wet scavenging and liquid-phase chemistry in a regional online-coupled chemistry transport model
publisher Copernicus Publications
series Atmospheric Chemistry and Physics
issn 1680-7316
1680-7324
publishDate 2013-02-01
description 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 SO<sub>2</sub> trace gas concentrations by 0.3 ppbv (−30%) on average, while leaving O<sub>3</sub> and NO<sub>x</sub> unchanged. PM<sub>10</sub> aerosol mass was increased by 10% on average. While total PM<sub>2.5</sub> changes only little, chemical composition is improved notably. Overestimations of nitrate aerosols are reduced by typically 0.5–1 μg m<sup>−3</sup> (up to −2 μg m<sup>−3</sup> in the Po Valley) while sulfate mass is increased by 1–1.5 μg m<sup>−3</sup> on average (up to 2.5 μg m<sup>−3</sup> 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.
url http://www.atmos-chem-phys.net/13/1177/2013/acp-13-1177-2013.pdf
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