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Estimation of heterogeneous reaction rates for stratospheric trace gases with particular reference to the diffusional uptake of HCl and ClONO2 by polar stratospheric clouds
Authors:S Ghosh  D Lary  J A Pyle
Institution:(1) Department of Chemistry, Centre for Atmospheric Science, Lensfield Road, Cambridge, CB2 1EW, England
Abstract:The stratosphere holds a variety of particulates like polar stratospheric clouds (PSCs) and sulphate aerosols which catalyse chemical reactions. These reactions cause changes in the composition of the stratosphere, including the redistribution of active chlorine which might lead to ozone destruction. As a result during recent years a lot of effort has been directed towards the quantification of the uptake of trace gases like ClONO2, HCl, etc. into these particulates. However, it has been observed that many of the two and three dimensional models used in such studies are constrained by the lack of adequate rate constant data. This paper describes a theoretical approach to estimate the reaction rate constants for 23 gases on both types of polar stratospheric clouds (type I and II). It is found that for gases like N2O5, ClONO2 and HCl, diffusional uptake is important and contributes significantly to the heterogeneous reaction rate. A complete Lennard-Jones calculation is used to accurately compute the trace gas diffusion coefficients.
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