Modeling study of strong acids formation and partitioning in a polluted cloud during wintertime

Abstract

A multiphase chemistry model coupled with a quasi‐spectral microphysical model has been applied to measurements from the European Cloud Ice Mountain Experiment campaign to quantify the formation of the strong acids nitrate and sulfate and to evaluate the role of microphysical processes in redistributing reactive species among the different phases (gas versus cloud and/or rain). Significant formation of nitrate and sulfate are found to be due to the reaction of pernitric acid with the sulfite ion. Moreover, pernitric acid, because of its equilibrium in the gas phase and its high solubility, is always available both in cloud water and in rainwater via mass transfer from the gas phase. The sulfite ion comes from the mass transfer from the gas phase of sulfur dioxide in cloud water. When rain formation begins, it is efficiently transferred to the rainwater by collision/coalescence processes. This leads to an enhancement in strong acid production when microphysics is activated in the model. Modeled results have been compared with experimental data in an effort to retrieve a behavior law related to the partitioning between the gas and aqueous phases of the cloud. In particular, when collision/coalescence processes are considered, an improvement in retrieving the partitioning of soluble species and especially nitrate is observed. A higher production in sulfate could help interpret the discrepancy of global model calculations with observed sulfate concentrations in Europe in wintertime.