A cloud chemistry module for the 3-D cloud-resolving mesoscale model Meso-NH with application to idealized cases

A complete chemical module has been developed for use in the Meso-NH three-dimensional cloud resolving mesoscale model. This module includes gaseous and aqueous phase chemical reactions that are analysed by a pre-processor generating the Fortran90 code automatically. The kinetic solver is based on a Rosenbrock algorithm, which is robust and accurate for integrating stiff systems and especially multiphase chemistry. The exchange of chemical species between the gas phase and cloud droplets and raindrops is computed kinetically by mass transfers considering non-equilibrium between the gas and the condensed phases. Microphysical transfers of chemical species are considered for the various cloud microphysics schemes available, which are based on one-moment or two-moment schemes. The pH of the droplets and of the raindrops is diagnosed separately as the root of a high order polynomial equation. The chemical concentrations in the ice phase are modelled in a single phase encompassing the two categories of precipitating ice particles (snow and graupel) of the microphysical scheme. The only process transferring chemical species in ice is retention during freezing or riming of liquid hydrometeors. Three idealized simulations are reported, which highlight the sensitivity of scavenging efficiency to the choice of the microphysical scheme and the retention coefficient in the ice phase. A two-dimensional warm, shallow convection case is used to compare the impact of the microphysical schemes on the temporal evolution and rates of acid precipitation. Acid wet deposition rates are shown to be overestimated when a one-moment microphysics scheme is used compared to a two-moment scheme. The difference is induced by a better prediction of raindrop radius and raindrop number concentration in the latter scheme. A two-dimensional mixed-phase squall line and a three-dimensional mixed-phase supercell were simulated to test the sensitivity of cloud vertical transport to the retention efficiency of gases in the ice phase. The 2-D and 3-D simulations illustrate that the retention in ice of a moderately soluble gas such as formaldehyde substantially decreases its concentration in the upper troposphere. In these simulations, retention of highly soluble species in the ice phase significantly increased the wet deposition rates.