Atmos. Chem. Phys. Discuss., 9, 24361-24410, 2009
www.atmos-chem-phys-discuss.net/9/24361/2009/
doi:10.5194/acpd-9-24361-2009
© Author(s) 2009. This work is distributed
under the Creative Commons Attribution 3.0 License.
Review Status
This discussion paper has been under review for the journal Atmospheric Chemistry and Physics (ACP). Please refer to the corresponding final paper in ACP.
Modelling the reversible uptake of chemical species in the gas phase by ice particles formed in a convective cloud
V. Marécal1, M. Pirre1, E. D. Rivière2, N. Pouvesle3, J. N. Crowley3, S. R. Freitas4, and K. M. Longo4
1Laboratoire de Physique et Chimie de l'Environnement et de l'Espace, CNRS-Université d'Orléans, Orléans, France
2Groupe de Spectrométrie Moléculaire et Atmosphérique, Université de Reims-CNRS, Reims, France
3Max-Planck-Institut für Chemie, Division of Atmospheric Chemistry, Mainz, Germany
4Center for Weather Forecasts and Climate Studies, INPE, Cachoeira Paulista, Brazil

Abstract. The present paper is a preliminary study preparing the introduction of reversible trace gas uptake by ice particles into a 3-D cloud resolving model. For this a 3-D simulation of a tropical deep convection cloud was run with the BRAMS cloud resolving model using a two-moment bulk microphysical parameterization. Trajectories encountering the convective clouds were computed from these simulation outputs along which the variations of the pristine ice, snow and aggregate mixing ratios and size distributions were extracted. The reversible uptake of 11 trace gases by ice was examined assuming applicability of Langmuir isotherms using recently evaluated (IUPAC) laboratory data. The results show that ice uptake is only significant for HNO3, HCl, CH3COOH and HCOOH. For H2O2, using new results for the partition coefficient results in significant partitioning to the ice phase for this trace gas also. It was also shown that the uptake is largely dependent on the temperature for some species. The adsorption saturation at the ice surface for large gas concentrations is generally not a limiting factor except for HNO3 and HCl for gas concentration greater than 1 ppbv. For HNO3, results were also obtained using a trapping theory, resulting in a similar order of magnitude of uptake, although the two approaches are based on different assumptions. The results were compared to those obtained using a BRAMS cloud simulation based on a single-moment microphysical scheme instead of the two moment scheme. We found similar results with a slightly more important uptake when using the single-moment scheme which is related to slightly higher ice mixing ratios in this simulation. The way to introduce these results in the 3-D cloud model is discussed.

Citation: Marécal, V., Pirre, M., Rivière, E. D., Pouvesle, N., Crowley, J. N., Freitas, S. R., and Longo, K. M.: Modelling the reversible uptake of chemical species in the gas phase by ice particles formed in a convective cloud, Atmos. Chem. Phys. Discuss., 9, 24361-24410, doi:10.5194/acpd-9-24361-2009, 2009.
 
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