ACPD Atmospheric Chemistry and Physics Discussions ACPD 1680-7375 Copernicus GmbH Göttingen, Germany 10.5194/acpd-11-24413-2011 Toward a more physical representation of precipitation scavenging in global chemistry models: cloud overlap and ice physics and their impact on tropospheric ozone Neu J. L. 1 2 Prather M. J. 1 University of California, Department of Earth System Science, Irvine, California, USA now at: Jet Propulsion Laboratory, Pasadena, California, USA 31 08 2011 11 8 24413 24466 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys-discuss.net/11/24413/2011/acpd-11-24413-2011.html The full text article is available as a PDF file from http://www.atmos-chem-phys-discuss.net/11/24413/2011/acpd-11-24413-2011.pdf

Uptake and removal of soluble trace gases and aerosols by precipitation represents a major uncertainty in the processes that control the vertical distribution of atmospheric trace species. Model representations of precipitation scavenging vary greatly in their complexity, and most are divorced from the physics of precipitation formation and transformation. Here, we describe a new large-scale precipitation scavenging algorithm, developed for the UCI chemistry-transport model (UCI-CTM), that represents a step toward a more physical treatment of scavenging through improvements in the formulation of the removal in sub-gridscale cloudy and ambient environments and their overlap within the column as well as ice phase uptake of soluble species. The UCI algorithm doubles the lifetime of HNO<sub>3</sub> in the upper troposphere relative to a scheme with commonly made assumptions about cloud overlap and ice uptake, and provides better agreement with HNO<sub>3</sub> observations. We find that the process of ice phase scavenging of HNO<sub>3</sub> is a critical component of the tropospheric O<sub>3</sub> budget, but that differences in the formulation of ice phase removal, while generating large relative differences in HNO<sub>3</sub> abundance, have little impact on NO<sub>x</sub> and O<sub>3</sub>. The O<sub>3</sub> budget is much more sensitive to the lifetime of HNO<sub>4</sub>, highlighting the need for better understanding of its interactions with ice and for additional observational constraints.

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