ACP Atmospheric Chemistry and Physics ACP 1680-7324 Copernicus GmbH Göttingen, Germany 10.5194/acp-12-3289-2012 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 Department of Earth System Science, University of California, Irvine, California, USA now at: Jet Propulsion Laboratory, Pasadena, California, USA 05 04 2012 12 7 3289 3310 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.net/12/3289/2012/acp-12-3289-2012.html The full text article is available as a PDF file from http://www.atmos-chem-phys.net/12/3289/2012/acp-12-3289-2012.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 used fractional cloud cover assumptions and ice uptake determined by Henry's Law 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 NO<sub>x</sub> and O<sub>3</sub> mixing ratios are relatively insensitive to large differences in the removal rate. Ozone abundances are 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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