Toward a more physical representation of precipitation scavenging in global chemistry models: Cloud overlap and ice physics and their impact on tropospheric ozone

Abstract

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 3 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 3 observations. We find that the process of ice phase scavenging of HNO 3 is a critical component of the tropospheric O 3 budget, but that NO x and O 3 mixing ratios are relatively insensitive to large differences in the removal rate. Ozone abundances are much more sensitive to the lifetime of HNO 4, highlighting the need for better understanding of its interactions with ice and for additional observational constraints. © 2012 Author(s).