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

Abstract

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 HNO3 in the upper troposphere relative to a scheme with commonly made assumptions about cloud overlap and ice uptake, and provides better agreement with HNO3 observations. We find that the process of ice phase scavenging of HNO3 is a critical component of the tropospheric O3 budget, but that differences in the formulation of ice phase removal, while generating large relative differences in HNO3 abundance, have little impact on NOx and O3. The O3 budget is much more sensitive to the lifetime of HNO4, highlighting the need for better understanding of its interactions with ice and for additional observational constraints.