Academic Publications

Global chemistry-transport models (CTMs) typically use simplified parameterizations or relaxation to climatology to estimate the chemical behavior of the stratosphere only in the context of its impact on tropospheric chemistry. This limits investigation of stratospheric chemistry and interactions between tropospheric and stratospheric chemistry-transport processes. We incorporate stratospheric chemical and physical processes into the model GEOS-Chem in the form of a unified chemistry extension (UCX). The stratospheric chemistry framework from NASA’s Global Modeling Initiative (GMI) is updated in accordance with JPL 10-06 and combined with GEOS-Chem’s existing widely applied and validated tropospheric chemistry to form a single, unified gas-phase chemistry scheme. Aerosol calculations are extended to include heterogeneous halogen chemistry and the formation, sedimentation and evaporation of polar stratospheric clouds (PSCs) as well as background liquid binary sulfate (LBS) aerosols. The Fast-JX v7.0a photolysis scheme replaces a hybrid of Fast-J and Fast-JX v6.2, allowing photolytic destruction at frequencies relevant to the stratosphere and of species not previously modeled. Finally, new boundary conditions are implemented to cover both surface emissions of new species and mesospheric behavior. Results for four simulation years (2004-2007) are compared to those from the original, tropospheric model and to in situ and satellite-based measurements. We use these comparisons to show that the extended model is capable of modeling stratospheric chemistry efficiently without compromising the accuracy of the model at lower altitudes, perturbing mean OH below 250 hPa by less than 5% while successfully capturing stratospheric behavior not previously captured in GEOS-Chem such as formation and collapse of the Antarctic ozone hole. These extensions (with supporting validation and intercomparison) enable an existing and extensively validated tropospheric CTM to be used to investigate a broader set of atmospheric chemistry problems and leverages GEOS-Chem’s existing tropospheric treatment.