Interactions between tropospheric chemistry and aerosols in a unified general circulation model

Abstract

A unified tropospheric chemistry-aerosol model has been developed within the Goddard Institute for Space Studies general circulation model (GCM). The model includes a detailed simulation of tropospheric ozone-NO_x-hydrocarbon chemistry as well as aerosols and aerosol precursors. Predicted aerosol species include sulfate, nitrate, ammonium, black carbon, primary organic carbon, and secondary organic carbon. The partitioning of ammonia and nitrate between gas and aerosol phases is determined by on-line thermodynamic equilibrium, and the formation of secondary organic aerosols is based on equilibrium partitioning and experimentally determined parameters. Two-way coupling between aerosols and chemistry provides consistent chemical fields for aerosol dynamics and aerosol mass for heterogeneous processes and calculations of gas-phase photolysis rates. Although the current version of the unified model does not include a prognostic treatment of mineral dust, we include its effects on photolysis and heterogeneous processes by using three-dimensional off-line fields. We also simulate sulfate and nitrate aerosols that are associated with mineral dust based on currently available chemical understanding. Considering both mineral dust uptake of HNO₃ and wet scavenging of HNO₃ on ice leads to closer agreement between predicted gas-phase HNO₃ concentrations and measurements than in previous global chemical transport model simulations, especially in the middle to upper troposphere. As a result of the coupling between chemistry and aerosols, global burdens of both gas-phase and aerosol species are predicted to respond nonlinearly to changing emissions of NO_x, NH₃, and sulfur.