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Abstract We have coupled the GEOS‐Chem tropospheric‐stratospheric chemistry mechanism and the Community Aerosol and Radiation Model for Atmospheres (CARMA), a sectional aerosol microphysics module, within the NASA Goddard Earth Observing System Chemistry‐Climate Model (GEOS CCM) in order to simulate the interactions between stratospheric chemistry and aerosol microphysics. We use observations of the 1991 Mount Pinatubo volcanic cloud to evaluate this new version of the GEOS CCM. The GEOS‐Chem chemistry module is used to simulate the oxidation of sulfur dioxide (SO2) more realistically than assuming hydroxyl radical (OH) fields are constant, as OH concentrations in the plume decrease dramatically in the weeks following the eruption. CARMA simulates sulfate aerosols with dynamic microphysical and optical properties. The CARMA‐calculated aerosol surface area is coupled to the chemistry module from GEOS‐Chem for the calculation of heterogeneous chemistry. We use a set of observational and theoretical constraints for Pinatubo to evaluate the performance of this new version of the GEOS CCM. These simulations are specifically compared with satellite and in‐situ observations and provide insights into the connections between the gas‐phase chemistry and the aerosol microphysics of the early plume and how they impact the climatic and chemical changes following a large volcanic eruption. A second, smaller eruption is also included in these simulations, the 15 August 1991, eruption of Cerro Hudson in Chile, which we find essential in explaining the aerosol optical depth in the Southern Hemisphere in 1991.

Abstract Stratospheric injections of sulfur dioxide from major volcanic eruptions perturb the Earth's global radiative balance and dominate variability in stratospheric sulfur loading. The atmospheric component of the GFDL Earth System Model (ESM4.1) uses a bulk aerosol scheme and previously prescribed the distribution of aerosol optical properties in the stratosphere. To quantify volcanic contributions to the stratospheric sulfur cycle and the resulting climate impact, we modified ESM4.1 to simulate stratospheric sulfate aerosols prognostically. Driven by explicit volcanic emissions of aerosol precursors and non‐volcanic sources, we conduct ESM4.1 simulations from 1989 to 2014, with a focus on the Mt. Pinatubo eruption. We evaluate our interactive representation of the stratospheric sulfur cycle against data from Moderate Resolution Imaging Spectroradiometer, Multi‐angle Imaging SpectroRadiometer, Advanced Very High Resolution Radiometer, High Resolution Infrared Radiation Sounder, and Stratospheric Aerosol and Gas Experiment II. To assess the key processes associated with volcanic aerosols, we performed a sensitivity analysis of sulfate burden from the Mt. Pinatubo eruption by varying injection heights, emission amount, and stratospheric sulfate's dry effective radius. We find that the simulated stratospheric sulfate mass burden and aerosol optical depth in the model are sensitive to these parameters, especially volcanic SO2 injection height, and the optimal combination of parameters depends on the metric we evaluate.