Abstract
This project examined the potential large-scale influence of marine aerosol cycling on atmospheric chemistry, physics and radiative transfer. Measurements indicate that the size-dependent generation of marine aerosols by wind waves at the ocean surface and the subsequent production and cycling of halogen-radicals are important but poorly constrained processes that influence climate regionally and globally. A reliable capacity to examine the role of marine aerosol in the global-scale atmospheric system requires that the important size-resolved chemical processes be treated explicitly. But the treatment of multiphase chemistry across the breadth of chemical scenarios encountered throughout the atmosphere is sensitive to the initial conditions and the precision of the solution method. This study examined this sensitivity, constrained it using high-resolution laboratory and field measurements, and deployed it in a coupled chemical-microphysical 3-D atmosphere model. First, laboratory measurements of fresh, unreacted marine aerosol were used to formulate a sea-state based marine aerosol source parameterization that captured the initial organic, inorganic, and physical conditions of the aerosol population. Second, a multiphase chemical mechanism, solved using the Max Planck Institute for Chemistry's MECCA (Module Efficiently Calculating the Chemistry of the Atmosphere) system, was benchmarked across a broad set of observed chemical and physical conditions in the marine atmosphere. Using these results, the mechanism was systematically reduced to maximize computational speed. Finally, the mechanism was coupled to the 3-mode modal aerosol version of the NCAR Community Atmosphere Model (CAM v3.6.33). Decadal-scale simulations with CAM v.3.6.33, were run both with and without reactive-halogen chemistry and with and without explicit treatment of particulate organic carbon in the marine aerosol source function. Simulated results were interpreted (1) to evaluate influences of marine aerosol production on the microphysical properties of aerosol populations and clouds over the ocean and the corresponding direct and indirect effects on radiative transfer; (2) atmospheric burdens of reactive halogen species and their impacts on O3, NOx, OH, DMS, and particulate non-sea-salt SO42-; and (3) the global production and influences of marine-derived particulate organic carbon. The model reproduced major characteristics of the marine aerosol system and demonstrated the potential sensitivity of global, decadal-scale climate metrics to multiphase marine-derived components of Earth's troposphere. Due to the combined computational burden of the coupled system, the currently available computational resources were the limiting factor preventing the adequate statistical analysis of the overall impact that multiphase chemistry might have on climate-scale radiative transfer and climate.
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