Effect of Dust Morphology on Aerosol Optics in the GEOS-Chem Chemical Transport Model, on UV-Vis Trace Gas Retrievals, and on Surface Area Available for Reactive Uptake

Abstract

Many chemical transport models treat mineral dust as spherical. Solar backscatter retrievals of trace gases (e.g., OMI and TROPOMI) implicitly treat mineral dust as spherical. The impact of the morphology of mineral dust particles is studied to assess its implications for global chemical transport model (GEOS-Chem) simulations and solar backscatter trace gas retrievals at ultraviolet and visible (UV-Vis) wavelengths. We investigate how the morphology of mineral dust particles affects the simulated dust aerosol optical depth; surface area, reaction, and diffusion parameters for heterogeneous chemistry; phase function, and scattering weights for air mass factor (AMF) calculations used in solar backscatter retrievals. We use a mixture of various aspect ratios of spheroids to model the dust optical properties and a combination of shape and porosity to model the surface area, reaction, and diffusion parameters. We find that assuming spherical particles can introduce size-dependent and wavelength-dependent errors of up to 14% in simulated dust extinction efficiency with corresponding error in simulated dust optical depth typically within 5%. We find that use of spheroids rather than spheres increases forward scattered radiance and decreases backward scattering that in turn decrease the sensitivity of solar backscatter retrievals of NO₂ to aerosols by factors of 2.0–2.5. We develop and apply a theoretical framework based on porosity and surface fractal dimension with corresponding increase in the reactive uptake coefficient driven by increased surface area and species reactivity. Differences are large enough to warrant consideration of dust non-sphericity for chemical transport models and UV-Vis trace gas retrievals.