Interpreting the Ultraviolet Aerosol Index Observed with the OMI Satellite Instrument to Understand Absorption by Organic Aerosols: Implications for Atmospheric Oxidation and Direct Radiative Effects

• Published in: Atmospheric chemistry and physics Vol. 16; no. 4; pp. 2507 - 2523
• Main Authors: Hammer, Melanie S., Martin, Randall V., Donkelaar, Aaron van, Buchard, Virginie, Torres, Omar, Ridley, David A., Spurr, Robert J. D.
• Format: Journal Article
• Language: English
• Published: Goddard Space Flight Center Copernicus Publications 01.03.2016; Copernicus GmbH
• Subjects: Absorption; Aerosol absorption; Aerosol effects; Aerosol optical properties; Aerosols; Atmospheric particulates; Bias; Biodiesel fuels; Biomass; Biomass burning; Burning; Carbon; Carbon aerosols; Chemical properties; Chemical transport; Chloroform; Computer simulation; Dust storms; Environment Pollution; Environmental aspects; Estimates; Hydroxyl radicals; Monitoring instruments; Observations; Optical properties; Oxidation; Oxidation-reduction reactions; Ozone; Ozone monitoring; Photochemistry; Photolysis; Pollution monitoring; Radiation absorption; Radiative forcing; Radiative transfer; Regions; Satellite instruments; Satellite observation; Satellites; Simulation; Sky; Solar radiation; Surface chemistry; Three dimensional models; Ultraviolet absorption; Ultraviolet radiation; Aerosols; Atmospheric Chemistry; Air Pollution
• ISSN: 1680-7324; 1680-7316; 1680-7324
• DOI: 10.5194/acp-16-2507-2016

Satellite observations of the ultraviolet aerosol index (UVAI) are sensitive to absorption of solar radiation by aerosols; this absorption affects photolysis frequencies and radiative forcing. We develop a global simulation of the UVAI using the 3-D chemical transport model GEOSChem coupled with the Vector Linearized Discrete Ordinate Radiative Transfer model (VLIDORT). The simulation is applied to interpret UVAI observations from the Ozone Monitoring Instrument (OMI) for the year 2007. Simulated and observed values are highly consistent in regions where mineral dust dominates the UVAI, but a large negative bias (-0.32 to -0.97) exists between simulated and observed values in biomass burning regions. We determine effective optical properties for absorbing organic aerosol, known as brown carbon (BrC), and implement them into GEOS-Chem to better represent observed UVAI values over biomass burning regions. The inclusion of absorbing BrC decreases the mean bias between simulated and OMI UVAI values from -0.57 to -0.09 over West Africa in January, from -0.32 to +0.0002 over South Asia in April, from -0.97 to -0.22 over southern Africa in July, and from -0.50 to +0.33 over South America in September. The spectral dependence of absorption after including BrC in the model is broadly consistent with reported observations for biomass burning aerosol, with absorbing Angstrom exponent (AAE) values ranging from 2.9 in the ultraviolet (UV) to 1.3 across the UV-Near IR spectrum. We assess the effect of the additional UV absorption by BrC on atmospheric photochemistry by examining tropospheric hydroxyl radical (OH) concentrations in GEOS-Chem. The inclusion of BrC decreases OH by up to 30% over South America in September, up to 20% over southern Africa in July, and up to 15% over other biomass burning regions. Global annual mean OH concentrations in GEOS-Chem decrease due to the presence of absorbing BrC, increasing the methyl chloroform lifetime from 5.62 to 5.68 years, thus reducing the bias against observed values. We calculate the direct radiative effect (DRE) of BrC using GEOS-Chem coupled with the radiative transfer model RRTMG (GC-RT). Treating organic aerosol as containing more strongly absorbing BrC changes the global annual mean all-sky top of atmosphere (TOA) DRE by +0.03Wm(exp -2) and all-sky surface DRE by -0.08Wm(exp -2). Regional changes of up to +0.3Wm(exp -2) at TOA and down to -1.5Wm(exp -2) at the surface are found over major biomass burning regions.