ACPD Atmospheric Chemistry and Physics Discussions ACPD 1680-7375 Copernicus GmbH Göttingen, Germany 10.5194/acpd-10-18919-2010 Global analysis of the relation between aerosols and short-lived trace gases Veefkind J. P. 1 Boersma K. F. 1 Wang J. 2 Kurosu T. 3 Krotkov N. 4 Levelt P. F. 1 5 Royal Netherlands Meteorological Institute, De Bilt, The Netherlands University of Nebraska-Lincoln, Lincoln, Nebraska, USA Harvard-Smithsonian Center for Astrophysics, Cambridge, Massachusetts, USA Goddard Earth Sciences and Technology Center, University of Maryland Baltimore County, Baltimore, Maryland, USA Eindhoven University of Technology, Eindhoven, The Netherlands 11 08 2010 10 8 18919 18951 This is an open-access article ditributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are credited. This article is available from http://www.atmos-chem-phys-discuss.net/10/18919/2010/acpd-10-18919-2010.html The full text article is available as a PDF file from http://www.atmos-chem-phys-discuss.net/10/18919/2010/acpd-10-18919-2010.pdf

The spatial and temporal correlations between concurrent satellite observations of aerosol optical thickness (AOT) from the Moderate Resolution Imaging Spectroradiometer (MODIS) and tropospheric columns of nitrogen dioxide, sulfur dioxide, and formaldehyde from the Ozone Monitoring Instrument (OMI) are used to infer information on the global composition of aerosol particles. When averaging the satellite data over large regions and longer time periods, we find significant correlation between MODIS AOT and OMI trace gas columns for various regions in the world. This suggests that enhanced aerosol and trace gas concentrations originate from common sources, such as fossil fuel combustion, biomass burning, and organic compounds released from the biosphere. This leads us to propose that satellite-inferred AOT to NO<sub>2</sub> ratios for regions with comparable photochemical regimes can be used as indicators for the relative (local) efficiency of combustion processes. Indeed, satellites observe low AOT to NO<sub>2</sub> ratios over the eastern United States and western Europe, and high AOT to NO<sub>2</sub> ratios over comparably industrialized regions in eastern Europe and China. Emission databases and OMI SO<sub>2</sub> observations over these regions suggest a much stronger sulfur contribution to aerosol formation than over the well-regulated areas of the eastern United States and western Europe. Furthermore, satellite observations show AOT to NO<sub>2</sub> ratios are a factor 100 higher over biomass burning regions than over industrialized areas, reflecting the unregulated burning practices with strong primary particle emissions in the tropics compared to the heavily controlled combustion processes in the industrialized Northern Hemisphere. Simulations with a global chemistry transport model (GEOS-Chem) capture most of these differences, providing some confidence in our understanding of aerosol sources, formation mechanisms, and sinks. Wintertime aerosol concentrations show strongest correlations with NO<sub>2</sub> throughout most of the Northern Hemisphere. During summertime, AOT is often (also) correlated with enhanced HCHO concentrations, reflecting the importance of secondary organic aerosol formation in that season. We also find significant correlations between AOT and HCHO over biomass burning regions, the tropics in general, and over industrialized regions in southeastern Asia. The distinct summertime maximum in AOT (0.4 at 550 nm) and HCHO over the southeastern United States strengthens existing hypotheses that local emissions of volatile organic compounds lead to the formation of secondary organic aerosols there. GEOS-Chem underestimates the AOT over the southeastern United States by a factor of 2, most likely due to too strong precipitation and too low SOA yield in the model.

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