[1] Understanding the roles of human and natural sources in contributing to aerosol concentrations around the world is an important step toward developing efficient and effective mitigation measures for local and regional air quality degradation and climate change. In this study we test the hypothesis that changes in aerosol optical depth (AOD) over time are caused by the changing patterns of anthropogenic emissions of aerosols and aerosol precursors. We present estimated trends of contributions to AOD for eight world regions from 1980 to 2006, built upon a full run of the Goddard Chemistry Aerosol Radiation and Transport model for the year 2001, extended in time using trends in emissions of man-made and natural sources. Estimated AOD trends agree well (R > 0.5) with observed trends in surface solar radiation in Russia, the United States, south Asia, southern Africa, and East Asia (before 1992) but less well for Organization for Economic Co-operative Development (OECD) Europe (R < 0.5). The trends do not agree well for southeast Asia and for East Asia (after 1992) where large-scale inter-and intraannual variations in emissions from forest fires, volcanic eruptions, and dust storms confound our approach. Natural contributions to AOD, including forest and grassland fires, show no significant long-term trends (<1%/a), except for a small increasing trend in OECD Europe and a small decreasing trend in South America. Trends in man-made contributions to AOD follow the changing patterns of industrial and economic activity. We quantify the average contributions of key source types to regional AOD over the entire time period.

Organic aerosols (OAs) in the atmosphere affect Earth's energy budget by not only scattering but also absorbing solar radiation due to the presence of the so-called "brown carbon" (BrC) component. However, the absorptivities of OAs are not represented or are poorly represented in current climate and chemical transport models. In this study, we provide a method to constrain the BrC absorptivity at the emission inventory level using recent laboratory and field observations. We review available measurements of the light-absorbing primary OA (POA), and quantify the wavelength-dependent imaginary refractive indices (kOA, the fundamental optical parameter determining the particle's absorptivity) and their uncertainties for the bulk POA emitted from biomass/biofuel, lignite, propane, and oil combustion sources. In particular, we parametrize the kOA of biomass/biofuel combustion sources as a function of the black carbon (BC)-to-OA ratio, indicating that the absorptive properties of POA depend strongly on burning conditions. The derived fuel-type-based kOA profiles are incorporated into a global carbonaceous aerosol emission inventory, and the integrated kOA values of sectoral and total POA emissions are presented. Results of a simple radiative transfer model show that the POA absorptivity warms the atmosphere significantly and leads to ∼27% reduction in the amount of the net global average POA cooling compared to results from the nonabsorbing assumption.

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