Aerosols serve as cloud condensation nuclei (CCN) and thus have a substantial effect on cloud properties and the initiation of precipitation. Large concentrations of human-made aerosols have been reported to both decrease and increase rainfall as a result of their radiative and CCN activities. At one extreme, pristine tropical clouds with low CCN concentrations rain out too quickly to mature into long-lived clouds. On the other hand, heavily polluted clouds evaporate much of their water before precipitation can occur, if they can form at all given the reduced surface heating resulting from the aerosol haze layer. We propose a conceptual model that explains this apparent dichotomy.

Biomass burning is widespread, especially in the tropics. It serves to clear land for shifting cultivation, to convert forests to agricultural and pastoral lands, and to remove dry vegetation in order to promote agricultural productivity and the growth of higher yield grasses. Furthermore, much agricultural waste and fuel wood is being combusted, particularly in developing countries. Biomass containing 2 to 5 petagrams of carbon is burned annually (1 petagram = 10¹⁵grams), producing large amounts of trace gases and aerosol particles that play important roles in atmospheric chemistry and climate. Emissions of carbon monoxide and methane by biomass burning affect the oxidation efficiency of the atmosphere by reacting with hydroxyl radicals, and emissions of nitric oxide and hydrocarbons lead to high ozone concentrations in the tropics during the dry season. Large quantities of smoke particles are produced as well, and these can serve as cloud condensation nuclei. These particles may thus substantially influence cloud microphysical and optical properties, an effect that could have repercussions for the radiation budget and the hydrological cycle in the tropics. Widespread burning may also disturb biogeochemical cycles, especially that of nitrogen. About 50 percent of the nitrogen in the biomass fuel can be released as molecular nitrogen. This pyrodenitrification process causes a sizable loss of fixed nitrogen in tropical ecosystems, in the range of 10 to 20 teragrams per year (1 teragram = 10¹²grams).

Although the definition and measurement techniques for atmospheric "black carbon" ("BC") or "elemental carbon'' ("EC") have long been subjects of scientific controversy, the recent discovery of light-absorbing carbon that is not black ("brown carbon, C_brown") makes it imperative to reassess and redefine the components that make up light-absorbing carbonaceous matter (LAC) in the atmosphere. Evidence for the atmospheric presence of C_brown comes from (1) spectral aerosol light absorption measurements near specific combustion sources, (2) observations of spectral properties of water extracts of continental aerosol, (3) laboratory studies indicating the formation of light-absorbing organic matter in the atmosphere, and (4) indirectly from the chemical analogy of aerosol species to colored natural humic substances. We show that brown carbon may severely bias measurements of "BC" and "EC" over vast parts of the troposphere, especially those strongly polluted by biomass burning, where the mass concentration of C_brown is high relative to that of soot carbon. Chemical measurements to determine "EC" are biased by the refractory nature of C_brown as well as by complex matrix interferences. Optical measurements of "BC" suffer from a number of problems: (1) many of the presently used instruments introduce a substantial bias into the determination of aerosol light absorption, (2) there is no unique conversion factor between light absorption and "EC" or "BC" concentration in ambient aerosols, and (3) the difference in spectral properties between the different types of LAC, as well as the chemical complexity of C_brown, lead to several conceptual as well as practical complications. We also suggest that due to the sharply increasing absorption of C_brown towards the UV, single-wavelength light absorption measurements may not be adequate for the assessment of absorption of solar radiation in the troposphere. We discuss the possible consequences of these effects for our understanding of tropospheric processes, including their influence on UV-irradiance, atmospheric photochemistry and radiative transfer in clouds.

The Global Fire Assimilation System (GFASv1.0) calculates biomass burning emissions by assimilating Fire Radiative Power (FRP) observations from the MODIS instruments onboard the Terra and Aqua satellites. It corrects for gaps in the observations, which are mostly due to cloud cover, and filters spurious FRP observations of volcanoes, gas flares and other industrial activity. The combustion rate is subsequently calculated with land cover-specific conversion factors. Emission factors for 40 gas-phase and aerosol trace species have been compiled from a literature survey. The corresponding daily emissions have been calculated on a global 0.5^° × 0.5^° grid from 2003 to the present. General consistency with the Global Fire Emission Database version 3.1 (GFED3.1) within its accuracy is achieved while maintaining the advantages of an FRP-based approach: GFASv1.0 makes use of the quantitative information on the combustion rate that is contained in the FRP observations, and it detects fires in real time at high spatial and temporal resolution. GFASv1.0 indicates omission errors in GFED3.1 due to undetected small fires. It also exhibits slightly longer fire seasons in South America and North Africa and a slightly shorter fire season in Southeast Asia. GFASv1.0 has already been used for atmospheric reactive gas simulations in an independent study, which found good agreement with atmospheric observations. We have performed simulations of the atmospheric aerosol distribution with and without the assimilation of MODIS aerosol optical depth (AOD). They indicate that the emissions of particulate matter need to be boosted by a factor of 2–4 to reproduce the global distribution of organic matter and black carbon. This discrepancy is also evident in the comparison of previously published top-down and bottom-up estimates. For the time being, a global enhancement of the particulate matter emissions by 3.4 is recommended. Validation with independent AOD and PM₁₀ observations recorded during the Russian fires in summer 2010 show that the global Monitoring Atmospheric Composition and Change (MACC) aerosol model with GFASv1.0 aerosol emissions captures the smoke plume evolution well when organic matter and black carbon are enhanced by the recommended factor. In conjunction with the assimilation of MODIS AOD, the use of GFASv1.0 with enhanced emission factors quantitatively improves the forecast of the aerosol load near the surface sufficiently to allow air quality warnings with a lead time of up to four days.