Physical, chemical, and optical properties of regional hazes dominated by smoke in Brazil

Gas and particle measurements are described for optically thick regional hazes, dominated by aged smoke from biomass burning, in the cerrado and rain forested regions of Brazil. The hazes tended to be evenly mixed from the surface to the trade wind inversion at 3-4 km in altitude. The properties of aged gases and particles in the regional hazes were significantly different from those of young smoke (<4 min old). As the smoke aged, the total amount of carbon in non-methane hydrocarbon species (C<11) was depleted by about one third due to transformations into CO2, CO, and reactive molecules, and removed by dry deposition and/or by conversion to particulate matter. As the smoke particles aged, their sizes increased significantly due to coagulation and mass growth by secondary species (e.g., ammonium, organic acids and sulfate). During aging, condensation and gas-to-particle conversion of inorganic and organic vapors increased the aerosol mass by similar to 20-40%. One third to one half of this mass growth likely occurred in the first few hours of aging due to the condensation of large organic molecules. The remaining mass growth was probably associated with photochemical and cloud-processing mechanisms operating over several days. Changes in particle sizes and compositions during aging had a large impact on the optical properties of the aerosol. Over a 2 to 4 day period, the fine particle mass-scattering efficiency and single-scattering albedo increased by 1 m(2) g(-1), and similar to 0.06, respectively. Conversely, the Angstrom coefficient, backscatter ratio, and mass absorption efficiency decreased significantly with age.