Evolution of gases and particles from a savanna fire in South Africa

[1] Airborne measurements of particles and gases from a 1000- ha savanna fire in South Africa are presented. These measurements represent the most extensive data set reported on the aging of biomass smoke. The measurements include total concentrations of particles ( CN), particle sizes, particulate organic carbon and black carbon, light- scattering coefficients, downwelling UV fluxes, and mixing ratios for 42 trace gases and 7 particulate species. The ratios of excess nitrate, ozone, and gaseous acetic acid to excess CO increased significantly as the smoke aged over similar to 40 - 45 min, indicating that these species were formed by photochemistry in the plume. For 17 other species, the excess mixing ratio normalized by the excess mixing ratio of CO decreased significantly with smoke age. The relative rates of decrease for a number of chemical species imply that the average OH concentration in the plume was similar to 1.7 x 10(7) molecules cm(-3). Excess CN, normalized by excess CO, decreased rapidly during the first similar to 5 min of aging, probably due to coagulation, and then increased, probably due to gas- to- particle conversion. The CO- normalized concentrations of particles < 1.5 mu m in diameter decreased, and particles > 1.5 mum diameter increased, with smoke age. The spectral depletion of solar radiation by the smoke is depicted. The downwelling UV flux near the vertical center of the plume was about two- thirds of that near the top of the plume.