Emissions from savanna fires in southern Africa

Thesis (Ph. D.)--University of Washington, 2004Airborne measurements are presented of emissions from savanna fires in southern Africa during the dry season. Measurements were obtained aboard the University of Washington Convair-580 research aircraft during the SAFARI 2000 field project in August and September 2000. Savanna fires in southern Africa emit a wide range of gaseous and particulate species including carbon, sulfur, nitrogen, halogen, and oxygenated compounds. Emission factors, emission ratios, and regional emissions of fifty trace gas and particulate species were derived, including eight species not previously reported in the literature (dimethyl sulfide, methyl nitrate, five species of hydrocarbons, and particles with diameters from 0.1--3 mum diameter). The physical, chemical, and radiative properties of the plume from a large savanna fire in South Africa are characterized, including plume dimensions, secondary formation of ozone and organic acids, oxidation of hydrocarbons, coagulation of particles, and gas-to-particle conversion in aged smoke. Numerous fires, thermodynamically stable layers aloft, and large-scale anticylonic flow result in high concentrations of air pollution distributed throughout the lower troposphere over southern Africa during the dry season. Average regional concentrations of CO (261 +/- 81 ppbv), SO2 (2.5 +/- 1.6 ppbv), O3 (64 +/- 13 ppbv), black particulate carbon (2.3 +/- 1.9 mug m-3), organic particulate carbon (6.2 +/- 5.2 mug m-3), total particle mass (26.0 +/- 4.7 mug m-3) are comparable to those found in polluted urban environments. The GEOS-CHEM model of tropospheric chemistry is used to characterize the transport of biomass burning emissions from southern Africa to the neighboring Atlantic and Indian Oceans during the dry season (May--October) of 2000. A large quantity of biomass burning emissions from southern Africa is transported westward over the latitudes 0--20°S to the southern Atlantic Ocean (∼40 Tg CO from May--October), contributing to a pollution anomaly in the south Atlantic Ocean. However, most of this material is transported back eastward over higher latitudes to the south (21--60°S) eventually reaching the southern Indian Ocean. As a result, ∼60 Tg of CO from biomass burning in southern Africa is transported eastward to the Indian Ocean across the latitude band 0--60°S from May--October, enhancing background CO concentrations by ∼4--13 ppbv per month over the southern subtropical Indian Ocean during the dry season