Aerosol chemical composition and distribution during the Pacific Exploratory Mission (PEM) Tropics

Distributions of aerosol-associated soluble ions over much of the South Pac ific were determined by sampling from the NASA DC-8 as part of the Pacific Exploratory Mission (PEM) Tropics campaign. The mixing ratios of all ionic species were surprisingly low throughout the free troposphere (2-12 km), de spite the pervasive influence from biomass burning plumes advecting over th e South Pacific from the west during PEM-Tropics. At the same time, the spe cific activity of Be-7 frequently exceeded 1000 fCi m(-3) through much of t he depth of the troposphere. These distributions indicate that the plumes m ust have been efficiently scavenged by precipitation (removing the soluble ions), but that the scavenging must have occurred far upwind of the DC-8 sa mpling regions (otherwise Be-7 activities would also have been low). This i nference is supported by large enhancements of HNO3 and carboxylic acids in many of the plumes, as these soluble acidic gases would also be readily sc avenged in any precipitation events. Decreasing mixing ratios of NH4+ with altitude in all South Pacific regions sampled provide support for recent su ggestions that oceanic emissions of NH3 constitute a significant source far from continents. Our sampling below 2 km reaffirms the latitudinal pattern in the methylsulfonate/non-sea-salt sulfate (MSA/nss SO4=) molar ratio est ablished through surface-based and shipboard sampling, with values increasi ng from <0.05 in the tropics to nearly 0.6 at 70 degrees S. However, we als o found very high values of this ratio (0.2-0.5) at 10 km altitude above th e intertropical, convergence zone near 10 degrees N, It appears that wet co nvective pumping of dimethylsulfide from the tropical marine boundary layer is responsible for the high values of the MSA/nss SO4= ratio in the tropic al upper troposphere. This finding complicates use of this ratio to infer t he zonal origin of biogenic S transported long distances.