Seasonal distributions of fine aerosol sulfate in the North American Arctic basin during TOPSE

Abstract

We used the mist chamber/ion chromatography technique to quantify fine aerosol SO4= (<2.7 μm) in the Arctic during the Tropospheric Ozone Production about the Spring Equinox Experiment (TOPSE) with about 2.5 min time resolution. Our effective sample area ranged from 50° to 86°N and 53° to 100°W. The seasonal evolution of fine aerosol sulfate in the Arctic troposphere during TOPSE was consistent with the phenomenon of Arctic haze. Arctic haze has been attributed to pollution from sources in the Arctic and pollution transported meridionally along stable isentropes into the Arctic in geographically broad but vertically narrow bands. These layers became more prevalent at higher altitudes as the season progressed toward summer, and the relevant isentropes are not held so close to the surface. Mean fine particle SO4= mixing ratios during TOPSE in February below 1000 m were elevated (112 pptv) and highly variable (between 28 and 290 pptv) but were significantly lower at higher altitudes (about 40 pptv). As the season progressed, elevated mixing ratios and higher variability were observed at higher altitudes, up to 7 km. In May, mixing ratios at the lowest altitudes declined but still remained higher than in February at all altitudes. The high variability in our measurements likely reflects the vertical heterogeneity of the wintertime Arctic atmosphere as the airborne sampling platform passed in and out of these layers. It is presumed that mixing ratios and variability will continue to decline at all altitudes into the summer as wet deposition processes become important in removing aerosol SO4= from the troposphere.