As part of the 2009 Operation Ice Bridge campaign, the NASA DC-8 aircraft was used to fill the data-time gap in laser observation of the changes in ice sheets, glaciers and sea ice between ICESat-I (Ice, Cloud, and land Elevation Satellite) and ICESat-II. Complementing the cryospheric instrument payload were four in situ atmospheric sampling instruments integrated onboard to measure trace gas concentrations of CO2, CO, N2O, CH 4, water vapor and various VOCs (Volatile Organic Compounds). This paper examines two plumes encountered at high altitude (12 km) during the campaign; one during a southbound transit flight (13°S) and the other at 86°S over Antarctica. The data presented are especially significant as the Southern Hemisphere is heavily under-sampled during the austral spring, with few if any high-resolution airborne observations of atmospheric gases made over Antarctica. Strong enhancements of CO, CH4, N2O, CHCl 3, OCS, C2H6, C2H2 and C3H8 were observed in the two intercepted air masses that exhibited variations in VOC composition suggesting different sources. The transport model FLEXPART showed that the 13°S plume contained predominately biomass burning emissions originating from Southeast Asia and South Africa, while both anthropogenic and biomass burning emissions were observed at 86° S with South America and South Africa as indicated source regions. The data presented here show evidence that boundary layer pollution is transported from lower latitudes toward the upper troposphere above the South Pole, which may not have been observed in the past. © 2012. American Geophysical Union. All Rights Reserved.