Exploring the inorganic composition of the Asian Tropopause Aerosol Layer using medium-duration balloon flights

Abstract. Satellite observations have revealed an enhanced aerosol layer near the tropopause over Asia during the summer monsoon, called the Asian Tropopause Aerosol Layer (ATAL). In this work, aerosol particles in the ATAL were collected with a balloon-borne impactor near the tropopause region over India, using extended duration balloon flights, in summer 2017 and winter 2018. Their chemical composition was further investigated by quantitative analysis using offline ion chromatography. Nitrate (NO3−) and nitrite (NO2−) were found to be the dominant ions in the collected aerosols with values ranging between 87–343 ng/m3 STP during the summer campaign. In contrast, sulfate (SO42−) levels were found above the detection limit (> 10 ng/m3 STP) only in winter. In addition, we determined the origin of the air masses sampled during the flights through analysis of back trajectories along with convective influence. The results obtained therein were put into a context of large-scale transport and aerosol distribution with GEOS-Chem chemical transport model simulations. The first flight of summer 2017 which sampled air mass within the Asian monsoon anticyclone (AMA), influenced by convection over Western China, was associated with particle size radius (0.05–2 μm). In contrast, the second flight sampled air mass at the edge of the AMA associated with larger particle size radius (> 2 μm) with higher nitrite concentration. The sampled air masses in winter 2018 were likely affected by smoke from the Pacific Northwest fire event in Canada, which occurred 7 months prior to our campaign, leading to concentration enhancements of SO42− and Ca2+. Overall, our results suggest that nitrogen-containing particles represent a large fraction of aerosols populating the ATAL, in agreement with the results from aircraft measurements during the StratoClim campaign. Furthermore, GEOS-Chem model simulations suggest that lightning NOx emissions had a significant impact on the production of nitrate aerosols sampled during the summer 2017.