Regional characteristics of atmospheric sulfate formation in East Antarctica imprinted on 17O-excess signature

Sakiko Ishino,Shohei Hattori,Michel Legrand,Qianjie Chen,Becky Alexander,Jingyuan Shao,Jiayue Huang,Lyatt Jaegle,Bruno Jourdain,Susanne Preunkert,Akinori Yamada,Naohiro Yoshida,Savarino Joel

crossref（2021）

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摘要

17O-excess (Δ17O = δ17O − 0.52 × δ18O) of sulfate trapped in Antarctic ice cores has been proposed as a potential tool for assessing past oxidant chemistry, while insufficient understanding of atmospheric sulfate formation around Antarctica hampers its interpretation. To probe influences of regional specific chemistry, we compared year-round observations of Δ17O of non-sea-salt sulfate in aerosols (Δ17O(SO42−)nss) at Dome C and Dumont d’Urville, inland and coastal sites in East Antarctica, throughout the year 2011. Although Δ17O(SO42–)nss at both sites showed consistent seasonality with summer minima (~1.0 ‰) and winter maxima (~2.5 ‰) owing to sunlight-driven changes in the relative importance of O3-oxidation to OH- and H2O2-oxidation, significant inter-site differences were observed in austral spring–summer and autumn. The co-occurrence of higher Δ17O(SO42–)nss at inland (2.0 ± 0.1 ‰) than the coastal site (1.2 ± 0.1 ‰) and chemical destruction of methanesulfonate (MS–) in aerosols at inland during spring–summer (October to December), combined with the first estimated Δ17O(MS–) of ~16 ‰, implies that MS– destruction produces sulfate with high Δ17O(SO42–)nss of ~12 ‰. If contributing to the known post-depositional decrease of MS– in snow, this process should also cause a significant post-depositional increase in Δ17O(SO42–)nss over 1 ‰, that can reconcile the discrepancy between Δ17O(SO42–)nss in the atmosphere and ice.

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