Regional Characteristics of Atmospheric Sulfate Formation in East Antarctica Imprinted on 17O-Excess Signature

O-17-excess (Delta O-17 = delta O-17 - 0.52 x delta O-18) 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 Delta O-17 of non-sea-salt sulfate in aerosols (Delta O-17(SO42-)(nss)) at Dome C and Dumont d'Urville, inland and coastal sites in East Antarctica, throughout the year 2011. Although Delta O-17(SO42-)(nss) at both sites showed consistent seasonality with summer minima (similar to 1.0 parts per thousand) and winter maxima (similar to 2.5 parts per thousand) owing to sunlight-driven changes in the relative importance of O-3 oxidation to OH and H2O2 oxidation, significant intersite differences were observed in austral spring-summer and autumn. The cooccurrence of higher Delta O-17(SO42-)(nss) at inland (2.0 parts per thousand +/- 0.1 parts per thousand) than the coastal site (1.2 parts per thousand +/- 0.1 parts per thousand) and chemical destruction of methanesulfonate (MS-) in aerosols at inland during spring-summer (October-December), combined with the first estimated Delta O-17(MS-) of similar to 16 parts per thousand, implies that MS- destruction produces sulfate with high Delta O-17(SO42-)(nss) of similar to 12 parts per thousand. If contributing to the known postdepositional decrease of MS- in snow, this process should also cause a significant postdepositional increase in Delta O-17(SO42-)(nss) over 1 parts per thousand, that can reconcile the discrepancy between Delta O-17(SO42-)(nss) in the atmosphere and ice. The higher Delta O-17(SO42-)(nss) at the coastal site than inland during autumn (March-May) may be associated with oxidation process involving reactive bromine and/or sea-salt particles around the coastal region.

Automated summary

The study compared Delta O-17 of non-sea-salt sulfate in aerosols between inland and coastal sites in East Antarctica throughout 2011. Results showed consistent seasonality with summer minima and winter maxima, but significant intersite differences were observed in spring-summer and autumn.