Detection of organosulfates and nitrooxy-organosulfates in Arctic and Antarctic atmospheric aerosols, using ultra-high resolution FT-ICR mass spectrometry.

Organosulfates (OSs) are recognized as important secondary organic aerosols (SOAs) in recent years. Due to their amphipathy and light absorptive capacity, OSs may potentially impact climate. Moreover, OSs can serve as molecular tracers for precursors and multiple processes leading to the generation of SOA. However, studies on OSs are lacking in the polar regions which limits our understanding of both their formation pathways and impacts on the polar environment. Here we present the first investigation into OSs in both the Arctic and Antarctic. Organic compounds in aerosol samples collected from the polar regions during the 2013/2014 Chinese National Arctic/Antarctic Research Expedition (CHINARE) were analyzed by Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) coupled with negative ion mode electrospray ionization (ESI(-)). Hundreds to thousands of OSs were detected at the polar sampling sites. The estimated total concentrations of OSs were in the range of 46-670 ng/m in the Arctic sampling area, and 47-260 ng/m in the Antarctic sampling area, accounting for 1-16% of total OM. OSs were found to have undergone a high degree of oxidation in the aerosol samples, which might be due to the combined effects of enhanced photo-oxidation in summertime or continuous oxidation during transport to the polar region. The potential appointment of OS precursors highlights the important role of long-range air-mass transport on the OSs derived from biogenic precursors and a notably large contribution from anthropogenic emissions, suggesting that human activities have significant impacts in remote polar environments. The results of this study provide important insights into the characteristics of OSs in the polar atmosphere. However, the need for further research focusing on the quantification, formation mechanisms and impacts of OSs on climate is emphasized.