Sources of Dimethyl Sulfide in the Canadian Arctic Archipelago and Baffin Bay
Résumé
Dimethyl sulfide plays a major role in the global sulfur cycle, meaning that it is important to the formation of sulfate aerosol and thus to cloud condensation nuclei populations and cloud formation. The summertime Arctic atmosphere sometimes resides in a cloud condensation nuclei limited regime, making it very susceptible to changes in their number. Despite the interest generated by this situation, dimethyl sulfide has only rarely been measured in the summertime Arctic. This work presents the first high time resolution (10 Hz) DMS mixing ratio measurements for the Eastern Canadian Archipelago and Baffin Bay in summer performed on an icebreaker cruise as one component of the Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments (NETCARE). Measured mixing ratios ranged from below the detection limit of 4 pptv to 1155 pptv with a median value of 186 pptv. We used transfer velocity parameterizations from the literature to generate the first flux estimates for this region in summer, which ranged from 0.02-12 μmol m-2 d-1. DMS has a lifetime against OH oxidation of 1-2 days, allowing both local sources and transport to play roles in its atmospheric mixing ratio. Through air mass trajectory analysis using FLEXPART-WRF and chemical transport modeling using GEOS-Chem, we have identified the relative contributions of local sources (Lancaster Sound and Baffin Bay) as well as transport from further afield (the Hudson Bay System and the Beaufort Sea) and find that the local sources dominate. GEOS-Chem is able to reproduce the major features of the measured time series, but is biased low overall (median 72 pptv). We discuss non-marine sources that could account for this low bias and estimate the possible contributions to DMS mixing ratios from lakes, biomass burning, melt ponds and coastal tundra. Our results show that local marine sources of DMS dominate the summer Arctic atmosphere, but that non-local and possibly non-marine contributions have a detectable influence.