Search

Understanding the mercury cycle in the Arctic is important due to the harmful bioaccumulation of its toxic form, methylmercury, in wildlife and ultimately Arctic residents. Gaseous elemental mercury (Hg(0)) is relatively well-mixed across the northern hemisphere atmosphere due to its long atmospheric lifetime. Hg(0) can be oxidized, especially in the Arctic spring during halogen-driven depletion events. The resulting gaseous oxidized mercury (Hg(II)) is relatively quickly deposited onto snow, either directly or via condensing onto particles, forming particulate mercury (PHg). It is generally understood that a large fraction of the deposited Hg(II) and PHg is photoreduced to Hg(0) and re-emitted to the atmosphere. However, mercury remaining in the snowpack till melt can become bioavailable through entering the ocean.There is a severe lack of Hg(II) and PHg observations in the central Arctic, particularly over sea ice, limiting our understanding of the mercury cycle in that region and inhibiting us from quantifying mercury budgets in all environmental compartments and particularly where it unfolds its harmful neurotoxic effects. Moreover, most of the observational efforts aiming at creating process understanding focused on spring during mercury depletion events or the snow melt period, leaving large knowledge gaps for fall and winter.Here, we show atmospheric observations of PHg during MOSAiC, measured with an aerosol mass spectrometer in fall and spring over the central Arctic pack ice. In both seasons, PHg concentrations correlate strongly with wind speed and chloride, suggesting a mechanical (wind-driven) process behind atmospheric PHg related partly to blowing snow. In addition, there are significant differences between fall and spring observations (e.g. no atmospheric mercury depletion events in fall), suggesting that various processes are at play.This wind-driven process has hitherto not been reported and is different from observations at land-based stations as well as previous measurements over sea ice that ascribed the formation of PHg to adsorption of Hg(II) onto pre-existing aerosols or diamond dust rather than aerosolization from the snow pack. We hypothesize, based on snow chemical analyzes and literature, that the elevated halide content in snow on sea ice creates complexes of PHg, which are much harder to photoreduce than Hg(II), leading to a larger PHg content in snow. These processes of forming PHg and wind-driven aerosolization have implications for the mercury content of snow and the distances over which PHg is re-deposited after atmospheric transport given that the lifetime of PHg is about one order of magnitude larger than that of Hg(II) in the atmosphere.

Near-surface mercury and ozone depletion events occur in the lowest part of the atmosphere during Arctic spring. Mercury depletion is the first step in a process that transforms long-lived elemental mercury to more reactive forms within the Arctic that are deposited to the cryosphere, ocean, and other surfaces, which can ultimately get integrated into the Arctic food web. Depletion of both mercury and ozone occur due to the presence of reactive halogen radicals that are released from snow, ice, and aerosols. In this work, we added a detailed description of the Arctic atmospheric mercury cycle to our recently published version of the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem 4.3.3) that includes Arctic bromine and chlorine chemistry and activation/recycling on snow and aerosols. The major advantage of our modelling approach is the online calculation of bromine concentrations and emission/recycling that is required to simulate the hourly and daily variability of Arctic mercury depletion. We used this model to study coupling between reactive cycling of mercury, ozone, and bromine during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) spring season in 2020 and evaluated results compared to land-based, ship-based, and remote sensing observations. The model predicts that elemental mercury oxidation is driven largely by bromine chemistry and that particulate mercury is the major form of oxidized mercury. The model predicts that the majority (74%) of oxidized mercury deposited to land-based snow is re-emitted to the atmosphere as gaseous elemental mercury, while a minor fraction (4%) of oxidized mercury that is deposited to sea ice is re-emitted during spring. Our work demonstrates that hourly differences in bromine/ozone chemistry in the atmosphere must be considered to capture the springtime Arctic mercury cycle, including its integration into the cryosphere and ocean.

6 pags., 2 figs., Unlike bromine, the effect of iodine chemistry on the Arctic surface ozone budget is poorly constrained. We present ship-based measurements of halogen oxides in the high Arctic boundary layer from the sunlit period of March to October 2020 and show that iodine enhances springtime tropospheric ozone depletion. We find that chemical reactions between iodine and ozone are the second highest contributor to ozone loss over the study period, after ozone photolysis-initiated loss and ahead of bromine., This study received funding from the European Research Council Executive Agency under the European Union’s Horizon 2020 Research and Innovation Program (project ERC‐2016‐COG 726349 CLIMAHAL and ERC-2016-STG 714621 GASPARCON) and the European Commission via the EMME-CARE project and was supported by the Consejo Superior de Investigaciones Científicas of Spain. This work was supported by the European Union’s Horizon 2020 Research and Innovation Programme under grant agreement no. 856612 and the Academy of Finland (project no. 334514). The Indian Institute of Tropical Meteorology is funded by the Ministry of Earth Sciences, Government of India. Ozone, CO, CH4 and AMS measurements were funded by the Swiss National Science Foundation (grant 200021_188478), the Swiss Polar Institute and U.S. National Science Foundation grants 1914781 and 1807163. J.S. holds the Ingvar Kamprad chair for extreme environments research, sponsored by Ferring Pharmaceuticals. Data reported in this manuscript were produced as part of the international MOSAiC expedition with tag MOSAiC20192020, with activities supported by Polarstern expedition AWI-PS122_00. H.S. was funded by the European ERA-PLANET projects iGOSP and iCUPE (consortium agreement no. 689443 for both projects). We thank FORMAS and the Swedish Polar Research Secretariat for support. We gratefully acknowledge funding by the Deutsche Forschungsgemeinschaft (project no. 268020496 – TRR 172) within the Transregional Collaborative Research Center ‘ArctiC Amplification: Climate Relevant Atmospheric and SurfaCe Processes, and Feedback Mechanisms (AC)3’ in subproject C03. We thank I. Bourgeois (NOAA/CIRES) for providing the ATom NOx data.

International audience; With the Arctic rapidly changing, the needs to observe, understand, and model the changes are essential. To support these needs, an annual cycle of observations of atmospheric properties, processes, and interactions were made while drifting with the sea ice across the central Arctic during the Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition from October 2019 to September 2020. An international team designed and implemented the comprehensive program to document and characterize all aspects of the Arctic atmospheric system in unprecedented detail, using a variety of approaches, and across multiple scales. These measurements were coordinated with other observational teams to explore cross-cutting and coupled interactions with the Arctic Ocean, sea ice, and ecosystem through a variety of physical and biogeochemical processes. This overview outlines the breadth and complexity of the atmospheric research program, which was organized into 4 subgroups: atmospheric state, clouds and precipitation, gases and aerosols, and energy budgets. Atmospheric variability over the annual cycle revealed important influences from a persistent large-scale winter circulation pattern, leading to some storms with pressure and winds that were outside the interquartile range of past conditions suggested by long-term reanalysis. Similarly, the MOSAiC location was warmer and wetter in summer than the reanalysis climatology, in part due to its close proximity to the sea ice edge. The comprehensiveness of the observational program for characterizing and analyzing atmospheric phenomena is demonstrated via a winter case study examining air mass transitions and a summer case study examining vertical atmospheric evolution. Overall, the MOSAiC atmospheric program successfully met its objectives and was the most comprehensive atmospheric measurement program to date conducted over the Arctic sea ice. The obtained data will support a broad range of coupled-system scientific research and provide an important foundation for advancing multiscale modeling capabilities in the Arctic.

The aim of this study was to evaluate the effects of processed dietary supplements derived from two seaweeds, Saccharina latissima (SL) and Ascophyllum nodosum (AN), on microbial methane production and fermentation profile using in vitro methods. Four dual-flow continuous culture fermenters were utilized in a 4x4 Latin Square design to assess these 4 supplements: unwashed, coarsely milled SL (UNW), 3-min rinsed SL (3MR), 20-sec blanched SL (20SB), and a crude phlorotannin extract from AN (PHLT). Treatments were randomly assigned to fermenters and were top dressed on the total mixed ration (TMR) at 5% of total dry matter (DM). Four, 10-d experimental periods were conducted, consisting of a 7-d equilibration period followed by a 3-d sampling period. Vessel pH was continually measured, and effluent samples were collected for volatile fatty acid (VFA) analysis and calculation of DM, organic matter (OM), neutral detergent fiber (NDF) and acid detergent fiber (ADF) digestibilities. Methane was measured prior to the first AM and PM feedings during the 3-d sampling period. Data were analyzed using the PROC MIXED procedure of SAS (9.4) with fermenter as the random effect and period and treatment as fixed effects. Processed treatments (3MR= 7.86, 20SB= 5.75, PHLT= 10.46 mg/dL) yielded less methane (P < 0.02) than unprocessed (UNW= 24.06 mg/dL). Apparent digestibilities of DM, OM, NDF and ADF were not affected by treatment. Total VFA (mM) was greater (P = 0.02) in 3MR than PHLT. The acetate to propionate ratio (A:P) was greater (P < 0.01) in PHLT compared with 20SB, 3MR and UNW (5.62 vs 1.47, 1.27 and 1.54, respectively). Time spent below pH 5.8 during fermentation was not affected by treatment. These results indicate that seaweed processing method can affect methane production in vitro without negatively impacting rumen fermentation and should be further investigated using in vivo models.