Mercury Isotopes Reveal Atmospheric Gaseous Mercury Deposition Directly to the Arctic Coastal Snowpack

Springtime atmospheric mercury depletion events (AMDEs) lead to snow with elevated mercury concentrations (>200 ng Hg/L) in the Arctic and Antarctic. During AMDEs gaseous elemental mercury (GEM) is photochemically oxidized by halogens to reactive gaseous mercury which is deposited to the snowpack. This reactive mercury is either photochemically reduced back to GEM and re-emitted to the atmosphere or remains in the snowpack until spring snowmelt. GEM is also deposited to the snowpack and tundra vegetation by reactive surface uptake (dry deposition) from the atmosphere. There is little consensus on the proportion of AMDE-sourced Hg versus Hg from dry deposition that is released in spring runoff. We used mercury stable isotope measurements of GEM, snowfall, snowpack, snowmelt, surface water, vegetation, and peat from a northern Alaska coastal watershed to quantify Hg sources. Although high Hg concentrations are deposited to the snowpack during AMDEs, we estimate that similar to 76 to 91% is released back to the atmosphere prior to snowmelt. Mercury deposited to the snowpack as GEM comprises the majority of snowmelt Hg and has a Hg stable isotope composition similar to Hg deposited by reactive surface uptake of GEM into the leaves of trees in temperate forests. This GEM-sourced Hg is the dominant Hg we measured in the spring snowpack and in tundra peat permafrost deposits.