Mercury isotope evidence for Arctic summertime re-emission of mercury from the cryosphere

During Arctic springtime, halogen radicals oxidize atmospheric elemental mercury (Hg-0), which deposits to the cryosphere. This is followed by a summertime atmospheric Hg-0 peak that is thought to result mostly from terrestrial Hg inputs to the Arctic Ocean, followed by photoreduction and emission to air. The large terrestrial Hg contribution to the Arctic Ocean and global atmosphere has raised concern over the potential release of permafrost Hg, via rivers and coastal erosion, with Arctic warming. Here we investigate Hg isotope variability of Arctic atmospheric, marine, and terrestrial Hg. We observe highly characteristic Hg isotope signatures during the summertime peak that reflect re-emission of Hg deposited to the cryosphere during spring. Air mass back trajectories support a cryospheric Hg emission source but no major terrestrial source. This implies that terrestrial Hg inputs to the Arctic Ocean remain in the marine ecosystem, without substantial loss to the global atmosphere, but with possible effects on food webs.Arctic warming thaws permafrost, leading to enhanced soil mercury transport to the Arctic Ocean. Mercury isotope signatures in arctic rivers, ocean and atmosphere suggest that permafrost mercury is buried in marine sediment and not emitted to the global atmospherePeer reviewe

Updated trends for atmospheric mercury in the Arctic: 1995–2018

The Arctic region forms a unique environment with specific physical, chemical, and biological processes affecting mercury (Hg) cycles and limited anthropogenic Hg sources. However, historic global emissions and long range atmospheric transport has led to elevated Hg in Arctic wildlife and waterways. Continuous atmospheric Hg measurements, spanning 20 years, and increased monitoring sites has allowed a more comprehensive understanding of how Arctic atmospheric mercury is changing over time. Time-series trend analysis of TGM (Total Gaseous Mercury) in air was performed from 10 circumpolar air monitoring stations, comprising of high-Arctic, and sub-Arctic sites. GOM (gaseous oxidised mercury) and PHg (particulate bound mercury) measurements were also available at 2 high-Arctic sites. Seasonal mean TGM for sub-Arctic sites were lowest during fall ranging from 1.1 ng m−3 Hyytiälä to 1.3 ng m−3, Little Fox Lake. Mean TGM concentrations at high-Arctic sites showed the greatest variability, with highest daily means in spring ranging between 4.2 ng m−3 at Amderma and 2.4 ng m−3 at Zeppelin, largely driven by local chemistry. Annual TGM trend analysis was negative for 8 of the 10 sites. High-Arctic seasonal TGM trends saw smallest decline during summer. Fall trends ranged from −0.8% to −2.6% yr−1. Across the sub-Arctic sites spring showed the largest significant decreases, ranging between −7.7% to −0.36% yr−1, while fall generally had no significant trends. High-Arctic speciation of GOM and PHg at Alert and Zeppelin showed that the timing and composition of atmospheric mercury deposition events are shifting. Alert GOM trends are increasing throughout the year, while PHg trends decreased or not significant. Zeppelin saw the opposite, moving towards increasing PHg and decreasing GOM. Atmospheric mercury trends over the last 20 years indicate that Hg concentrations are decreasing across the Arctic, though not uniformly. This is potentially driven by environmental change, such as plant productivity and sea ice dynamics

Updated trends for atmospheric mercury in the Arctic: 1995–2018

The Arctic region forms a unique environment with specific physical, chemical, and biological processes affecting mercury (Hg) cycles and limited anthropogenic Hg sources. However, historic global emissions and long range atmospheric transport has led to elevated Hg in Arctic wildlife and waterways. Continuous atmospheric Hg measurements, spanning 20 years, and increased monitoring sites has allowed a more comprehensive understanding of how Arctic atmospheric mercury is changing over time. Time-series trend analysis of TGM (Total Gaseous Mercury) in air was performed from 10 circumpolar air monitoring stations, comprising of high-Arctic, and sub-Arctic sites. GOM (gaseous oxidised mercury) and PHg (particulate bound mercury) measurements were also available at 2 high-Arctic sites. Seasonal mean TGM for sub-Arctic sites were lowest during fall ranging from 1.1 ng m−3 Hyytiälä to 1.3 ng m−3, Little Fox Lake. Mean TGM concentrations at high-Arctic sites showed the greatest variability, with highest daily means in spring ranging between 4.2 ng m−3 at Amderma and 2.4 ng m−3 at Zeppelin, largely driven by local chemistry. Annual TGM trend analysis was negative for 8 of the 10 sites. High-Arctic seasonal TGM trends saw smallest decline during summer. Fall trends ranged from −0.8% to −2.6% yr−1. Across the sub-Arctic sites spring showed the largest significant decreases, ranging between −7.7% to −0.36% yr−1, while fall generally had no significant trends. High-Arctic speciation of GOM and PHg at Alert and Zeppelin showed that the timing and composition of atmospheric mercury deposition events are shifting. Alert GOM trends are increasing throughout the year, while PHg trends decreased or not significant. Zeppelin saw the opposite, moving towards increasing PHg and decreasing GOM. Atmospheric mercury trends over the last 20 years indicate that Hg concentrations are decreasing across the Arctic, though not uniformly. This is potentially driven by environmental change, such as plant productivity and sea ice dynamics

Mercury isotope evidence for Arctic summertime re-emission of mercury from the cryosphere

During Arctic springtime, halogen radicals oxidize atmospheric elemental mercury (Hg-0), which deposits to the cryosphere. This is followed by a summertime atmospheric Hg-0 peak that is thought to result mostly from terrestrial Hg inputs to the Arctic Ocean, followed by photoreduction and emission to air. The large terrestrial Hg contribution to the Arctic Ocean and global atmosphere has raised concern over the potential release of permafrost Hg, via rivers and coastal erosion, with Arctic warming. Here we investigate Hg isotope variability of Arctic atmospheric, marine, and terrestrial Hg. We observe highly characteristic Hg isotope signatures during the summertime peak that reflect re-emission of Hg deposited to the cryosphere during spring. Air mass back trajectories support a cryospheric Hg emission source but no major terrestrial source. This implies that terrestrial Hg inputs to the Arctic Ocean remain in the marine ecosystem, without substantial loss to the global atmosphere, but with possible effects on food webs.Arctic warming thaws permafrost, leading to enhanced soil mercury transport to the Arctic Ocean. Mercury isotope signatures in arctic rivers, ocean and atmosphere suggest that permafrost mercury is buried in marine sediment and not emitted to the global atmospherePeer reviewe

Modelling the coupled mercury-halogen-ozone cycle in the central Arctic during spring

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.Peer reviewe