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Limited information exists on mercury concentrations and environmental drivers of mercury bioaccumulation in high latitude terrestrial carnivores. Spatial patterns of mercury concentrations in wolverine ( Gulo gulo , n = 419) were assessed across a 1,600,000 km 2 study area in relation to landscape, climate, diet and biological factors in Arctic and boreal biomes of western Canada. Hydrogen stable isotope ratios were measured in wolverine hair from a subset of 80 animals to assess the spatial scale for characterizing environmental conditions of their habitat. Habitat characteristics were determined using GIS methods and raster datasets at two scales, the collection location point and a 150 km radius buffer, which was selected based on results of a correlation analysis between hydrogen stable isotopes in precipitation and wolverine hair. Total mercury concentrations in wolverine muscle ranged >2 orders of magnitude from 0.01 to 5.72 μg/g dry weight and varied geographically, with the highest concentrations in the Northwest Territories followed by Nunavut and Yukon. Regression models at both spatial scales indicated diet (based on nitrogen stable isotope ratios) was the strongest explanatory variable of mercury concentrations in wolverine, with smaller though statistically significant contributions from landscape variables (soil organic carbon, percent cover of wet area, percent cover of perennial snow-ice) and distance to the Arctic Ocean coast. The carbon and nitrogen stable isotope ratios of wolverine muscle suggested greater mercury bioaccumulation could be associated with feeding on marine biota in coastal habitats. Landscape variables identified in the modelling may reflect habitat conditions which support enhanced methylmercury transfer to terrestrial biota. Spatially-explicit estimates of wet atmospheric deposition were positively correlated with wolverine mercury concentrations but this variable was not selected in the final regression models. These landscape patterns provide a basis for further research on underlying processes enhancing methylmercury uptake in high latitude terrestrial food webs.

Wildfire frequency has increased in past four decades in Canada and is expected to increase in future as a result of climate change (Wotton et al., 2010). Mercury (Hg) emissions from biomass burning are known to be significant; however, the impact of biomass burning on air concentration and deposition fluxes in Canada has not been previously quantified. We use estimates of burned biomass from FINN (Fire INventory from NCAR) and vegetation-specific emission factors (EFs) of mercury to investigate the spatiotemporal variability of Hg emissions in Canada. We use Environment and Climate Change Canada's GEM-MACH-Hg (Global Environmental Multi-scale, Modelling Air quality and Chemistry model, mercury version) to quantify the impact of biomass burning in Canada on spatiotemporal variability of air concentrations and deposition fluxes of mercury in Canada. We use North American gaseous elemental mercury (GEM) observations (2010–2015), GEM-MACH-Hg, and an inversion technique to optimize the EFs for GEM for five vegetation types represented in North American fires to constrain the biomass burning impacts of mercury. The inversion results suggest that EFs representing more vegetation types – specifically peatland – are required. This is currently limited by the sparseness of measurements of Hg from biomass burning plumes. More measurements of Hg concentration in the air, specifically downwind of fires, would improve the inversions. We use three biomass burning Hg emissions scenarios in Canada to conduct three sets of model simulations for 2010–2015: two scenarios where Hg is emitted only as GEM using literature or optimized EFs and a third scenario where Hg is emitted as GEM using literature EFs and particle bound mercury (PBM) emitted using the average GEM∕PBM ratio from lab measurements. The three biomass burning emission scenarios represent a range of possible values for the impacts of Hg emissions from biomass burning in Canada on Hg concentration and deposition.We find total biomass burning Hg emissions to be highly variable from year to year and estimate average 2010–2015 total atmospheric biomass burning emissions of Hg in Canada to be between 6 and 14 t during the biomass burning season (i.e. from May to September), which is 3–7 times the mercury emission from anthropogenic sources in Canada for this period. On average, 65 % of the emissions occur in the provinces west of Ontario. We find that while emissions from biomass burning have a small impact on surface air concentrations of GEM averaged over individual provinces/territories, the impact at individual sites can be as high as 95 % during burning events. We estimate average annual mercury deposition from biomass burning in Canada to be between 0.3 and 2.8 t, compared to 0.14 t of mercury deposition from anthropogenic sources during the biomass burning season in Canada. Compared to the biomass burning emissions, the relative impact of fires on mercury deposition is shifted eastward, with on average 54 % percent of the deposition occurring in provinces west of Ontario. While the relative contribution of Canadian biomass burning to the total mercury deposition over each province/territory is no more than 9 % between 2010 and 2015, the local contribution in some locations (including areas downwind of biomass burning) can be as high as 80 % (e.g. northwest of Great Slave Lake in 2014) from May to September. We find that northern Alberta and Saskatchewan, central British Columbia, and the area around Great Slave Lake in the Northwest Territories are at greater risk of mercury contamination from biomass burning. GEM is considered to be the dominant mercury species emitted from biomass burning; however, there remains an uncertainty in the speciation of mercury released from biomass burning. We find that the impact of biomass burning emissions on mercury deposition is significantly affected by the uncertainty in speciation of emitted mercury because PBM is more readily deposited closer to the emission sources than GEM; an addition of  ∼ 18 % percent of mercury emission from biomass burning in the form of PBM in the model increases the 6-year average deposition by  ∼ 4 times.

We implement a detailed representation of aerosol mixing state in the Global Environmental Multiscale – Modelling Air quality and CHemistry (GEM-MACH) air quality and weather forecast model. Our mixing-state representation includes three categories: one for more hygroscopic aerosol, one for less hygroscopic aerosol with a high black carbon (BC) mass fraction, and one for less hygroscopic aerosol with a low BC mass fraction. The more detailed representation allows us to better resolve two different aspects of aerosol mixing state: differences in hygroscopicity due to aerosol composition and the amount of absorption enhancement of BC due to non-absorbing coatings. Notably, this three-category representation allows us to account for BC thickly coated with primary organic matter, which enhances the absorption of the BC but has a low hygroscopicity. We compare the results of the three-category representation (1L2B, (one hydrophilic, two hydrophobic)) with a simulation that uses two categories, split by hygroscopicity (HYGRO), and a simulation using the original size-resolved internally mixed assumption (SRIM). We perform a case study that is focused on North America during July 2016, when there were intense wildfires over northwestern North America. We find that the more detailed representation of the aerosol hygroscopicity in both 1L2B and HYGRO decreases wet deposition, which increases aerosol concentrations, particularly of less hygroscopic species. The concentration of PM2.5 increases by 23 % on average. We show that these increased aerosol concentrations increase cloud droplet number concentrations and cloud reflectivity in the model, decreasing surface temperatures. Using two categories based on hygroscopicity yields only a modest benefit in resolving the coating thickness on black carbon, however. The 1L2B representation resolves BC with thinner coatings than the HYGRO simulation, resulting in absorption aerosol optical depths that are 3 % less on average, with greater differences over strong anthropogenic source regions. We did not find strong subsequent effects of this decreased absorption on meteorology.

Oil sands upgrading facilities in the Athabasca oil sands region (AOSR) in Alberta, Canada, have been reporting mercury (Hg) emissions to public government databases (National Pollutant Release Inventory (NPRI)) since the year 2000, yet the relative contribution of these emissions to ambient Hg deposition remains unknown. The impact of oil sands emissions (OSE) on Hg levels in and around the AOSR, relative to contributions from global (anthropogenic, geogenic and legacy) emissions and regional biomass burning emissions (BBE), was assessed using a global 3D-process-based Hg model, GEM-MACH-Hg, from 2012 to 2015. In addition, the relative importance of year-to-year changes in Hg emissions from the above sources and meteorological conditions to inter-annual variations in Hg deposition was examined. Surface air concentrations of Hg species and annual snowpack Hg loadings simulated by the model were found comparable to measured levels in the AOSR, suggesting consistency between reported Hg emissions from oil sands activities and Hg levels in the region. As a result of global-scale transport and the long lifetime of gaseous elemental Hg (Hg(0)), surface air concentrations of Hg(0) in the AOSR reflected the background Hg(0) levels in Canada. By comparison, average air concentrations of total oxidized Hg (efficiently deposited Hg species) in the AOSR were elevated up to 60 % within 50 km of the oil sands Hg emission sources. Hg emissions from wildfire events led to episodes of high ambient Hg(0) concentrations and deposition enrichments in northern Alberta, including the AOSR, during the burning season. Hg deposition fluxes in the AOSR were within the range of the deposition fluxes measured for the entire province of Alberta. On a broad spatial scale, contribution from imported Hg from global sources dominated the annual background Hg deposition in the AOSR, with present-day global anthropogenic emissions contributing to 40 % (< 1 % from Canada excluding OSE) and geogenic and legacy emissions contributing to 60 % of the background Hg deposition. In contrast, oil sands Hg emissions were responsible for significant enhancements in Hg deposition in the immediate vicinity of oil sands Hg emission sources, which were ∼ 10 times larger in winter than summer (250 %–350 % in winter and ∼ 35 % in summer within 10 km of OSE, 2012–2013). The spatial extent of the influence of oil sands emissions on Hg deposition was also greater in winter relative to summer (∼ 100 km vs. 30 km from Hg-emitting facilities). In addition, inter-annual changes in meteorological conditions and oil sands emissions also led to significantly higher inter-annual variations in wintertime Hg deposition compared to summer. In 2015, within 10 km of major oil sands sources, relative to 2012, Hg deposition declined by 46 % in winter but 22 % annually, due to a larger OSE-led reduction in wintertime deposition. Inter-annual variations in meteorological conditions were found to both exacerbate and diminish the impacts of OSE on Hg deposition in the AOSR, which can confound the interpretation of trends in short-term environmental Hg monitoring data. Hg runoff in spring flood, comprising the majority of annual Hg runoff, is mainly derived from seasonal snowpack Hg loadings and mobilization of Hg deposited in surface soils, both of which are sensitive to Hg emissions from oil sands developments in the proximity of sources. Model results suggest that sustained efforts to reduce anthropogenic Hg emissions from both global and oil sands sources are required to reduce Hg deposition in the AOSR.

Current understanding of mercury (Hg) behavior in the atmosphere contains significant gaps. Some key characteristics of Hg processes, including anthropogenic and geogenic emissions, atmospheric chemistry, and air–surface exchange, are still poorly known. This study provides a complex analysis of processes governing Hg fate in the atmosphere involving both measured data from ground-based sites and simulation results from chemical transport models. A variety of long-term measurements of gaseous elemental Hg (GEM) and reactive Hg (RM) concentration as well as Hg wet deposition flux have been compiled from different global and regional monitoring networks. Four contemporary global-scale transport models for Hg were used, both in their state-of-the-art configurations and for a number of numerical experiments to evaluate particular processes. Results of the model simulations were evaluated against measurements. As follows from the analysis, the interhemispheric GEM gradient is largely formed by the prevailing spatial distribution of anthropogenic emissions in the Northern Hemisphere. The contributions of natural and secondary emissions enhance the south-to-north gradient, but their effect is less significant. Atmospheric chemistry has a limited effect on the spatial distribution and temporal variation of GEM concentration in surface air. In contrast, RM air concentration and wet deposition are largely defined by oxidation chemistry. The Br oxidation mechanism can reproduce successfully the observed seasonal variation of the RM ∕ GEM ratio in the near-surface layer, but it predicts a wet deposition maximum in spring instead of in summer as observed at monitoring sites in North America and Europe. Model runs with OH chemistry correctly simulate both the periods of maximum and minimum values and the amplitude of observed seasonal variation but shift the maximum RM ∕ GEM ratios from spring to summer. O3 chemistry does not predict significant seasonal variation of Hg oxidation. Hence, the performance of the Hg oxidation mechanisms under study differs in the extent to which they can reproduce the various observed parameters. This variation implies possibility of more complex chemistry and multiple Hg oxidation pathways occurring concurrently in various parts of the atmosphere.

Mercury (Hg) is a worldwide contaminant that can cause adverse health effects to wildlife and humans. While atmospheric modeling traces the link from emissions to deposition of Hg onto environmental surfaces, large uncertainties arise from our incomplete understanding of atmospheric processes (oxidation pathways, deposition, and re-emission). Atmospheric Hg reactivity is exacerbated in high latitudes and there is still much to be learned from polar regions in terms of atmospheric processes. This paper provides a synthesis of the atmospheric Hg monitoring data available in recent years (2011–2015) in the Arctic and in Antarctica along with a comparison of these observations with numerical simulations using four cutting-edge global models. The cycle of atmospheric Hg in the Arctic and in Antarctica presents both similarities and differences. Coastal sites in the two regions are both influenced by springtime atmospheric Hg depletion events and by summertime snowpack re-emission and oceanic evasion of Hg. The cycle of atmospheric Hg differs between the two regions primarily because of their different geography. While Arctic sites are significantly influenced by northern hemispheric Hg emissions especially in winter, coastal Antarctic sites are significantly influenced by the reactivity observed on the East Antarctic ice sheet due to katabatic winds. Based on the comparison of multi-model simulations with observations, this paper discusses whether the processes that affect atmospheric Hg seasonality and interannual variability are appropriately represented in the models and identifies research gaps in our understanding of the atmospheric Hg cycling in high latitudes.

Atmospheric chemistry and transport of mercury play a key role in the global mercury cycle. However, there are still considerable knowledge gaps concerning the fate of mercury in the atmosphere. This is the second part of a model intercomparison study investigating the impact of atmospheric chemistry and emissions on mercury in the atmosphere. While the first study focused on ground-based observations of mercury concentration and deposition, here we investigate the vertical and interhemispheric distribution and speciation of mercury from the planetary boundary layer to the lower stratosphere. So far, there have been few model studies investigating the vertical distribution of mercury, mostly focusing on single aircraft campaigns. Here, we present a first comprehensive analysis based on various aircraft observations in Europe, North America, and on intercontinental flights. The investigated models proved to be able to reproduce the distribution of total and elemental mercury concentrations in the troposphere including interhemispheric trends. One key aspect of the study is the investigation of mercury oxidation in the troposphere. We found that different chemistry schemes were better at reproducing observed oxidized mercury patterns depending on altitude. High concentrations of oxidized mercury in the upper troposphere could be reproduced with oxidation by bromine while elevated concentrations in the lower troposphere were better reproduced by OH and ozone chemistry. However, the results were not always conclusive as the physical and chemical parameterizations in the chemistry transport models also proved to have a substantial impact on model results.

The Multi-Compartment Hg (mercury) Modeling and Analysis Project (MCHgMAP) is an international multimodel research initiative intended to simulate and analyze the geospatial distributions and temporal trends of environmental Hg to inform effectiveness evaluations of two multilateral environmental agreements (MEAs): the Minamata Convention on Mercury (MC) and the Convention on Long-Range Transboundary Air Pollution (LRTAP). This MCHgMAP overview paper presents its science objectives, background, and rationale; experimental design (multimodel ensemble (MME) architecture, inputs and evaluation data, simulations, and reporting framework); and methodologies for the evaluation and analysis of simulated environmental Hg levels. The primary goals of the project are to facilitate detection and attribution of recent (observed) and future (projected) spatial patterns and temporal trends of global environmental Hg levels and identification of key knowledge gaps in Hg science and modeling to improve future effectiveness evaluation cycles of the MEAs. The current advances and challenges of Hg models, emission inventories, and observational data are examined, and an optimized multimodel experimental design is introduced to address the key policy questions of the MEAs. A common set of emissions, environmental conditions, and observation datasets is proposed (where possible) to enhance the MME comparability. A novel harmonized simulation approach between atmospheric, land, oceanic, and multimedia models is proposed to account for the short- and long-term changes in secondary Hg exchanges and to achieve mechanistic consistency of Hg levels across environmental matrices. A comprehensive set of model experiments is proposed and prioritized to ensure systematic analysis and participation of a variety of models from the scientific community.

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.

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.