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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.

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. A 3D process-based global Hg model, GEM-MACH-Hg, was applied to simulate the Hg burden in and around the AOSR using NPRI reported oil sands Hg emissions from 2012 (59 kg) to 2015 (25 kg) and other regional and global Hg emissions. The impact of oil sands emissions (OSE) on Hg levels in the AOSR, relative to contributions from sources such as global anthropogenic and biomass burning emissions (BBE), was assessed. 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. Model simulated surface air concentrations of Hg species and annually accumulated Hg in snowpacks were found comparable to independently obtained measurements 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 of gaseous elemental Hg (Hg(0)), surface air concentrations of Hg(0) in the AOSR reflected the background Hg(0) levels in Canada (1.4 ng m−3, AOSR; 1.2 1.6 ng m−3, Canada) with negligible impact from OSE. Highly spatiotemporally variable wildfire Hg emission events led to episodes of high ambient Hg(0) air concentrations of up to 2.5 ng m−3 during the burning season. By comparison, average air concentrations of total oxidised Hg (gaseous plus particulate; efficiently deposited Hg species) in the AOSR were elevated by 60 % above background levels (2012–2013) within 50 km of the oil sands major upgraders as a result of OSE. Annual average Hg deposition fluxes in the AOSR were within the range of the deposition fluxes measured for the entire province of Alberta (15.6–18.3 µg m−2 y−1, AOSR (2012–2015); ~14–25 µg m−2 y−1, Alberta (2015)). Winter (November–April) and summer (June–August), respectively, accounted for 20 % and 50 % of the annual Hg deposition in the AOSR. On a broad spatial scale, imported Hg from global sources dominated the annual Hg deposition in the AOSR, with present-day global anthropogenic emissions contributing to 40 % (

Passive air samplers (PASs), which provide time-averaged concentrations of gaseous mercury over the timescale of weeks to months, are promising for filling a gap in the monitoring of atmospheric mercury worldwide. Their usefulness will depend on their ease of use and robustness under field conditions, their availability and affordability, and most notably, their ability to provide results of acceptable precision and accuracy. Here we describe a comparative evaluation of three PASs with respect to their ability to precisely and accurately record atmospheric background mercury concentrations at sites in both southern Italy and southern Ontario, Canada. The study includes the CNR-PAS with gold nanoparticles as a sorbent, developed by the Italian National Research Council, the IVL-PAS using an activated carbon-coated disk, developed by the Swedish Environmental Research Institute, and the MerPAS® using a sulfur-impregnated activated carbon sorbent, developed at the University of Toronto and commercialized by Tekran. Detection limits are deduced from the variability in the amount of mercury quantified in more than 20 field blank samples for each PAS. Analytical and sampling precision is quantified through 22 triplicate deployments for each PAS, ranging in duration from 2 to 12 weeks. Accuracy and bias are assessed through comparison with gaseous elemental mercury concentrations recorded by Tekran 2537 automated mercury analyzers operating alongside the PASs at both locations. The performance of the PASs was significantly better in Italy, with all of them providing concentrations that are not significantly different from the average concentrations of the Tekran 2537 instruments. In Canada, where weather conditions were much harsher and more variable during the February through April deployment period, there are differences amongst the PASs. At both sites, the MerPAS® is currently the most sensitive, precise, and accurate among the three PASs. A key reason for this is the larger size and the radial configuration of the MerPAS®, which results in lower blank levels relative to the sequestered amounts of mercury when compared to the other two PASs, which rely on axial diffusion geometries. Since blank correction becomes relatively smaller with longer deployments, performance tends to be closer amongst the PASs during deployments of 8 and 12 weeks.

Wildfire impacts on air quality and climate are expected to be exacerbated by climate change with the most pronounced impacts in the boreal biome. Despite the large geographic coverage, there is a lack of information on boreal forest wildfire emissions, particularly for organic compounds, which are critical inputs for air quality model predictions of downwind impacts. In this study, airborne measurements of 250 compounds from 15 instruments, including 228 non-methane organics compounds (NMOG), were used to provide the most detailed characterization, to date, of boreal forest wildfire emissions. Highly speciated measurements showed a large diversity of chemical classes highlighting the complexity of emissions. Using measurements of the total NMOG carbon (NMOGT), the ΣNMOG was found to be 46.2 % of NMOGT, of which, the intermediate- and semi-volatile organic compounds (I/SVOCs) were estimated to account for 7.4 %. These estimates of I/SVOC emission factors expand the volatility range of NMOG typically reported. Despite extensive speciation, a substantial portion of NMOGT remained unidentified (46.4 %), with expected contributions from more highly-functionalized VOCs and I/SVOCs. The emission factors derived in this study improve wildfire chemical speciation profiles and are especially relevant for air quality modelling of boreal forest wildfires. These aircraft-derived emission estimates were further linked with those derived from satellite observations demonstrating their combined value in assessing variability in modelled emissions. These results contribute to the verification and improvement of models that are essential for reliable predictions of near-source and downwind pollution resulting from boreal forest wildfires.

Tracing emission sources and transformations of atmospheric mercury with Hg stable isotopes depends on the ability to collect amounts sufficient for reliable quantification. Commonly employed active sampling methods require power and long pumping times, which limits the ability to deploy in remote locations and at high spatial resolution and can lead to compromised traps. In order to overcome these limitations, we conducted field and laboratory experiments to assess the preservation of isotopic composition during sampling of gaseous elemental mercury (GEM) with a passive air sampler (PAS) that uses a sulfur-impregnated carbon sorbent and a diffusive barrier. Whereas no mass independent fractionation (MIF) was observed during sampling, the mass dependent fractionation (MDF, δ

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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.

Atmospheric mercury (Hg) is deposited to Polar Regions during springtime atmospheric mercury depletion events (AMDEs) that require halogens and snow or ice surfaces. The fate of this Hg during and following snowmelt is largely unknown. We measured Hg, major ions, and stable water isotopes from the snowpack through the entire spring melt runoff period for two years. Our small (2.5 ha) watershed is near Barrow (now Utqiaġvik), Alaska. We measured discharge, made 10 000 snow depths, and collected over 100 samples of snow and meltwater for chemical analysis in 2008 and 2009 from the watershed snowpack and ephemeral stream channel. Our results suggest AMDE Hg complexed with Cl⁻ or Br⁻ may be less likely to be photochemically reduced and re-emitted to the atmosphere prior to snowmelt, and we estimate that roughly 25% of the Hg in snowmelt is attributable to AMDEs. Projected Arctic warming, with more open sea ice leads providing halogen sources that promote AMDEs, may provide enhanced Hg deposition, reduced Hg emission and, ultimately, an increase in snowpack and snowmelt runoff Hg concentrations.

Bromine atoms play a central role in atmospheric reactive halogen chemistry, depleting ozone and elemental mercury, thereby enhancing deposition of toxic mercury, particularly in the Arctic near-surface troposphere. However, direct bromine atom measurements have been missing to date, due to the lack of analytical capability with sufficient sensitivity for ambient measurements. Here we present direct atmospheric bromine atom measurements, conducted in the springtime Arctic. Measured bromine atom levels reached 14 parts per trillion (ppt, pmol mol −1 ; 4.2 × 10 8 atoms per cm −3 ) and were up to 3–10 times higher than estimates using previous indirect measurements not considering the critical role of molecular bromine. Observed ozone and elemental mercury depletion rates are quantitatively explained by the measured bromine atoms, providing field validation of highly uncertain mercury chemistry. Following complete ozone depletion, elevated bromine concentrations are sustained by photochemical snowpack emissions of molecular bromine and nitrogen oxides, resulting in continued atmospheric mercury depletion. This study provides a breakthrough in quantitatively constraining bromine chemistry in the polar atmosphere, where this chemistry connects the rapidly changing surface to pollutant fate.

Mercury (Hg) is a global pollutant released from both natural and human sources. Here we compare long-term records of wet deposition loadings of total Hg (THg) in the open to dry deposition loadings of THg in throughfall and litterfall under four boreal mixedwood canopy types at the remote Experimental Lakes Area (ELA) in Northwestern Ontario, Canada. We also present long-term records of atmospheric concentrations of gaseous elemental (GEM), gaseous oxidized (GOM), and particle bound (PBM) Hg measured at the ELA. We show that dry THg loadings in throughfall and litterfall are 2.7 to 6.1 times greater than wet THg loadings in the open. GEM concentrations showed distinct monthly and daily patterns, correlating positively in spring and summer with rates of gross ecosystem productivity and respiration. GOM and PBM concentrations were less variable throughout the year but were highest in the winter, when concentrations of anthropogenically sourced particles and gases were also high. Forest fires, Arctic air masses, and road salt also impacted GEM, GOM, and PBM concentrations at the ELA. A nested GEOS-Chem simulation for the ELA region produced a dry/wet deposition ratio of >5, suggesting that the importance of dry deposition in forested regions can be reasonably modeled by existing schemes for trace gases.

Thin solid films 735, 138862 (2021). doi:10.1016/j.tsf.2021.138862, Published by Elsevier, Amsterdam [u.a.]

The specific properties of gaseous elemental mercury (GEM) allow it to undergo bidirectional exchange between the atmosphere and the Earth’s surface. Determining the direction and the magnitude of GEM’s atmosphere-surface flux is possible and has been accomplished using micrometeorological and chamber techniques, but (i) is complex and labor-intensive, and (ii) often only yields fluxes over relatively short time scales. A recently developed passive air sampler for GEM has the precision required for identifying and quantifying vertical concentration gradients above the Earth’s surface. The feasibility and performance of this approach is currently being tested in a number of field studies aimed at the: (i) measurement of GEM concentration gradients above both mercury-contaminated and background forest soils, (ii) quantification of vertical concentration gradients on a tower through a temperate deciduous forest canopy, and (iii) measurement of mercury concentration gradients over stable and thawing permafrost to determine the effect of permafrost degradation on GEM evasion. Contrasting with earlier flux studies, these investigations cover long time periods (up to 1.5 years) and have coarse temporal resolution (monthly to seasonally). Significant gradients of GEM air concentrations, both increasing and decreasing with height above ground, were observed, implying that at a minimum, the method is able to identify the flux direction of GEM. Under the right circumstances, this method can also be used to estimate the approximate magnitude of the GEM air-surface exchange flux. The measured gradients also reveal the impact of factors such as temperature, solar irradiance, and snow cover on air-surface exchange. The method holds promise for establishing the direction and size of exchange fluxes at long time scales of months to a year, especially in study areas where access, effort and cost are prohibitive to longer duration studies with existing approaches.

The Arctic plays a critical role in the global Hg cycle as both a sink of Hg and, in response to rapid global warming, an emerging source of Hg due to release from permafrost and glaciers. Human activities have led to significant mercury (Hg) contamination in the Arctic over many decades, potentially impacting the health of Arctic ecosystems and indigenous people. Thus, it is crucial to understand the sources and transformations of Hg in the Arctic in order to predict how Hg behaves as emissions and the global climate change. Here we examine Hg stable isotopes in atmospheric particulate Hg (PHg), gaseous elemental Hg (GEM) and surface snow in the high Arctic (Alert, Canada) during polar spring from 2011 to 2015, in order to trace the sources of atmospheric Hg and its fate in Arctic surface environment. Isotope signatures of GEM (δ202Hg = 0.67 ± 0.24‰, Δ199Hg = −0.23 ± 0.04‰, Δ200Hg = −0.06 ± 0.04‰, 2SD) are similar to the average Northern Hemisphere background, suggesting that GEM in the high Arctic atmosphere is well mixed with those from lower latitudes. Surprisingly, the isotope composition of PHg has negative Δ199Hg, which is similar to GEM but distinct from the positive Δ199Hg typically observed for oxidized Hg species elsewhere. Furthermore, Hg in surface snow shows more negative MIF than PHg, indicating post-depositional loss of Hg via photoreduction. We suggest that PHg is primarily sourced from in situ oxidation of GEM and subsequent scavenging by particles, and thus inherited the isotope composition of GEM when the oxidation is near-complete. The photoreduction re-emission of Hg from snow is strongly affected by Hg speciation, but the overall extent of re-emission (20 ± 31%) is lower than previous estimations for other locations, suggesting potentially a greater loading of Hg to Arctic ecosystem via snowmelt.

Ferromagnetic insulator thin films can convey information by spin waves, avoiding charge displacement and Eddy current losses. The sparsity of high-temperature insulating ferromagnetic materials hinders the development of spin wave based devices. Stoichiometric magnesium titanate, MgTiO$_3$, has an electronic-energy-band structure in which all bands are either full or empty, being a paramagnetic insulator. The MgTiO$_3$ ilmenite consists of ordered octahedra and cation network in which one third of the octahedra are vacant, one third host magnesium and one third titanium. By giving up these characteristics, a rich variety of different magnetic structures can be formed. Our experiments and electronic-energy-band-structure computations show that the magnetic and electric properties of Mg-Ti-O films can drastically be changed and controlled by Mg- and Ti-cation arrangement and abundancy in the octahedra. Insulating titanium- and semiconducting magnesium-rich films were ferromagnetic up to elevated temperatures. The presence and origin of ferromagnetic insulating phase in the films is not apparent - the expectation, based on the well-established rules set by Goodenough and Kanamori, is paramagnetic or antiferromagnetic ordering. We show that ferro- and paramagnetic phases, possessing the same stoichiometry, can be obtained by merely rearranging the cations, thus allowing defect-free interfaces in multilayer structures.

Passive air samplers (PASs) for gaseous mercury (Hg) were deployed for time periods between 1 month and 1 year at 20 sites across the globe with continuous atmospheric Hg monitoring using active Tekran instruments. The purpose was to evaluate the accuracy of the PAS vis-à-vis the industry standard active instruments and to determine a sampling rate (SR; the volume of air stripped of gaseous Hg per unit of time) that is applicable across a wide range of conditions. The sites spanned a wide range of latitudes, altitudes, meteorological conditions, and gaseous Hg concentrations. Precision, based on 378 replicated deployments performed by numerous personnel at multiple sites, is 3.6 ± 3.0 %1, confirming the PAS's excellent reproducibility and ease of use. Using a SR previously determined at a single site, gaseous Hg concentrations derived from the globally distributed PASs deviate from Tekran-based concentrations by 14.2 ± 10 %. A recalibration using the entire new data set yields a slightly higher SR of 0.1354 ± 0.016 m3 day−1. When concentrations are derived from the PAS using this revised SR the difference between concentrations from active and passive sampling is reduced to 8.8 ± 7.5 %. At the mean gaseous Hg concentration across the study sites of 1.54 ng m−3, this represents an ability to resolve concentrations to within 0.13 ng m−3. Adjusting the sampling rate to deployment specific temperatures and wind speeds does not decrease the difference in active–passive concentration further (8.7 ± 5.7 %), but reduces its variability by leading to better agreement in Hg concentrations measured at sites with very high and very low temperatures and very high wind speeds. This value (8.7 ± 5.7 %) represents a conservative assessment of the overall uncertainty of the PAS due to inherent uncertainties of the Tekran instruments. Going forward, the recalibrated SR adjusted for temperature and wind speed should be used, especially if conditions are highly variable or deviate considerably from the average of the deployments in this study (9.89 °C, 3.41 m s−1). Overall, the study demonstrates that the sampler is capable of recording background gaseous Hg concentrations across a wide range of environmental conditions with accuracy similar to that of industry standard active sampling instruments. Results at sites with active speciation units were inconclusive on whether the PASs take up total gaseous Hg or solely gaseous elemental Hg primarily because gaseous oxidized Hg concentrations were in a similar range as the uncertainty of the PAS. 1Subscripted numbers are not significant, but are reported to reduce rounding errors in subsequent studies (see Sect. 2.3 for details).

Passive air samplers (PASs) provide an opportunity to improve the spatial range and resolution of gaseous mercury (Hg) measurements. Here, we propose a sampler design that combines a sulfur-impregnated activated carbon sorbent, a Radiello diffusive barrier, and a protective shield for outdoor deployments. The amount of gaseous Hg taken up by the sampler increased linearly with time for both an 11-week indoor (r2 = 0.990) and 12-month outdoor (r2 = 0.996) deployment, yielding sampling rates of 0.158 ± 0.008 m3 day–1 indoors and 0.121 ± 0.005 m3 day–1 outdoors. These sampling rates are close to modeled estimates of 0.166 m3 day–1 indoors and 0.129 m3 day–1 outdoors. Replicate precision is better than for all previous PASs for gaseous Hg, especially during outdoor deployments (2 ± 1.3%). Such precision is essential for discriminating the relatively small concentration variations occurring at background sites. Deployment times for obtaining reliable time-averaged atmospheric gaseous Hg concentrations range fr...

Long-range atmospheric transport and deposition are important sources of mercury (Hg) to Arctic aquatic and terrestrial ecosystems. We review here recent progress made in the study of the transport, transformation, deposition and reemission of atmospheric Hg in the Canadian Arctic, focusing on field measurements (see Dastoor et al., this issue for a review of modeling studies on the same topics). Redox processes control the speciation of atmospheric Hg, and thus impart an important influence on Hg deposition, particularly during atmospheric mercury depletion events (AMDEs). Bromine radicals were identified as the primary oxidant of atmospheric Hg during AMDEs. Since the start of monitoring at Alert (NU) in 1995, the timing of peak AMDE occurrence has shifted to earlier times in the spring (from May to April) in recent years, and while AMDE frequency and GEM concentrations are correlated with local meteorological conditions, the reasons for this timing-shift are not understood. Mercury is subject to various post-depositional processes in snowpacks and a large portion of deposited oxidized Hg can be reemitted following photoreduction; how much Hg is deposited and reemitted depends on geographical location, meteorological, vegetative and sea-ice conditions, as well as snow chemistry. Halide anions in the snow can stabilize Hg, therefore it is expected that a smaller fraction of deposited Hg will be reemitted from coastal snowpacks. Atmospheric gaseous Hg concentrations have decreased in some parts of the Arctic (e.g., Alert) from 2000 to 2009 but at a rate that was less than that at lower latitudes. Despite numerous recent advances, a number of knowledge gaps remain, including uncertainties in the identification of oxidized Hg species in the air (and how this relates to dry vs. wet deposition), physical–chemical processes in air, snow and water—especially over sea ice—and the relationship between these processes and climate change.

Atmospheric mercury (Hg) is deposited to Polar Regions during springtime atmospheric mercury depletion events (AMDEs) that require halogens and snow or ice surfaces. The fate of this Hg during and following snowmelt is largely unknown. We measured Hg, major ions, and stable water isotopes from the snowpack through the entire spring melt runoff period for two years. Our small (2.5 ha) watershed is near Barrow (now Utqiaġvik), Alaska. We measured discharge, made 10 000 snow depths, and collected over 100 samples of snow and meltwater for chemical analysis in 2008 and 2009 from the watershed snowpack and ephemeral stream channel. Results show an "ionic pulse" of mercury and major ions in runoff during both snowmelt seasons, but major ion and Hg runoff concentrations were roughly 50% higher in 2008 than in 2009. Though total discharge as a percent of total watershed snowpack water equivalent prior to the melt was similar in both years (36% in 2008 melt runoff and 34% in 2009), it is possible that record low precipitation in the summer of 2007 led to the higher major ion and Hg concentrations in 2008 melt runoff. Total dissolved Hg meltwater runoff of 14.3 (± 0.7) mg/ha in 2008 and 8.1 (± 0.4) mg/ha in 2009 is five to seven times higher than that reported from other arctic watersheds. We calculate 78% of snowpack Hg was exported with snowmelt runoff in 2008 and 41% in 2009. Our results suggest AMDE Hg complexed with Cl

Mercury contamination in the Great Lakes continues to have important public health and wildlife ecotoxicology impacts, and atmospheric deposition is a significant ongoing loading pathway. The objective of this study was to estimate the amount and source-attribution for atmospheric mercury deposition to each lake, information needed to prioritize amelioration efforts. A new global, Eulerian version of the HYSPLIT-Hg model was used to simulate the 2005 global atmospheric transport and deposition of mercury to the Great Lakes. In addition to the base case, 10 alternative model configurations were used to examine sensitivity to uncertainties in atmospheric mercury chemistry and surface exchange. A novel atmospheric lifetime analysis was used to characterize fate and transport processes within the model. Model-estimated wet deposition and atmospheric concentrations of gaseous elemental mercury (Hg(0)) were generally within ∼10% of measurements in the Great Lakes region. The model overestimated non-Hg(0) concentrations by a factor of 2–3, similar to other modeling studies. Potential reasons for this disagreement include model inaccuracies, differences in atmospheric Hg fractions being compared, and the measurements being biased low. Lake Erie, downwind of significant local/regional emissions sources, was estimated by the model to be the most impacted by direct anthropogenic emissions (58% of the base case total deposition), while Lake Superior, with the fewest upwind local/regional sources, was the least impacted (27%). The U.S. was the largest national contributor, followed by China, contributing 25% and 6%, respectively, on average, for the Great Lakes. The contribution of U.S. direct anthropogenic emissions to total mercury deposition varied between 46% for the base case (with a range of 24–51% over all model configurations) for Lake Erie and 11% (range 6–13%) for Lake Superior. These results illustrate the importance of atmospheric chemistry, as well as emissions strength, speciation, and proximity, to the amount and source-attribution of mercury deposition.