Winter Dust Storms Impact the Physical and Biogeochemical Functioning of a Large High Arctic Lake.

We found that a winter of abnormally low snowfall and numerous dust storms from eolian processes acting on exposed landscapes (including a major 4-day dust storm while onsite in May 2014) caused a cascade of impacts on the physical, chemical, and ecological functioning of the largest lake by volume in the High Arctic (Lake Hazen; Nunavut, Canada). MODIS imagery revealed that dust deposited in snowpacks on the lake's ice acted as light-absorbing impurities (LAIs), reducing surface reflectance and increasing surface temperatures relative to normal snowpack years, causing early snowmelt and drainage of meltwaters into the lake. LAIs remaining on the ice surface melted into the ice, causing premature candling and one of the earliest ice-offs and longest ice-free seasons on record for Lake Hazen. Meltwater inputs from snowpacks resulted in dilution of dissolved, and increased concentration of particulate bound, chemical species in Lake Hazen's upper water column. Spring inputs of nutrients increased both heterotrophy and algal productivity under the surface ice following snowmelt, with a net consumption of dissolved oxygen. As climate change continues to alter High Arctic temperatures and precipitation patterns, we can expect further changes in dust storm frequency and severity with corresponding impacts for freshwater ecosystems.

Investigation of perfluoroalkyl substances in proglacial rivers and permafrost seep in a high Arctic watershed.

We measured perfluoroalkyl substances (PFAS) in proglacial rivers and along a non-glacial freshwater continuum to investigate the role of snow and ice melting in their transport and fate within the Lake Hazen watershed (82° N). PFAS concentrations in glacial rivers were higher than those in surface waters of Lake Hazen, suggesting melting glacial ice increased PFAS concentrations in the lake. Stream water derived from subsurface soils along a non-glacial (permafrost thaw and snowmelt) freshwater continuum was a source of PFAS to Lake Hazen. Lower concentrations were found downstream of a meadow wetland relative to upstream locations along the continuum, suggesting PFAS partitioning into vegetation and soil as water flowed downstream towards Lake Hazen. Our estimations indicate that total PFAS inputs from glacial rivers and snowmelt were 1.6 kg (78%) and 0.44 kg (22%), respectively, into Lake Hazen, totalling 2.04 kg, and the output of PFAS from Lake Hazen was 0.64 kg. A positive net annual change of 1.4 kg indicates PFAS had notable residence times and/or net storage in Lake Hazen.

Warming Climate Is Reducing the Diversity of Dominant Microbes in the Largest High Arctic Lake.

Temperatures in the Arctic are expected to increase dramatically over the next century, and transform high latitude watersheds. However, little is known about how microbial communities and their underlying metabolic processes will be affected by these environmental changes in freshwater sedimentary systems. To address this knowledge gap, we analyzed sediments from Lake Hazen, NU Canada. Here, we exploit the spatial heterogeneity created by varying runoff regimes across the watershed of this uniquely large high-latitude lake to test how a transition from low to high runoff, used as one proxy for climate change, affects the community structure and functional potential of dominant microbes. Based on metagenomic analyses of lake sediments along these spatial gradients, we show that increasing runoff leads to a decrease in taxonomic and functional diversity of sediment microbes. Our findings are likely to apply to other, smaller, glacierized watersheds typical of polar or high latitude ecosystems; we can predict that such changes will have far reaching consequences on these ecosystems by affecting nutrient biogeochemical cycling, the direction and magnitude of which are yet to be determined.

Glacial Melt Inputs of Organophosphate Ester Flame Retardants to the Largest High Arctic Lake.

Organophosphate esters (OPEs) have been detected in the Arctic environment, but the influence of glacial melt on the environmental behavior of OPEs in recipient Arctic aquatic ecosystems is still unknown. In this study, water samples were collected from Lake Hazen (LH) and its tributaries to investigate the distribution of 14 OPEs in LH and to explore the input of OPEs from glacial rivers to LH and the output of OPEs from LH in 2015 and 2018. Σ14OPE concentrations in water of LH were lower than glacial rivers and its outflow, the Ruggles River. In 2015, a high melt year, we estimated that glacial rivers contributed 7.0 ± 3.2 kg OPEs to LH, compared to a 16.5 ± 0.3 kg OPEs output by the Ruggles River, suggesting that residence time and/or additional inputs via direct wet and dry deposition and permafrost melt likely result in OPE retention in the LH watershed. In 2018, a lower melt year, Σ14OPE concentrations in glacial rivers were much lower, indicating that the rate of glacier melt may govern, in part, the concentrations of OPEs in the tributaries of LH. This study highlights long-range transport of OPEs, their deposition in Arctic glaciers, landscapes, and lakes.

The use of hair as a proxy for total and methylmercury burdens in polar bear muscle tissue.

Polar bears (Ursus maritimus) are an ecologically important species in the Arctic, whose health, and that of the people whose livelihoods depend on them, are increasingly affected by climate change and the bioaccumulation of contaminants such as mercury (Hg). Although methylmercury (MeHg) is the toxic form of Hg that biomagnifies up food webs, risk assessment studies typically only report on total Hg (THg) concentrations because it is cheaper to quantify. Furthermore, hair is commonly analysed for THg in polar bear as well as human risk assessment studies because it is relatively non-invasive to collect, yet we know little of how THg and MeHg concentrations differ between hair and muscle tissues. In this study, we quantified THg and MeHg concentrations in hair and muscle from 44 polar bears (24 sub-adults: 9 females, 15 males; 18 adults: 5 females, 13 males, and 2 males of unknown age group), harvested in 2015 and 2016 from four subpopulations in Nunavut, Canada (Davis Strait, n = 3; Gulf of Boothia, n = 8; Baffin Bay, n = 15; Foxe Basin, n = 18). We found only moderately positive correlations (0.4 ≤ r ≤ 0.5) between THg concentrations in hair and THg and MeHg concentrations in muscle. Further, 75% and 88% of THg was MeHg in hair and muscle, respectively. High concentrations of THg in hair - 71% of the samples were above the suggested neurochemical no observed effect level for polar bears - suggest some of the bears may be adversely affected by Hg-related health effects. Despite this, all MeHg concentrations in muscle (0.1 to 0.4 mg/kg (wet weight, ww)) were below the consumption maximum Hg concentration of 0.5 mg/kg (ww) set by Canadian health authorities.

Fate and Transport of Perfluoroalkyl Substances from Snowpacks into a Lake in the High Arctic of Canada.

The delivery of perfluoroalkyl substances (PFAS) from snowpacks into Lake Hazen, located on Ellesmere Island (Nunavut, Canada, 82° N) indicates that annual atmospheric deposition is a major source of PFAS that undergo complex cycling in the High Arctic. Perfluoroalkyl carboxylic acids (PFCA) in snowpacks display odd-even concentration ratios characteristic of long-range atmospheric transport and oxidation of volatile precursors. Major ion analysis in snowpacks suggests that sea spray, mineral dust, and combustion aerosol are all relevant to the fate of PFAS in the Lake Hazen watershed. Distinct drifts of light and dark snow (enriched with light absorbing particles, LAPs) facilitate the study of particle loads on the fate of PFAS in the snowpack. Total PFAS (ΣPFAS, ng m-2) loads are lower in snowpacks enriched with LAPs and are attributed to reductions in snowpack albedo combined with enhanced post-depositional melting. Elevated concentrations of PFCA are observed in the top 5 m of the water column during snowmelt periods compared to ice-covered or ice-free periods. PFAS concentrations in deep waters of the Lake Hazen water column were consistent between snowmelt, ice-free, and ice-covered periods, which is ascribed to the delivery of dense and turbid glacier meltwaters mixing PFAS throughout the Lake Hazen water column. These observations highlight the underlying mechanisms in PFAS cycling in High Arctic Lakes particularly in the context of increased particle loads and melting.

Proglacial freshwaters are significant and previously unrecognized sinks of atmospheric CO2.

Carbon dioxide (CO2) emissions from freshwater ecosystems are almost universally predicted to increase with climate warming. Glacier-fed rivers and lakes, however, differ critically from those in nonglacierized catchments in that they receive little terrestrial input of organic matter for decomposition and CO2 production, and transport large quantities of easily mobilized comminuted sediments available for carbonate and silicate weathering reactions that can consume atmospheric CO2 We used a whole-watershed approach, integrating concepts from glaciology and limnology, to conclusively show that certain glacier-fed freshwater ecosystems are important and previously overlooked annual CO2 sinks due to the overwhelming influence of these weathering reactions. Using the glacierized Lake Hazen watershed (Nunavut, Canada, 82°N) as a model system, we found that weathering reactions in the glacial rivers actively consumed CO2 up to 42 km downstream of glaciers, and cumulatively transformed the High Arctic's most voluminous lake into an important CO2 sink. In conjunction with data collected at other proglacial freshwater sites in Greenland and the Canadian Rockies, we suggest that CO2 consumption in proglacial freshwaters due to glacial melt-enhanced weathering is likely a globally relevant phenomenon, with potentially important implications for regional annual carbon budgets in glacierized watersheds.

Atmospheric Concentrations and Wet/Dry Loadings of Mercury at the Remote Experimental Lakes Area, Northwestern Ontario, Canada.

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.

Tailings ponds of the Athabasca Oil Sands Region, Alberta, Canada, are likely not significant sources of total mercury and methylmercury to nearby ground and surface waters.

Tailings ponds created during industrial bitumen extraction from the Athabasca Oil Sands Region (AOSR), Alberta, Canada, have been shown to contain numerous contaminants, such as polycyclic aromatic compounds and naphthenic acids, and to slowly leak into adjacent ground and surface waters. Despite elevated concentrations of total mercury (THg) in nearby Athabasca River waters downstream of the AOSR developments, to date there are no published studies of THg or methylmercury (MeHg; a potent neurotoxin) in the AOSR tailings ponds. Here we present concentrations of THg and MeHg, as well as various water chemistry parameters, within four AOSR tailings ponds. Concentrations of SO42-, NH3, Na, and Cl were elevated in tailings ponds relative to nearby freshwaters. Surface water concentrations of THg (filtered: 0.15-0.57 ng/L) and MeHg (unfiltered: <0.02-0.53 ng/L; filtered: <0.02-0.32 ng/L), though, were generally low in the tailings ponds, with the highest concentrations observed in the oldest pond. In the mature fine tailings that settle out in the ponds, concentrations of THg (37.0-197 ng/g) and MeHg (0.10-0.52 ng/g) were also low, with the highest concentrations again in the oldest pond. We calculated that if all the dissolved THg and MeHg potentially leaking annually from the tailings ponds entered the nearby Athabasca River, river THg and MeHg concentrations would increase by only 0.01% and 0.03%, respectively. Overall, these ponds are likely not significant sources of THg or MeHg to nearby ground and surface waters, although due to the potential for Hg methylation to occur in the ponds themselves, other tailings ponds in the AOSR should be monitored to ensure that concentrations of MeHg in them are also low.

Unprecedented Increases in Total and Methyl Mercury Concentrations Downstream of Retrogressive Thaw Slumps in the Western Canadian Arctic.

Retrogressive thaw slumps (RTSs) are thermokarst features created by the rapid thaw of ice-rich permafrost, and can mobilize vast quantities of sediments and solutes downstream. However, the effect of slumping on downstream concentrations and yields of total mercury (THg) and methylmercury (MeHg) is unknown. Fluvial concentrations of THg and MeHg downstream of RTSs on the Peel Plateau (Northwest Territories, Canada) were up to 2 orders of magnitude higher than upstream, reaching concentrations of 1,270 ng L-1 and 7 ng L-1, respectively, the highest ever measured in uncontaminated sites in Canada. MeHg concentrations were particularly elevated at sites downstream of RTSs where debris tongues dammed streams to form reservoirs where microbial Hg methylation was likely enhanced. However, > 95% of the Hg downstream was typically particle-bound and potentially not readily bioavailable. Mean open-water season yields of THg (610 mg km-2 d-1) and MeHg (2.61 mg km-2 d-1) downstream of RTSs were up to an order of magnitude higher than those for the nearby large Yukon, Mackenzie and Peel rivers. We estimate that ∼5% of the Hg stored for centuries or millennia in northern permafrost soils (88 Gg) is susceptible to release into modern-day Hg biogeochemical cycling from further climate changes and thermokarst formation.

Physicochemical Drivers of Microbial Community Structure in Sediments of Lake Hazen, Nunavut, Canada.

The Arctic is undergoing rapid environmental change, potentially affecting the physicochemical constraints of microbial communities that play a large role in both carbon and nutrient cycling in lacustrine environments. However, the microbial communities in such Arctic environments have seldom been studied, and the drivers of their composition are poorly characterized. To address these gaps, we surveyed the biologically active surface sediments in Lake Hazen, the largest lake by volume north of the Arctic Circle, and a small lake and shoreline pond in its watershed. High-throughput amplicon sequencing of the 16S rRNA gene uncovered a community dominated by Proteobacteria, Bacteroidetes, and Chloroflexi, similar to those found in other cold and oligotrophic lake sediments. We also show that the microbial community structure in this Arctic polar desert is shaped by pH and redox gradients. This study lays the groundwork for predicting how sediment microbial communities in the Arctic could respond as climate change proceeds to alter their physicochemical constraints.

The world's largest High Arctic lake responds rapidly to climate warming.

Using a whole-watershed approach and a combination of historical, contemporary, modeled and paleolimnological datasets, we show that the High Arctic's largest lake by volume (Lake Hazen) has succumbed to climate warming with only a ~1 °C relative increase in summer air temperatures. This warming deepened the soil active layer and triggered large mass losses from the watershed's glaciers, resulting in a ~10 times increase in delivery of glacial meltwaters, sediment, organic carbon and legacy contaminants to Lake Hazen, a >70% decrease in lake water residence time, and near certainty of summer ice-free conditions. Concomitantly, the community assemblage of diatom primary producers in the lake shifted dramatically with declining ice cover, from shoreline benthic to open-water planktonic species, and the physiological condition of the only fish species in the lake, Arctic Char, declined significantly. Collectively, these changes place Lake Hazen in a biogeochemical, limnological and ecological regime unprecedented within the past ~300 years.