A 50 year record for perfluoroalkyl acids in the high arctic: implications for global and local transport.

Perfluoroalkyl acids (PFAAs) are persistent compounds that are ubiquitous globally, though some uncertainties remain in the understanding of their long-range transport mechanisms. They are frequently detected in remote locations, where local sources may be unimportant. We collected a 16.

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.

Mercury deposition to lake sediments near historic gold mines in northern Canada.

Mercury (Hg) contamination in aquatic systems can lead to adverse human and environmental health outcomes. Yellowknife, a city in Canada's Northwest Territories, is a historic mining community, with two large gold mines (Giant Mine and Con Mine) that used Hg amalgamation methods to extract gold between ∼1938 and 1960. We analyzed dated sediment cores from 20 small lakes to investigate the spatial and temporal Hg deposition patterns within 50 km of Giant Mine.

Canadian high arctic ice core records of organophosphate flame retardants and plasticizers.

Organophosphate esters (OPEs) have been used as flame retardants, plasticizers, and anti-foaming agents over the past several decades. Of particular interest is the long range transport potential of OPEs given their ubiquitous detection in Arctic marine air. Here we report 19 OPE congeners in ice cores drilled on remote icefields and ice caps in the Canadian high Arctic.

Mercury at the top of the world: A 31-year record of mercury in Arctic char in the largest High Arctic lake, linked to atmospheric mercury concentrations and climate oscillations.

Lake Hazen, the largest lake north of the Arctic circle, is being impacted by mercury (Hg) pollution and climate change. The lake is inhabited by two morphotypes of land-locked Arctic char (Salvelinus alpinus), a sensitive indicator species for pollution and climatic impacts. The objectives of this study were to describe the trends in Hg concentration over time and to determine the relationship of climate to length-at-age and Hg concentrations in each char morphotype, as well as the relationship to atmospheric Hg measurements at a nearby monitoring station.

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.

Methylmercury Transport and Fate Shows Strong Seasonal and Spatial Variability along a High Arctic Freshwater Hydrologic Continuum.

The presence of toxic methylmercury (MeHg) in Arctic freshwater ecosystems and foodwebs is a potential health concern for northern Indigenous people. Addressing this issue requires a better understanding of MeHg production, fate during transport, and uptake into foodwebs. We used methylation assays and spatiotemporal surveys of MeHg concentrations, during the ice-covered and open water seasons, across a hydrologic continuum (composed of thaw seeps, lake/ponds, and a wetland) to identify Hg methylation hotspots and seasonal differences in MeHg cycling unique to Arctic ecosystems.

The tree-ring mercury record of Klondike gold mining at Bear Creek, central Yukon.

Use of elemental mercury (Hg) to enhance placer gold recovery is an effective method dating back centuries, but is associated with significant atmospheric Hg losses. This method was widely used in the Canadian Klondike region during most of the 20th century when the mining industry experienced rapid growth. While the health risks associated with Hg pollution are now well understood, few studies have assessed the environmental legacy of Hg use in the Klondike.

Contrasting the ecological effects of decreasing ice cover versus accelerated glacial melt on the High Arctic's largest lake.

Lake Hazen, the High Arctic's largest lake, has received an approximately 10-fold increase in glacial meltwater since its catchment glaciers shifted from net mass gain to net mass loss in 2007 common era (CE), concurrent with recent warming. Increased glacial meltwater can alter the ecological functioning of recipient aquatic ecosystems via changes to nutrient budgets, turbidity and thermal regimes. Here, we examine a rare set of five high-resolution sediment cores collected in Lake Hazen between 1990 and 2017 CE to investigate the influence of increased glacial meltwater versus alterations to lake ice phenology on ecological change.

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. ΣOPE concentrations in water of LH were lower than glacial rivers and its outflow, the Ruggles River.

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

Carbon dioxide (CO) 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 CO production, and transport large quantities of easily mobilized comminuted sediments available for carbonate and silicate weathering reactions that can consume atmospheric CO 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 CO 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 CO up to 42 km downstream of glaciers, and cumulatively transformed the High Arctic's most voluminous lake into an important CO sink.

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.

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.

Contemporary limnology of the rapidly changing glacierized watershed of the world's largest High Arctic lake.

Glacial runoff is predicted to increase in many parts of the Arctic with climate change, yet little is known about the biogeochemical impacts of meltwaters on downstream freshwater ecosystems. Here we document the contemporary limnology of the rapidly changing glacierized watershed of the world's largest High Arctic lake (Lake Hazen), where warming since 2007 has increased delivery of glacial meltwaters to the lake by up to 10-times. Annually, glacial meltwaters accounted for 62-98% of dissolved nutrient inputs to the lake, depending on the chemical species and year.

Characterization of perfluoroalkyl substances in sediment cores from High and Low Arctic lakes in Canada.

Perfluoroalkyl substances (PFASs) are synthetic environmentally-persistent pollutants that are amenable to long-range transport and accumulation in remote Arctic ecosystems. In this study, historical inventories of twenty-three PFASs (i.e.

Drivers of Mercury Cycling in the Rapidly Changing Glacierized Watershed of the High Arctic's Largest Lake by Volume (Lake Hazen, Nunavut, Canada).

Across the Arctic, glaciers are melting and permafrost is thawing at unprecedented rates, releasing not only water to downstream aquatic systems, but also contaminants like mercury, archived in ice over centuries. Using concentrations from samples collected over 4 years and calibrated modeled hydrology, we calculated methylmercury (MeHg) and total mercury (THg) mass balances for Lake Hazen, the world's largest High Arctic lake by volume, for 2015 and 2016. Glacial rivers were the most important source of MeHg and THg to Lake Hazen, accounting for up to 53% and 94% of the inputs, respectively.

400-Year Record of Atmospheric Mercury from Tree-Rings in Northwestern Canada.

Tree-rings are a promising high-resolution archive for gaseous atmospheric mercury (composed primarily of Hg) reconstruction, but the influence of cambial age (ring number from pith) and tree-specific differences are uncertainties with potential implications for interpreting tree-ring Hg signals. We address these uncertainties and reconstruct the last 400 years of Hg change using a tree-ring Hg data set from 20 white spruce ( Picea glauca) trees from a pristine site in central Yukon. Cambial age has no significant influence on tree-ring Hg concentration, but tree-specific differences in mean concentration are prevalent and must be normalized to a common mean to accurately constrain long-term trends in the mean tree-ring Hg record.

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.

Sources of Methylmercury to Snowpacks of the Alberta Oil Sands Region: A Study of In Situ Methylation and Particulates.

Snowpacks in the Alberta Oil Sands Region (AOSR) of Canada contain elevated loadings of methylmercury (MeHg; a neurotoxin that biomagnifies through foodwebs) due to oil sands related activities. At sites ranging from 0 to 134 km from the major AOSR upgrading facilities, we examined sources of MeHg by quantifying potential rates of MeHg production in snowpacks and melted snow using mercury stable isotope tracer experiments, as well as quantifying concentrations of MeHg on particles in snowpacks (pMeHg). At four sites, methylation rate constants were low in snowpacks (k = 0.

Importance of open marine waters to the enrichment of total mercury and monomethylmercury in lichens in the Canadian High Arctic.

Caribou, which rely on lichens as forage, are a dietary source of monomethylmercury (MMHg) to many of Canada's Arctic Aboriginal people. However, little is understood about the sources of MMHg to lichens in the High Arctic. We quantified MMHg, total mercury (THg) and other chemical parameters (e.

Atmospheric mercury in the Canadian Arctic. Part II: insight from modeling.

A review of mercury in the Canadian Arctic with a focus on field measurements is presented in part I (see Steffen et al., this issue). Here we provide insights into the dynamics of mercury in the Canadian Arctic from new and published mercury modeling studies using Environment Canada's mercury model.

Atmospheric mercury in the Canadian Arctic. Part I: a review of recent field measurements.

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).

Determination of monomethylmercury and dimethylmercury in the Arctic marine boundary layer.

Our understanding of the biogeochemical cycling of monomethylmercury (MMHg) in the Arctic is incomplete because atmospheric sources and sinks of MMHg are still unclear. We sampled air in the Canadian Arctic marine boundary layer to quantify, for the first time, atmospheric concentrations of methylated Hg species (both MMHg and dimethylmercury (DMHg)), and, estimate the importance of atmospheric deposition as a source of MMHg to Arctic land- and sea-scapes. Overall atmospheric MMHg and DMHg concentrations (mean ± SD) were 2.

Mercury in freshwater ecosystems of the Canadian Arctic: recent advances on its cycling and fate.

The Canadian Arctic has vast freshwater resources, and fish are important in the diet of many Northerners. Mercury is a contaminant of concern because of its potential toxicity and elevated bioaccumulation in some fish populations. Over the last decade, significant advances have been made in characterizing the cycling and fate of mercury in these freshwater environments.

Mercury in the marine environment of the Canadian Arctic: review of recent findings.

This review summarizes data and information which have been generated on mercury (Hg) in the marine environment of the Canadian Arctic since the previous Canadian Arctic Contaminants Assessment Report (CACAR) was released in 2003. Much new information has been collected on Hg concentrations in marine water, snow and ice in the Canadian Arctic. The first measurements of methylation rates in Arctic seawater indicate that the water column is an important site for Hg methylation.