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. Lake Hazen was a strong sink for NO3--NO2-, NH4+ and DOC, but a source of DIC to its outflow the Ruggles River. Most nutrients entering Lake Hazen were, however, particle-bound and directly transported well below the photic zone via dense turbidity currents, thus reinforcing ultraoligotrophy in the lake rather than overcoming it. For the first time, we apply the land-to-ocean aquatic continuum framework in a large glacierized Arctic watershed, and provide a detailed and holistic description of the physical, chemical and biological limnology of the rapidly changing Lake Hazen watershed. Our findings highlight the sensitivity of freshwater ecosystems to the changing cryosphere, with implications for future water quality and productivity at high latitudes.

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. However, due to the MeHg and THg being primarily particle-bound, Lake Hazen was an annual MeHg and THg sink. Exports of MeHg and THg out the Ruggles River outflow were consequently very low, but erosion and permafrost slumping downstream of the lake increased river MeHg and THg concentrations significantly before entering coastal waters in Chandler Fjord. Since 2001, glacial MeHg and THg inputs to Lake Hazen have increased by 0.01 and 0.400 kg yr-1, respectively, in step with dramatic increases in glacial melt. This study highlights the potential for increases in mercury inputs to arctic ecosystems downstream of glaciers despite recent reductions in global mercury emissions.

Mercury and cortisol in Western Hudson Bay polar bear hair.

Non-invasive methods of assessing animal health and life history are becoming increasingly popular in wildlife research; hair samples from polar bears (Ursus maritimus), are being used to study an ever broader range of anthropogenic and endocrine compounds. A number of contaminants are known to disrupt endocrine function in polar bears. However, the relationship between mercury and cortisol remains unknown, although mercury is an endocrine disruptor in other species. Here, we examine the relationship between concentrations of cortisol and total mercury (THg) analyzed in guard hair from 378 polar bears (184 females, 194 males) sampled in Western Hudson Bay, 2004-2012. The difference in mean cortisol concentration between female (0.8 ± 0.6 pg/mg) and male (0.7 ± 0.5 pg/mg) polar bears bordered on significance (p = 0.054). However, mean mercury concentration was significantly greater (p = 0.009) in females (4.7 ± 1.4 µg/g) than males (4.3 ± 1.2 µg/g). Hair cortisol in males was significantly influenced by mercury, age, and fatness, as well as interactions between mercury and year, mercury and fatness, and year and fatness (all: p < 0.03) (multiple regression analysis, whole model: r(2) = 0.14, F(7,185) = 4.43, p = 0.0001). Fatness was the only significant variable in the multiple regression analysis for females (r(2) = 0.06, F(1,182) = 13.0, p = 0.0004). In conclusion, a significant, but complex, relationship was found between mercury and cortisol concentrations in hair from male, but not female, polar bears.

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.g., marine and crustal elements, δ(13)C, δ(15)N, organic carbon, calcium carbonate) in lichen and soil samples collected along transects extending from the coast on Bathurst and Devon islands, Nunavut, to determine factors driving lichen MMHg and THg concentrations in the High Arctic. Lichen MMHg and THg concentrations ranged from 1.41 to 17.1 ng g(-1) and from 36.0 to 361 ng g(-1), respectively. Both were highly enriched over concentrations in underlying soils, indicating a predominately atmospheric source of Hg in lichens. However, MMHg and THg enrichment at coastal sites on Bathurst Island was far greater than on Devon Island. We suggest that this variability can be explained by the proximity of the Bathurst Island transect to several polynyas, which promote enhanced Hg deposition to adjacent landscapes through various biogeochemical processes. This study is the first to clearly show a strong marine influence on MMHg inputs to coastal terrestrial food webs with implications for MMHg accumulation in caribou and the health of the people who depend on them as part of a traditional diet.

Assessment of modeled mercury dry deposition over the Great Lakes region.

Three sets of model predicted values for speciated mercury concentrations and dry deposition fluxes over the Great Lakes region were assessed using field measurements and model intercomparisons. The model predicted values were produced by the Community Multiscale Air Quality Modeling System for the year 2002 (CMAQ2002) and for the year 2005 (CMAQ2005) and by the Global/Regional Atmospheric Heavy Metals Model for the year 2005 (GRAHM2005). Median values of the surface layer ambient concentration of gaseous elemental mercury (GEM) from all three models were generally within 30% of measurements. However, all three models overpredicted surface-layer concentrations of gaseous oxidized mercury (GOM) and particulate bound mercury (PBM) by a factor of 2-10 at the majority of the 15 monitoring locations. For dry deposition of GOM plus PBM, CMAQ2005 showed a clear gradient with the highest deposition in Pennsylvania and its surrounding areas while GRAHM2005 showed no such gradient in this region; however, GRAHM2005 had more hot spots than those of CMAQ2005. Predicted dry deposition of GOM plus PBM from these models should be treated as upper-end estimates over some land surfaces in this region based on the tendencies of all the models to overpredict GOM and PBM concentrations when compared to field measurements. Model predicted GEM dry deposition was found to be as important as GOM plus PBM dry deposition as a contributor to total dry deposition. Predicted total annual mercury dry deposition were mostly lower than 5 µg m(-2) to the surface of the Great lakes, between 5 and 15 µg m(-2) to the land surface north of the US/Canada border, and between 5 and 40 µg m(-2) to the land surface south of the US/Canada border. Predicted dry deposition from different models differed from each other by as much as a factor of 2 at regional scales and by a greater extent at local scales.

Nitrous oxide fluxes in three experimental boreal forest reservoirs.

Global atmospheric concentrations of nitrous oxide (N2O), a powerful greenhouse gas, continue to increase. While many sources and sinks have been identified, there is little known about how existing and newly constructed reservoirs, such as those created for hydroelectric production, impact current atmospheric N2O concentrations. We hypothesized that N2O fluxes to the atmosphere would increase because enhanced nutrient availability and increased soil respiration following the flooding of soils during reservoir creation would favor denitrification. Furthermore, we hypothesized that emissions would be linked to the amount of organic carbon contained in the flooded landscape. These hypotheses were tested by creating three experimental reservoirs over boreal upland subcatchments that ranged in the amount of organic carbon stored in soils and vegetation. Diffusive surface N2O fluxes within each reservoir were estimated using surface water concentrations of N2O and the thin boundary layer method. Surface fluxes ranged from -1.0 to -3.5 microg N2O m(-2) d(-1), and water column N2O concentrations indicated that contrary to expectations, the reservoirs were acting as slight sinks for atmospheric N2O. This net consumption of N2O was likely related to an excess of labile carbon and low concentrations of oxygen (O2) and nitrate (NO3-) in the flooded soils. Therefore, it is postulated that reservoir creation by flooding boreal soils will likely have little or no net effect of adding additional N2O to the current greenhouse gas (GHG) atmospheric burden, at least over the short term.

Importance of the forest canopy to fluxes of methyl mercury and total mercury to boreal ecosystems.

The forest canopy was an important contributor to fluxes of methyl mercury (MeHg) and total mercury (THg) to the forest floor of boreal uplands and wetlands and potentially to downstream lakes, at the Experimental Lakes Area (ELA), northwestern Ontario. The estimated fluxes of MeHg and THg in throughfall plus litterfall below the forest canopy were 2 and 3 times greater than annual fluxes by direct wet deposition of MeHg (0.9 mg of MeHg ha(-1)) and THg (71 mg of THg ha(-1)). Almost all of the increased flux of MeHg and THg under the forest canopy occurred as litterfall (0.14-1.3 mg of MeHg ha(-1) yr(-1) and 110-220 mg of THg ha(-1) yr(-1)). Throughfall added no MeHg and approximately 9 mg of THg ha(-1) yr(-1) to wet deposition at ELA, unlike in other regions of the world where atmospheric deposition was more heavily contaminated. These data suggest that dry deposition of Hg on foliage as an aerosol or reactive gaseous Hg (RGM) species is low at ELA, a finding supported by preliminary measurements of RGM there. Annual total deposition from throughfall and litterfall under a fire-regenerated 19-yr-old jack pine/birch forest was 1.7 mg of MeHg ha(-1) and 200 mg of THg ha(-1). We found that average annual accumulation of MeHg and THg in the surficial litter/fungal layer of soils since the last forest fire varied between 0.6 and 1.6 mg of MeHg ha(-1) and between 130 and 590 mg of THg ha(-1) among sites differing in drainage and soil moisture. When soil Hg accumulation sites were matched with similar sites where litterfall and throughfall were collected, measured fluxes of THg to the forest floor (sources) were similar to our estimates of longterm soil accumulation rates (sinks), suggesting that the Hg in litterfall and throughfall is a new and not a recycled input of Hg to forested ecosystems. However, further research is required to determine the proportion of Hg in litterfall that is being biogeochemically recycled within forest and wetland ecosystems and, thus, does not represent new inputs to the forest ecosystem.

The effects of experimental reservoir creation on the bioaccumulation of methylmercury and reproductive success of tree swallows (Tachycineta bicolor).

Reservoir creation results in decomposition of flooded organic matter and increased rates of mercury methylation. Methylmercury (MeHg), the most toxic form of mercury, bioaccumulates through aquatic food webs. Our objective was to quantify the transfer of MeHg from aquatic food webs into terrestrial organisms. We examined rates of MeHg bioaccumulation in an insectivorous songbird, the tree swallow, breeding near an experimentally created reservoir. We also determined the impact of flooding and MeHg bioaccumulation on the reproductive success of these birds. Mean MeHg burdens in nestling swallows from near the experimental reservoir increased from 1,210 +/- 150 ng before flooding to 2,200 +/- 102 ng after flooding. Postflood MeHg concentrations in both the body and feathers of the birds were significantly greater than preflood MeHg concentrations. Although MeHg burdens in swallows were elevated in postflood years, we found no overt toxicological affects. An increase in dipteran productivity (the primary food source of tree swallows) after reservoir creation resulted in earlier nest initiation, larger eggs, and faster growth rates of wing and bill length in nestlings raised during postflood years.