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Critical loads (CLs) are frequently used to quantify terrestrial ecosystem impacts from nitrogen (N) deposition using ecological responses such as the growth and mortality of tree species. Typically, CLs are reported as a single value, with uncertainty, for an indicator across a species' entire range. Mediating factors such as climate and soil conditions can influence species' sensitivity to N, but the magnitudes of these effects are rarely calculated explicitly. Here, we quantify the spatial variability and estimation error in N CLs for the growth and survival of 10 different tree species while accounting for key environmental factors that mediate species sensitivity to N (e.g., soil characteristics). We used a bootstrapped machine learning approach to determine the level of N deposition at which a 1% decrease occurs in growth rate or survival probability at forest plot locations across the United States. We found minimal differences (<5 kg N ha -1 year -1 ) when comparing a single species' CLs across climatic regimes but found considerable variability in species' local N CLs (>8.5 kg N ha -1 year -1 ) within these regimes. We also evaluated the most important factors for predicting tree growth rates and mortality and found that climate, competition, and air pollution generally have the greatest influence on growth rates and survival probability. Lastly, we developed a new probability of exceedance metric for each species and found high likelihoods of exceedance across large portions (46%) of some species' ranges. Our analysis demonstrates that machine learning approaches provide a unique capability to: (1) quantify mediating factor influences on N sensitivity of trees, (2) estimate the error in local N CL estimates, and (3) generate localized N CLs with probabilities of exceedance for tree species., Competing Interests: CONFLICT OF INTEREST STATEMENT The authors declare no conflicts of interest.

Mercury (Hg) inputs have particularly impacted the northeastern United States due to its proximity to anthropogenic emissions sources and abundant habitats that efficiently convert inorganic Hg into methylmercury. Intensive research and monitoring efforts over the past 50 years in New York State, USA, have informed the assessment of the extent and impacts of Hg exposure on fishes and wildlife. By synthesizing Hg data statewide, this study quantified temporal trends of Hg exposure, spatiotemporal patterns of risk, the role that habitat and Hg deposition play in producing spatial patterns of Hg exposure in fish and other wildlife, and the effectiveness of current monitoring approaches in describing Hg trends. Most temporal trends were stable, but we found significant declines in Hg exposure over time in some long-sampled fish. The Adirondack Mountains and Long Island showed the greatest number of aquatic and terrestrial species with elevated Hg concentrations, reflecting an unequal distribution of exposure risk to fauna across the state. Persistent hotspots were detected for aquatic species in central New York and the Adirondack Mountains. Elevated Hg concentrations were associated with open water, forests, and rural, developed habitats for aquatic species, and open water and forested habitats for terrestrial species. Areas of consistently elevated Hg were found in areas driven by atmospheric and local Hg inputs, and habitat played a significant role in translating those inputs into biotic exposure. Continued long-term monitoring will be important in evaluating how these patterns continue to change in the face of changing land cover, climate, and Hg emissions., (© 2023. The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature.)

Ongoing salinization and alkalinization in U.S. rivers have been attributed to inputs of road salt and effects of human-accelerated weathering in previous studies. Salinization poses a severe threat to human and ecosystem health, while human derived alkalinization implies increasing uncertainty in the dynamics of terrestrial sequestration of atmospheric carbon dioxide. A mechanistic understanding of whether and how human activities accelerate weathering and contribute to the geochemical changes in U.S. rivers is lacking. To address this uncertainty, we compiled dissolved sodium (salinity proxy) and alkalinity values along with 32 watershed properties ranging from hydrology, climate, geomorphology, geology, soil chemistry, land use, and land cover for 226 river monitoring sites across the coterminous U.S. Using these data, we built two machine-learning models to predict monthly-aggregated sodium and alkalinity fluxes at these sites. The sodium-prediction model detected human activities (represented by population density and impervious surface area) as major contributors to the salinity of U.S. rivers. In contrast, the alkalinity-prediction model identified natural processes as predominantly contributing to variation in riverine alkalinity flux, including runoff, carbonate sediment or siliciclastic sediment, soil pH and soil moisture. Unlike prior studies, our analysis suggests that the alkalinization in U.S. rivers is largely governed by local climatic and hydrogeological conditions., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

Critical loads (CLs) and target loads (TLs) of atmospheric deposition of sulfur (S) and nitrogen (N) specify the thresholds of air pollution above which damage to ecosystems is expected to occur and are used to inform environmental regulation and natural resource management. Model estimates of CL and TL can vary for a given location, and these differences can be important for characterization of ecosystem effects from elevated S and N deposition. Moreover, TLs are used to evaluate associated timeframes of ecosystem recovery. We compared published CLs and TLs based on soil acidity criteria derived from steady-state versus dynamic models for terrestrial ecosystems. We examined the magnitude of differences in the CL/TL results from the two types of models for the same regions in the Eastern U.S. Results showed that CLs/TLs from dynamic models (or from steady state modeling using soil base cation weathering estimates from dynamic models) generally produce a broader range of values of acid-sensitivity, including lower CLs/TLs, as compared with a steady-state approach. Applications of dynamic biogeochemical models capable of developing CLs/TLs are relatively data intensive and typically limited to locations where measured soil and soil solution (or nearby stream water) chemistry are available for model parameterization, calibration, and testing. We recommend that CLs/TLs derived from dynamic models be used, where data permit, as they are likely more accurate and allow for evaluation of time-dependent phenomena and period needed for recovery. However, CLs derived from steady-state models remain a useful tool for understanding broad spatial patterns in soil acid-sensitivity throughout the U.S. Future work should focus on the development of more reliable model input parameters, particularly soil base cation weathering, and the extent to which CLs and TLs at a given location may vary and be altered with anticipated future climate change. In addition, dynamic models could be further developed to estimate CLs/TLs for nutrient N., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022. Published by Elsevier Ltd.)

Critical loads (CLs) of atmospheric deposition for nitrogen (N) and sulfur (S) are used to support decision making related to air regulation and land management. Frequently, CLs are calculated using empirical methods, and the certainty of the results depends on accurate representation of underlying ecological processes. Machine learning (ML) models perform well in empirical modeling of processes with non-linear characteristics and significant variable interactions. We used bootstrap ensemble ML methods to develop CL estimates and assess uncertainties of CLs for the growth and survival of 108 tree species in the conterminous United States. We trained ML models to predict tree growth and survival and characterize the relationship between deposition and tree species response. Using four statistical methods, we quantified the uncertainty of CLs in 95 % confidence intervals (CI). At the lower bound of the CL uncertainty estimate, 80 % or more of tree species have been impacted by nitrogen deposition exceeding a CL for tree survival over >50 % of the species range, while at the upper bound the percentage is much lower (<20 % of tree species impacted across >60 % of the species range). Our analysis shows that bootstrap ensemble ML can be effectively used to quantify critical loads and their uncertainties. The range of the uncertainty we calculated is sufficiently large to warrant consideration in management and regulatory decision making with respect to atmospheric deposition., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 The Authors. Published by Elsevier B.V. All rights reserved.)

In this article marking the 40th anniversary of the US National Science Foundation's Long Term Ecological Research (LTER) Network, we describe how a long-term ecological research perspective facilitates insights into an ecosystem's response to climate change. At all 28 LTER sites, from the Arctic to Antarctica, air temperature and moisture variability have increased since 1930, with increased disturbance frequency and severity and unprecedented disturbance types. LTER research documents the responses to these changes, including altered primary production, enhanced cycling of organic and inorganic matter, and changes in populations and communities. Although some responses are shared among diverse ecosystems, most are unique, involving region-specific drivers of change, interactions among multiple climate change drivers, and interactions with other human activities. Ecosystem responses to climate change are just beginning to emerge, and as climate change accelerates, long-term ecological research is crucial to understand, mitigate, and adapt to ecosystem responses to climate change., (© The Author(s) 2022. Published by Oxford University Press on behalf of the American Institute of Biological Sciences.)

Federal policy changes in the management of carbon emissions from power plants offer a potent real-world example for examining air-land-water interactions and their implications for coastal water quality. We integrate models of energy (Integrated Planning Model (IPM)), air quality (Community Multiscale Air Quality (CMAQ) and water quality (SPAtially Referenced Regression On Watershed attributes (SPARROW)) to investigate the potential water quality impacts of policy-driven changes in total nitrogen deposition in watersheds draining to US coastal areas. We estimate the combined effects of three recently proposed energy policy scenarios, population growth, and climate change. We decompose the combined effects into the roles of the individual components on the supply of riverine nitrogen for the entire US and eight coastal regions. We find that population growth is the most important driver of changes in coastal nitrogen flux. Energy policies play a minor role in offsetting the negative effects of population growth, although the effect varies by energy policy and region. The greatest population and policy effects are projected for the Gulf of Mexico. Given limited reductions in nitrogen emissions and deposition associated with energy policies, the net effect of policy and population changes is an increase in total nitrogen flux to all estuaries relative to the 2010 baseline. While population growth increases flux, and energy policies decrease flux in all regions, climate change can either increase or decrease flux depending on the region. That is because the relatively large individual effects of temperature and precipitation on watershed nitrogen processes work in opposing directions. The net result of the offsetting nature of individual climate processes varies in both magnitude and direction by coastal region. Further research is needed to sort out individual temperature and precipitation effects in different regions., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier B.V. All rights reserved.)

Photochemical and microbial processing are the prevailing mechanisms that shape the composition and reactivity of dissolved organic matter (DOM); however, prior research has not comparatively evaluated the impacts of these processes on the photoproduction of reactive intermediates (RIs) from freshly sourced terrestrial DOM. We performed controlled irradiation and incubation experiments with leaf and soil samples collected from an acid-impacted lake watershed in the Adirondack Mountain region of New York to examine the effects of DOM processing on the apparent quantum yields of RIs (Φ app,RI ), including excited triplet states of DOM ( 3 DOM*), singlet oxygen ( 1 O 2 ), and hydroxyl radicals ( • OH). Photodegradation led to net reductions in Φ app, 1 O 2 , Φ app, 3 DOM* , and Φ app, • OH , whereas (photo-)biodegradation resulted in increases in Φ app, 1 O 2 and Φ app, 3 DOM* . Photodegradation and (photo-)biodegradation also shifted the energy distribution of 3 DOM* in different directions. Multivariate statistical analyses revealed the potential relevance of photo-biodegradation in driving changes in Φ app, 1 O 2 and Φ app, 3 DOM* and prioritized five bulk DOM optical and redox properties that best explained the variations in Φ app, 1 O 2 and Φ app, 3 DOM* along the watershed terrestrial-aquatic continuum. Our findings highlight the contrasting impacts of photochemical and microbial processes on the photoreactivity of freshly sourced terrestrial DOM and invite further studies to develop a more holistic understanding of their implications for aquatic photochemistry.

Mercury emissions from artisanal and small-scale gold mining throughout the Global South exceed coal combustion as the largest global source of mercury. We examined mercury deposition and storage in an area of the Peruvian Amazon heavily impacted by artisanal gold mining. Intact forests in the Peruvian Amazon near gold mining receive extremely high inputs of mercury and experience elevated total mercury and methylmercury in the atmosphere, canopy foliage, and soils. Here we show for the first time that an intact forest canopy near artisanal gold mining intercepts large amounts of particulate and gaseous mercury, at a rate proportional with total leaf area. We document substantial mercury accumulation in soils, biomass, and resident songbirds in some of the Amazon's most protected and biodiverse areas, raising important questions about how mercury pollution may constrain modern and future conservation efforts in these tropical ecosystems., (© 2022. The Author(s).)

Modeling studies project that in the future surface waters in the northeast US will continue to recover from acidification over decades following reductions in atmospheric sulfur dioxide and nitrogen oxides emissions. However, these studies generally assume stationary climatic conditions over the simulation period and ignore the linkages between soil and surface water recovery from acid deposition and changing climate, despite fundamental impacts to watershed processes and comparable time scales for both phenomena. In this study, the integrated biogeochemical model PnET-BGC was applied to two montane forest watersheds in the Adirondack region of New York, USA to evaluate the recovery of surface waters from historical acidification in response to possible future changes in climate and atmospheric sulfur and nitrogen deposition. Statistically downscaled climate scenarios on average project warmer temperatures and greater precipitation for the Adirondack by the end of the century. Model simulations suggest under constant climate, acid-sensitive Buck Creek would gain 12.8 μeq L -1 of acid neutralizing capacity (ANC) by 2100 from large reductions in deposition, whereas acid insensitive Archer Creek is projected to gain 7.9 μeq L -1 of ANC. However, climate change could limit those improvements in acid-base status. Under climate change, a negative offset relative to the ANC increases with no climate change are projected for both streams by 2100. In acid-insensitive Archer Creek the negative offset (-8.5 μeq L -1 ) was large enough that ANC is projected to decrease by -0.6 μeq L -1 , whereas in acid-sensitive Buck Creek, the negative offset (-0.4 μeq L -1 ) resulted in a slight decline of the projected future ANC increase to 12.4 μeq L -1 . Calculated target loads for 2150 for both sites decreased when future climate change was considered in model simulations, which suggests further reductions in acid deposition may be necessary to restore ecosystem structure and function under a changing climate., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier B.V. All rights reserved.)

Acidic deposition contributes to a range of environmental impacts across forested landscapes, including acidification of soil and drainage water, toxic aluminum mobilization, depletion of available soil nutrient cations, and impacts to forest and aquatic species health and biodiversity. In response to decreasing levels of acidic deposition, soils and drainage waters in some regions of North America have become gradually less acidic. Thresholds of atmospheric deposition at which adverse ecological effects are manifested are called critical loads (CLs) and/or target loads (TLs). Target loads are developed based on approaches that account for spatial and temporal aspects of acidification and recovery. Exceedance represents the extent to which current or projected future levels of acidic deposition exceed the level expected to cause ecological harm. We report TLs of sulfur (S) and nitrogen (N) deposition and the potential for ecosystem recovery of watershed soils and streams in the Adirondack region of New York State, resources that have been less thoroughly investigated than lakes. Regional TLs were calculated by statistical extrapolation of hindcast and forecast simulations of 25 watersheds using the process-based model PnET-BGC coupled with empirical observations of stream hydrology and established sensitivity of sugar maple (Acer saccharum) to soil base saturation and brook trout (Salvelinus fontinalis) to stream acid neutralizing capacity (ANC). Historical impacts and the expected recovery timeline of regional soil and stream chemistry and fish community condition within the Adirondack Park were evaluated. Analysis suggests that many low-order Adirondack streams and associated watershed soils have low TLs (<40 meq/m 2 /yr of N + S deposition) to achieve specified benchmarks for recovery of soil base saturation or stream ANC. Acid-sensitive headwater and low-order streams and watershed soils in the region are expected to experience continued adverse effects from N and S deposition well into the future even under aggressive emissions reductions. Watershed soils and streams in the western Adirondack Park are particularly vulnerable to acidic deposition and currently in exceedance of TLs. The methods used for linking statistical and process-based models to consider chemical and biological response under varying flow conditions at the regional scale in this study can be applied to other areas of concern., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

Process ecosystem models are useful tools to provide insight on complex, dynamic ecological systems, and their response to disturbances. The biogeochemical model PnET-BGC was modified and tested using field observations from an experimentally whole-tree harvested northern hardwood watershed (W5) at the Hubbard Brook Experimental Forest (HBEF), New Hampshire, USA. In this study, the confirmed model was used as a heuristic tool to investigate long-term changes in hydrology, biomass accumulation, and soil solution and stream water chemistry for three different watershed cutting intensities (40%, 60%, 80%) and three rotation lengths (30, 60, 90 years) under both constant (current climate) and changing (MIROC5-RCP4.5) future climate scenarios and atmospheric CO 2 through the year 2200. For the no future cutting scenario, total ecosystem stored carbon (i.e., sum of aboveground biomass, woody debris and soil) reached a maximum value of 207 t C ha -1 under constant climate but increased to 452 t C ha -1 under changing climate in 2200 due to a CO 2 fertilization effect. Harvesting of trees decreased total ecosystem stored carbon between 7 and 36% for constant climate and 7-60% under changing climate, respectively, with greater reductions for shorter logging rotation lengths and greater watershed cutting intensities. Harvesting under climate change resulted in noticeable losses of soil organic matter (12-56%) coinciding with loss of soil nutrients primarily due to higher rates of soil mineralization associated with increases in temperature, compared with constant climate conditions (3-22%). Cumulative stream leaching of nitrate under climate change (181-513 kg N ha -1 ) exceeded constant climate values (139-391 kg N ha -1 ) for the various cutting regimes. Under both climate conditions the model projected greater sensitivity to varying the length of cutting period than cutting intensities. Hypothetical model simulations highlight future challenges in maintaining long-term productivity of managed forests under changing climate due to a potential for a deterioration of soil fertility., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier B.V. All rights reserved.)

Solid-gas-water phase partitioning of mercury (Hg) and the processes governing its diffusivity within soils are poorly studied. In this study, landscape and forest species dependences of gaseous elemental Hg (Hg(0)) in soil profiles (0-50 cm) were investigated over four seasons in eight subtropical (130 days) and temperate (96 days) forest plots. The vertical soil pore Hg(0) concentrations differed between subtropical (Masson pine, broad-leaved forest, and open field) and temperate (Chinese pine, larch, mixed broad-leaf forests, and open field) catchments, with annual averages ranging from 6.73 to 15.8 and 0.95 to 2.08 ng m -3 , respectively. The highest Hg(0) concentrations in soil gas consistently occurred in the upper mineral or organic horizons, indicating immobilization of Hg(0) in mineral soils. A strongly positive relationship between pore Hg(0) concentrations and ratios of Hg to organic matter (SOM) in soils suggests that the vertical distribution of Hg(0) is related to soil Hg(0) formation by Hg(II) reduction and sorption to SOM. Temperature was also an important driver of Hg(0) production in soil pores. Based on measurements of soil-air Hg(0) exchange, diffusion coefficients ( D s ) of Hg(0) between soil and atmosphere were calculated for field sites, providing a foundation for future development and validation of terrestrial Hg models.

Acid deposition has declined across eastern North America and northern Europe due to reduced emissions of sulfur and nitrogen oxides. Ecosystem recovery has been slow with limited improvement in surface water chemistry. Delayed recovery has encouraged acid-neutralization strategies to accelerate recovery of impaired biological communities. Lime application has been shown to increase pH and dissolved organic carbon (DOC), which could also drive increased mobilization of mercury (Hg) to surface waters. A four-year study was conducted within Honnedaga Lake's watershed in the Adirondack region of New York to compare the effects of watershed and direct channel lime additions on Hg in stream water and macroinvertebrates. All treatments sharply increased stream pH and DOC concentrations, but large differences in the duration of impacts were apparent. The watershed treatment resulted in multi-year increases in concentrations and loads of total Hg (150%; 390%), DOC (190%; 350%) and nutrients, whereas total Hg and DOC increased for short periods (72-96 h) after channel treatments. No response of Hg in macroinvertebrates was evident following the watershed treatment, but a potential short-term and spatially constrained increase occurred after the channel treatment. Our observations indicate that both treatment approaches mobilize Hg, but that direct channel liming mobilizes considerably less than watershed liming over any period longer than a few days. During the final study year, increased methyl Hg concentrations were observed across reference and treated streams, which may reflect an extended dry period, highlighting that climate variation may also affect Hg dynamics.

Atmospheric deposition is a major input of mercury (Hg) to aquatic and terrestrial ecosystems. To evaluate Hg pollution mitigation strategies for inland lakes, the two Great Lakes (Ontario and Erie) adjacent to New York State (NYS), and rural land areas of Upstate New York, the relative contributions to atmospheric Hg deposition from anthropogenic emission reductions and meteorological variations were investigated using a regional three-dimensional chemical transport model with detailed Hg and bromine chemistry (CMAQ-newHg-Br). Our simulations suggested that NYS in-state emissions and the Northeastern US emission reductions from 2005 to 2011 did not significantly alter Hg wet and dry deposition in all study areas when averaged over time and space. However, such emission changes significantly altered intensive emission sources (>10 lb/year) with subsequent effects on deposition to nearby water bodies. For the Great Lakes, Hg dry deposition was enhanced by a factor of 2-5 in the adjacent model grids (within distances of ~12 km downwind), and the enhancements decreased to negligible values over ~50 km distances. Over land, anthropogenic emissions contributed 30% of the spatial variation in Hg dry deposition and 46% in ambient concentrations of gaseous oxidized Hg (GOM). Spatial and temporal variations in meteorology and foliar characteristics were found to affect both Hg wet and dry deposition. Convective precipitation significantly contributed to spatial and seasonal variations (~65%) in Hg wet deposition over both lake and land surfaces, whereas wind speed and surface heat flux were the main factors contributing to the spatial variation in Hg dry deposition over the lake surfaces through their impacts on dry deposition velocities of GOM and PBM. Leaf area index, which regulates deposition velocity, contributed 14% of the spatial variation in dry deposition flux over land. Variation in solar radiation, which influences photochemical formation of GOM and PBM, explained ~10% of the spatial variation over lake and land surfaces alike. Findings from our highly focused study suggested broad implications. Future climate change will likely serve to enhance Hg concentrations in biota via increases in Hg dry and wet deposition to varying degrees contingent on land surface type. Hence, liminating the health risks of Hg requires mitigation of both anthropogenic Hg emission hotspots and human-induced climate change.

Nearly half of freshwater wetlands have been lost due to human disturbance. In response, wetlands are being restored to retain their ecosystem services. A potentially adverse consequence of wetland function is the production of methylmercury (MeHg). We measured concentrations of mercury (Hg) species and ancillary parameters in groundwaters and surface waters from four natural and 16 restored wetlands in northern New York State, USA to investigate differences in concentrations of Hg species among wetlands. We found no obvious differences in concentrations of total mercury (THg) and methylmercury in pond waters between natural and restored wetlands. High values of %methylmercury were evident in both ground (38.8 ± 27.6%) and surface waters (43.4 ± 25.6%) suggesting these wetland complexes are highly efficient in converting ionic Hg to methylmercury, regardless if restored or natural. High methylation efficiency may be due to observed drying and rewetting cycles. Hg in pond waters is likely derived from direct atmospheric deposition or by mobilization from near-wetland shallow sediments, in addition to groundwater inflows. Water flow of groundwaters from the associated watershed into pond waters resulted in increases in concentrations of THg and methylmercury. Dissolved organic matter likely plays an important role in the supply of Hg to pond waters. Relationships between methylmercury and %methylmercury with sulfate and nitrate in groundwaters may suggest some chemical limitation on Hg methylation at higher concentrations of these anions. Because of the similarity in Hg dynamics for natural and restored wetlands, the most effective strategy to mitigate methylmercury production would be to decrease atmospheric Hg deposition.

Mercury (Hg), a neurotoxic pollutant, can be transported long distances through the atmosphere and deposited in remote areas, threatening aquatic wildlife through methylation and bioaccumulation. Over the last two decades, air quality management has resulted in decreases in Hg emissions from waste incinerators and coal-fired power plants across North America. The common loon (Gavia immer) is an apex predator of the aquatic food web. Long-term monitoring of Hg in loons can help track biological recovery in response to the declines in atmospheric Hg that have been documented in the northeastern USA. To assess spatial patterns and temporal trends in Hg exposure of the common loon in the Adirondack Park of New York State, we analyzed Hg concentrations in loon blood and egg samples from 116 lakes between 1998 and 2016. We found spatially variable Hg concentrations in adult loon blood and feathers across the Park. Loon Hg concentrations (converted to female loon units) increased 5.7% yr -1 from 1998 to 2010 (p = 0.04), and then stabilized at 1.70 mg kg -1 from 2010 to 2016 (p = 0.91), based on 760 observations. Concentrations of Hg in juvenile loons also increased in the early part of the record, stabilizing 2 years before Hg concentrations stabilized in adults. For 52 individual lakes with samples from at least 4 different years, loon Hg increased in 34 lakes and decreased in 18 lakes. Overall, we found a delayed recovery of Hg concentrations in loons, despite recent declines in atmospheric Hg.

Mercury (Hg) pollution is an environmental problem that adversely affects human and ecosystem health at local, regional, and global scales-including within New York State. More than two-thirds of the Hg currently released to the environment originates, either directly or indirectly, from human activities. Since the early 1800s, global atmospheric Hg concentrations have increased by three- to eight-fold over natural levels. In the U.S., atmospheric emissions and point-source releases to waterways increased following industrialization into the mid-1980s. Since then, water discharges have largely been curtailed. As a result, Hg emissions, atmospheric concentrations, and deposition over the past few decades have declined across the eastern U.S. Despite these decreases, Hg pollution persists. To inform policy efforts and to advance public understanding, the New York State Energy Research and Development Authority (NYSERDA) sponsored a scientific synthesis of information on Hg in New York State. This effort includes 23 papers focused on Hg in atmospheric deposition, water, fish, and wildlife published in Ecotoxicology. New York State experiences Hg contamination largely due to atmospheric deposition. Some landscapes are inherently sensitive to Hg inputs driven by the transport of inorganic Hg to zones of methylation, the conversion of inorganic Hg to methylmercury, and the bioaccumulation and biomagnification along food webs. Mercury concentrations exceed human and ecological risk thresholds in many areas of New York State, particularly the Adirondacks, Catskills, and parts of Long Island. Mercury concentrations in some biota have declined in the Eastern Great Lakes Lowlands and the Northeastern Highlands over the last four decades, concurrent with decreases in water releases and air emissions from regional and U.S. sources. However, widespread changes have not occurred in other ecoregions of New York State. While the timing and magnitude of the response of Hg levels in biota varies, policies expected to further diminish Hg emissions should continue to decrease Hg concentrations in food webs, yielding benefits to the fish, wildlife, and people of New York State. Anticipated improvements in the Hg status of aquatic ecosystems are likely to be greatest for inland surface waters and should be roughly proportional to declines in atmospheric Hg deposition. Efforts that advance recovery from Hg pollution in recent years have yielded significant progress, but Hg remains a pollutant of concern. Indeed, due to this extensive compilation of Hg observations in biota, it appears that the extent and intensity of the contamination on the New York landscape and waterscape is greater than previously recognized. Understanding the extent of Hg contamination and recovery following decreases in atmospheric Hg deposition will require further study, underscoring the need to continue existing monitoring efforts.

Mercury (Hg) concentrations and speciation were measured in nine tributaries to Lake Ontario as part of two independent field-sampling programs. Among the study tributaries, mean total Hg (THg) concentrations ranged from 0.9 to 2.6 ng/L; mean dissolved Hg (THg D ) ranged from 0.5 to 1.5 ng/L; mean particulate Hg (THg P ) ranged from 0.3 to 2.0 ng/L; and mean methylmercury (MeHg) ranged from 0.06 to 0.14 ng/L. Watershed land cover, total suspended solids (TSS), and dissolved organic carbon (DOC) were evaluated as potential controls of tributary Hg. Significant relationships between THg D and DOC were limited, whereas significant relationships between THg P and TSS were common across watersheds. Total suspended solids was strongly correlated with the percentage of agricultural land in watersheds. Particle enrichment of Hg (mass Hg/mass TSS) was highly variable, but distinctly higher in US tributaries likely due to higher TSS in Canadian tributaries associated with higher urban and agricultural land cover. MeHg was largely associated with the aqueous phase, and MeHg as a fraction of THg was positively correlated to percent open water coverage in the watershed. Wetland cover was positively correlated to THg and MeHg concentrations, while urban land cover was only related to higher THg P .

Mercury (Hg) is a potent neurotoxin that biomagnifies within food webs. Adverse effects have been documented for avian species related to exposure of elevated Hg levels. High elevation, boreal forests generally receive higher atmospheric Hg deposition and regional studies have subsequently identified elevated blood Hg concentrations in songbird species inhabiting these montane habitats. The overall goal of this study was to investigate spatial and seasonal Hg exposure patterns in songbird species along an elevational gradient on Whiteface Mountain in the Adirondack Park of New York State. Songbird blood samples were collected from June-July in 2009 and 2010 along an elevational gradient at 13 study plots (450-1400 m) with a focus on Catharus thrushes, including the hermit thrush, Swainson's thrush, and Bicknell's thrush. The main results of this study documented: (1) an overall linear pattern of increasing blood Hg concentrations with increasing elevation, with additional analysis suggesting a nonlinear elevational pattern of increasing blood Hg concentrations to 1075 m, followed by decreasing concentrations thereafter, for all Catharus thrush species across the elevational gradient; and (2) an overall nonlinear seasonal pattern of increasing, followed by decreasing blood Hg concentrations across target species. Avian exposure patterns appear driven by elevated atmospheric Hg deposition and increased methylmercury bioavailability within high elevation habitats as compared with low elevation forests. Seasonal patterns are likely influenced by a combination of complex and dynamic variables related to dietary selection and annual molting cycles. Considering that few high elevation analyses have been conducted within the context of regional songbird research, this project complements the results from similar studies and highlights the need for further monitoring efforts to investigate environmental Hg contamination within avian communities.

Mercury (Hg) is a potent neurotoxin that biomagnifies within both aquatic and terrestrial food webs resulting in adverse physiological and reproductive effects on impacted wildlife populations, including songbird communities. Due to reducing conditions, wetland ecosystems promote the formation of methylmercury. Regional studies have documented elevated blood mercury concentrations in songbird species within these habitat types. The overall goal of this research was to examine spatial and seasonal patterns of Hg exposure for targeted songbird species within Sphagnum bog wetland systems and compare these patterns with adjacent upland forests in the Adirondack Park of New York State. Project sampling was conducted at study plots within four Sphagnum bog and associated upland forest sites from May - August during the 2008, 2009, and 2011 field seasons. The overall results documented: (1) blood Hg concentrations were elevated in songbird species inhabiting Sphagnum bog habitats as compared to nearby upland forest species; (2) target species within each habitat type exhibited consistent species-level patterns in blood Hg concentrations at each study site; and (3) no seasonal change in blood Hg concentrations within Sphagnum bog habitats was documented, but an increasing, followed by a decreasing seasonal pattern in mercury exposure was detected for upland forest species. Habitat type was demonstrated to influence avian Hg exposure levels. Moreover, Sphagnum bog ecosystems may be contributing to elevated Hg concentrations in biota within the surrounding environment. Seasonal patterns for blood Hg concentrations were found to vary between habitat type and are likely related to a combination of variables including habitat-driven Hg concentrations in prey items, seasonal dietary shifts, and annual molting cycles. This project emphasizes the importance of prioritizing future research efforts within identified high Hg habitat types, specifically wetland systems, to better characterize associated avian exposure levels, estimate the spatial extent of wetland systems on the surrounding environment, and identify locations of potential biological hotspots across the Adirondack Park.

Mercury is a neurotoxic pollutant and contamination in remote ecosystems due to atmospheric mercury deposition coupled with watershed characteristics that influence mercury bioavailability. Biological interactions that affect mercury bioaccumulation are especially relevant as fish assemblages change in response to species introductions and lake management practices. We studied the influence of shifting food web dynamics on mercury in fisheries of Little Moose Lake in the southwestern Adirondack Mountains of New York, USA. Annual removal of non-native Smallmouth Bass (Micropterus dolomieu) has been used as a management strategy since 2000 to restore the native fish assemblage and food web in favor of Lake Trout (Salvelinus namaycush). Changes in total mercury, stable carbon ( 13 C/ 12 C) and nitrogen ( 15 N/ 14 N) isotopes, and growth were evaluated for Lake Trout and Smallmouth Bass. Growth rates increased for both predators and trophic position increased for Lake Trout post-removal. Mercury concentrations in Lake Trout increased over the 16-year study period influenced by a diet shift from invertebrates to higher trophic level prey fish, regardless of increased growth. Smallmouth Bass mercury concentrations decreased with compensatory growth from a reduced population size. These contrasting trends indicate that changes in mercury deposition were not the primary driver for mercury bioaccumulation responses in Little Moose Lake. Stable isotope values changed for both predators and for several lower trophic level organisms, likely reflecting changes in nutrient cycling and/or inputs. Our findings emphasize the potential role of fisheries management on whole-lake and predatory fish responses to mercury contamination in temperate lakes.

Ice storms are a type of extreme winter weather event common to north temperate and boreal forests worldwide. Recent climate modelling studies suggest that these storms may become more frequent and severe under a changing climate. Compared to other types of storm events, relatively little is known about the direct and indirect impacts of these storms on forests, as naturally occurring ice storms are inherently difficult to study. Here we describe a novel experimental approach used to create a suite of ice storms in a mature hardwood forest in New Hampshire, USA. The experiment included five ice storm intensities (0, 6.4, 12.7 and 19.1 mm radial ice accretion) applied in a single year, and one ice storm intensity (12.7 mm) applied in two consecutive years. Results demonstrate the feasibility of this approach for creating experimental ice storms, quantify the increase in fine and coarse woody debris mass and nutrients transferred from the forest canopy to the soil under the different icing conditions, and show an increase in the damage to the forest canopy with increasing icing that evolves over time. In this forest, little damage occurred below 6.4 mm radial ice accretion, moderate damage occurred with up to 12.7 mm of accretion, and significant branch breakage and canopy damage occurred with 19.1 mm of ice. The icing in consecutive years demonstrated an interactive effect of ice storm frequency and severity such that some branches damaged in the first year of icing appeared to remain in the canopy and then fall to the ground in the second year of icing. These results have implications for National Weather Service ice storm warning levels, as they provide a quantitative assessment of ice-load related inputs of forest debris that will be useful to municipalities creating response plans for current and future ice storms., Competing Interests: We declare that one of the authors (FB) is employed by a commercial company: Research Designs. FB is the sole proprietor of Research Designs, and he provided specialized design services for this experiment. This does not alter our adherence to PLOS ONE policies on sharing data and materials.

The Adirondack Mountain region of New York, a historical hotspot for atmospheric sulfur and nitrogen deposition, features abundant lakes that are experiencing browning associated with recovery from acidification. Yet, much remains unknown about the photoreactivity of Adirondack lake waters. We quantified the apparent quantum yields (Φ app,RI ) of photochemically produced reactive intermediates (RIs), such as excited triplet states of dissolved organic matter ( 3 DOM*), singlet oxygen ( 1 O 2 ), and hydroxyl radicals ( • OH), for surface waters collected from 16 representative Adirondack lakes. Φ app, 3 DOM* and Φ app, 1 O 2 for native Adirondack lake waters fell within ranges reported for whole waters and DOM isolates from various sources, while Φ app, • OH were substantially lower than those measured for other aquatic samples. Orthogonal partial least squares and multiple linear regression analyses identified the spectral slope coefficient from 290 to 400 nm ( S 290-400 ) as the most effective predictor of Φ app,RI among measured water chemistry parameters and bulk DOM properties. Φ app,RI also exhibited divergent responses to controlled pH adjustment and aluminum or iron addition simulating hypothetical scenarios relevant to past and future water chemistry conditions of Adirondack lakes. This study highlights the need for continued research on changes in photoreactivity of acid-impacted aquatic ecosystems in response to browning and subsequent impacts on photochemical processes.

Ice storms can have profound and lasting effects on the structure and function of forest ecosystems in regions that experience freezing conditions. Current models suggest that the frequency and intensity of ice storms could increase over the coming decades in response to changes in climate, heightening interest in understanding their impacts. Because of the stochastic nature of ice storms and difficulties in predicting when and where they will occur, most past investigations of the ecological effects of ice storms have been based on case studies following major storms. Since intense ice storms are exceedingly rare events it is impractical to study them by waiting for their natural occurrence. Here we present a novel alternative experimental approach, involving the simulation of glaze ice events on forest plots under field conditions. With this method, water is pumped from a stream or lake and sprayed above the forest canopy when air temperatures are below freezing. The water rains down and freezes upon contact with cold surfaces. As the ice accumulates on trees, the boles and branches bend and break; damage that can be quantified through comparisons with untreated reference stands. The experimental approach described is advantageous because it enables control over the timing and amount of ice applied. Creating ice storms of different frequency and intensity makes it possible to identify critical ecological thresholds necessary for predicting and preparing for ice storm impacts.

The present-day acid-base chemistry of surface waters can be directly linked to contemporary observations of acid deposition; however, pre-industrial conditions are key to predicting the potential future recovery of stream ecosystems under decreasing loads of atmospheric sulfur (S) and nitrogen (N) deposition. The integrated biogeochemical model PnET-BGC was applied to 25 forest watersheds that represent a range of acid sensitivity in the Adirondack region of New York, USA to simulate the response of streams to past and future changes in atmospheric S and N deposition, and calculate the target loads of acidity for protecting and restoring stream water quality and ecosystem health. Using measured data, the model was calibrated and applied to simulate soil and stream chemistry at all study sites. Model hindcasts indicate that historically stream water chemistry in the Adirondacks was variable, but inherently sensitive to acid deposition. The median model-simulated acid neutralizing capacity (ANC) of the streams was projected to be 55 μeq L -1 before the advent of anthropogenic acid deposition (~1850), decreasing to minimum values of 10 μeq L -1 around the year 2000. The median simulated ANC increased to 13 μeq L -1 by 2015 in response to decreases in acid deposition that have occurred over recent decades. Model projections suggest that simultaneous decreases in sulfate, nitrate and ammonium deposition are more effective in restoring stream ANC than individual decreases in sulfur or nitrogen deposition. However, the increases in stream ANC per unit equivalent decrease in S deposition is greater compared to decreases in N deposition. Using empirical algorithms, fish community density and biomass are projected to increase under several deposition-control scenarios that coincide with increases in stream ANC. Model projections suggest that even under the most aggressive deposition-reduction scenarios, stream chemistry and fisheries will not fully recover from historical acidification by 2200., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 The Authors. Published by Elsevier B.V. All rights reserved.)

Dimethyl mercury (CH 3 HgCH 3 , DMeHg) has been observed in upwelling marine environments and the deep ocean. However, little is known about the occurrence and mechanisms of DMeHg formation in freshwater environments. In this study, concentrations of dissolved gaseous DMeHg were investigated in floodwaters of rice paddies in China that have been contaminated by mercury from mining. Values of DMeHg in rice paddies were compared with measurements from nearshore surface seawater in the Bohai Gulf. High concentrations of dissolved gaseous DMeHg occurred in rice paddies. Average DMeHg concentration was 12 ± 22 pg L -1 with range of 0.39 to 91 pg L -1 in rice paddies at Shuijing, China, a site impacted by an abandoned mercury mine. These concentrations are comparable to those previously observed in the deep seawater and coastal upwelling environments (2.3-115pg L -1 ). An alkaline environment was found to be necessary for DMeHg formation in rice paddies. Associated incubation experiments showed that production of DMeHg in paddy soil was limited by Hg availability. Although iron amendments accelerated the production of gaseous methylmercury (MeHg) species to floodwaters, available Hg 2+ is crucial for this production in flooded rice paddies. These observations are the first to demonstrate the occurrence of DMeHg and reveal factors affecting DMeHg production in rice paddies. Given the high volatility of DMeHg, these measurements also suggest a source for observations of MeHg in atmospheric deposition and advance understanding of a potentially important aspect of the biogeochemical cycling of Hg.

Statistically downscaled climate change scenarios from four General Circulation Models for two Representative Concentration Pathways (RCP) were applied as inputs to a biogeochemical model, PnET-BGC, to examine potential future dynamics of water, carbon, and nitrogen in an old-growth Douglas-fir forest in the western Cascade Range. Projections show 56% to 77% increases in stomatal conductance throughout the year from 1986-2010 to 2076-2100, and 65% to 104% increases in leaf carbon assimilation between October and June over the same period. However, future dynamics of water and carbon under the RCP scenarios are affected by a 49% to 86% reduction in foliar biomass resulting from severe air temperature and humidity stress to the forest in summer. Important implications of future decreases in foliar biomass include 1) 20% to 71% decreases in annual transpiration which increase soil moisture by 7% to 15% in summer and fall; 2) decreases in photosynthesis by 77% and soil organic matter by 62% under the high radiative forcing scenario; and 3) altered foliar and soil carbon to nitrogen stoichiometry. Potential carbon dioxide fertilization effects on vegetation are projected to 1) amplify decreases in transpiration by 4% to 9% and increases in soil moisture in summer and fall by 1% to 2%; and 2) alleviate decreases in photosynthesis by 4%; while 3) having negligible effects on the dynamics of nitrogen. Our projections suggest that future decrease in transpiration and moderate water holding capacity may mitigate soil moisture stress to the old-growth Douglas-fir forest. Future increases in nitrogen concentration in soil organic matter are projected to alleviate the decrease in net nitrogen mineralization despite a reduction in decomposition of soil organic matter by the end of the century., (Copyright © 2018 Elsevier B.V. All rights reserved.)

Using statistically downscaled future climate scenarios and a version of the biogeochemical model (PnET-BGC) that was modified for use in the alpine tundra, we investigated changes in water, carbon, and nitrogen dynamics under the Representative Concentration Pathways at Niwot Ridge in Colorado, USA. Our simulations indicate that future hydrology will become more water-limited over the short-term due to the temperature-induced increases in leaf conductance, but remains energy-limited over the longer term because of anticipated future decreases in leaf area and increases in annual precipitation. The seasonal distribution of the water supply will become decoupled from energy inputs due to advanced snowmelt, causing soil moisture stress to plants during the growing season. Decreases in summer soil moisture are projected to not only affect leaf production, but also reduce decomposition of soil organic matter in summer despite increasing temperature. Advanced future snowmelt in spring and increasing rain to snow ratio in fall are projected to increase soil moisture and decomposition of soil organic matter. The extended growing season is projected to increase carbon sequestration by 2% under the high radiative forcing scenario, despite a 31% reduction in leaf display due to the soil moisture stress. Our analyses demonstrate that future nitrogen uptake by alpine plants is regulated by nitrogen supply from mineralization, but plant nitrogen demand may also affect plant uptake under the warmer scenario. PnET-BGC simulations also suggest that potential CO 2 effects on alpine plants are projected to cause larger increases in plant carbon storage than leaf and root production., (Copyright © 2018 Elsevier B.V. All rights reserved.)

Historical increases in emissions and atmospheric deposition of oxidized and reduced nitrogen (N) provided the impetus for extensive, global-scale research investigating the effects of excess N in terrestrial and aquatic ecosystems, with several regions within the Eastern Deciduous Forest of the United States found to be susceptible to negative effects of excess N. The Clean Air Act and associated rules have led to decreases in emissions and deposition of oxidized N, especially in eastern U.S., representing a research challenge and opportunity for ecosystem ecologists and biogeochemists. The purpose of this paper is to predict changes in the structure and function of North American forest ecosystems in a future of decreased N deposition. Hysteresis is a property of a system wherein output is not a strict function of corresponding input, incorporating lag, delay, or history dependence, particularly when the response to decreasing input is different from the response to increasing input. We suggest a conceptual hysteretic model predicting varying lag times in recovery of soil acidification, plant biodiversity, soil microbial communities, forest carbon (C) and N cycling, and surface water chemistry toward pre-N impact conditions. Nearly all of these can potentially respond strongly to reductions in N deposition. Most responses are expected to show some degree of hysteresis, with the greatest delays in response occurring in processes most tightly linked to "slow pools" of N in wood and soil organic matter. Because experimental studies of declines in N loads in forests of North America are lacking and because of the expected hysteresis, it is difficult to generalize from experimental results to patterns expected from declining N deposition. These will likely be long-term phenomena, difficult to distinguish from other, concurrent environmental changes, including elevated atmospheric CO 2 , climate change, reductions in acidity, invasions of new species, and long-term vegetation responses to past disturbance., (Copyright © 2018 Elsevier Ltd. All rights reserved.)

Understanding the impacts of clear-cutting is critical to inform sustainable forest management associated with net primary productivity and nutrient availability over the long-term. Few studies have rigorously tested model simulations against field measurements which would provide more confidence in efforts to quantify logging impacts over the long-term. The biogeochemical model, PnET-BGC has been used to simulate forest production and stream chemistry at the Hubbard Brook Experimental Forest (HBEF), New Hampshire, USA. Previous versions of PnET-BGC could accurately simulate the longer-term biogeochemical response to harvesting, but were unable to reproduce the marked changes in stream NO 3 - immediately after clear-cutting which is an important impact of forest harvesting. Moreover, the dynamics of nutrients in major pools including mineralization and plant uptake were poorly predicted. In this study, the model was modified and parametrized allowing for a lower decomposition rate during the earlier years after the clear-cut and increased NH 4 + plant uptake with the regrowth of new vegetation to adequately reproduce hydrology, aboveground forest biomass, and soil solution and stream water chemistry in response to a whole-tree harvest of a northern hardwood forest watershed (W5) at the HBEF. Modeled soil solution and stream water chemistry successfully captured the rapid recovery of leaching nutrients to pre-cut levels within four years after the treatment. The model simulated a substantial increase in aboveground net primary productivity (NPP) from around 36% to 97% of pre-cut aboveground values within years 2 to 4 of the cut, which closely reproduced the measured values. The projected accumulation of aboveground biomass 70 years following the harvest was almost 190 t ha -1 , which is close to the pre-cut measured value. A first-order sensitivity analysis showed greater sensitivity of projections of the model outputs for the mature forest than the strongly aggrading forest., (Copyright © 2018 Elsevier B.V. All rights reserved.)

In many temperate forested watersheds, hydrologic nitrogen export has declined substantially in recent decades, and many of these watersheds show enduring effects from historic acid deposition. A watershed acid remediation experiment in New Hampshire reversed many of these legacy effects of acid deposition and also increased watershed nitrogen export, suggesting that these two phenomena may be coupled. Here we examine stream nitrate dynamics in this watershed acid remediation experiment for indicators of nitrogen saturation in the terrestrial and aquatic ecosystems. Post-treatment, the (positive) slope of the relationship between nitrate concentration and discharge increased by a median of 82% ( p = 0.004). This resulted in greater flushing of nitrate during storm events, a key indicator of early stage nitrogen saturation. Hysteretic behavior of the concentration-discharge relationship indicated that the mobilization of soil nitrate pools was responsible for this increased flushing. In contrast to this evidence for nitrogen saturation in the terrestrial ecosystem, we found that nitrogen uptake increased, post-treatment, in the aquatic ecosystem, substantially attenuating growing-season nitrate flux by up to 71.1% ( p = 0.025). These results suggest that, as forests slowly recover from acid precipitation, terrestrial, and aquatic ecosystem nitrogen balance may be substantially altered.

Rice consumption is the primary pathway for methylmercury (MeHg) exposure at inland mercury (Hg) mining areas of China. The sources and processes of formation and translocation for MeHg in rice plant are complex and remain largely unknown. In this study, rice ( Oryza sativa L.) was exposed to isotopically labeled dimethylmercury (DMe 199 Hg) in field experiments using open top chambers to explore the response of MeHg accumulation in rice tissues to different levels of DMe 199 Hg in air. Rice leaves assimilated DMeHg from air, which was subsequently largely stored in aboveground tissues, including the rice grain, with only a small amount reaching the root. Combining these experimental results with field investigations of DMeHg concentrations in air beneath the rice canopy in a Hg mining area, we estimate that 15.5%, 10.8%, and 8.50% MeHg in the brown rice, the leaf, and the upper stalk, respectively, could be derived from atmospheric sources of DMeHg, while 99.5% of MeHg in rice root originated from the rice soil-water system. These findings help refine the mechanism of MeHg accumulation in rice that, in addition to soil, a fraction of MeHg in rice plants can be derived from DMeHg emissions from flooded rice paddies in Hg mining areas.

Mercury is a global pollutant released into the biosphere by varied human activities including coal combustion, mining, artisanal gold mining, cement production, and chemical production. Once released to air, land and water, the addition of carbon atoms to mercury by bacteria results in the production of methylmercury, the toxic form that bioaccumulates in aquatic and terrestrial food chains resulting in elevated exposure to humans and wildlife. Global recognition of the mercury contamination problem has resulted in the Minamata Convention on Mercury, which came into force in 2017. The treaty aims to protect human health and the environment from human-generated releases of mercury curtailing its movement and transformations in the biosphere. Coincident with the treaty's coming into force, the 13th International Conference of Mercury as a Global Pollutant (ICMGP-13) was held in Providence, Rhode Island USA. At ICMGP-13, cutting edge research was summarized and presented to address questions relating to global and regional sources and cycling of mercury, how that mercury is methylated, the effects of mercury exposure on humans and wildlife, and the science needed for successful implementation of the Minamata Convention. Human activities have the potential to enhance mercury methylation by remobilizing previously released mercury, and increasing methylation efficiency. This synthesis concluded that many of the most important factors influencing the fate and effects of mercury and its more toxic form, methylmercury, stem from environmental changes that are much broader in scope than mercury releases alone. Alterations of mercury cycling, methylmercury bioavailability and trophic transfer due to climate and land use changes remain critical uncertainties in effective implementation of the Minamata Convention. In the face of these uncertainties, important policy and management actions are needed over the short-term to support the control of mercury releases to land, water and air. These include adequate monitoring and communication on risk from exposure to various forms of inorganic mercury as well as methylmercury from fish and rice consumption. Successful management of global and local mercury pollution will require integration of mercury research and policy in a changing world.

Artisanal and small-scale gold mining (ASGM) in Madre de Dios, Peru, continues to expand rapidly, raising concerns about increases in loading of mercury (Hg) to the environment. We measured physicochemical parameters in water and sampled and analyzed sediments and fish from multiple sites along one ASGM-impacted river and two unimpacted rivers in the region to examine whether Hg concentrations were elevated and possibly related to ASGM activity. We also analyzed the 308 fish samples, representing 36 species, for stable isotopes (δ 15 N and δ 13 C) to estimate their trophic position. Trophic position was positively correlated with the log-transformed Hg concentrations in fish among all sites. There was a lack of relationship between Hg concentrations in fish and either Hg concentrations in sediments or ASGM activity among sites, suggesting that fish Hg concentrations alone is not an ideal bioindicator of site-specific Hg contamination in the region. Fish Hg concentrations were not elevated in the ASGM-impacted river relative to the other two rivers; however, sediment Hg concentrations were highest in the ASGM-impacted river. Degraded habitat conditions and commensurate shifts in fish species and ecological processes may influence Hg bioaccumulation in the ASGM-impacted river. More research is needed on food web dynamics in the region to elucidate any effects caused by ASGM, especially through feeding relationships and food sources.

In this paper we present the results of a four-year study of water quality in runoff from an extensive, sedum covered, vegetated roof on an urban commercial building. Monitoring commenced seven months after the roof was constructed, with the first growing season. Stormwater drainage quality function of the vegetated roof was compared to a conventional (impermeable, high-albedo) membrane roof in addition to paired measurements of wet and bulk depositions at the study site. We present concentrations and fluxes of nutrients and major solutes. We discuss seasonal and year-to-year variation in water quality of drainage from the vegetated roof and how it compares with atmospheric deposition and drainage from the impermeable roof. Drainage waters from the vegetated roof exhibited a high concentration of nutrients compared to atmospheric deposition, particularly during the warm temperature growing season. However, nutrient losses were generally low because of the strong retention of water by the vegetated roof. There was marked variation in the retention of nutrients by season due to variations in concentrations in drainage from the vegetated roof. The vegetated roof was a sink of nitrogen, total phosphorus and chloride, and a source of phosphate and dissolved inorganic and organic carbon. Chloride exhibited elevated inputs and leaching during the winter. The drainage from the vegetated and impermeable roofs met the United States Environmental Protection Agency freshwater standards for all parameters, except for total phosphorus., (Copyright © 2017 Elsevier B.V. All rights reserved.)

Surface waters in Europe and North America previously impacted by acid deposition are recovering in conjunction with declining precursor emissions since the 1980s. Lime has been applied to some impacted watersheds to accelerate recovery. The response to liming can be considered a proxy for future recovery from acid deposition. Increases in dissolved organic carbon concentrations have been observed in surface waters in response to increased pH associated with recovery from acid deposition. Although not previously described, recovery-related increases in dissolved organic carbon could drive increases in mercury concentrations and loads because of the affinity of mercury for dissolved organic matter. We used a before-after impact-response approach to describe the response of stream mercury cycling to the application of lime to the watershed of a small stream in the Adirondack Mountains of New York, USA. Dissolved organic carbon, total mercury and methylmercury concentrations increased significantly in streamwater within two weeks of treatment, to previously unobserved concentrations. After six months, post-treatment before-after impact-control (BACI) tests indicate that mean dissolved organic carbon concentrations and total mercury to dissolved organic carbon ratios remained significantly higher and limed site fluxes of methylmercury were lower than those at the reference stream. This pattern suggests total mercury is leaching at elevated levels from the limed watershed, but limitations in production and transport to the stream channel likely resulted in increases in methylmercury concentration that were of limited duration.

Mercury (Hg) is deposited from the atmosphere to remote areas such as forests, but the amount of Hg in trees is not well known. To determine the importance of Hg in trees, we analyzed foliage, bark and bole wood of eight tree species at four sites in the northeastern USA (Huntington Forest, NY; Sleepers River, VT; Hubbard Brook, NH; Bear Brook, ME). Foliar concentrations of Hg averaged 16.3 ng g-1 among the hardwood species, which was significantly lower than values in conifers, which averaged 28.6 ng g-1 (p < 0.001). Similarly, bark concentrations of Hg were lower (p < 0.001) in hardwoods (7.7 ng g-1) than conifers (22.5 ng g-1). For wood, concentrations of Hg were higher in yellow birch (2.1-2.8 ng g-1) and white pine (2.3 ng g-1) than in the other species, which averaged 1.4 ng g-1 (p < 0.0001). Sites differed significantly in Hg concentrations of foliage and bark (p = 0.02), which are directly exposed to the atmosphere, but the concentration of Hg in wood depended more on species (p < 0.001) than site (p = 0.60). The Hg contents of tree tissues in hardwood stands, estimated from modeled biomass and measured concentrations at each site, were higher in bark (mean of 0.10 g ha-1) and wood (0.16 g ha-1) than in foliage (0.06 g ha-1). In conifer stands, because foliar concentrations were higher, the foliar pool tended to be more important. Quantifying Hg in tree tissues is essential to understanding the pools and fluxes of Hg in forest ecosystems.

Concurrent regional and global environmental changes are affecting freshwater ecosystems. Decadal-scale data on lake ecosystems that can describe processes affected by these changes are important as multiple stressors often interact to alter the trajectory of key ecological phenomena in complex ways. Due to the practical challenges associated with long-term data collections, the majority of existing long-term data sets focus on only a small number of lakes or few response variables. Here we present physical, chemical, and biological data from 28 lakes in the Adirondack Mountains of northern New York State. These data span the period from 1994-2012 and harmonize multiple open and as-yet unpublished data sources. The dataset creation is reproducible and transparent; R code and all original files used to create the dataset are provided in an appendix. This dataset will be useful for examining ecological change in lakes undergoing multiple stressors.

From the 1970s to 1990s, more stringent air quality regulations were implemented across North America and Europe to reduce chemical emissions that contribute to acid rain. Surface water pH slowly increased during the following decades, but biological recovery lagged behind chemical recovery. Fortunately, this situation is changing. In the past few years, northeastern US fish populations have begun to recover in lakes that were historically incapable of sustaining wild fish due to acidic conditions. As lake ecosystems across the eastern United States recover from acid deposition, the stress to the most susceptible populations of native coldwater fish appears to be shifting from acidification effects to thermal impacts associated with changing climate. Extreme summer temperature events - which are expected to occur with increasing frequency in the coming century - can stress and ultimately kill native coldwater fish in lakes where thermal stratification is absent or highly limited. Based on data from northeastern North America, we argue that recovery from acid deposition has the potential to improve the resilience of coldwater fish populations in some lakes to impacts of climate change. This will occur as the amount of dissolved organic carbon (DOC) in the water increases with increasing lake pH. Increased DOC will reduce water clarity and lead to shallower and more persistent lake thermoclines that can provide larger areas of coldwater thermal refuge habitat. Recovery from acidification will not eliminate the threat of climate change to coldwater fish, but secondary effects of acid recovery may improve the resistance of coldwater fish populations in lakes to the effects of elevated summer temperatures in historically acidified ecosystems. This analysis highlights the importance of considering the legacy of past ecosystem impacts and how recovery or persistence of those effects may interact with climate change impacts on biota in the coming decades., (© 2016 John Wiley & Sons Ltd.)

A cross-site analysis was conducted on seven diverse, forested watersheds in the northeastern United States to evaluate hydrological responses (evapotranspiration, soil moisture, seasonal and annual streamflow, and water stress) to projections of future climate. We used output from four atmosphere-ocean general circulation models (AOGCMs; CCSM4, HadGEM2-CC, MIROC5, and MRI-CGCM3) included in Phase 5 of the Coupled Model Intercomparison Project, coupled with two Representative Concentration Pathways (RCP 8.5 and 4.5). The coarse resolution AOGCMs outputs were statistically downscaled using an asynchronous regional regression model to provide finer resolution future climate projections as inputs to the deterministic dynamic ecosystem model PnET-BGC. Simulation results indicated that projected warmer temperatures and longer growing seasons in the northeastern United States are anticipated to increase evapotranspiration across all sites, although invoking CO 2 effects on vegetation (growth enhancement and increases in water use efficiency (WUE)) diminish this response. The model showed enhanced evapotranspiration resulted in drier growing season conditions across all sites and all scenarios in the future. Spruce-fir conifer forests have a lower optimum temperature for photosynthesis, making them more susceptible to temperature stress than more tolerant hardwood species, potentially giving hardwoods a competitive advantage in the future. However, some hardwood forests are projected to experience seasonal water stress, despite anticipated increases in precipitation, due to the higher temperatures, earlier loss of snow packs, longer growing seasons, and associated water deficits. Considering future CO 2 effects on WUE in the model alleviated water stress across all sites. Modeled streamflow responses were highly variable, with some sites showing significant increases in annual water yield, while others showed decreases. This variability in streamflow responses poses a challenge to water resource management in the northeastern United States. Our analyses suggest that dominant vegetation type and soil type are important attributes in determining future hydrological responses to climate change., (© 2016 John Wiley & Sons Ltd.)

We estimated the potential economic value of recreational fisheries in lakes altered by acid pollution in the Adirondack Mountains (USA). We found that the expected value of recreational fisheries has been diminished because of acid deposition but may improve as lakes recover from acidification under low emissions scenarios combined with fish stocking. Fishery value increased with lake pH, from a low of $4.41 angler day -1 in lakes with pH < 4.5, to a high of $38.40 angler day -1 in lakes with pH > 6.5 that were stocked with trout species. Stocking increased the expected fishery value by an average of $11.50 angler day -1 across the entire pH range of the lakes studied. Simulating the future long-term trajectory of a subset of lakes, we found that pH and expected fishery value increased over time in all future emissions scenarios. Differences in estimated value among pollution reduction scenarios were small (<$1 angler day -1 ) compared to fish stocking scenarios (>$4 angler day -1 ). Our work provides a basis for assessing the costs and benefits of emissions reductions and management efforts that can hasten recovery of the economic and cultural benefits of ecosystems degraded by chronic pollution.

Syracuse, New York is working under a court-ordered agreement to limit combined sewer overflows (CSO) to local surface waters. Green infrastructure technologies, including green roofs, are being implemented as part of a CSO abatement strategy and to develop co-benefits of diminished stormwater runoff, including decreased loading of contaminants to the wastewater system and surface waters. The objective of this study was to examine the quantity and quality of discharge associated with precipitation events over an annual cycle from a green roof in Syracuse, NY and to compare measurements from this monitoring program with results from a roof irrigation experiment. Wet deposition, roof drainage, and water quality were measured for 87 storm events during an approximately 12 month period over 2011-2012. Water and nutrient (total phosphorus, total nitrogen, and dissolved organic carbon) mass balances were conducted on an event basis to evaluate retention annually and during the growing and non-growing seasons. These results are compared with a hydrological manipulation experiment, which comprised of artificially watering of the roof. Loadings of nutrients were calculated for experimental and actual storms using the concentration of nutrients and the flow data of water discharging the roof. The green roof was effective in retaining precipitation quantity from storm events (mean percent retention 96.8%, SD = 2.7%, n = 87), although the relative fraction of water retained decreased with increases in the size of the event. There was no difference in water retention of the green roof for the growing and non-growing seasons. Drainage waters exhibited high concentration of nutrients during the warm temperature growing season, particularly total nitrogen and dissolved organic carbon. Overall, nutrient losses were low because of the strong retention of water. However, there was marked variation in the retention of nutrients by season due to variations in concentrations in roof runoff., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

Although there has been a decline in U.S. mercury emissions, the effects of this change on remote ecosystems are not well understood. We examine decadal (2004-2015) responses of atmospheric mercury deposition, along with total mercury (THg) and methylmercury (MeHg) concentrations and fluxes, to decrease in mercury emissions at Arbutus Lake-watershed in the remote forested Adirondack region of New York, a biological mercury hotspot. Although wet mercury deposition remains constant, THg deposition has decreased through decreases in litter mercury inputs (17.9 to 10.8 μg/m 2 -yr) apparently driven by decreases in atmospheric concentrations of gaseous elemental mercury (Hg o ). While the lake is a net sink for THg and MeHg, concentrations and fluxes of THg and MeHg have decreased in the inlet stream and lake water apparently in response to decreases in Hg o deposition. Decreases in surface water mercury have occurred despite decadal increases in concentrations of dissolved organic carbon. Moreover, the fraction of THg as MeHg at the inlet has not changed despite decadal decreases in atmospheric sulfate deposition and surface water concentrations of sulfate. Our results indicate that recent decreases in U.S. mercury emissions have resulted in decreases in litter mercury deposition, and stream and lake THg and MeHg concentrations and fluxes, suggesting the first steps toward ecosystem recovery.

With decreases in acid deposition, nitrogen : phosphorus (N:P) ratios in lakes are anticipated to decline, decreasing P limitation of phytoplankton and potentially changing current food web dynamics. This effect could be particularly pronounced in the Adirondack Mountains of New York State, a historic hotspot for effects of acid deposition. In this study, we evaluate spatial patterns of nutrient dynamics in Adirondack lakes and use these to infer potential future temporal trends. We calculated Mann-Kendall tau correlations among total phosphorus (TP), chlorophyll a, dissolved organic carbon (DOC), acid neutralizing capacity (ANC), and nitrate (NO 3 - ) concentrations in 52 Adirondack Long Term Monitoring (ALTM) program lakes using samples collected monthly during 2008-2012. We evaluated the hypothesis that decreased atmospheric N and S deposition will decrease P limitation in freshwater ecosystems historically impacted by acidification. We also compared these patterns among lake watershed characteristics (i.e., seepage or lacking a surface outlet, chain drainage, headwater drainage, thin glacial till, medium glacial till). We found that correlations (P < 0.05) were highly dependent upon the different hydrologic flowpaths of seepage vs. drainage lakes. Differentiations among watershed till depth were also important in determining correlations due to water interaction with surficial geology. Additionally, we found low NO 3 - :TP (N:P mass) values in seepage lakes (2.0 in winter, 1.9 in summer) compared to chain drainage lakes (169.4 in winter, 49.5 in summer) and headwater drainage lakes (97.0 in winter, 10.9 in summer), implying a high likelihood of future shifts in limitation patterns for seepage lakes. With increasing DOC and decreasing NO 3 - concentrations coinciding with decreases in acid deposition, there is reason to expect changes in nutrient dynamics in Adirondack lakes. Seepage lakes may become N-limited, while drainage lakes may become less P-limited, both resulting in increased productivity. Long-term measurements of TP and chlorophyll a from the Adirondacks are needed to inform how future decreases in atmospheric N and S deposition will influence the trophic status of lake ecosystems throughout the region., (© 2016 by the Ecological Society of America.)

Decades of acid rain have acidified forest soils and freshwaters throughout montane forests of the northeastern United States; the resulting loss of soil base cations is hypothesized to be responsible for limiting rates of forest growth throughout the region. In 1999, an experiment was conducted that reversed the long-term trend of soil base cation depletion and tested the hypothesis that calcium limits forest growth in acidified soils. Researchers added 1,189 kg Ca(2+) ha(-1) as the pelletized mineral wollastonite (CaSiO3) to a 12-ha forested watershed within the Hubbard Brook Experimental Forest in the White Mountains of New Hampshire. Significant increases in the pH and acid-neutralizing capacity of soils and streamwater resulted, and the predicted increase in forest growth occurred. An unanticipated consequence of this acidification mitigation experiment began to emerge a decade later, with marked increases in dissolved inorganic nitrogen (DIN) exports in streamwater from the treated watershed. By 2013, 30-times greater DIN was exported from this base-treated watershed than from adjacent reference watersheds, and DIN exports resulting from this experiment match or exceed earlier reports of inorganic N losses after severe ice-storm damage within the study watershed. The discovery that CaSiO3 enrichment can convert a watershed from a sink to a source of N suggests that numerous potential mechanisms drive watershed N dynamics and provides new insights into the influence of acid deposition mitigation strategies for both carbon cycling and watershed N export.

Assessments of future climate change impacts on ecosystems typically rely on multiple climate model projections, but often utilize only one downscaling approach trained on one set of observations. Here, we explore the extent to which modeled biogeochemical responses to changing climate are affected by the selection of the climate downscaling method and training observations used at the montane landscape of the Hubbard Brook Experimental Forest, New Hampshire, USA. We evaluated three downscaling methods: the delta method (or the change factor method), monthly quantile mapping (Bias Correction-Spatial Disaggregation, or BCSD), and daily quantile regression (Asynchronous Regional Regression Model, or ARRM). Additionally, we trained outputs from four atmosphere-ocean general circulation models (AOGCMs) (CCSM3, HadCM3, PCM, and GFDL-CM2.1) driven by higher (A1fi) and lower (B1) future emissions scenarios on two sets of observations (1/8º resolution grid vs. individual weather station) to generate the high-resolution climate input for the forest biogeochemical model PnET-BGC (eight ensembles of six runs).The choice of downscaling approach and spatial resolution of the observations used to train the downscaling model impacted modeled soil moisture and streamflow, which in turn affected forest growth, net N mineralization, net soil nitrification, and stream chemistry. All three downscaling methods were highly sensitive to the observations used, resulting in projections that were significantly different between station-based and grid-based observations. The choice of downscaling method also slightly affected the results, however not as much as the choice of observations. Using spatially smoothed gridded observations and/or methods that do not resolve sub-monthly shifts in the distribution of temperature and/or precipitation can produce biased results in model applications run at greater temporal and/or spatial resolutions. These results underscore the importance of carefully considering field observations used for training, as well as the downscaling method used to generate climate change projections, for smaller-scale modeling studies. Different sources of variability including selection of AOGCM, emissions scenario, downscaling technique, and data used for training downscaling models, result in a wide range of projected forest ecosystem responses to future climate change., (© 2016 by the Ecological Society of America.)