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 CO2, climate change, reductions in acidity, invasions of new species, and long-term vegetation responses to past disturbance.

The influence of coastal ecosystems on global greenhouse gas (GHG) budgets and their response to increasing inundation and salinization remains poorly constrained. In this study, we have integrated an uncertainty quantification (UQ) and ensemble machine learning (ML) framework to identify and rank the most influential processes, properties, and conditions controlling methane behavior in a freshwater floodplain responding to recently restored seawater inundation. Our unique multivariate, multiyear, and multi-site dataset comprises tidal creek and floodplain porewater observations encompassing water level, salinity, pH, temperature, dissolved oxygen (DO), dissolved organic carbon (DOC), total dissolved nitrogen (TDN), partial pressure of carbon dioxide (pCO2), nitrous oxide (pN2O), methane (pCH4), and the stable isotopic composition of methane (δ13CH4). Additionally, we incorporated topographical data, soil porosity, hydraulic conductivity, and water retention parameters for UQ analysis using a previously developed 3D variably saturated flow and transport floodplain model for a physical mechanistic understanding of factors influencing groundwater levels and salinity and, therefore, CH4. Principal component analysis revealed that groundwater level and salinity are the most significant predictors of overall biogeochemical variability. The ensemble ML models and UQ analyses identified DO, water level, salinity, and temperature as the most influential factors for porewater methane levels and indicated that approximately 80% of the total variability in hourly water levels and around 60% of the total variability in hourly salinity can be explained by permeability, creek water level, and two van Genuchten water retention function parameters: the air-entry suction parameter α and the pore size distribution parameter m. These findings provide insights on the physicochemical factors in methane behavior in coastal ecosystems and their representation in local- to global-scale Earth system models.

The people of New York have long benefited from the state's diversity of ecosystems, which range from coastal shorelines and wetlands to extensive forests and mountaintop alpine habitat, and from lakes and rivers to greenspaces in heavily populated urban areas. These ecosystems provide key services such as food, water, forest products, flood prevention, carbon storage, climate moderation, recreational opportunities, and other cultural services. This chapter examines how changes in climatic conditions across the state are affecting different types of ecosystems and the services they provide, and considers likely future impacts of projected climate change. The chapter emphasizes how climate change is increasing the vulnerability of ecosystems to existing stressors, such as habitat fragmentation and invasive species, and highlights opportunities for New Yorkers to adapt and build resilience.

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.

First posted October 25, 2022 For additional information, contact: Program Manager, Next Generation Water Observing SystemWater Resources Mission AreaU.S. Geological Survey12201 Sunrise Valley DriveReston, VA 20192Contact Pubs Warehouse Groundwater-stream connectivity across mountain watersheds is critical for supporting streamflow during dry times and keeping streams cool during warm times, yet U.S. Geological Survey (USGS) stream measurements are often sparse in headwaters. Starting in 2019, the USGS Next Generation Water Observing System Program developed a multiscale methods and technology testbed approach to monitoring groundwater discharge to streams in the Neversink Reservoir watershed in the Catskill Mountains of New York. Groundwater discharge dynamics are complex across space and time because of geographic variability, topography, and preferential groundwater flow patterns, and the monitoring of discharge processes necessitates an innovative approach that includes emerging water tracing methods and enhanced local geologic mapping. This fact sheet describes the multiscale monitoring approach applied in the Neversink Reservoir watershed and specifically how the varied data types are complimentary in understanding groundwater-stream connectivity, with elements transferable to other mountain watersheds.

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/m2/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.

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.

This data note describes the Biscuit Brook and Neversink Reservoir watershed long-term monitoring data that includes: 1) stream discharge, (1983-2020 for Biscuit Brook and 1937-2020 for the Neversink Reservoir watershed), 2) stream water chemistry, 1983-2020, at 4 stations, 3) fish survey data from 16 locations in the watershed 1990-2019, 4) soil chemistry data from 2 headwater sub-watersheds, 1993-2012 and 5) periodic stream water chemistry sampling data from 364 locations throughout the watershed, 1983-2020. The Neversink Reservoir watershed in the Catskill Mountains of New York, USA drains an area of 172.5 km(2). The watershed feeds one of six reservoirs in New York City's West of Hudson water supply, which accounts for about 90% of the city's water supply. Biscuit Brook is a 9.63 km(2) tributary sub-watershed within the Neversink Reservoir watershed.

First posted November 10, 2021 For additional information, contact: Director, Pennsylvania Water Science CenterU.S. Geological Survey215 Limekiln RoadNew Cumberland, PA 17070 Sustaining the quality of the Nation's water resources and the health of our diverse ecosystems depends on the availability of sound water-resources data and information to develop effective, science-based policies. Effective management of water resources also brings more certainty and efficiency to important economic sectors. Taken together, these actions lead to immediate and long-term economic, social, and environmental benefits that will make a difference to the lives of the almost 400 million people projected to live in the United States by 2050.The Chesapeake Bay is the largest and most productive estuary in the United States and is a vital environmental and economic resource. Approximately half of the water volume of the Chesapeake Bay originates from streams and rivers that drain the 64,243 mi2 Chesapeake Bay watershed. The Bay and its tributaries have been degraded by excessive nutrients, such as nitrogen, from contributing watersheds. Inputs of nitrogen to the Bay lead to increased algal growth, decreased dissolved oxygen, and declining fisheries. In 2000, the Chesapeake Bay was listed as impaired under the Clean Water Act and Total Maximum Daily Loads (TMDLs) for nutrients and sediment have been established to assist with management actions aimed at nutrient reductions. Effective nutrient management requires an understanding of past, present, and future nutrient sources, fate, and transport in the watershed.The Chesapeake Bay community has been a pioneer in science, management, and regulation to improve water quality. Factors like climate, hydrology, source inputs, and management controls play a vital role in determining the delivery and magnitude of nitrogen inputs to the Bay. Science in the form of monitoring data, predictive tools, and interpretive reports can help inform decisions to better balance the use and control of nitrogen in coastal areas. The findings in this report can contribute to effective management of the Bay and its watershed by providing a synthesis of the understanding of how human activities and environmental change in the watershed in the past, present, and future will influence the export of nitrogen to the Bay.We hope this publication will provide you with insights and information to meet your water resource needs and will foster increased civilian awareness and involvement in the protection and restoration of our Nation's waters. The information in this report is intended primarily for those interested or involved in resource management and protection, conservation, regulation, and policymaking at the regional and national levels.

Acid rain was first recognized in the 1970s in North America and Europe as an atmospheric pollutant that was causing harm to ecosystems. In response, the U.S. Congress enacted Title IV of the Clean Air Act Amendments (CAA) in 1990 to reduce sulfur and nitrogen emissions from fossil fuel burning power plants. This study reports trends in wet-precipitation chemistry in response to emissions reductions implemented as part of the CAA. Trends were calculated for sulfate (SO4), nitrate (NO3) and ammonium (NH4) from 1985 to 2017 at 168 stations operated by the National Atmospheric Deposition Program (NADP); stations were divided into 9 regions across the United States. Trend analyses were conducted for three time periods: Period 1 (1985-1999), Period 2 (2000-2017), and the entire study period (1985-2017). Seasonal and regional Kendall trend analyses reveal significant decreasing trends in mean wet-precipitation SO4 concentrations in all 9 regions during the entire study period. The largest decreasing trends in monthly mean SO4 precipitation-weighted concentrations were measured in the Mid-Atlantic (-1.29 mu eq/l/yr), Midwest (-1.15 mu eq/l/yr), and Northeast regions (-1.10 mu eq/l/ yr). The trends in monthly mean NO3 concentrations were not as strong as those for SO4, but all of the regions had significant decreasing trends in NO3 and again the Mid-Atlantic (-0.53 mu eq/l/yr), Midwest (-0.44 mu eq/l/yr), and Northeast regions (-0.50 mu eq/l/yr) had the strongest trends. Trends were steepest during Period 2 for SO4 and NO3, in fact for NO3 86% of the stations had significant decreasing trends during Period 2 while only 8% of the stations had significant decreasing trends during Period 1. The stations with the highest concentrations of SO4 and NO3 at the beginning of the study had the strongest decreasing trends and the relations were stronger during Period 2 than Period 1. For NH4, 22% of the stations had statistically significant increasing trends in concentration during Period 1. The largest increasing trends in wet-precipitation NH4 concentration occurred in the North-Central region during Period 1, Period 2 and throughout the entire study. By comparison, NH4 trends in the Rocky-North and Rocky-South regions were about half as steep and trends in the South-Central and Midwest regions were about one-third as steep. We compared trends in SO4 and NO3 concentrations from NADP stations to emissions of sulfur dioxide and nitrogen oxides, respectively to determine whether there was a relation between emissions and wet-precipitation concentration trends within proximity to NADP stations. There was a statistically significant relation (r(2) = 0.62-0.69, p < 0.01) between the trend in SO4 concentrations at individual NADP stations and total and mean sulfur dioxide (SO2) emissions from power plants within a range of 750 km and 1000 km from each station. There were also significant relations between NO3 concentration trends at NADP stations and power plant emissions of nitrogen oxides, but they were not nearly as strong (r(2) = 0.18-0.36, p < 0.01) as those for SO4 and were strongest for emissions within a range of 1000 km and 1500 km from each NADP station. Decreases in wet-precipitation SO4 concentrations were more consistent across regions and through time than decreases in NO3 and SO4 trends were more closely linked to stationary emissions sources than NO3 trends. There were statistically significant increases in NH4 wet-precipitation concentrations, as have been reported in previous studies, but this study found that those increases were strongest during Period 1 and were not consistent across the United States. During the first 3 years of the study period, wet-precipitation acidity was dominated by SO4 in 8 of the 9 regions; by 2017 NO3 dominated the acidity of wet-precipitation in 7 of the 9 regions. There has also been a downward shift in the NO3:NH4 ratio of wet-precipitation as the emissions of nitrogen oxides have declined while ammonia emissions have remained essentially constant. This shift has resulted in an increase in wet-precipitation total nitrogen concentrations in 7 of the 9 regions and indicate that efforts to control NH3 emissions will become increasingly important as emissions of nitrogen oxides continue to decline.

The Panola Mountain Research Watershed (PMRW) is a 41‐hectare forested catchment within the Piedmont Province of the Southeastern United States. Observations, experimentation, and numerical modelling have been conducted at Panola over the past 35 years. But to date, these studies have not been fully incorporated into a more comprehensive synthesis. Here we describe the evolving perceptual understanding of streamflow generation mechanisms at the PMRW. We show how the long‐term study has enabled insights that were initially unforeseen but are also unachievable in short‐term studies. In particular, we discuss how the accumulation of field evidence, detailed site characterization, and modelling enabled a priori hypotheses to be formed, later rejected, and then further refined through repeated field campaigns. The extensive characterization of the soil and bedrock provided robust process insights not otherwise achievable from hydrometric measurements and numerical modelling alone. We focus on two major aspects of streamflow generation: the role of hillslopes (and their connection to the riparian zone) and the role of catchment storage in controlling fluxes and transit times of water in the catchment. Finally, we present location‐independent hypotheses based on our findings at PMRW and suggest ways to assess the representativeness of PMRW in the broader context of headwater watersheds.

The Chesapeake Bay watershed has been the focus of pioneering studies of the role of atmospheric nitrogen (N) deposition as a nutrient source and driver of estuarine trophic status. Here, we review the history and evolution of scientific investigations of the role of atmospheric N deposition, examine trends from wet and dry deposition networks, and present century-long (1950-2050) atmospheric N deposition estimates. Early investigations demonstrated the importance of atmospheric deposition as an N source to the Bay, providing 25%-40% among all major N sources. These early studies led to the unprecedented inclusion of targeted decreases in atmospheric N deposition as part of the multi-stakeholder effort to reduce N loads to the Bay. Emissions of nitrogen oxides (NOx) and deposition of wet nitrate, oxidized dry N, and dry ammonium (NH4+) sharply and synchronously declined by 60%-73% during 1995-2019. These decreases largely resulted from implementation of Title IV of the 1990 Clean Air Act Amendments, which began in 1995. Wet NH4+ deposition shows no significant trend during this period. The century-long atmospheric N deposition estimates indicate an increase in total atmospheric N deposition in the Chesapeake watershed from 1950 to a peak of ~15 kg N/ha/yr in 1979, trailed by a slight decline of <10% through the mid-1990s, and followed by a sharp decline of about 40% thereafter through 2019. An additional 21% decline in atmospheric N deposition is projected from 2015 to 2050. A comparison of the Potomac River and James River watersheds indicates higher atmospheric N deposition in the Potomac, likely resulting from greater emissions from higher proportions of agricultural and urban land in this basin. Atmospheric N deposition rose from 30% among all N sources to the Chesapeake Bay watershed in 1950 to a peak of 40% in 1973, and a decline to 28% by 2015. These data highlight the important role of atmospheric N deposition in the Chesapeake Bay watershed and present a potential opportunity for decreases in deposition to contribute to further reducing N loads and improving the trophic status of tidal waters.

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.

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.

First posted August 28, 2020 Revised December 3, 2020 For additional information, contact: Director, New York Water Science CenterU.S. Geological Survey425 Jordan RoadTroy, NY 12180–8349 Mercury is an environmentally ubiquitous neurotoxin, and its methylated form presents health risks to humans and other biota, primarily through dietary intake. Because methylmercury bioaccumulates and biomagnifies in living tissue, concentrations progressively increase at higher trophic positions in ecosystem food webs. Therefore, the greatest health risks are for organisms at the highest trophic positions and for humans who consume organisms such as fish from these high trophic positions. Data on environmental mercury concentrations in various media and biota provide a basis for comparison among sites and regions and for evaluating ecosystem health risks. The U.S. Geological Survey, in cooperation with the Natural Resources Department, Bad River Band of Lake Superior Chippewa, have compiled a dataset from analyses of mercury concentrations in surface water, bed sediment, fish tissue, Rana clamitans (green frog) tissue, Haliaeetus leucocephalus (bald eagle) feathers, Lontra canadensis (North American river otter) hair, Zizania palustris (northern wild rice), and litterfall from samples collected in the Bad River watershed, Wisconsin during 2004–18. These data originated from either the Natural Resources Department or another agency based on samples collected within or near to Bad River Tribal lands before transfer to the U.S. Geological Survey for compilation and analysis at the onset of the project. This report describes the compiled mercury dataset, provides comparisons to similar measurements in the region and elsewhere, and evaluates health risks to humans and to the sampled biota. Except for litterfall, data were not collected on a consistent, regular basis over a sufficient period to evaluate temporal patterns. The reported mercury concentrations are generally similar to those reported elsewhere in the upper Great Lakes region. Reported values are consistent with atmospheric deposition as the principal source and reflect a favorable environment for mercury methylation. Fish mercury concentrations increased at higher food web positions and generally increased with length in most species measured. Sander vitreus (walleye) present the greatest risk to humans among fishes considered here because of their high trophic position and associated elevated mercury concentrations in combination with relatively high walleye consumption rates by the Native American community. Methylmercury concentrations in wild rice are generally low and likely pose little health risk. Despite reports of declining atmospheric mercury deposition across eastern North America during the past decade, a downward trend in litterfall mercury deposition was not evident in samples collected during 2012–18. Limitations in this data compilation and analysis were noted due to missing information such as collection dates and site locations for some samples. Regular monitoring of mercury in litterfall and surface waters along with periodic collection of fish would enable evaluation of temporal change in the mercury cycle that might affect future risk to humans and aquatic ecosystem inhabitants.

Mercury (Hg) concentrations in freshwater fish across the state of New York frequently exceed guidelines considered harmful to humans and wildlife, but statewide distribution and temporal changes are not well known for the state’s streams and rivers. We analyzed existing data to describe recent spatial patterns, identify key environmental drivers, and assess temporal changes. Size classes within sportfishes and prey fishes formed ‘functional taxa’ (FT), and standardized scores were generated from 2007–2016 data for 218 sites. Muscle Hg in ≥1 sportfish FT exceeded human-health guidelines of 50 ng/g (sensitive populations) and 300 ng/g (general population, GP) at 93 and 56% of sites, respectively, but exceeded 1000 ng/g (a state threshold) at only 10% of sites. Whole-body Hg in ≥1 prey fish FT exceeded wildlife thresholds of 40 ng/g and 100 ng/g at 91 and 51% of sites, respectively. Environmental drivers of recent spatial patterns include extent of forest cover and storage, the latter an indicator of wetlands. Standardized Hg scores increased with increasing atmospheric Hg deposition and storage across rural ‘upland’ regions of New York. However, scores were not related to atmospheric deposition in more-developed ‘lowland’ regions due to the limited methylation potential of urban landscapes. Comparisons of 2010–2015 sportfish Hg concentrations with those of 1998 and 2000–2005 showed inconsistent temporal changes both among and within eight sites examined. Some recent stream and river fish Hg spatial patterns differed from those of lake-based studies, highlighting the importance of New York’s flowing waters to future Hg monitoring and risk assessment.

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.

Acidic atmospheric deposition has adversely affected aquatic ecosystems globally. As emissions and deposition of sulfur (S) and nitrogen (N) have declined in recent decades across North America and Europe, ecosystem recovery is evident in many surface waters. However, persistent chronic and episodic acidification remain important concerns in vulnerable regions. We evaluated acidification in 269 headwater streams during 2010-2012 along the Appalachian Trail (AT) that transits several ecoregions and is located downwind of high levels of S and N emission sources. Discharge was estimated by matching sampled streams to those of a nearby gaged stream and assuming equivalent daily mean flow percentiles. Charge balance acid-neutralizing capacity (ANC) values were adjusted to the 15th (Q15) and 85th flow percentiles (Q85) by applying the ANC/discharge slope among sample pairs collected at each stream. A site-based approach was applied to streams sampled twice or more and a second regression-based approach to streams sampled once to estimate episodic acidification magnitudes as the ANC difference from Q15 to Q85. Streams with ANC <0 mu eq/L doubled from 16% to 32% as discharge increased from Q15 to Q85 according to the site-based approach. The proportion of streams with ANC <0 mu eq/L at low flow and high flow decreased from north to south. Base cation dilution explained the greatest amount of episodic acidification among streams and variation in sulfate (SO42-) concentrations was a secondary explanatory variable. Episodic SO42- patterns varied geographically with dilution dominant in northern streams underlain by soils developed in glacial sediment and increased concentrations dominant in southern streams with older, highly weathered soils. Episodic acidification increased as low-flow ANC increased, exceeding 90 mu eq/L in 25% of streams. Episodic increases in ANC were the dominant pattern in streams with low-flow ANC values <30 mu eq/L. Chronic and episodic acidification remain an ecological concern among AT streams. The approach developed here could be applied to estimate the magnitude and extent of chronic and episodic acidification in other regions recovering from decreasing levels of atmospheric S and N deposition.

Little is known about the regional extent and variability of nitrate from atmospheric deposition that is transported to streams without biological processing in forests. We measured water chemistry and isotopic tracers (δ18O and δ15N) of nitrate sources across the Northern Forest Region of the U.S. and Canada and reanalyzed data from other studies to determine when, where, and how unprocessed atmospheric nitrate was transported in catchments. These inputs were more widespread and numerous than commonly recognized, but with high spatial and temporal variability. Only 6 of 32 streams had high fractions (>20%) of unprocessed atmospheric nitrate during baseflow. Seventeen had high fractions during stormflow or snowmelt, which corresponded to large fractions in near-surface soil waters or groundwaters, but not deep groundwater. The remaining 10 streams occasionally had some (<20%) unprocessed atmospheric nitrate during stormflow or baseflow. Large, sporadic events may continue to be cryptic due to atmospheric deposition variation among storms and a near complete lack of monitoring for these events. A general lack of observance may bias perceptions of occurrence; sustained monitoring of chronic nitrogen pollution effects on forests with nitrate source apportionments may offer insights needed to advance the science as well as assess regulatory and management schemes.