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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.)

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.

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.)

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.

Critical loads (CLs) and dynamic critical loads (DCLs) are important tools to guide the protection of ecosystems from air pollution. In order to quantify decreases in acidic deposition necessary to protect sensitive aquatic species, we calculated CLs and DCLs of sulfate (SO4(2-))+nitrate (NO3-) for 20 lake-watersheds from the Adirondack region of New York using the dynamic model, PnET-BGC. We evaluated lake water chemistry and fish and total zooplankton species richness in response to historical acidic deposition and under future deposition scenarios. The model performed well in simulating measured chemistry of Adirondack lakes. Current deposition of SO4(2-)+NO3-, calcium (Ca2+) weathering rate and lake acid neutralizing capacity (ANC) in 1850 were related to the extent of historical acidification (1850-2008). Changes in lake Al3+ concentrations since the onset of acidic deposition were also related to Ca2+ weathering rate and ANC in 1850. Lake ANC and fish and total zooplankton species richness were projected to increase under hypothetical decreases in future deposition. However, model projections suggest that lake ecosystems will not achieve complete chemical and biological recovery in the future., (Copyright © 2014. Published by Elsevier B.V.)

Changes in lake water chemistry between 1984 and 2001 at 130 stratified random sites across the northeastern United States were studied to evaluate the population-level effects of decreases in acidic deposition. Surface-water S04(2-) concentrations decreased across the region at a median rate of -1.53 microequiv L(-1) year(-1). Calcium concentrations also decreased, with a median rate of -1.73 microequiv L(-1) year(-1). This decrease in Ca2+ retarded the recovery of surface water acid neutralizing capacity (Gran ANC), which increased at a median rate of 0.66 microequiv L(-1) year(-1). There were small increases in pH in all subregions except central New England and Maine, where the changes were not statistically significant. Median NO3- trends were not significant except in the Adirondacks, where NO3- concentrations increased at a rate of 0.53 microequiv L(-1) year(-1). A regionwide decrease in the concentration of total Al, especially in ponds with low ANC values (ANC < 25 microequiv L(-1)), was observed in the Adirondack subregion. These changes in Al were consistent with the general pattern of increasing pH and ANC. Despite the general pattern of chemical recovery, many ponds remain chronically acidic or are susceptible to episodic acidification. The continued chemical and biological recovery at sites in the northeastern United States will depend on further controls on S and N emissions.

High rates of acidic deposition in the Adirondack region of New York have accelerated acidification of soils and surface waters. Annual input-output budgets for major solutes and acid-neutralizing capacity (ANC) were estimated for 43 drainage lake-watersheds in the Adirondacks from 1998 to 2000. Sulfate was the predominant anion on an equivalent basis in both precipitation and drainage export. Calcium ion had the largest cation drainage export, followed by Mg2+. While these watersheds showed net nitrogen (N) retention, the drainage losses of SO4(2-), Cl-, base cations, and ANC exceeded their respective inputs from precipitation. Land cover (forest type and wetlands) affected the export of SO4(2-), N solutes, and dissolved organic carbon (DOC). The relationships of solute export with elevation (negative for base cations and Cl-, positive for NO3- and H+) suggest the importance of the concomitant changes of biotic and abiotic watershed characteristics associated with elevational gradients. The surface water ANC increased with the sum of base cations and was greatest in the lakes with watersheds characterized by thick deposits of glacial till. The surface water ANC was also higher in the lake-watersheds with lower DOC export. Some variation in lake ANC was associated with variability in acidic deposition. Using a classification system previously developed for Adirondack lakes on the basis primarily of surficial geology, lake-watersheds were grouped into five classes. The calculated ANC fluxes based on the major sinks and sources of ANC were comparable with measured ANC for the thick-till (I) and the medium-till lake-watersheds with low DOC (II). The calculated ANC was overestimated for the medium-till with high DOC (III) and the thin-till with high DOC (V) lake-watersheds, suggesting the importance of naturally occurring organic acids as an ANC sink, which was not included in the calculations. The lower calculated estimates than the measured ANC for the thin-till lake-watersheds with low DOC (IV) were probably due to the mobilization of Al as an ANC source in these watersheds that were highly sensitive to strong acid inputs. Our analysis of various drainage lakes across the Adirondacks on the basis of solute mass balances, coupled with the use of a lake classification system and GIS data, demonstrates that the lake-watersheds characterized by shallow deposits of glacial till are highly sensitive to acidic deposition not only in the southwestern Adirondack region where previous field-based studies were intensively conducted but also across the entire Adirondack region. Moreover, the supply of organic acids and Al mobilization substantially modify the acid-base status of surface waters.

Understanding the response of soil and surface waters to changes in atmospheric deposition is critical for guiding future legislation on air pollution. The Adirondack region of New York experiences among the most severe ecological impacts from acidic deposition. The region is characterized by considerable variability in atmospheric deposition, surficial and bedrock geology, hydrologic flow paths, and vegetation resulting in variability in effects of acidic deposition. In this study, an integrated biogeochemical model (PnET-BGC) was applied to 37 forest lake watersheds to assess the response of soil and surface waters of the Adirondacks to changes in atmospheric deposition at a regional scale. Model-simulated surface water chemistry was validated against data from two synoptic surveys conducted in 1984 and 2001. Results indicate that the model is able to capture the observed changes in surface water chemistry during this period. The model was further used to forecast the response of soil and surface waters to three future emission control scenarios. Results indicate that under the Clean Air Act, surface water SO4(2-) concentrations will continue to decrease at a median rate of -0.38 microeq/L-yr, and surface water ANC is predicted to increase at a median rate of 0.11 microeq/L-yr. More aggressive emission reductions will accelerate the rate of recovery. Under an aggressive control scenario, which represents an additional 75% reduction in SO2 emissions beyond the implementation of the Clean Air Act, surface water SO4(2-) concentrations are predicted to decrease at a median rate of -0.88 microeq/L-yr, and surface water ANC is predicted to increase at a median rate of 0.43 microeq/L-yr. Model predictions of several biologically relevant chemical indicators are also reported.

Long-term changes in the chemistry of wet deposition and lake water were investigated in the Adirondack Region of New York. Marked decreases in concentrations of SO4(2-) and H+ in wet deposition have occurred at two sites since the late 1970s. These decreases are consistent with long-term declines in emissions of sulfur dioxide (SO2) in the eastern United States. Changes in wet NO3- deposition and nitrogen oxides (NOx) emissions have been minor over the same interval. Virtually all Adirondack Lakes have shown marked decreases in concentrations of SO4(2-), which coincide with decreases in atmospheric S deposition. Concentrations of NO3- have also decreased in several Adirondack lakes. As atmospheric N deposition has not changed over this period, the mechanism contributing to this apparent increase in lake/watershed N retention is not evident. Decreases in concentrations of SO4(2-) + NO3- have resulted in increases in acid-neutralizing capacity (ANC) and pH and resulted in a shift in the speciation of monomeric Al from toxic inorganic species toward less toxic organic forms in some lakes. Nevertheless, many lakes continue to exhibit pH values and concentrations of inorganic monomeric Al that are critical to aquatic biota. Extrapolation of rates of ANC increase suggests that the time frame of chemical recovery of Adirondack Lakes will be several decades if current decreases in acidic deposition are maintained.

Acidic deposition is comprised of sulfuric and nitric acids and ammonium derived from atmospheric emissions of sulfur dioxide, nitrogen oxides, and ammonia, respectively. Acidic deposition has altered soil through depletion of labile pools of nutrient cations (i.e. calcium, magnesium), accumulation of sulfur and nitrogen, and the mobilization of elevated concentrations of inorganic monomeric aluminum to soil solutions in acid-sensitive areas. Acidic deposition leaches essential calcium from needles of red spruce, making this species more susceptible to freezing injury. Mortality among sugar maples appears to result from deficiencies of nutrient cations, coupled with other stresses such as insect defoliation or drought. Acidic deposition has impaired surface water quality in the Adirondack and Catskill regions of New York by lowering pH levels, decreasing acid-neutralizing capacity, and increasing aluminum concentrations. Acidification has reduced the diversity and abundance of aquatic species in lakes and streams. There are also linkages between acidic deposition and fish mercury contamination and eutrophication of estuaries.

The 1970 and 1990 Amendments of the Clean Air Act (CAAA) have resulted in a decline in acidic deposition in the northeastern United States. Results from the application of a biogeochemical model (PnET-BGC) at the Hubbard Brook Experimental Forest in New Hampshire suggest that, without the implementation of the CAAAs, soil base saturation and soil solution molar Ca/Al ratio would decrease to values below 6% and 1.0, respectively, while S would continue to accumulate in organic matter and adsorbed pools at rates of 2 and 3 kg of S ha(-1) yr(-1), respectively. This scenario of conditions without the CAAAs was projected to result in higher stream concentrations of SO4(2-), NO3-, and Ca2+; monomeric Al; pH below 4.8; and acid-neutralizing capacity (ANC) less than -15 microequiv L(-1). The implementation of the CAAAs has led to a slight improvement in the soil base saturation, while recovery of soil solution Ca/Al cannot be fully assessed because of variability in observed values. Our evaluation of the relative benefits of the 1970 and 1990 CAAAs indicate that although the magnitude of the cumulative decrease in strong acid deposition was greater following the 1970 CAAA as compared to the 1990 CAAA, the extent of ecosystem recovery relative to the changes in acidic deposition suggests that the 1990 CAAA was also beneficial. The slow recovery rates might be the result of a legacy of chemical effects of acidic deposition for the last 150 years and suggests that additional controls in emissions might be required to show significant changes.