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Soil microbial community composition routinely correlates with pH, reflecting both direct pH effects on microbial physiology and long-term biogeochemical feedbacks. We used two watershed-scale liming experiments to identify short- (2 years) and long-term (25 years) changes in the structure and function of bacterial and fungal communities in organic horizons (O

Mortality of brook trout Salvelinus fontinalis and water chemistry were characterized in 6 headwater streams in the western Adirondacks of New York during spring 2015, 2016, and 2017 and compared with results from analogous tests done between 1980 and 2003 in many of the same streams, to assess temporal changes in toxicity and inorganic monomeric aluminum (Ali) concentrations, and the role of Ali exposure duration on brook trout survival. The Ali concentrations of 2 and 4 µmol L–1 corresponded to low‐to‐moderate and high mortality thresholds, but prolonged exposure to ≥1 µmol Ali L–1 also produced mortality. The variability, mean, and highest Ali concentrations in Buck Creek year round, and in several other streams during spring, have decreased significantly over the past 3 decades. Logistic models indicate that Ali surpassed highly toxic concentrations in Buck Creek for 3 to 4 mo annually during 2001 to 2003 and for 2 to 3 wk annually during 2015 to 2017. The loss of extremely high Ali episodes indicates that toxicity has declined markedly between the 1989 to 1990, 2001 to 2003, and 2015 to 2017 test periods, yet Ali concentrations can still cause moderate‐to‐high and complete (100%) mortality. The logistic models illustrate how mortality of brook trout in several Adirondack streams likely decreased in response to the 1990 Amendments to the United States' Clean Air Act (which decreased acidity, Ali concentrations, and duration of toxic episodes) and offer a means to predict how changes in US regulations that limit emissions of NOx and SOx (and N and S deposition loads) could affect fish survival and stream ecosystems in this region and across the Northeast. Environ Toxicol Chem 2020;39:623–636. © 2019 The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals, Inc. on behalf of SETAC., Logistic regression models derived from toxicity tests using young‐of‐year brook trout in 6 western Adirondack streams during 2001 to 2003 and 2015 to 2017 show how inorganic monomeric aluminum (Ali) concentrations >0 and ≥1, 2, 4, and 8 µmol L–1 and exposure durations ranging from 0 to 30 d interact to affect the probability of death (100% mortality). Although contemporary Ali concentrations still reach levels that can cause 100% morality in several streams, the models predict how mortality should change, because the duration that Ali surpassed highly toxic concentrations (e.g., 4 µmol L–1) at Buck Creek declined from 3 to 4 mo annually in 2001 to 2003 to 2 to 3 wk annually in 2015 to 2017.

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

Surface waters across much of New York’s Adirondack Mountains were acidified in the late 20th century but began to recover following the 1990 amendments to the Clean Air Act. Little data, however, are available to characterize biological impacts and predict recovery of fish assemblages in streams of the region. Quantitative fish and chemistry surveys were completed in 47 headwater streams during summer 2014–2016 to develop logistic (probabilistic) models that characterize the status of contemporary fish assemblages and predict how different nitrogen (N) and sulfur (S) deposition loads may affect future fish assemblages. Models for inorganic monomeric aluminum (Ali) and richness ≥1 species and for acid neutralizing capacity (ANC) and total density >400 fish/0.1 ha, total biomass >1500 g/0.1 ha, brook trout (Salvelinus fontinalis) density >0 or >200 fish/0.1 ha, and brook trout biomass >1000 g/0.1 ha were suitable for evaluating community and population responses to changes in acid–base chemistry. Anticipated changes in national (US) secondary standards for atmospheric emissions of nitrogen oxides (NOx) and sulfur oxides (SOx) to achieve target N and S deposition loads will alter acid–base chemistry and the probabilities for observing various levels of fish metrics in streams across the region and elsewhere.

Reductions in acidic deposition rates through legislative actions in North America and Europe have stemmed further environmental degradation and shifted the focus to potential recovery [...]

The Buck Creek‐Boreas River Adirondack Watershed Monitoring Program, located in the Adirondack region of New York State, United States, combines the monitoring of headwater streams, soils, and vegetation based on a watershed design. Continuous monitoring of six watersheds is linked to the sampling of more than 400 additional Adirondack streams between 2003 and 2019 for chemical analysis of 14 constituents throughout the highly valued Adirondack ecoregion that covers an area of more than 24 000 km². Much of this landscape has a low capacity for acid buffering, but due to spatial variation in geologic features, some areas are moderately to well acid buffered. This program includes data that extends back to the early 1980s and is ongoing. The focus of the program is on the watersheds of headwater Adirondack streams. Soil, vegetation and stream data are used to better understand environmental effects on the linkages of these ecosystem components. Documentation of the long‐term responses of Adirondack ecosystems to environmental disturbances such as acid rain, climate change and other unforeseen factors is the primary objective of the program.

A century of atmospheric deposition of sulfur and nitrogen has acidified soils and undermined the health and recruitment of foundational tree species in the northeastern US. However, effects of acidic deposition on the forest understory plant communities of this region are poorly documented. We investigated how forest understory plant species composition and richness varied across gradients of acidic deposition and soil acidity in the Adirondack Mountains of New York State. We surveyed understory vegetation and soils in hardwood forests on 20 small watersheds and built models of community composition and richness as functions of soil chemistry, nitrogen and sulfur deposition, and other environmental variables. Community composition varied significantly with gradients of acidic deposition, soil acidity, and base cation availability (63% variance explained). Several species increased with soil acidity while others decreased. Understory plant richness decreased significantly with increasing soil acidity (r = 0.60). The best multivariate regression model to predict richness (p

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 (

AIM: Severity and heterogeneity of stress are major constraints of beta diversity, but their relative influence is poorly understood. Here, we addressed this question by examining the patterns of beta diversity in stress‐sensitive versus stress‐tolerant stream diatoms and their response to local versus regional factors along gradients of stress severity and heterogeneity. LOCATION: The Adirondack region of New York. METHODS: Beta diversity was measured as multivariate dispersion of communities across high stress, low stress, and high + low stress (heterogeneous) environments, encompassing 200 stream samples. Null models were implemented to assess community similarity relative to randomly assembled communities and the importance of local assembly processes versus the regional species pool. RESULTS: The overall beta diversity was influenced by a combination of severity and heterogeneity of stress, while beta diversity of sensitive species increased with heterogeneity. Beta diversity of tolerant species did not vary with either severity or heterogeneity of stress. Heterogeneity decreased community similarity relative to the null expectation in all groups of species. Stress reduced the importance of local assembly mechanisms for the overall beta diversity and sensitive species beta diversity. In contrast, the importance of local assembly mechanisms increased with stress regarding beta diversity of tolerant species. MAIN CONCLUSIONS: Beta diversity responded to both severity and heterogeneity of stress, but turnover along these gradients was mostly driven by sensitive species. The overall beta diversity and beta diversity of sensitive species became more constrained by the depauperate regional species pool, as opposed to local assembly mechanisms. While heterogeneous stress contributed to beta diversity, severe stress suppressed beta diversity through elimination of sensitive species. Therefore, an increase in beta diversity in an environmentally‐stressed region may serve as a forewarning for future loss of sensitive species, should the stress continue to intensify.

Declines in acidic deposition across Europe and North America have led to decreases in surface water acidity and signs of chemical recovery of soils from acidification. To better understand the link between recovery of soils and surface waters, chemical trends in precipitation, soils, and streamwater were investigated in three watersheds representing a depositional gradient from high to low across the northeastern United States. Significant declines in concentrations of H (ranging from -1.2 to -2.74 microequivalents [μeq] L yr), NO (ranging from -0.6 to -0.84 μeq L yr), and SO (ranging from -0.95 to -2.13 μeq L yr) were detected in precipitation in the three watersheds during the period 1999 to 2013. Soil chemistry in the A horizon of the watershed with the greatest decrease in deposition showed significant decreases in exchangeable Al and increases in exchangeable bases. Soil chemistry did not significantly improve during the study in the other watersheds, and base saturation in the Oa and upper B horizons significantly declined in the watershed with the smallest decrease in deposition. Streamwater SO concentrations significantly declined in all three streams (ranging from -2.01 to -2.87 μeq L yr) and acid neutralizing capacity increased (ranging from 1.38 to 1.60 μeq L yr) in the two streams with the greatest decreases in deposition. Recovery of soils has likely been limited by decades of acid deposition that have leached base cations from soils with base-poor parent material.

Plant phenology studies rarely consider controlling factors other than air temperature. We evaluate here the potential significance of physical and chemical properties of soil (edaphic factors) as additional important controls on phenology. More specifically, we investigate causal connections between satellite-observed green-up dates of small forest watersheds and soil properties in the Adirondack Mountains of New York, USA. Contrary to the findings of previous studies, where edaphic controls of spring phenology were found to be marginal, our analyses show that at least three factors manifest themselves as significant controls of seasonal patterns of variation in vegetated land surfaces observed from remote sensing: 1) thickness of the forest floor, 2) concentration of exchangeable soil potassium, and 3) soil acidity. For example, a thick forest floor appears to delay the onset of green-up. Watersheds with elevated concentrations of potassium are associated with early surface greening. We also found that trees growing in strongly acidified watersheds demonstrate delayed green-up dates. Overall, our work demonstrates that, at the scale of small forest watersheds, edaphic factors can explain a significant percentage of the observed spatial variation in Land Surface Phenology that is comparable to the percentage that can be explained by climatic and landscape factors. We conclude that physical and chemical properties of forest soil play important roles in forest ecosystems as modulators of climatic drivers controlling the rate of spring soil warming and the transition of trees out of winter dormancy.

Dissolved organic carbon (DOC) has received considerable attention in freshwater research, particularly since the early 2000s when increasing trends became apparent. However, remaining questions need to be resolved to address future effects of DOC on surface waters. This study was undertaken to determine (1) the relative importance of acidity and ionic strength in driving DOC increases in waters recovering from acidification and (2) the role played by long-term acid rain effects on soil. Data obtained from temporal and spatial monitoring of 142 headwater streams throughout the Adirondack region of New York (USA) were used to evaluate chemical relationships involving DOC. Year-round monitoring of three streams of differing acidification status were combined with intermittent stream surveys during spring snowmelt throughout this 24,243 km2 region that is recovering from acidification of soils and surface waters. Despite acidic deposition decreases reaching levels estimated for the early 1900s, DOC concentrations exhibited linear increases from the early 2000s through 2019. Ionic strength or conductivity showed consistent inverse relationships with DOC in all data comparisons from 2004‐05 to 2018‐19. In contrast, relationships between pH and DOC did not support increasing pH as an important factor in DOC increases. Inconsistent relationships between pH and DOC were due to strongly acidic organic acids that remain unprotonated throughout the pH range of these waters and limited weak-acid deprotonation below pH 6.2. Decreasing ionic strength increases DOC solubility by expanding the diffuse double layer, which fosters disaggregation of organic matter and dispersion of colloids. This affect controlled DOC solubilization below a pH of approximately 6.2. Distinguishing between ionic strength and pH effects is important because further large reductions in acidic deposition are not expected but continued soil-water dilution is likely from soil-Ca2+ depletion and the decreasing rate of Ca2+ leaching by SO42− and NO3−, which are still being released from soil organic matter.

Sugar maple, an abundant and highly valued tree species in eastern North America, has experienced decline from soil calcium (Ca) depletion by acidic deposition, while beech, which often coexists with sugar maple, has been afflicted with beech bark disease (BBD) over the same period. To investigate how variations in soil base saturation combine with effects of BBD in influencing stand composition and structure, measurements of soils, canopy, subcanopy, and seedlings were taken in 21 watersheds in the Adirondack region of NY (USA), where sugar maple and beech were the predominant canopy species and base saturation of the upper B horizon ranged from 4.4 to 67%. The base saturation value corresponding to the threshold for Al mobilization (16.8%) helped to define the species composition of canopy trees and seedlings. Canopy vigor and diameter at breast height (DBH) were positively correlated (P

Reductions in sulfur emissions have initiated chemical recovery of surface waters impacted by acidic deposition in the Adirondack region of New York State. However, acidified streams remain common in the region, which limits recovery of brook trout (Salvelinus fontinalis) populations. To investigate liming as a method to accelerate recovery of brook trout, the channels of two acidified streams were limed annually from 2012 to 2015, and an entire watershed of a third acidified tributary was limed by helicopter in 2013. Stream flow, water chemistry, and density of young-of-year (YOY) brook trout were measured in limed streams, an untreated acidified stream, and a buffered reference stream. Lime additions increased pH and acid-neutralizing capacity and decreased inorganic monomeric aluminum concentrations to less than 2.0 μmol/L, the minimum concentration at which in situ brook trout mortality has been documented. However, of the two channel-limed streams, only stream T8 showed a significant response (P

[This corrects the article DOI: 10.1371/journal.pone.0205296.].

Mobilization of toxic forms of aluminum (Ali) have been one of the most harmful effects of acidic deposition on aquatic ecosystems. Large decreases in acidic deposition levels have resulted in decreases in Ali concentrations in surface waters starting in the 1990s. However, recent studies indicate that fish communities are still being impaired by elevated Ali concentrations in streams, suggesting the need for a present-day assessment of the recovery status of Al chemistry in impacted regions such as the Adirondack region of New York, United States. Therefore, the recovery status of Al was assessed from long-term high-frequency monitoring of three Adirondack streams up through 2019, and multiple resampling of 127 headwater streams throughout the Adirondack region between 2004/2005 and 2018/2019. Results indicated that concentrations of Ali have continued to decrease throughout the Adirondack region, but that harmful conditions still exist in a substantial number of streams during spring snowmelt. In the western Adirondack region, 35 percent of streams during spring snowmelt, (typically the most acidic period), and 10 percent of streams during summer were still experiencing harmful concentrations of Ali (>1.0 μmol L−1) in 2018/2019. In the less-impacted east-central Adirondack region, 10 percent of streams during snowmelt, and 4 percent of streams during summer were experiencing harmful Ali concentrations in 2018. Temporal decreases in Ali concentrations were due in part to a shift in speciation from Ali to non-toxic organically complexed Al as dissolved organic carbon concentrations increased, which was also a response to decreasing acidic deposition. Increased availability of calcium resulting from acid-neutralization processes such as weathering also contributed to the decrease in Ali over the past 5–8 years. The current low levels of acidic deposition may have begun to enhance recovery by increasing the effectiveness of ambient acid-neutralization processes.

Soil calcium depletion has been strongly linked to acidic deposition in eastern North America and recent studies have begun to document the recovery of soils in response to large decreases in acidic deposition. However, increased calcium availability has not yet been seen in the B horizon, where calcium depletion has been most acute, but mineral weathering is critically important for resupplying ecosystem calcium. This study provides new data in seven watersheds in the Adirondack region (New York, USA), where acidic deposition impacts on soils and surface waters have been substantial and recovery remains slow. Initial sampling in 1997&ndash, 1998 and 2003&ndash, 2004 was repeated in 2009&ndash, 2010, 2014, 2016 and 2017. Exchangeable calcium concentrations increased by an average of 43% in the Oe horizon of three watersheds where this horizon was sampled (10.7&ndash, 15.3 cmolc kg&minus, 1). Changes in calcium were not seen in the individual watersheds of the Oa and B horizons, but as a group, a significant increase in calcium was measured in the upper B horizon. Liming of a calcium-depleted watershed also tripled calcium concentration in the upper B horizon in 5 years. However, stream calcium in unlimed watersheds decreased over the study period. Small increases in B-horizon calcium may be underway.

Sugar maple (Acer saccharum) is among the most ecologically and economically important tree species in North America, and its growth and regeneration is often the focus of silvicultural practices in northern hardwood forests. A key stressor for sugar maple (SM) is acid rain, which depletes base cations from poorly-buffered forest soils and has been associated with much lower SM vigor, growth, and recruitment. However, the potential interactions between forest management and soil acidification – and their implications for the sustainability of SM and its economic and cultural benefits – have not been investigated. In this study, we simulated the development of 50 extant SM stands in the western Adirondack region of NY (USA) for 100years under different soil chemical conditions and silvicultural prescriptions. We found that interactions between management prescription and soil base saturation will strongly shape the ability to maintain SM in managed forests. Below 12% base saturation, SM did not regenerate sufficiently after harvest and was replaced mainly by red maple (Acer rubrum) and American beech (Fagus grandifolia). Loss of SM on acid-impaired sites was predicted regardless of whether the shelterwood or diameter-limit prescriptions were used. On soils with sufficient base saturation, models predicted that SM will regenerate after harvest and be sustained for future rotations. We then estimated how these different post-harvest outcomes, mediated by acid impairment of forest soils, would affect the potential monetary value of ecosystem services provided by SM forests. Model simulations indicated that a management strategy focused on syrup production – although not feasible across the vast areas where acid impairment has occurred – may generate the greatest economic return. Although pollution from acid rain is declining, its long-term legacy in forest soils will shape future options for sustainable forestry and ecosystem stewardship in the northern hardwood forests of North America.

The application of lime (calcium carbonate) may be a cost-effective strategy to promote forest ecosystem recovery from acid impairment, under contemporary low levels of acidic deposition. However, liming acidified soils may create more suitable habitat for invasive earthworms that cause significant damage to forest floor communities and may disrupt ecosystem processes. We investigated the potential effects of liming in acidified soils where earthworms are rare in conjunction with a whole-ecosystem liming experiment in the chronically acidified forests of the western Adirondacks (USA). Using a microcosm experiment that replicated the whole-ecosystem treatment, we evaluated effects of soil liming on Lumbricus terrestris survivorship and biomass growth. We found that a moderate lime application (raising pH from 3.1 to 3.7) dramatically increased survival and biomass of L. terrestris, likely via increases in soil pH and associated reductions in inorganic aluminum, a known toxin. Very few L. terrestris individuals survived in unlimed soils, whereas earthworms in limed soils survived, grew, and rapidly consumed leaf litter. We supplemented this experiment with field surveys of extant earthworm communities along a gradient of soil pH in Adirondack hardwood forests, ranging from severely acidified (pH 5). In the field, no earthworms were observed where soil pH 4.4 and human dispersal vectors, including proximity to roads and public fishing access, were most prevalent. Overall our results suggest that moderate lime additions can be sufficient to increase earthworm invasion risk where dispersal vectors are present.

Decreasing trends in acidic deposition levels over the past several decades have led to partial chemical recovery of surface waters. However, depletion of soil Ca from acidic deposition has slowed surface water recovery and led to the impairment of both aquatic and terrestrial ecosystems. Nevertheless, documentation of acidic deposition effects on soils has been limited, and little is known regarding soil responses to ongoing acidic deposition decreases. In this study, resampling of soils in eastern Canada and the northeastern U.S. was done at 27 sites exposed to reductions in wet SO4(2-) deposition of 5.7-76%, over intervals of 8-24 y. Decreases of exchangeable Al in the O horizon and increases in pH in the O and B horizons were seen at most sites. Among all sites, reductions in SO4(2-) deposition were positively correlated with ratios (final sampling/initial sampling) of base saturation (P < 0.01) and negatively correlated with exchangeable Al ratios (P < 0.05) in the O horizon. However, base saturation in the B horizon decreased at one-third of the sites, with no increases. These results are unique in showing that the effects of acidic deposition on North American soils have begun to reverse.

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.

Recent soils research has shown that important chemical soil characteristics can change in less than a decade, often the result of broad environmental changes. Repeated sampling to monitor these changes in forest soils is a relatively new practice that is not well documented in the literature and has only recently been broadly embraced by the scientific community. The objective of this protocol is therefore to synthesize the latest information on methods of soil resampling in a format that can be used to design and implement a soil monitoring program. Successful monitoring of forest soils requires that a study unit be defined within an area of forested land that can be characterized with replicate sampling locations. A resampling interval of 5 years is recommended, but if monitoring is done to evaluate a specific environmental driver, the rate of change expected in that driver should be taken into consideration. Here, we show that the sampling of the profile can be done by horizon where boundaries can be clearly identified and horizons are sufficiently thick to remove soil without contamination from horizons above or below. Otherwise, sampling can be done by depth interval. Archiving of sample for future reanalysis is a key step in avoiding analytical bias and providing the opportunity for additional analyses as new questions arise.

For over 40 years, acid deposition has been recognized as a serious international environmental problem, but efforts to restore acidified streams and biota have had limited success. The need to better understand the effects of different sources of acidity on streams has become more pressing with the recent increases in surface water organic acids, or 'brownification,' associated with climate change and decreased inorganic acid deposition. Here, we carried out a large scale multi-seasonal investigation in the Adirondacks, one of the most acid-impacted regions in the United States, to assess how acid stream producers respond to local and watershed influences and whether these influences can be used in acidification remediation. We explored the pathways of wetland control on aluminum chemistry and diatom taxonomic and functional composition. We demonstrate that streams with larger watershed wetlands have higher organic content, lower concentrations of acidic anions, and lower ratios of inorganic to organic monomeric aluminum, all beneficial for diatom biodiversity and guilds producing high biomass. Although brownification has been viewed as a form of pollution, our results indicate that it may be a stimulating force for biofilm producers with potentially positive consequences for higher trophic levels. Our research also reveals that the mechanism of watershed control of local stream diatom biodiversity through wetland export of organic matter is universal in running waters, operating not only in hard streams, as previously reported, but also in acid streams. Our findings that the negative impacts of acid deposition on Adirondack stream chemistry and biota can be mitigated by wetlands have important implications for biodiversity conservation and stream ecosystem management. Future acidification research should focus on the potential for wetlands to improve stream ecosystem health in acid-impacted regions and their direct use in stream restoration, for example, through stream rechanneling or wetland construction in appropriate hydrologic settings.

Declines of acidic deposition levels by as much as 50% since 1990 have led to partial recovery of surface waters in the northeastern USA but continued depletion of soil calcium through this same period suggests a disconnection between soil and surface water chemistry. To investigate the role of soil-surface water interactions in recovery from acidification, the first regional survey to directly relate soil chemistry to stream chemistry during high flow was implemented in a 4144-km2 area of the Catskill region of New York, where acidic deposition levels are among the highest in the East. More than 40% of 95 streams sampled in the southern Catskill Mountains were determined to be acidified and had inorganic monomeric aluminum concentrations that exceeded a threshold that is toxic to aquatic biota. More than 80% likely exceeded this threshold during the highest flows, but less than 10% of more than 100 streams sampled were acidified in the northwestern portion of the region. Median Oa horizon soil base saturation ranged from 50% to 80% at 200 sites across the region, but median base saturation in the upper 10 cm of the B horizon was less than 20% across the region and was only 2% in the southern area. Aluminum is likely to be interfering with root uptake of calcium in the mineral horizon in approximately half the sampled watersheds. Stream chemistry was highly variable over the Catskill region and, therefore, did not always reflect the calcium depletion of the B horizon that our sampling suggested was nearly ubiquitous throughout the region. Published 2013. This article is a U.S. Government work and is in the public domain in the USA.

Environmental change is monitored in North America through repeated measurements of weather, stream and river flow, air and water quality, and most recently, soil properties. Some skepticism remains, however, about whether repeated soil sampling can effectively distinguish between temporal and spatial variability, and efforts to document soil change in forest ecosystems through repeated measurements are largely nascent and uncoordinated. In eastern North America, repeated soil sampling has begun to provide valuable information on environmental problems such as air pollution. This review synthesizes the current state of the science to further the development and use of soil resampling as an integral method for recording and understanding environmental change in forested settings. The origins of soil resampling reach back to the 19th century in England and Russia. The concepts and methodologies involved in forest soil resampling are reviewed and evaluated through a discussion of how temporal and spatial variability can be addressed with a variety of sampling approaches. Key resampling studies demonstrate the type of results that can be obtained through differing approaches. Ongoing, large-scale issues such as recovery from acidification, long-term N deposition, C sequestration, effects of climate change, impacts from invasive species, and the increasing intensification of soil management all warrant the use of soil resampling as an essential tool for environmental monitoring and assessment. Furthermore, with better awareness of the value of soil resampling, studies can be designed with a long-term perspective so that information can be efficiently obtained well into the future to address problems that have not yet surfaced.

[1] Increased greening of northern forests, measured by the Normalized Difference Vegetation Index (NDVI), has been presented as evidence that a warmer climate has increased both net primary productivity (NPP) and the carbon sink in boreal forests. However, higher production and greener canopies may accompany changes in carbon allocation that favor foliage or fine roots over less decomposable woody biomass. Furthermore, tree core data throughout mid- and northern latitudes have revealed a divergence problem (DP), a weakening in tree ring responses to warming over the past half century that is receiving increasing attention, but remains poorly understood. Often, the same sites exhibit trend inconsistency phenomenon (TIP), namely positive, or no trends in growing season NDVI where negative trends in tree ring indexes are observed. Here we studied growth of two Norway spruce (Picea abies) stands in western Russia that exhibited both the DP and TIP but were subject to soil acidification and calcium depletion of differing timing and severity. Our results link the decline in radial growth starting in 1980 to a shift in carbon allocation from wood to roots driven by a combination of two factors: (a) soil acidification that depleted calcium and impaired root function and (b) earlier onset of the growing season that further taxed the root system. The latter change in phenology appears to act as a trigger at both sites to push trees into nutrient limitation as the demand for Ca increased with the longer growing season, thereby causing the shift in carbon allocation.

Sustaining recent progress in mitigating acid pollution could require lower emissions caps that will give rise to real or perceived tradeoffs between healthy ecosystems and inexpensive energy. Because most impacts of acid rain affect ecosystem functions that are poorly understood by policy-makers and the public, an ecosystem services (ES) framework can help to measure how pollution affects human well-being. Focused on the Adirondack region (USA), a global ‘hot-spot’ of acid pollution, we measured how the chronic acidification of the region's forests, lakes, and streams has affected the potential economic and cultural benefits they provide to society. We estimated that acid-impaired hardwood forests provide roughly half of the potential benefits of forests on moderate to well-buffered soils – an estimated loss of ∼ $10,000 ha−1 in net present value of wood products, maple syrup, carbon sequestration, and visual quality. Acidic deposition has had only nominal impact – relative to the effects of surficial geology and till depth – on the capacity of Adirondack lakes and streams to provide water suitable for drinking. However, as pH declines in lakes, the estimated value of recreational fishing decreases significantly due to loss of desirable fish such as trout. Hatchery stocking programs have partially offset the pollution-mediated losses of fishery value, most effectively in the pH range 4.8–5.5, but are costly and limited in scope. Although any estimates of the monetary ‘damages’ of acid rain have significant uncertainties, our findings highlight some of the more tangible economic and cultural benefits of pollution mitigation efforts, which continue to face litigation and political opposition.

Acidic deposition caused by fossil fuel combustion has degraded aquatic and terrestrial ecosystems in North America for over four decades. The only management option other than emissions reductions for combating the effects of acidic deposition has been the application of lime to neutralize acidity after it has been deposited on the landscape. For this reason, liming has been a part of acid rain science from the beginning. However, continued declines in acidic deposition have led to partial recovery of surface water chemistry, and the start of soil recovery. Liming is therefore no longer needed to prevent further damage, so the question becomes whether liming would be useful for accelerating recovery of systems where improvement has lagged. As more is learned about recovering ecosystems, it has become clear that recovery rates vary with watershed characteristics and among ecosystem components. Lakes appear to show the strongest recovery, but recovery in streams is sluggish and recovery of soils appears to be in the early stages. The method in which lime is applied is therefore critical in achieving the goal of accelerated recovery. Application of lime to a watershed provides the advantage of increasing Ca availability and reducing or preventing mobilization of toxic Al, an outcome that is beneficial to both terrestrial and aquatic ecosystems. However, the goal should not be complete neutralization of soil acidity, which is naturally produced. Liming of naturally acidic areas such as wetlands should also be avoided to prevent damage to indigenous species that rely on an acidic environment.

Four decades after the passage of the US Clean Air Act, air-quality standards are set to protect ecosystems from damage caused by gas-phase nitrogen (N) and sulfur (S) compounds, but not from the deposition of these air pollutants to land and water. Here, we synthesize recent scientific literature on the ecological effects of N and S air pollution in the US. Deposition of N and S is the main driver of ecosystem acidification and contributes to nutrient enrichment in many natural systems. Although surface-water acidification has decreased in the US since 1990, it remains a problem in many regions. Perturbations to ecosystems caused by the nutrient effects of N deposition continue to emerge, although gas-phase concentrations are generally not high enough to cause phytotoxicity. In all, there is overwhelming evidence of a broad range of damaging effects to ecosystems in the US under current air-quality conditions.

Forty to fifty percent decreases in acidic deposition through the 1980s and 1990s led to partial recovery of acidified surface waters in the northeastern United States; however, the limited number of studies that have assessed soil change found increased soil acidification during this period. From existing data, it's not clear whether soils continued to worsen in the 1990s or if recovery had begun. To evaluate possible changes in soils through the 1990s, soils in six red spruce (Picea rubens Sarg.) stands in New York, Vermont, New Hampshire, and Maine, first sampled in 1992 to 1993, were resampled in 2003 to 2004. The Oa-horizon pH increased (P < 0.01) at three sites, was marginally higher (P < 0.1) at one site, and lower (P < 0.05) at the New York site. Total C concentrations in Oa horizons decreased (P < 0.05) at sites where the pH increased, but the cause is uncertain. Exchangeable Al concentrations in Oa horizons decreased (P < 0.05) 20 to 40% at all sites except New York, which showed no change. The Al decrease can be attributed to decreased deposition of SO42-, which decreased the mobility of Al throughout the upper soil profi le. Results indicate a nascent recovery driven largely by vegetation processes.

Depletion of Ca from forest soils due to acidic deposition has had potentially pervasive effects on forest commun- ities, but these impacts remain largely unknown. Because snails, salamanders, and plants play essential roles in the Ca cycle of northern hardwood forests, we hypothesized that their community diversity, abundance, and structure would vary with differences in biotic Ca availability. To test this hypothesis, we sampled 12 upland hardwood forests representing a soil Ca gradient in the Adirondack Mountains, New York (USA), where chronic deposition has resulted in acidified soils but where areas of well-buffered soils remain Ca rich due to parent materials. Along the gradient of increasing soil (Ca 2+ ), we ob- served increasing trends in snail community richness and abundance, live biomass of redback salamanders (Plethodon ciner- eus (Green, 1818)), and canopy tree basal area. Salamander communities were dominated by mountain dusky salamanders (Desmognathus ochrophaeus Cope, 1859) at Ca-poor sites and changed continuously along the Ca gradient to become domi- nated by redback salamanders at the Ca-rich sites. Several known calciphilic species of snails and plants were found only at the highest-Ca sites. Our results indicated that Ca availability, which is shaped by geology and acidic deposition inputs, in- fluences northern hardwood forest ecosystems at multiple trophic levels, although the underlying mechanisms require further study. Resume : L'epuisement du Ca dans les sols forestiers a cause des depots acides a eu des repercussions potentiellement ge- neralisees sur les communautes forestieres mais ces impacts demeurent largement inconnus. Etant donne que les escargots, les salamandres et les plantes jouent un role essentiel dans le cycle du Ca des forets feuillues nordiques, nous avons emis l'hypothese que la diversite, l'abondance et la structure de leurs communautes varieraient en fonction de la disponibilite du Ca. Pour tester cette hypothese, nous avons echantillonne 12 forets feuillues en milieu sec dans les monts Adirondacks, dans l'Etat de New York aux Etats-Unis d'Amerique, ou des depots chroniques ont acidifie les sols mais ou il y a encore des en- droits ou les sols ont un pouvoir tampon eleve et demeurent riches en Ca a cause du materiau originel. A mesure que la

Limited stream chemistry and macroinvertebrate data indicate that acidic deposition has adversely affected benthic macroinvertebrate assemblages in numerous headwater streams of the western Adirondack Mountains of New York. No studies, however, have quantified the effects that acidic deposition and acidification may have had on resident fish and macroinvertebrate communities in streams of the region. As part of the Western Adirondack Stream Survey, water chemistry from 200 streams was sampled five times and macroinvertebrate communities were surveyed once from a subset of 36 streams in the Oswegatchie and Black River Basins during 2003–2005 and evaluated to: (a) document the effects that chronic and episodic acidification have on macroinvertebrate communities across the region, (b) define the relations between acidification and the health of affected species assemblages, and (c) assess indicators and thresholds of biological effects. Concentrations of inorganic Al in 66% of the 200 streams periodically reached concentrations toxic to acid-tolerant biota. A new acid biological assessment profile (acidBAP) index for macroinvertebrates, derived from percent mayfly richness and percent acid-tolerant taxa, was strongly correlated (R2 values range from 0.58 to 0.76) with concentrations of inorganic Al, pH, ANC, and base cation surplus (BCS). The BCS and acidBAP index helped remove confounding influences of natural organic acidity and to redefine acidification-effect thresholds and biological-impact categories. AcidBAP scores indicated that macroinvertebrate communities were moderately or severely impacted by acidification in 44–56% of 36 study streams, however, additional data from randomly selected streams is needed to accurately estimate the true percentage of streams in which macroinvertebrate communities are adversely affected in this, or other, regions. As biologically relevant measures of impacts caused by acidification, both BCS and acidBAP may be useful indicators of ecosystem effects and potential recovery at the local and regional scale.

Elevated N deposition is continuing on many forested landscapes around the world and our understanding of ecosystem response is incomplete. Soil processes, especially nitrification, are critical. Many studies of soil N transformations have focused on identifying relationships within a single watershed but these results are often not transferable. We studied 10 small forested research watersheds in the northeastern USA to determine if there were common factors related to soil ammonification and nitrification. Vegetation varied between mixed northern hardwoods and mixed conifers. Watershed surface soils (Oa or A horizons) were sampled at grid or transect points and analyzed for a suite of chemical characteristics. At each sampling point, vegetation and topographic metrics (field and GIS-based) were also obtained. Results were examined by watershed averages (n = 10), seasonal/watershed averages (n = 28), and individual sampling points (n = 608). Using both linear and tree regression techniques, the proportion of conifer species was the single best predictor of nitrification rates, with lower rates at higher conifer dominance. Similar to other studies, the soil C/N ratio was also a good predictor and was well correlated with conifer dominance. Unlike other studies, the presence of Acer saccharum was not by itself a strong predictor, but was when combined with the presence of Betula alleghaniensis. Topographic metrics (slope, aspect, relative elevation, and the topographic index) were not related to N transformation rates across the watersheds. Although found to be significant in other studies, neither soil pH, Ca nor Al was related to nitrification. Results showed a strong relationship between dominant vegetation, soil C, and soil C/N.

The 24 ha Dry Creek watershed in the Catskill Mountains of southeastern New York State USA was clearcut during the winter of 1996–1997. The interactions among acidity, nitrate (NO 3 − ), aluminum (Al), and calcium (Ca2+) in streamwater, soil water, and groundwater were evaluated to determine how they affected the speciation, solubility, and concentrations of Al after the harvest. Watershed soils were characterized by low base saturation, high exchangeable Al concentrations, and low exchangeable base cation concentrations prior to the harvest. Mean streamwater NO 3 − concentration was about 20 μmol l−1 for the 3 years before the harvest, increased sharply after the harvest, and peaked at 1,309 μmol l−1 about 5 months after the harvest. Nitrate and inorganic monomeric aluminum (Alim) export increased by 4−fold during the first year after the harvest. Alim mobilization is of concern because it is toxic to some fish species and can inhibit the uptake of Ca2+ by tree roots. Organic complexation appeared to control Al solubility in the O horizon while ion exchange and possibly equilibrium with imogolite appeared to control Al solubility in the B horizon. Alim and NO 3 − concentrations were strongly correlated in B-horizon soil water after the clearcut (r 2 = 0.96), especially at NO 3 − concentrations greater than 100 μmol l−1. Groundwater entering the stream from perennial springs contained high concentrations of base cations and low concentrations of NO 3 − which mixed with acidic, high Alim soil water and decreased the concentration of Alim in streamwater after the harvest. Five years after the harvest soil water NO 3 − concentrations had dropped below preharvest levels as the demand for nitrogen by regenerating vegetation increased, but groundwater NO 3 − concentrations remained elevated because groundwater has a longer residence time. As a result streamwater NO 3 − concentrations had not fallen below preharvest levels, even during the growing season, 5 years after the harvest because of the contribution of groundwater to the stream. Streamwater NO 3 − and Alim concentrations increased more than reported in previous forest harvesting studies and the recovery was slower likely because the watershed has experienced several decades of acid deposition that has depleted initially base-poor soils of exchangeable base cations and caused long-term acidification of the soil.

Water chemistry, discharge, and mortality of caged brook trout Salvelinus fontinalis were characterized in six headwater streams in the southwestern Adirondack Mountains of New York during spring 2001–2003. Results were compared with mortality recorded during similar tests during 1984–1985, 1988–1990, and 1997 to assess contemporary relations between stream acidification and brook trout mortality, the effects of exposure duration on mortality, and the effects of decreased rates of acidic deposition on water quality and fish mortality. Water quality and mortality of caged, young-of-the-year brook trout were evaluated during 30-d exposure periods from mid-April to late May during the most recent tests. In 2001–2003, mortality ranged from 0% to 100% and varied among streams and years, depending on the timing of toxicity tests in relation to the annual snowmelt and on the ability of each watershed to neutralize acids and prevent acutely toxic concentrations of inorganic monomeric aluminum (Alim) duri...

Funding for Open Access provided by the UMD Libraries Open Access Publishing Fund., Decline of sugar maple in North American forests has been attributed to changes in soil calcium (Ca) and nitrogen (N) by acidic precipitation. Although N is an essential and usually a limiting factor in forests, atmospheric N deposition may cause N-saturation leading to loss of soil Ca. Such changes can affect carbon gain and growth of sugar maple trees and seedlings. We applied a 2^2 factorial arrangement of N and dolomitic limestone containing Ca and Magnesium (Mg) to 12 forest plots in the Catskill Mountain region of NY, USA. To quantify the short-term effects, we measured photosynthetic-light responses of sugar maple mature trees and seedlings two or three times during two summers. We estimated maximum net photosynthesis (An-max) and its related light intensity (PAR at An-max), apparent quantum efficiency (Aqe), and light compensation point (LCP). To quantify the long-term effects, we measured basal area of living mature trees before and 4 and 8 years after treatment applications. Soil and foliar chemistry variables were also measured. Dolomitic limestone increased Ca, Mg, and pH in the soil Oe horizon. Mg was increased in the B horizon when comparing the plots receiving N with those receiving CaMg. In mature trees, foliar Ca and Mg concentrations were higher in the CaMg and N+CaMg plots than in the reference or N plots; foliar Ca concentration was higher in the N+CaMg plots compared with the CaMg plots, foliar Mg was higher in the CaMg plots than the N+CaMg plots; An-max was maximized due to N+CaMg treatment; Aqe decreased by N addition; and PAR at An-max increased by N or CaMg treatments alone, but the increase was maximized by their combination. No treatment effect was detected on basal areas of living mature trees four or eight years after treatment applications. In seedlings, An-max was increased by N+CaMg addition. The reference plots had an open herbaceous layer, but the plots receiving N had a dense monoculture of common woodfern in the forest floor, which can impede seedling survival.

The relationship between algal species richness and diversity, and pH is controversial. Furthermore, it is still unknown how episodic stream acidification following atmospheric deposition affects species richness and diversity. Here we analyzed water chemistry and diatom epiphyton dynamics and showed their contrasting behavior in chronically vs. episodically acidic streams in the Adirondack region. Species richness and diversity were significantly higher in the chronically acidic brown water stream, where organic acidity was significantly higher and the ratio of inorganic to organic monomeric aluminum significantly lower. Conversely, in the episodically acidic clear water stream, the inorganic acidity and pH were significantly higher and the diatom communities were very species-poor. This suggests that episodic acidification in the Adirondacks may be more stressful for stream biota than chronic acidity. Strong negative linear relationships between species diversity, Eunotia exigua, and dissolved organic carbon against pH were revealed after the influence of non-linear temporal trends was partialled out using a novel way of temporal modeling. (© 2006 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)

The US Environmental Protection Agency established the Adirondack Effects Assessment Program (AEAP) to evaluate and monitor the status of biological communities in lakes in the Adirondack region of New York that have been adversely affected by acid deposition. This program includes chemical analysis of 30 lakes, sampled two to three times each summer. Results of trends analysis for lake chemistry and chlorophyll a (chlor a) are presented for 1994 to 2003, and a general comparison is made with recent results of the Adirondack Long-Term Monitoring (ALTM) Program, which included chemical analysis of all but two of these lakes (plus an additional 24 lakes) monthly, year-round for 1992–2004. Increases in pH were found in 25 of the 30 AEAP lakes (P < 0.05) and increases in acid-neutralizing capacity (ANC) were found in 12 of the 30 lakes (P < 0.05). Concentrations of both SO42− and Mg2+ decreased in 11 lakes (P < 0.05), whereas concentrations of NO3− decreased in 20 lakes (P < 0.05). Concentrations of NH4+ decreased in 10 lakes at a significance level of P < 0.05 and in three other lakes based on P < 0.1. Concentrations of inorganic and organic monomeric aluminum generally were below the reporting limit of 1.5 μmol L−1, but decreases were detected in four and five lakes, respectively (P < 0.1). Concentrations of chlor a increased in seven lakes at a significance level of P < 0.05 and two lakes at a significance level of P < 0.1. A significant inverse correlation was also found between chlor a and NO3− concentrations in nine lakes at a significance level of P < 0.05 and two lakes at a significance level of P < 0.1. Results of AEAP analysis of lake chemistry were similar to those of the ALTM Program, although decreases in SO42− concentrations were more evident in the year-round ALTM record. Overall, the results suggest (a) a degree of chemical recovery from acidification during the summer, (b) an increase in phytoplankton productivity, and (c) a decreasing trend in NO3− concentrations resulting from the increased productivity.

Assessments of acidic deposition effects on aquatic ecosystems have often been hindered by complications from naturally occurring organic acidity. Measurements of pH and ANCG, the most commonly used indicators of chemical effects, can be substantially influenced by the presence of organic acids. Relationships between pH and inorganic Al, which is toxic to many forms of aquatic biota, are also altered by organic acids. However, when inorganic Al concentrations are plotted against ANC (the sum of Ca2+, Mg2+, Na+, and K+, minus S042-, N03-, and Cl-), a distinct threshold for Al mobilization becomes apparent. If the concentration of strong organic anions is included as a negative component of ANC, the threshold occurs at an ANC value of approximately zero, the value expected from theoretical charge balance constraints. This adjusted ANC is termed the base-cation surplus. The threshold relationship between the base-cation surplus and Al was shown with data from approximately 200 streams in the Adirondack region of New York, during periods with low and high dissolved organic carbon concentrations, and for an additional stream from the Catskill region of New York. These results indicate that (1) strong organic anions can contribute to the mobilization of inorganic Al in combination with SO42- and N03-, and (2) the presence of inorganic Al in surface waters is an unambiguous indication of acidic deposition effects.

Measurements of net nitrification rates in forest soils have usually been performed by extended sample incubation (2–8 weeks), either in the field or in the lab. Because of disturbance effects, these measurements are only estimates of nitrification potential and shorter incubations may suffice. In three separate studies of northeastern USA forest soil surface horizons, we found that laboratory nitrification rates measured over 1 day related well to those measured over 4 weeks. Soil samples of Oa or A horizons were mixed by hand and the initial extraction of subsamples, using 2 mol L−1 KCl, occurred in the field as soon as feasible after sampling. Soils were kept near field temperature and subsampled again the following day in the laboratory. Rates measured by this method were about three times higher than the 4-week rates. Variability in measured rates was similar over either incubation period. Because NO3− concentrations were usually quite low in the field, average rates from 10 research watersheds could be estimated with only a single, 1-day extraction. Methodological studies showed that the concentration of NH4+ increased slowly during contact time with the KCl extractant and, thus, this contact time should be kept similar during the procedure. This method allows a large number of samples to be rapidly assessed.

Nitrogen transformation rates in eight northeastern US research sites were measured in soil samples taken in the early season of 2000 and the late season of 2001. Net mineralization and nitrification rates were determined on Oa or A horizon samples by two different sampling methods—intact cores and repeated measurements on composite samples taken from around the cores. Net rates in the composite samples (n=30) showed three different temporal patterns: high net nitrification with minimal NH4+ accumulation, high net nitrification and high NH4+ accumulation, and minimal net nitrification and moderate NH4+ accumulation. The 4-week net rates in intact cores were about half that of the rates from the composite samples but were well related (R2>0.70). Composite samples from sites that exhibited high net nitrification were incubated with acetylene and net nitrification was completely stopped, suggesting an autotrophic pathway. Gross mineralization and nitrification (2000 only) rates were estimated using the isotope dilution technique. Gross rates of nitrification and consumption in intact cores were relatively low. Gross rates of mineralization and net rates of nitrification were both related to the soil C/N ratio, with higher rates generally occurring in sites containing Acer saccharum as a dominant or co-dominant species. The comparison of methods suggests that all provide a similar hierarchy of potential rates but that the degree of net nitrification is strongly influenced by the degree of sample disturbance. Differences between sites appear to be related to an interaction of soil (C/N) and vegetation (A. saccharum contribution) characteristics.