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Abstract Soils are a principal global reservoir of mercury (Hg), a neurotoxic pollutant that is accumulating through anthropogenic emissions to the atmosphere and subsequent deposition to terrestrial ecosystems. The fate of Hg in global soils remains uncertain, however, particularly to what degree Hg is re-emitted back to the atmosphere as gaseous elemental mercury (GEM). Here we use fallout radionuclide (FRN) chronometry to directly measure Hg accumulation rates in soils. By comparing these rates with measured atmospheric fluxes in a mass balance approach, we show that representative Arctic, boreal, temperate, and tropical soils are quantitatively efficient at retaining anthropogenic Hg. Potential for significant GEM re-emission appears limited to a minority of coniferous soils, calling into question global models that assume strong re-emission of legacy Hg from soils. FRN chronometry poses a powerful tool to reconstruct terrestrial Hg accumulation across larger spatial scales than previously possible, while offering insights into the susceptibility of Hg mobilization from different soil environments.

Abstract Fluvial silicon (Si) plays a critical role in controlling primary production, water quality, and carbon sequestration through supporting freshwater and marine diatom communities. Geological, biogeochemical, and hydrological processes, as well as climate and land use, dictate the amount of Si exported by streams. Understanding Si regimes—the seasonal patterns of Si concentrations—can help identify processes driving Si export. We analyzed Si concentrations from over 200 stream sites across the Northern Hemisphere to establish distinct Si regimes and evaluated how often sites moved among regimes over their period of record. We observed five distinct regimes across diverse stream sites, with nearly 60% of sites exhibiting multiple regime types over time. Our results indicate greater spatial and interannual variability in Si seasonality than previously recognized and highlight the need to characterize the watershed and climate variables that affect Si cycling across diverse ecosystems.

Abstract Elevated salt concentrations in streams draining developed watersheds are well documented, but the effects of hydrologic variability and the role of groundwater in surface water salinization are poorly understood. To characterize these effects, we use long‐term data (12–19 yr) and high‐frequency specific conductance (SPC) data collected from 13 streams across New Hampshire, USA. Concentration–discharge (C–Q) relationships for chloride (Cl−) derived from high‐frequency SPC showed distinct seasonal variability. Diluting behavior was common, but flushing behavior occurred in autumn and winter, suggesting that both groundwater and surface runoff contribute salts to streams. Long‐term data show that although extreme flood events initially reduced salt concentrations in groundwater and rural streams, concentrations recovered to preflood conditions in about a decade. Chronic Cl− exceedances occurred in urban streams during all seasons. This research suggests that variation in stream flow, extreme events and application of deicing agents play a role in freshwater salinization.

Abstract Hurricanes and other extreme events are increasing in many regions, yet their long‐term impacts on ecosystem function are uncertain. In forested ecosystems, soil solution chemistry provides an important tool to assess the impacts of disturbance on nutrient cycling and dissolved organic carbon dynamics. Here, we address the dependence of soil solution chemistry on disturbance regime using a novel combination of both experimental and observational results collected over a period of 16 years in montane tropical sites in the Luquillo Experimental Forest of Puerto Rico. Soil solution was sampled following various combinations of canopy trimming and detrital manipulation (2004), repeated manipulation (2014), drought (2015), and Hurricane Maria (2017). Soil solution was sensitive to disturbance but resilient, with return to baseline after 12–18 months. Any disturbance regime that involved loss of canopy and detrital inputs to the forest floor resulted in increased nitrate concentrations, but the response declined with repeated disturbance. Lysimeters in plots that had received no experimental manipulation had 1.5 times higher response to Hurricane Maria than those previously manipulated. The response to disturbance thus showed clear context dependence, with disturbance history affecting disturbance response. Among the nutrients and major ions, only nitrate showed a response to experimental manipulations, drought, and Hurricane Maria. In contrast to nitrate, soil solution potassium was unaltered by initial experimental manipulation but increased dramatically following drought and Hurricane Maria. Phosphorus only increased following Hurricane Maria and only in plots that had twice received experimental trimming and deposition of cut branches on the forest floor. Stoichiometry of dissolved organic matter also changed in these plots, with decreased carbon to nitrogen ratios. The potassium response suggests that damage to roots from tropical cyclones and drought is an important driver of the biogeochemical response to tropical storms. Dampening of soil nitrogen losses and increases in phosphorus losses following successive disturbance events indicates that increased frequency of tropical storms and droughts will result in fundamental alteration of soil biogeochemical cycles, with uncertain effects on forest structure.

The Lotic Intersite Nitrogen eXperiments (LINX I and II) were a series of replicated in situ manipulations of 15N across biomes and land-uses designed to assess the factors that control the removal, retention, and ultimate fate of inorganic nitrogen in stream ecosystems. By studying streams at the continental scale, the lessons learned provide some of the best data available to understand the functional role of streams across the landscape, the management implications of nitrogen uptake in streams and rivers, and the value of small streams in elucidating fundamental principles of ecosystem science. Because small streams are characterized by high throughput and low standing stocks of primary producers and stored carbon and nutrients, they provide unique opportunities to assess the fundamental drivers of nitrogen cycling that would be difficult to conduct in other ecosystems. In addition to the water quality implications of understanding controls on nitrogen delivery to downstream systems, LINX I and II also provide unique insights for ecosystem science and stream ecology more broadly. Here we review a series of ecosystem and network-scale lessons that can be inferred from LINX I and II. We then propose three emergent research questions motivated by the LINX projects which are amenable to future continental-scale work. LINX I and II also demonstrate the value of a highly collaborative, distributed approach to ecosystem science that requires each member of the team to conduct a standardized protocol while simultaneously encouraging team member to improve protocols and develop cross-site projects in his or her specific area of expertise.

Concentration-discharge relationships are a key tool for understanding the sources and transport of material from watersheds to fluvial networks. Storm events in particular provide insight into variability in the sources of solutes and sediment within watersheds, and the hydrologic pathways that connect hillslope to stream channel. Here we examine high-frequency sensor-based specific conductance and turbidity data from multiple storm events across two watersheds (Quebrada Sonadora and Rio Icacos) with different lithology in the Luquillo Mountains of Puerto Rico, a forested tropical ecosystem. Our analyses include Hurricane Maria, a category 5 hurricane. To analyze hysteresis, we used a recently developed set of metrics to describe and quantify storm events including the hysteresis index (HI), which describes the directionality of hysteresis loops, and the flushing index (FI), which can be used to infer whether the mobilization of material is source or transport limited. We also examine the role of antecedent discharge to predict hysteretic behavior during storms. Overall, specific conductance and turbidity showed contrasting responses to storms. The hysteretic behavior of specific conductance was similar across sites, displaying clockwise hysteresis and a negative FI indicating proximal sources of solutes and consistent source limitation. In contrast, the directionality of turbidity hysteresis was significantly different between watersheds, although both had strong flushing behavior indicative of transport limitation. Overall, models that included antecedent discharge did not perform any better than models with peak discharge alone, suggesting that the magnitude and trajectory of an individual event was the strongest driver of material flux and hysteretic behavior. Hurricane Maria produced unique hysteresis metrics within both watersheds, indicating a distinctive response to this major hydrological event. The similarity in response of specific conductance to storms suggests that solute sources and pathways are similar in the two watersheds. The divergence in behavior for turbidity suggests that sources and pathways of particulate matter vary between the two watersheds. The use of high-frequency sensor data allows the quantification of storm events while index-based metrics of hysteresis allow for the direct comparison of complex storm events across a heterogeneous landscape and variable flow conditions.

Streams and rivers of the Luquillo Experimental Forest, Puerto Rico, have been the subject of extensive watershed and aquatic research since the 1980s. This research includes understanding stream export of nutrients and coarse particulate organic matter, physicochemical constituents, aquatic fauna populations and community structure. However, many of the streams and watersheds studied do not appear in standard scale maps. We document recent collaborative and multi-institutional work to improve hydrological network information and identify knowledge gaps. The methods used to delimit and densify stream networks include establishment and incorporation of an updated new vertical datum for Puerto Rico, LIDAR derived elevation, and a combination of visual-manual and automated digitalization processes. The outcomes of this collaborative effort have resulted in improved watershed delineation, densification of hydrologic networks to reflect the scale of on-going studies, and the identification of constraining factors such as unmapped roadways, culverts, and other features of the built environment that interrupt water flow and alter runoff pathways. This work contributes to enhanced knowledge for watershed management, including attributes of riparian areas, effects of road and channel intersections and ridge to reef initiatives with broad application to other watersheds.

Dissolved organic matter (DOM) plays a crucial role in many important processes that take place in terrestrial and aquatic systems. These include carbon and nutrient cycling, pedogenesis, and microbial metabolism. Here we highlight the results of studies that demonstrate the role of DOM in linking terrestrial and aquatic systems. We emphasize three fundamental aspects of the research, which together show the importance of DOM in linking terrestrial and aquatic systems: First, tracing DOM properties during its transport through terrestrial and aquatic systems is a powerful tool for improving our conceptual understanding of the mechanistic drivers of DOM dynamics. Second, linking DOM dynamics to important physical processes such as hydrology provides important insights into the nature of terrestrial–aquatic links. Third, interrelations between DOM dynamics and human impacts on ecosystems highlight how the role of DOM in coupled terrestrial–aquatic systems may change in the future. New measurement and modeling approaches have enabled a more thorough assessment of all three aspects of DOM dynamics. They show that both natural and anthropogenic drivers not only greatly influence DOM dynamics in soils, but owing to the mobility of DOM, also have substantial influence on aquatic systems. This physical connection of soils and surface waters demonstrates the importance of understanding fundamental processes such as nutrient cycling, pedogenesis, and microbial metabolism at a whole‐landscape scale.

Streamwater is affected by several processes in the watershed including anthropogenic activities that result in changes in water quality as well as in the functioning of these stream ecosystems. Therefore, this work aims to evaluate the concentration of major ions (Ca2+, Mg2+, Na+, K+, NH4+, NO3-, NO2-, Cl-, SO4(2-), PO4(3-), HCO3-) in streams in the state of São Paulo (southeast Brazil). The sampling sites are located at undisturbed (ombrophilus dense forest, semideciduous forest and savanna - cerrado) and disturbed areas (pasture, urbanization and sugar cane crops). Streamwater chemistry varied according to land use change and, in general, was higher in disturbed sites. Streams located in undisturbed sites at Ribeira de Iguape/Alto Paranapanema watershed (streams 1, 2 and 3) seem to be regulated by soil characteristics, as the disturbed streams located at the same watershed covered by pasture (stream 7) showed high concentration for the most of the variables. Exception to streams located at Pontal do Paranapanema watershed where both disturbed (stream 8) and undisturbed streams (stream 4 and 5) presented similar patterns for almost all variables measured.A química da água é afetada por diversos processos que ocorrem no entorno da bacia de drenagem incluindo atividades antropogênicas que resultam em mudanças na qualidade da água bem como, no funcionamento desses ecossistemas. Portanto, o objetivo deste estudo foi avaliar a concentração dos íons dissolvidos (Ca2+, Mg2+, Na+, K+, NH4+, NO3-, NO2-, CL-, SO4(2-), PO4(3-), HCO3-) em riachos no Estado de São Paulo (sudeste brasileiro). Os pontos de amostragem estão localizados em bacias não alteradas (floresta ombrófila densa, floresta estacional semidecidual e cerrado) e alteradas (pastagem, urbanização e cana de açúcar). A química dos riachos variou de acordo com o uso da terra, sendo as maiores concentrações encontradas, em geral, nas bacias alteradas. Riachos localizados em áreas pouco alteradas na Bacia de Ribeira do Iguape/Alto Paranapanema (riachos 1, 2 e 3) são, provavelmente, regulados pelas propriedades do solo desde que os riachos alterados (riacho 7) localizados na mesma bacia sob pastagem apresentaram maiores concentrações para a maioria dos parâmetros avaliados. Exceção aos riachos localizados na Bacia do Pontal do Paranapanema onde ambos os riachos, alterados (riacho 8) e pouco alterados (riachos 4 e 5), apresentaram padrões similares para a maioria das variáveis avaliadas.

The establishment of sown pasture is an important agricultural practice in many landscapes. Although both native grassland and sown pasture play a key role in the global carbon cycle, due to lack of data and field experiments, our understanding of grassland CH4 fluxes and CO2 emissions remains limited, especially when it comes to sown pasture. We measured ecosystem respiration and CH4 fluxes in response to a variety of potential drivers (soil temperature, soil moisture, ammonium nitrogen, nitrate nitrogen and dissolved organic carbon) in CG (continuous grazing), RG (rotational grazing) and UG (ungrazed) plots in sown grassland for one year in Inner Mongolia. Fluxes of CH4 and ecosystem respiration were measured using static opaque chambers and gas chromatography. Grazing significantly reduced ecosystem respiration (p < 0.01), and grazing pattern significantly influenced respiration in CG and RG plots (p < 0.01). We find that the sown grassland is a net sink for atmospheric CH4. No influence of grazing pattern was observed on CH4 flux in CG, RG and UG (p > 0.05). Soil temperature is the most important factor influencing ecosystem respiration and CH4 flux in the sown grassland, with soil moisture playing a secondary role to soil temperature. Variation in levels of ammonium nitrogen, nitrate nitrogen and dissolved organic carbon had little influence on ecosystem respiration or CH4 flux (except in UG plots). The values obtained for ecosystem respiration of grasslands have a large uncertainty range, which may be due to spatial variability as well as differences in research methods. Mean CH4 fluxes measured only during the growing season were much higher than the annual mean CH4 fluxes.

Ecologists have developed terminology to distinguish ecosystems based on the degree of human alteration. To this end, ecosystems can be characterized as "novel ecosystems," "impacted ecosystems," or "designed ecosystems," depending on the role of human management in ecosystem development and effects on ecosystem properties. Properly classifying an ecosystem as novel, impacted, or designed has critical implications for its conservation and management, but a broadly applicable definition for a "novel ecosystem" does not exist. We have provided a formal definition of "novel ecosystem" that facilitates its use in practical applications and have described four characteristics of such an ecosystem. A novel ecosystem can be identified by its origins rooted in human agency, the ecological thresholds it has crossed, a significantly altered species composition, and a capacity to sustain itself. Ecosystem classification in the literature has been inconsistent. We have illustrated the application of our definition using multiple case studies representing impacted, designed, and novel ecosystems.

The forests of central Europe have undergone remarkable transitions in the past 40 years as air quality has improved dramatically. Retrospective analysis of Norway spruce (Picea abies) tree rings in the Czech Republic shows that air pollution (e.g. SO2 concentrations, high acidic deposition to the forest canopy) plays a dominant role in driving forest health. Extensive soil acidification occurred in the highly polluted "Black Triangle" in Central Europe, and upper mineral soils are still acidified. In contrast, acidic atmospheric deposition declined by 80% and atmospheric SO2 concentration by 90% between the late 1980s and 2010s. In this study we oserved that annual tree ring width (TRW) declined in the 1970s and subsequently recovered in the 1990s, tracking SO2 concentrations closely. Furthermore, recovery of TRW was similar in unlimed and limed stands. Despite large increases in soil base saturation, as well as soil pH, as a result of repeated liming starting in 1981, TRW growth was similar in limed and unlimed plots. TRW recovery was interrupted in 1996 when highly acidic rime (originating from more pronounced decline of alkaline dust than SO2 from local power plants) injured the spruce canopy, but recovered soon to the pre-episode growth. Across the long-term site history, changes in soil chemistry (pH, base saturation, Bc/Al soil solution ratio) cannot explain observed changes in TRW at the two study sites where we tracked soil chemistry. Instead, statistically significant recovery in TRW is linked to the trajectory of annual SO2 concentrations or sulfur deposition at all three stands.

Mobilization of trace metals from soils to surface waters can impact both human and ecosystem health. This study resamples a water sample archive to explore the spatial pattern of streamwater total concentrations of arsenic, cadmium, copper, lead, and zinc and their associations with biogeochemical controls in northern New England. Road deicing appears to result in elevated trace metal concentrations, as trace metal concentrations are strongly related to sodium concentrations and are most elevated when the sodium: chloride ratio is near 1.0 (~halite). Our results are consistent with previous laboratory and field studies that indicate cation exchange as a metal mobilization mechanism when road salt is applied to soils containing metals. This study also documents associations among sodium, chloride, dissolved organic carbon, iron, and metal concentrations, suggesting cation exchange mechanisms related to road deicing are not the only mechanisms that increase trace metal concentrations in surface waters. In addition to cation exchange, this study considers dissolved organic carbon complexation and oxidation-reduction conditions affecting metal mobility from soils in a salt-rich environment. These observations demonstrate that road deicing has the potential to increase streamwater trace metal concentrations across broad spatial scales and increase risks to human and ecosystem health.

Stream water dissolved organic carbon (DOC) correlates positively with soil organic carbon (SOC) in many biomes. Does this relationship hold in a small geographic region when variations of temperature, precipitation and vegetation are driven by a significant altitudinal gradient? We examined the spatial connectivity between concentrations of DOC in headwater stream and contents of riparian SOC and water-soluble soil organic carbon (WSOC), riparian soil C:N ratio, and temperature in four vegetation types along an altitudinal gradient in the Wuyi Mountains, China. Our analyses showed that annual mean concentrations of headwater stream DOC were lower in alpine meadow (AM) than in subtropical evergreen broadleaf forest (EBF), coniferous forest (CF), and subalpine dwarf forest (SDF). Headwater stream DOC concentrations were negatively correlated with riparian SOC as well as WSOC contents, and were unrelated to riparian soil C:N ratio. Our findings suggest that DOC concentrations in headwater streams are affected by different factors at regional and local scales. The dilution effect of higher precipitation and adsorption of soil DOC to higher soil clay plus silt content at higher elevation may play an important role in causing lower DOC concentrations in AM stream of the Wuyi Mountains. Our results suggest that upscaling and downscaling of the drivers of DOC export from forested watersheds when exploring the response of carbon flux to climatic change or other drivers must done with caution.