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The pace and trajectory of ecosystem development are governed by the availability and cycling of limiting nutrients, and anthropogenic disturbances such as acid rain and deforestation alter these trajectories by removing substantial quantities of nutrients via titration or harvest. Here, we use six decades of continuous chemical and hydrologic data from three adjacent headwater catchments in the Hubbard Brook Experimental Forest, New Hampshire—one deforested (W5), one CaSiO3-enriched (W1), and one reference (W6)—to quantify long-term nutrient and mineral fluxes. Acid deposition since 1900 drove pronounced depletion and export of base cations, particularly calcium, across all watersheds. Experimental deforestation of W5 intensified loss of biomass and nutrient cations and triggered sustained increases in streamwater pH, Ca2+, and SiO2 exports over nearly four decades, greatly exceeding the effects of direct CaSiO3 enrichment in both duration and magnitude. We detect no long-term changes in water yield or water flow paths in the experimental watersheds, and we attribute this multidecadal increase in weathering rates following deforestation to biological responses to severe nutrient limitation. Our evidence suggests that in the regrowing forest, plants are investing photosynthate into belowground processes that amplify mineral weathering to access phosphorus and micronutrients, consequently elevating the export of less limiting elements present in silicate parent material. Throughout decades of forest regrowth, enhanced biotic weathering has continued to deplete the acid buffering capacity of the terrestrial ecosystem while the export of weathering products has elevated the pH of the receiving stream. 

Abstract Riverine silicon (Si) plays a vital role in governing primary production, water quality, and carbon cycling. Climate and land cover change have altered how dissolved Si (DSi) is processed on land, transported to rivers, and cycled through aquatic ecosystems. The Global Aggregation of Stream Silica (GlASS) database was constructed to assess changes in river Si concentrations and fluxes, their relationship to other nutrients (nitrogen (N) and phosphorus (P)), and to evaluate mechanisms driving the availability of Si. GlASS includes concentrations of DSi, dissolved inorganic N (NO₃, NO_x, and NH₄), and dissolved inorganic P (as soluble reactive P or PO₄-P) at daily to quarterly time steps from 1963 to 2024; daily discharge; and watershed characteristics for 421 rivers spanning eight climate zones. Original data sources are cited, data quality assurance workflows are public, and input files to a common load model are provided. GlASS offers critical data to address questions about patterns, controls, and trajectories of global river Si biogeochemistry and stoichiometry. 

The Lamprey River watershed, located in southeastern New Hampshire (USA), drains 554 km² of low elevation land before discharging into the Great Bay Estuary (Wymore and others 2021). The watershed is classified as suburban with mixed land-use that includes forests (73%), wetlands (10%), development (7%), and agriculture (NOAA Coastal Change Analysis Program 2016). We selected four distinct sites within the watershed to capture the dynamics of both tributaries and the mainstem, while accounting for variations in land use, land cover, and nutrient availability. Wednesday Hill Brook (WHB) is a 1st-order stream that drains a residential landscape and has the highest NO3 concentrations among the sites due to a high density of septic systems (Flint and McDowell 2015). Dowst Cate Forest (DCF) is a 2nd-order stream draining a headwater wetland and forested landscape and is characterized by the highest concentrations of dissolved organic carbon (DOC). The two main stem Lamprey River sites, LMP72 and LMP73, exhibit moderate concentrations of both DOC and NO3 and are located approximately 1 km apart. LMP72 is located at a low-head run-of-river dam while LMP73 is free-flowing water downstream of the reservoir. Our dataset includes weekly water chemistry and dissolved gas data collected from April 2014 through May 2023, except for DCF where data collection ended in 2021, resulting in a total of 1,179 observations across the four different sites. 

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 Climate and atmospheric deposition interact with watershed properties to drive dissolved organic carbon (DOC) concentrations in lakes. Because drivers of DOC concentration are inter-related and interact, it is challenging to assign a single dominant driver to changes in lake DOC concentration across spatiotemporal scales. Leveraging forty years of data across sixteen lakes, we used structural equation modeling to show that the impact of climate, as moderated by watershed characteristics, has become more dominant in recent decades, superseding the influence of sulfate deposition that was observed in the 1980s. An increased percentage of winter precipitation falling as rain was associated with elevated spring DOC concentrations, suggesting a mechanistic coupling between climate and DOC increases that will persist in coming decades as northern latitudes continue to warm. Drainage lakes situated in watersheds with fine-textured, deep soils and larger watershed areas exhibit greater variability in lake DOC concentrations compared to both seepage and drainage lakes with coarser, shallower soils, and smaller watershed areas. Capturing the spatial variability in interactions between climatic impacts and localized watershed characteristics is crucial for forecasting lentic carbon and nutrient dynamics, with implications for lake ecology and drinking water quality. 

Abstract The seasonal behavior of fluvial dissolved silica (DSi) concentrations, termedDSi regime, mediates the timing of DSi delivery to downstream waters and thus governs river biogeochemical function and aquatic community condition. Previous work identified five distinct DSi regimes across rivers spanning the Northern Hemisphere, with many rivers exhibiting multiple DSi regimes over time. Several potential drivers of DSi regime behavior have been identified at small scales, including climate, land cover, and lithology, and yet the large‐scale spatiotemporal controls on DSi regimes have not been identified. We evaluate the role of environmental variables on the behavior of DSi regimes in nearly 200 rivers across the Northern Hemisphere using random forest models. Our models aim to elucidate the controls that give rise to (a) average DSi regime behavior, (b) interannual variability in DSi regime behavior (i.e., Annual DSi regime), and (c) controls on DSi regime shape (i.e., minimum and maximum DSi concentrations). Average DSi regime behavior across the period of record was classified accurately 59% of the time, whereas Annual DSi regime behavior was classified accurately 80% of the time. Climate and primary productivity variables were important in predicting Average DSi regime behavior, whereas climate and hydrologic variables were important in predicting Annual DSi regime behavior. Median nitrogen and phosphorus concentrations were important drivers of minimum and maximum DSi concentrations, indicating that these macronutrients may be important for seasonal DSi drawdown and rebound. Our findings demonstrate that fluctuations in climate, hydrology, and nutrient availability of rivers shape the temporal availability of fluvial DSi. 

Abstract Nitrogen (N) wet deposition chemistry impacts watershed biogeochemical cycling. The timescale and magnitude of (a)synchrony between wet deposition N inputs and watershed N outputs remains unresolved. We quantify deposition‐river N (a)synchrony with transfer entropy (TE), an information theory metric enabling quantification of lag‐dependent feedbacks in a hydrologic system by calculating directional information flow between variables. Synchrony is defined as a significant amount of TE‐calculated reduction in uncertainty of river N from wet deposition N after conditioning for antecedent river N conditions. Using long‐term timeseries of wet deposition and river DON, NO₃⁻, and NH₄⁺concentrations from the Lamprey River watershed, New Hampshire (USA), we constrain the role of wet deposition N to watershed biogeochemistry. Wet deposition N contributed information to river N at timescales greater than quick‐flow runoff generation, indicating that river N losses are a lagged non‐linear function of hydro‐biogeochemical forcings. River DON received the most information from all three wet deposition N solutes while wet deposition DON and NH₄⁺contributed the most information to all three river N solutes. Information theoretic algorithms facilitated data‐driven inferences on the hydro‐biogeochemical processes influencing the fate of N wet deposition. For example, signals of mineralization and assimilation at a timescale of 12 to 21‐weeks lag display greater synchrony than nitrification, and we find that N assimilation is a positive lagged function of increasing N wet deposition. Although wet deposition N is not the main driver of river N, it contributes a significant amount of information resolvable at time scales of transport and transformations.