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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 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. 

After 4.5 billion years as an evolving and dynamic planet, the Earth continues to evolve but with human‐altered dynamics. Earth scientists have special opportunities and responsibilities to accelerate our understanding of Earth's changes that are transforming our most remarkable home. 

Key Points We re‐evaluate equations proposed by Francis Hall to assess concentration‐discharge ( C ‐ Q ) relationships using newly available long‐term and high‐frequency data sets Across time steps we find that log‐log and log‐linear models perform equally well to describe C ‐ Q relationships Parametrization of storage‐discharge relationships via recession analyses provides additional insight to C ‐ Q relationships 

Abstract Dissolved organic matter (DOM) is a heterogeneous mixture of organic compounds that is produced through both microbial degradation and abiotic leaching of solid phase organic matter, and by a wide range of metabolic processes in algae and higher plants. DOM is ubiquitous throughout the hydrologic cycle and plays an important role in watershed management for drinking water supply as well as many aspects of aquatic ecology and geochemistry. Due to its wide-ranging effects in natural waters and analytical challenges, the focal research questions regarding DOM have varied since the 1920s. A standard catchment-scale model has emerged to describe the environmental controls on DOM concentrations. Modest concentrations of DOM are found in atmospheric deposition, large increases occur in throughfall and shallow soil flow paths, and variable concentrations in surface waters occur largely as a result of the extent to which hydrologic flow paths encounter deeper mineral soils, wetlands or shallow organic-rich riparian soils. Both production and consumption of DOM occur in surface waters but appear to frequently balance, resulting in relatively constant concentrations with distance downstream in most streams and rivers. Across biomes the concentration and composition of DOM in flowing waters is driven largely by soil processes or direct inputs to channels, but high levels can be found in streams and rivers from the tropics to the poles. Seven central challenges and opportunities in the study of DOM should frame ongoing research. These include maintaining or establishing long-term records of changes in concentrations and fluxes over time, capitalizing on the use of sensors to describe short-term DOM dynamics in aquatic systems, integrating the full carbon cycle into understanding of watershed and aquatic DOM dynamics, understanding the role of DOM in evasion of greenhouse gases from inland waters, unraveling the enigma of dissolved organic nitrogen, documenting gross versus net DOM fluxes, and moving beyond an emphasis on functional ecological significance to understanding the evolutionary significance of DOM in a wide range of environments.