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Understanding how subsurface water storage—created and structured by the geology and geomorphology of the critical zone—governs hydrologic connectivity between landscapes and streams is essential for explaining spatial and temporal variation in stream water chemistry. Most headwater studies have focused on high‐resolution stream water chemistry at the catchment outlet, rarely examining the spatial variability among tributaries and the main channel, or how these patterns relate to the underlying geology and geomorphology. Linking upstream spatial and temporal variability with chemical dynamics at the outlet over time is even less common. We conducted weekly synoptic sampling along Lookout Creek, located within the HJ Andrews Experimental Forest Long Term Ecological Research programme. Lookout Creek is in the volcanic terrain of the western Cascades, Oregon. The catchment spans multiple geologic units (e.g., lava flows) and geomorphic features (e.g., earthflows). We measured stream chemistry along the main stem and five tributaries to assess how varying degrees of hydrologic connectivity influence solute concentrations and transport across this geologic and geomorphologic template. To identify the timing and magnitude of hydrologic connectivity between tributaries, the main stem, and the catchment outlet, we analysed spatiotemporal patterns in stream chemistry using concentration‐discharge relationships, principal component analysis, and a metric of subcatchment synchrony. We found that in previously glaciated catchments with active earthflows, solute concentrations and base‐cation‐to‐silica ratios were higher, and more solutes had a chemostatic or mobilising behaviour, indicating high subsurface storage. This variability in subsurface storage, and its influence on hydrologic connectivity, ultimately determined the degree of chemical synchrony with the catchment outlet. Our findings suggest that, under future climate scenarios with shifts in precipitation phase and timing, headwater systems with substantial subsurface storage are likely to be more chemically resilient. 

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. 

Biogeochemical properties of soils play a crucial role in soil and stream chemistry throughout a watershed. How water interacts with soils during subsurface flow can have impacts on water quality, thus, it is fundamental to understand where and how certain soil water chemical processes occur within a catchment. In this study, ~200 soil samples were evaluated throughout a small catchment in the Front Range of Colorado, USA to examine spatial and vertical patterns in major soil solutes among different landscape units: riparian areas, alluvial/colluvial fans, and steep hillslopes. Solutes were extracted from the soil samples in the laboratory and analyzed for major cation (Li, K, Mg, Br, and Ca) and anion (F, Cl, NO 2 , NO 3 , PO 4 , and SO 4 ) concentrations using ion chromatography. Concentrations of most solutes were greater in near surface soils (10 cm) than in deeper soils (100 cm) across all landscape units, except for F which increased with depth, suggestive of surface accumulation processes such as dust deposition or enrichment due to biotic cycling. Potassium had the highest variation between depths, ranging from 1.04 mg/l (100 cm) to 3.13 mg/l (10 cm) sampled from riparian landscape units. Nearly every solute was found to be enriched in riparian areas where vegetation was visibly denser, with higher mean concentrations than the hillslopes and fans, except for NO 3 which had higher concentrations in the fans. Br, NO 2 , and PO 4 concentrations were often below the detectable limit, and Li and Na were not variable between depths or landscape units. Ratioed stream water concentrations (K:Na, Ca:Mg, and NO 3 :Cl) vs. discharge relationships compared to the soil solute ratios indicated a hydraulic disconnection between the shallow soils (<100 cm) and the stream. Based on the comparisons among depths and landscape units, our findings suggest that K, Ca, F, and NO 3 solutes may serve as valuable tracers to identify subsurface flowpaths as they are distinct among landscape units and depth within this catchment. However, interflow and/or shallow groundwater flow likely have little direct connection to streamflow generation. 

Riverine silicon (Si) plays a vital role in governing primary production, water quality, and carbon sequestration. The Global Aggregation of Stream Silica (GlASS) database was constructed to assess changes in riverine Si concentrations and fluxes, their relationship to available nutrients, and to evaluate mechanisms driving these patterns. GlASS includes dissolved Si (DSi), dissolved inorganic nitrogen, and dissolved inorganic phosphorus concentrations at daily to quarterly time steps, daily discharge, and watershed characteristics for rivers with drainage areas ranging < 1 km2 to 3 million km2 and spanning eight climate zones, mainly in the northern hemisphere. Data range between years 1963 and 2023. GlASS uses publicly available datasets, ensuring transparency and reproducibility. Original data sources are cited, data quality assurance workflows are public, and input files to a common load estimator are provided. 

This dataset includes monthly dissolved silicon (DSi) concentration data from 198 rivers across the Northern Hemisphere. Concentration and discharge data were sourced from public and/or published datasets and the Weighted Regressions on Time, Discharge, and Season model (Hirsch et al. 2010) was used to estimate monthly concentrations and flow-normalized concentrations for all sites over their period of record. Sites span eight climate zones, ranged from 18 degrees N to 70 degrees N, and vary in drainage area from < 1 km2 to nearly 3 million km2. These monthly concentration data were then used to cluster sites into average (i.e., average of all years) and annual (i.e., each year individually) seasonal regimes using a time-series clustering approach. The annual regimes were used to quantify how often a site moved among regimes over its period of record (i.e., stability). Site characteristics including climate zone, discharge, and concentration-discharge behavior were explored as potential drivers of cluster membership and stability. 

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.