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Abstract. Large sample datasets are transforming the catchment sciences, but there are few off-the-shelf stream water chemistry datasets with complementary atmospheric deposition, streamflow, meteorology, and catchment physiographic attributes. The existing CAMELS (Catchment Attributes and Meteorology for Large-sample Studies) dataset includes data on topography, climate, streamflow, land cover, soil, and geology across the continental US. With CAMELS-Chem, we pair these existing attribute data for 516 catchments with atmospheric deposition data from the National Atmospheric Deposition Program and water chemistry and instantaneous discharge data from the US Geological Survey over the period from 1980 through 2018 in a relational database and corresponding dataset. The data include 18 common stream water chemistry constituents: Al, Ca, Cl, dissolved organic carbon, total organic carbon, HCO3, K, Mg, Na, total dissolved N, total organic N, NO3, dissolved oxygen, pH (field and lab), Si, SO4, and water temperature. Annual deposition loads and concentrations include hydrogen, NH4, NO3, total inorganic N, Cl, SO4, Ca, K, Mg, and Na. We demonstrate that CAMELS-Chem water chemistry data are sampled effectively across climates, seasons, and discharges for trend analysis and highlight the coincident sampling of stream constituents for process-based understanding. To motivate their use by the larger scientific community across a variety of disciplines, we show examples of how these publicly available datasets can be applied to trend detection and attribution, biogeochemical process understanding, and new hypothesis generation via data-driven techniques. 

Abstract. Climate warming will cause mountain snowpacks to melt earlier, reducing summer streamflow and threatening water supplies and ecosystems. Quantifying how sensitive streamflow timing is to climate change and where it is most sensitive remain key questions. Physically based hydrological models are often used for this purpose; however, they have embedded assumptions that translate into uncertain hydrological projections that need to be quantified and constrained to provide reliable inferences. The purpose of this study is to evaluate differences in projected end-of-century changes to streamflow timing between a new empirical model based on diel (daily) streamflow cycles and regional land surface simulations across the mountainous western USA. We develop an observational technique for detecting streamflow responses to snowmelt using diel cycles of incoming solar radiation and streamflow to detect when snowmelt occurs. We measure the date of the 20th percentile of snowmelt days (DOS20) across 31 western USA watersheds affected by snow, as a proxy for the beginning of snowmelt-initiated streamflow. Historic DOS20 varies from mid-January to late May among our sites, with warmer basins having earlier snowmelt-mediated streamflow. Mean annual DOS20 strongly correlates with the dates of 25 % and 50 % annual streamflow volume (DOQ25 and DOQ50, both R2=0.85), suggesting that a 1 d earlier DOS20 corresponds with a 1 d earlier DOQ25 and 0.7 d earlier DOQ50. Empirical projections of future DOS20 based on a stepwise multiple linear regression across sites and years under the RCP8.5 scenario for the late 21st century show that DOS20 will occur on average 11±4 d earlier per 1 ∘C of warming. However, DOS20 in colder watersheds (mean November–February air temperature, TNDJF<-8 ∘C) is on average 70 % more sensitive to climate change than in warmer watersheds (TNDJF>0 ∘C). Moreover, empirical projections of DOQ25 and DOQ50 based on DOS20 are about four and two times more sensitive to climate change, respectively, than those simulated by a state-of-the-art land surface model (NoahMP-WRF) under the same scenario. Given the importance of changes in streamflow timing for water resources, and the significant discrepancies found in projected streamflow sensitivity, snowmelt detection methods such as DOS20 based on diel streamflow cycles may help to constrain model parameters, improve hydrological predictions, and inform process understanding. 

Understanding and predicting catchment responses to a regional disturbance is difficult because catchments are spatially heterogeneous systems that exhibit unique moderating characteristics. Changes in precipitation composition in the Northeastern U.S. is one prominent example, where reduction in wet and dry deposition is hypothesized to have caused increased dissolved organic carbon (DOC) export from many northern hemisphere forested catchments; however, findings from different locations contradict each other. Using shifts in acid deposition as a test case, we illustrate an iterative “process and pattern” approach to investigate the role of catchment characteristics in modulating the steam DOC response. We use a novel dataset that integrates regional and catchment-scale atmospheric deposition data, catchment characteristics and co-located stream Q and stream chemistry data. We use these data to investigate opportunities and limitations of a pattern-to-process approach where we explore regional patterns of reduced acid deposition, catchment characteristics and stream DOC response and specific soil processes at select locations. For pattern investigation, we quantify long-term trends of flow-adjusted DOC concentrations in stream water, along with wet deposition trends in sulfate, for USGS headwater catchments using Seasonal Kendall tests and then compare trend results to catchment attributes. Our investigation of climatic, topographic, and hydrologic catchment attributes vs. directionality of DOC trends suggests soil depth and catchment connectivity as possible modulating factors for DOC concentrations. This informed our process-to-pattern investigation, in which we experimentally simulated increased and decreased acid deposition on soil cores from catchments of contrasting long-term DOC response [Sleepers River Research Watershed (SRRW) for long-term increases in DOC and the Susquehanna Shale Hills Critical Zone Observatory (SSHCZO) for long-term decreases in DOC]. SRRW soils generally released more DOC than SSHCZO soils and losses into recovery solutions were higher. Scanning electron microscope imaging indicates a significant DOC contribution from destabilizing soil aggregates mostly from hydrologically disconnected landscape positions. Results from this work illustrate the value of an iterative process and pattern approach to understand catchment-scale response to regional disturbance and suggest opportunities for further investigations. 

Abstract Research at long‐term catchment monitoring sites has generated a great volume, variety, and velocity of data for analysis of stream water chemistry dynamics. To harness the potential of these big data and extract patterns that are indicative of underlying functional relationships, machine learning tools have advantages over traditional statistical methods, and are increasingly being applied for dimension reduction, feature extraction, and trend identification. Still, as examples of complex systems, catchments are characterized by multivariate factor interactions and equifinality that are not easily identified by most machine‐learning methods. Using dissolved organic carbon (DOC) dynamics as an illustration, we applied a new evolutionary algorithm (EA) to extract geologic, topographic, meteorologic, hydrologic, and land use attributes that were correlated to mean stream DOC concentration in forested catchments distributed across the continental United States. The EA reduced dimensionality of our attribute dataset to identify the combination of factors, and their specific value ranges, that interacted to drive membership in High or Low mean DOC clusters. High mean DOC concentrations were associated with two distinct geographic locations of variable climatic and vegetative conditions, indicating equifinality. Our findings underscore the importance of critical zone structure in mediating hydrological and biogeochemical processes to govern DOC dynamics at the catchment scale. This multi‐scale, pattern‐to‐process approach is being applied to refine hypotheses for process‐based modeling of DOC dynamics in forested headwater streams at catchment to site scales. 

Abstract The shallow and deep hypothesis suggests that stream concentration‐discharge (CQ) relationships are shaped by distinct source waters from different depths. Under this hypothesis, baseflows are typically dominated by groundwater and mostly reflect groundwater chemistry, whereas high flows are typically dominated by shallow soil water and mostly reflect soil water chemistry. Aspects of this hypothesis draw on applications like end member mixing analyses and hydrograph separation, yet direct data support for the hypothesis remains scarce. This work tests the shallow and deep hypothesis using co‐located measurements of soil water, groundwater, and streamwater chemistry at two intensively monitored sites, the W‐9 catchment at Sleepers River (Vermont, United States) and the Hafren catchment at Plynlimon (Wales). At both sites, depth profiles of subsurface water chemistry and stream CQ relationships for the 10 solutes analyzed are broadly consistent with the hypothesis. Solutes that are more abundant at depth (e.g., calcium) exhibit dilution patterns (concentration decreases with increasing discharge). Conversely, solutes enriched in shallow soils (e.g., nitrate) generally exhibit flushing patterns (concentration increases with increasing discharge). The hypothesis may hold broadly true for catchments that share such biogeochemical stratifications in the subsurface. Soil water and groundwater chemistries were estimated from high‐ and low‐flow stream chemistries with average relative errors ranging from 24% to 82%. This indicates that streams mirror subsurface waters: stream chemistry can be used to infer scarcely measured subsurface water chemistry, especially where there are distinct shallow and deep end members.