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One of the principal questions in hydrology is how and when water leaves the critical zone storage as either stream flow or evapotranspiration. We investigated subsurface water storage and storage selection of the Southern Sierra Critical Zone Observatory (California, USA) within the age-ranked storage selection framework, constrained by a novel combination of cosmogenic radioactive and stable isotopes: tritium, sodium-22, sulfur-35, and oxygen-18. We found a significant positive correlation between tritium and stream flow rate and between sulfur-35 and stream flow rate, indicating that the age distribution of stream flow varies with stream flow rate. Storage selection functions that vary with stream flow rate are better able to reproduce tritium concentrations in stream flow than functions that are constant in time. For the Southern Sierra Critical Zone, there is a strong preference to discharge the oldest water in storage during dry conditions but only a weak preference for younger water during wet conditions. The preference of evapotranspiration for younger water, constrained by oxygen-18 in stream water, is essential to parameterize subsurface storage but needs to be confirmed by isotopic or other investigations of evapotranspiration. This is the first study to illustrate how a combination of cosmogenic radioactive isotopes reveals the hydrochronology and water storage dynamics of catchments, constrains the subsurface architecture of the critical zone, and provides insight into landscape evolution.Plain Language Summary Watersheds store water underground in soils and weathered bedrock.How long it takes for water to flow through the subsurface to feed streams is difficult to measure but important to understand how watersheds function. We used a novel combination of isotopic tracer methods to study the mixture of water ages in Providence Creek, a stream in the southern Sierra Nevada, California (USA). We studied naturally occurring radioactive isotopes of hydrogen (tritium), sodium-22, and sulfur-35. The abundance of these isotopes decreases because of radioactive decay as water spends more time underground. Each of these isotopes has a distinct half-life (12.3 years, 2.6 years, and 87 days, respectively). By using this combination of isotopes we were able to tease out the mixture of water ages in the stream. This level of detail helps us understand how the subsurface "selects" water from storage to generate stream flow. We find that Providence Creek has a strong preference to remove the oldest water in storage during dry conditions but shows only a slight preference to remove younger water during wet conditions. Based on the age mixtures of stream water, we estimate that the Providence Creek watershed stores 3 m of water in the subsurface.

We present results from field studies at two central California dairies that demonstrate the prevalence of saturated-zone denitrification in shallow groundwater with 3H/ 3He apparent ages of < 35 years. Concentrated animal feeding operations are suspected to be major contributors of nitrate to groundwater, but saturated zone denitrification could mitigate their impact to groundwater quality. Denitrification is identified and quantified using N and O stable isotope compositions of nitrate coupled with measurements of excess N2 and residual NO3(-) concentrations. Nitrate in dairy groundwater from this study has delta15N values (4.3-61 per thousand), and delta18O values (-4.5-24.5 per thousand) that plot with delta18O/delta15N slopes of 0.47-0.66, consistent with denitrification. Noble gas mass spectrometry is used to quantify recharge temperature and excess air content. Dissolved N2 is found at concentrations well above those expected for equilibrium with air or incorporation of excess air, consistent with reduction of nitrate to N2. Fractionation factors for nitrogen and oxygen isotopes in nitrate appear to be highly variable at a dairy site where denitrification is found in a laterally extensive anoxic zone 5 m below the water table, and at a second dairy site where denitrification occurs near the water table and is strongly influenced by localized lagoon seepage.

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The NG-MIMS system is capable of providing analyses sufficiently accurate and precise for introduced noble gas tracers at managed aquifer recharge facilities, groundwater fingerprinting based on excess air and noble gas recharge temperature, and field and laboratory studies investigating ebullition and diffusive exchange.

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