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Historical use of fertilizer and manure on farmlands is known to have a lasting impact on ecosystems and water resources, but few studies assess the legacy of nitrate pollution on groundwater and surface water after farming applications were reduced. We studied the response of nitrate in spring water to a reduction of nitrogen fertilizer applications in agriculture realized since the mid-1980s. We assessed the travel time distribution of groundwater based on a time series of tritium measurements for 90 springs and small brooks that drain a dual porosity chalk aquifer. The travel time distributions were constrained using the tritium data in combination with time series of nitrate concentrations, applying a shape-free travel time distribution model. A clear trend reversal of nitrate concentrations was observed and simulated for springs with a large fraction of young water (< 30 years old) whereas the nitrate response in springs with relatively older water was attenuated and delayed. We conclude that obtaining a time series of tritium data helps to constrain age distributions of water that is discharged from dual permeability aquifers. The fraction of water aged <30 years was a meaningful parameter to distinguish between different types of springs. Nitrate trends in springs that drain large fractions of young water (> 0.6) show higher peak concentrations, shorter lag-time between leaching and outflow peaks and steeper declines after trend reversal, relative to trends in springs which are dominantly fed by older groundwater. The study thus shows that the nitrate legacy of groundwater systems is strongly determined by the range of their travel time distributions, and trend reversal in receiving springs and surface waters may appear within 10 to 15 years after measures to reduce nitrate losses from farming.

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Contamination from acid mine drainage affects ecosystems and usability of groundwater for domestic and municipal purposes. The Captain Jack Superfund Site outside of Ward, Boulder County, Colorado, USA, hosts a draining mine adit that was remediated through emplacement of a hydraulic bulkhead to preclude acid mine drainage from entering nearby Lefthand Creek. During impoundment of water within the mine workings in 2020, a diverse and novel dataset of stable isotopes of water, sulfate, and carbon (δ2H, δ18OH2O, δ18OSO4, δ34S, δ13CDIC), rare earth elements, and environmental tracers (noble gases and tritium) were collected to understand groundwater recharge and mixing, mechanisms of sulfide oxidation and water-rock interaction, and the influence of remediation on the hydrologic and geochemical system. Water isotopes indicate that groundwater distal from the mine workings has seasonally variable recharge sources whereas water within the workings has a distinctive composition with minimal temporal variability. Sulfate isotopes indicate that sulfide oxidation occurs both within the mine workings and in adjacent igneous dikes, and that sulfide oxidation may occur under suboxic conditions with ferric iron as the oxidant. Carbon isotopes track the neutralization of acidic waters and the carbon mass budget of the system. Rare earth elements corroborate stable isotopes in indicating groundwater compartmentalization, and additionally illustrate enhanced mineral weathering in the mine workings. Environmental tracers indicate mixing of modern and pre-modern groundwater and inform timelines that active remediation may be needed. Together these datasets provide a useful template for similar investigations of abandoned mine sites where physical mixing processes, sources of solute loading, or remediation timeframes are of importance.

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Krypton-81 was applied to investigate the age of groundwater in the aquifer system in the Bangkok metropolitan and vicinity areas. Stable (2H, 18O and 13C) and radioactive (3H, 85Kr and 14C) isotopes and noble gases were applied in parallel. Low levels of 14C and significant radiogenic 4He confirm that groundwater in the deep aquifers is older than 30 ka. 81Kr analysis identified groundwater with ages ranging from 17 to 300 ka. At some sites, large age discrepancies between 81Kr and 14C indicated that inter-aquifer mixing is likely occurring. The interpretation of the noble gases suggests that groundwaters in the deeper aquifers, with apparent ages of 300 to 10 ka, have recharged in slightly colder and wetter climates than those found in the upper aquifers with apparent ages < 10 ka. Degradation of water quality from seawater intrusion was identified in the upper four aquifers. This was also evidenced by higher δ18O and δ2H values, typical of seawater. The four deeper aquifers contain high quality water characterised by less enriched 18O and 2H. This work presents new findings of very old groundwater in the Bangkok aquifer system.

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Identifying nitrate sources and their temporal evolution in different land use is important for the sustainable management of groundwater resources. In this study, groundwater dating (3H-3He and time series of 3H) was combined with chemical and stable isotope analyses to resolve the evolution of nitrate sources and the driving mechanism of nitrate contamination. Approximately 75% of the groundwater samples (collected in 2014 and 2018) had nitrate concentrations exceeding World Health Organization's guideline for drinking water (50 mg/L), and 44% exceeded the groundwater quality standard of China (88.6 mg/L), indicating severe nitrate pollution. The shift of nitrate sources in different land use was identified using stable isotope composition of nitrate and groundwater age. The decreasing median value of δ15N from 10.6‰ to 7.5‰ of dated groundwater in farmland irrigated by clean water indicated the shift of nitrate sources from manure toward the mixing of fertilizer and manure due to the increased application of chemical fertilizers from intensive plant farming since 1980s. Comparably, the trend of increasing δ15N (the median value from 7‰ to 12‰) in farmland irrigated by wastewater might be attributed to the decreasing proportion of industrial wastewater since 2000s. The prevailing sources of nitrate in residential area were manure and sewage, and showed no obvious change along the recharge time. Driven by rapid urbanization, the nitrate sources of land use change area exhibited a marked shift from inorganic fertilizers toward manure and sewage. Principal component analysis (PCA) on nitrate concentrations with multiple parameters indicated nitrogen input in agricultural development and urbanization were the main controlling factors of nitrate contamination in the study area. The study results are a good reference for groundwater management in regions with nitrate source change during the process of rapid urbanization and agricultural intensification. The coupling of chemical, isotopic analyses and groundwater dating proved to be invaluable and should be applied in similar studies of nitrate contamination.

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Researching the watershed-scale spatiotemporal groundwater and surface water mixing function, groundwater recharge heights and age can provide important information to watershed water sources management and water pollution controlling. In this study, 20 groundwater samples, 6 precipitation samples, and 40 surface water samples in the Yiluo River watershed in middle China were collected, and the mixing function between groundwater and surface water, recharge height, and age of groundwater was studied by using hydrochemistry (Cl, DO, EC, pH), radioactive isotopes (14C), and stable isotopes (13C, 18O, 15N). The results showed that river and shallow groundwater had frequent interaction. Evaporation function played a major role in the groundwater recharging process. Groundwater age displayed spatial and seasonal variations, and the age ranged from 660 to 2800 years (dry season) and 560 to 1800 years (wet season) in downstream and midstream, while the age range from 12,025 to 143,600 years (dry season) and 10,560 to 12,650 years (wet season) in upstream. The average recharge height of downstream and midstream both in dry and wet seasons is about 576.00 to 908.70 m. While in upstream, both, in the dry and wet seasons, ranged from 1285 to 2680 m. The mixing function between groundwater and surface water displayed spatiotemporal variety. These results of this study can provide useful information for the watershed-scale water resources management.

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Nutrient and pesticide pollution are among the major threats to groundwater quality in agriculturally impacted aquifers. Understanding their legacy effects and drivers are important to protect aquifers from exposures to contamination. However, the complexities of groundwater flowpaths make it difficult to predict the time-scales of groundwater flow and contaminant transport. To determine these controls of groundwater nutrient and pesticides in an aquifer system underlying an intensive agricultural area in the Great Barrier Reef catchment, Australia, we sampled tritium (3H) to estimate groundwater-age, nutrient and pesticide concentrations to investigate groundwater contamination, and nitrogen (ẟ15N-NO3-) and oxygen (ẟ18O-NO3-) isotopes to determine groundwater nitrate dynamics. We, then, constructed high-resolution 3D geological and groundwater flow models of the aquifer system to determine the role of the geologic heterogeneity on the observed nutrient and pesticide concentrations. Groundwater 3H derived ages, and nutrient and pesticide concentrations did not follow distinct spatial trends. ẟ15N-NO3- and ẟ18O-NO3- values indicated that nitrification and denitrification processes influenced nitrate dynamics in the aquifer system; however, they were not solely able to explain the entire 3D variability. The 3D geologic modelling identified possible preferential flowpaths and perched systems, which helped to explain the observed groundwater-age, nutrient and pesticide variabilities. Old-groundwater (~100-years) was found in shallow depths (<15 m) where perched systems were identified. In areas with preferential flowpaths, young-groundwater (⁓1-year) with significant nitrate (~12 mg-N/L) and pesticides (up to 315 ng/L) concentrations were detected at deeper depths (>25 m), below perched and locally confined systems. Downward increasing groundwater-age, and decreasing nutrient and pesticide concentrations were detected in the unconfined aquifer, while old-groundwater (~160-years) and lower nitrate (<3 mg-N/L) and pesticides (<2 ng/L) concentrations were detected in the confined systems. This study demonstrates the importance of understanding both the geology and the hydrogeology of an area before deploying monitoring studies and/or making conclusions from tritium, nutrient and pesticide data alone.

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The Guaraní Aquifer System (SAG) is the largest transboundary aquifer in Latin America, extending beneath parts of Brazil, Paraguay, Argentina, and Uruguay. This paper presents the results of recent hydrogeological studies in the southern portion of the SAG. Locally, the abundance of surface water bodies precluded the use of conventional hydrological tools to characterize groundwater flows. Geological, hydrochemical and environmental isotope investigations were integrated to postulate a revised hydrogeological conceptual model. The revised geological model has provided a better definition of the geometry of the aquifer units and outlined the relevance of regional faults in controlling flow patterns. The new potentiometric map is consistent with groundwater flow from the SAG outcrops to the centre of the Corrientes Province, where upwards flows were identified. Hydrochemical and isotope data confirmed the widespread occurrence of mixing. Noble gas isotopes dissolved in groundwater (4He and 81Kr/Kr) provided residence times ranging from recent recharge up to 770 ± 130 ka. Groundwater age modelling confirmed the role of the geological structures in controlling groundwater flow. The southern sector of the SAG is a multilayer aquifer system with vertical flows and deep regional discharge near the Esteros del Iberá wetland area and along the Paraná and Uruguay rivers.

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As an important part of the water cycle, the hydrologic process and chemical compositions of groundwater have changed significantly due to the joint influence of climate change and human activities. Groundwater salinization becomes a serious threat to water security in coastal areas. In order to assess the relationships between surface water, groundwater and seawater in the coastal plain, we performed a synthesis study based on hydrochemical-isotopic data, hydro-dynamical records and environmental tracers. Deuterium and oxygen isotopes and water chemical indicators were used to identify pollution status, salt sources and migration processes. Radioactive isotopes and gaseous tracers were used to obtain reasonable groundwater age. With the help of multi-tracer approach, the surface-groundwater interaction, salinization of groundwater and nitrate pollution were identified in the Yang-Dai River plain, northern China. The estimated groundwater ages determined from chlorofluorocarbons (CFCs) and tritium (3H) ranges from 18 to 41 years in this area, suggesting a modern groundwater circulation. The spatial distribution of the groundwater age varies significantly due to horizontal hydrogeological heterogeneity. The total dissolved solids (TDS) content of the groundwater near the Well Field (average: 970 mg/L) was higher than the TDS values in samples derived from places located at an equivalent distance to the coastal line (average is 708 mg/L), which resulted from the vertical seawater intrusion through river channels and pollutant inputs from agriculture activities. The nitrate concentrations in groundwater were elevated up to 271 mg/L and increased with increasing groundwater age, which was another water environment problem that should be solved urgently but lacks sufficient attention for years. This study provides a conceptual model with a number of comparable hydrochemical information, which is significant for regional pollution control and water resources management.

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Radionuclide contamination of groundwater causes critical impacts on water resources, human lives, and ecosystems. The intrusion of radionuclides into the groundwater flow system in Fukushima, Japan, could be illuminated by determining groundwater age and mixing processes. To do this, periodical field surveys were conducted in catchments contaminated by the Fukushima Dai-ichi Nuclear Power Plant accident. Sampling began in May 2011, which was 2 months after the disaster, and continued through June 2012. Chlorofluorocarbon (CFCs), tritium, and oxygen and hydrogen stable isotopes were used as environmental tracers. The observed tritium concentrations suggested that the water contained accident-derived radionuclides that exceeded the natural background baseline. Groundwater ages in the selected two headwater catchments were estimated to be between 10 and 26 years by combined use of multiple CFCs concentrations. In addition, the governing groundwater flow system was mostly approximated by a piston flow model; however, modern water fraction was also suggested based on the relationship between CFC-11 and CFC-12. The estimated water age and isotopic signals among stream water, spring water, and groundwater revealed that the intrusion of radionuclides into the groundwater was caused by the mixing between groundwater and modern water sources such as soil water and precipitation with relatively high radionuclide concentrations. This mixing was facilitated by a weathered and fractured granite bedrock and a thin unsaturated subsurface layer in the study area. Continued long-term monitoring of radionuclides in the groundwater will be necessary for water resources management in the future. CAPSULE: Radionuclide intrusion into the groundwater is related to the mixing between radionuclide-poor groundwater and modern water with relatively high radionuclide concentration.

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This study presents a novel data set of noble gas compositions and 3H/3He measurements in groundwater samples from the Gardermoen Aquifer in Norway. The motivation was to test the applicability of noble gases as tracers in constraining the conceptual model and improve the understanding of deeper parts of the aquifer. Flow models have been used as tools for water resource management at the Oslo international airport, which is located within the aquifer recharge area, and bordering towards protected nature reserves. Current models are well calibrated for upper parts of the aquifer, and in line with new noble gas data. However, in some areas large inverse pressure gradients are observed. Interpretation of noble gas data proved useful in understanding these pressure deviations as a result of water retention in low permeability layers of clay and silt. Noble gas composition, isotopic ratios and tritium water ages define different water "types". Mixing along flow path or as a consequence of pumping were found to be indicators of geological heterogeneity, and were used to evaluate degree of flow separation as well as vertical versus horizontal flux. 3H/3He water ages varied between 0 and 50 years, increasing with depth below the groundwater table and along flow paths. These data indicate lower vertical permeability and longer residence times in deeper parts of the aquifer than suggested by previous models. This study is of high relevance in the continued water resource management scheme at Gardermoen, for improving existing models and in sound, long-term monitoring of groundwater, ensuring sustained influx towards sensitive biotopes.

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The combination of emerging antibiotic resistance and lack of discovery of new antibiotic classes poses a threat to future human welfare. Antibiotics are administered to livestock at a large scale and these may enter the environment by the spreading of manure on agricultural fields. They may leach to groundwater, especially in the Netherlands which has some of the most intensive livestock farming and corresponding excessive manure spreading in the world. This study investigates the presence of antibiotics in groundwater in two regions with the most intensive livestock farming in the Netherlands. If so, the hydrochemical conditions were further elaborated. Ten multi-level wells with in total 46 filters were sampled, focusing on relatively young, previously age-dated groundwater below agricultural fields. Twenty-two antibiotics were analyzed belonging to the following antibiotic groups: tetracyclines, sulfonamides, trimethoprims, ß-lactams, macrolides, lincosamides, quinolones, nitrofurans and chloramphenicol. The samples were analyzed for these antibiotics by LC-MS/MS ESI-POS/NEG (MRM) preceded by solid phase extraction which resulted in importantly low detection limits. Six antibiotics were found above detection limits in 31 filters in seven wells: sulfamethazine, sulfamethoxazole, lincomycin, chloramphenicol, ciprofloxacin, and sulfadiazine. The concentrations range from 0.3 to 18 ng L-1. Sulfonamides were detected at all measured depths down to 23 meters below surface level with apparent groundwater ages up to 40 years old. No antibiotics were detected below the nitrate/iron redox cline, which suggests that the antibiotics might undergo degradation or attenuation under nitrate-reducing redox conditions. This study provides proof that antibiotics are present in groundwater below agricultural areas in the Netherlands due to the spreading of animal manure.

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Estimating intermediate water residence times (a few years to a century) in shallow aquifers is critical to quantifying groundwater vulnerability to nutrient loading and estimating realistic recovery timelines. While intermediate groundwater residence times are currently determined with atmospheric tracers such as chlorofluorocarbons (CFCs), these analyses are costly and would benefit from other tracer approaches to compensate for the decreasing resolution of CFC methods in the 5-20 years range. In this context, we developed a framework to assess the capacity of dissolved silica (DSi) to inform residence times in shallow aquifers. We calibrated silicate weathering rates with CFCs from multiple wells in five crystalline aquifers in Brittany and in the Vosges Mountains (France). DSi and CFCs were complementary in determining apparent weathering reactions and residence time distributions (RTDs) in shallow aquifers. Silicate weathering rates were surprisingly similar among Brittany aquifers, varying from 0.20 to 0.23 mg L-1 yr-1 with a coefficient of variation of 7%, except for the aquifer where significant groundwater abstraction occurred, where we observed a weathering rate of 0.31 mg L-1 yr-1. The silicate weathering rate was lower for the aquifer in the Vosges Mountains (0.12 mg L-1 yr-1), potentially due to differences in climate and anthropogenic solute loading. Overall, these optimized silicate weathering rates are consistent with previously published studies with similar apparent ages range. The consistency in silicate weathering rates suggests that DSi could be a robust and cheap proxy of mean residence times for recent groundwater (5-100 years) at the regional scale. This methodology could allow quantification of seasonal groundwater contributions to streams, estimation of residence times in the unsaturated zone and improve assessment of aquifer vulnerability to anthropogenic pollution.

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Hydrochemical analysis and environmental isotopic tracing are successfully applied to study groundwater evolution processes. Located in eastern China, the Jiangsu Coastal Plain is characterized by an extensively exploited deep groundwater system, and groundwater salinization has become the primary water environmental problem. This paper provides a case study on the use of a hydrochemical and environmental isotopic approach to assess possible mixing and evolution processes at Yoco Port, Jiangsu Province, China. Hydrochemical and isotopic patterns of deep groundwater allow one to distinguish different origins in deep water systems. HCO3- is the dominant anion in the freshwater samples, whereas Na+ and Cl- are the dominant major ions in the saline samples. According to δ18O, δ2H and 14C dating, the fresh water is derived from precipitation under a colder climate during the Glacial Maximum (Dali Glacial), while the saline groundwater is influenced by glacial-interglacial cycles during the Holocene Hypsithermal. The δ18O, δ2H and 3H data confirm that deep groundwater in some boreholes is mixed with overlying saline water. The deep groundwater reservoir can be divided into a saline water sector and a fresh water sector, and each show distinct hydrochemical and isotopic compositions. The saline groundwater found in the deep aquifer cannot be associated with present seawater intrusion. Since the Last Glacial Maximum in the Late Pleistocene, the deep groundwater flow system has evolved to its current status with the decrease in ice cover and the rising of sea level. However, the hydraulic connection is strengthened by continuous overexploitation, and deep groundwater is mixed with shallow groundwater at some points.

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The spatial heterogeneity of dissolved arsenic (As) concentrations in shallow groundwater of the Bengal Basin has been attributed to transport of As (and reactive carbon) from external sources or to the release of As from within grey sand formations. We explore the latter scenario in this detailed hydrological and geochemical study along a 300 m transect of a shallow aquifer extending from a groundwater recharge area within a sandy channel bar to its discharge into a nearby stream. Within the 10-20 m depth range, groundwater ages along the transect determined by the 3H-3He method increase from <10 yr in the recharge area to a maximum of 40 yr towards the stream. Concentrations of groundwater As within the same grey sands increase from 10 to 100 to ∼500 µg/L along this transect. Evidence of reversible adsorption of As between the groundwater and sediment was obtained from a series of push-pull experiments, traditional batch adsorption experiments, and the accidental flooding of a shallow monitoring well. Assuming reversible adsorption and a distribution coefficient, Kd, of 0.15-1.5 L/kg inferred from these observations, a simple flushing model shows that the increase in As concentrations with depth and groundwater age at this site, and at other sites in the Bengal and Red River Basins, can be attributed to the evolution of the aquifer over 100-1000 years as aquifer sands are gradually flushed of their initial As content. A wide range of As concentrations can thus be maintained in groundwater with increases with depth governed by the history of flushing and local recharge rates, without external inputs of reactive carbon or As from other sources.

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Temporal changes in methyl tert-butyl ether (MtBE) concentrations in groundwater were evaluated in the northeastern United States, an area of the nation with widespread low-level detections of MtBE based on a national survey of wells selected to represent ambient conditions. MtBE use in the U.S. peaked in 1999 and was largely discontinued by 2007. Six well networks, each representing specific areas and well types (monitoring or supply wells), were each sampled at 10year intervals between 1996 and 2012. Concentrations were decreasing or unchanged in most wells as of 2012, with the exception of a small number of wells where concentrations continue to increase. Statistically significant increasing concentrations were found in one network sampled for the second time shortly after the peak of MtBE use, and decreasing concentrations were found in two networks sampled for the second time about 10years after the peak of MtBE use. Simulated concentrations from convolutions of estimates for concentrations of MtBE in recharge water with age distributions from environmental tracer data correctly predicted the direction of MtBE concentration changes in about 65% of individual wells. The best matches between simulated and observed concentrations were found when simulating recharge concentrations that followed the pattern of national MtBE use. Some observations were matched better when recharge was modeled as a plume moving past the well from a spill at one point in time. Modeling and sample results showed that wells with young median ages and narrow age distributions responded more quickly to changes in the contaminant source than wells with older median ages and broad age distributions. Well depth and aquifer type affect these responses. Regardless of the timing of decontamination, all of these aquifers show high susceptibility for contamination by a highly soluble, persistent constituent.

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Travel-time based models simplify the description of reactive transport by replacing the spatial coordinates with the groundwater travel time, posing a quasi one-dimensional (1-D) problem and potentially rendering the determination of multidimensional parameter fields unnecessary. While the approach is exact for strictly advective transport in steady-state flow if the reactive properties of the porous medium are uniform, its validity is unclear when local-scale mixing affects the reactive behavior. We compare a two-dimensional (2-D), spatially explicit, bioreactive, advective-dispersive transport model, considered as "virtual truth", with three 1-D travel-time based models which differ in the conceptualization of longitudinal dispersion: (i) neglecting dispersive mixing altogether, (ii) introducing a local-scale longitudinal dispersivity constant in time and space, and (iii) using an effective longitudinal dispersivity that increases linearly with distance. The reactive system considers biodegradation of dissolved organic carbon, which is introduced into a hydraulically heterogeneous domain together with oxygen and nitrate. Aerobic and denitrifying bacteria use the energy of the microbial transformations for growth. We analyze six scenarios differing in the variance of log-hydraulic conductivity and in the inflow boundary conditions (constant versus time-varying concentration). The concentrations of the 1-D models are mapped to the 2-D domain by means of the kinematic (for case i), and mean groundwater age (for cases ii & iii), respectively. The comparison between concentrations of the "virtual truth" and the 1-D approaches indicates extremely good agreement when using an effective, linearly increasing longitudinal dispersivity in the majority of the scenarios, while the other two 1-D approaches reproduce at least the concentration tendencies well. At late times, all 1-D models give valid approximations of two-dimensional transport. We conclude that the conceptualization of nonlinear bioreactive transport in complex multidimensional domains by quasi 1-D travel-time models is valid for steady-state flow fields if the reactants are introduced over a wide cross-section, flow is at quasi steady state, and dispersive mixing is adequately parametrized.

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The Waste Isolation Pilot Plant (WIPP) in New Mexico is the first geologic repository for disposal of transuranic nuclear waste from defense-related programs of the US Department of Energy. It is constructed within halite beds of the Permian-age Salado Formation. The Culebra Dolomite, confined within Rustler Formation evaporites overlying the Salado Formation, is a potential pathway for radionuclide transport from the repository to the accessible environment in the human-disturbed repository scenario. Although extensive subsurface characterization and numerical flow modeling of groundwater has been done in the vicinity of the WIPP, few studies have used natural isotopic tracers to validate the flow models and to better understand solute transport at this site. The advent of Atom-Trap Trace Analysis (ATTA) has enabled routine measurement of cosmogenic (81)Kr (half-life 229,000 yr), a near-ideal tracer for long-term groundwater transport. We measured (81)Kr in saline groundwater sampled from two Culebra Dolomite monitoring wells near the WIPP site, and compared (81)Kr model ages with reverse particle-tracking results of well-calibrated flow models. The (81)Kr model ages are ~130,000 and ~330,000 yr for high-transmissivity and low-transmissivity portions of the formation, respectively. Compared with flow model results which indicate a relatively young mean hydraulic age (~32,000 yr), the (81)Kr model ages imply substantial physical attenuation of conservative solutes in the Culebra Dolomite and provide limits on the effective diffusivity of contaminants into the confining aquitards.

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