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Stone, A. E. C., & Edmunds, W. M. (2014). Naturally-high nitrate in unsaturated zone sand dunes above the Stampriet Basin, Namibia. Journal of Arid Environments, 105, 41–51.
Abstract: Elevated groundwater nitrate levels are common in drylands, often in excess of WHO guidelines, with concern for human and animal health. In light of recent attempts to identify nitrate sources in the Kalahari this paper presents the first unsaturated zone (USZ) nitrate profiles and recharge rate estimates for the important transboundary Stampriet Basin, alongside the first rainfall chemistry records. Elevated subsurface nitrate reaches 100–250 and 250–525 mg/L NO3–N, with NO3–N/Cl of 4–12, indicating input above evapotranspiration. Chloride mass balance recharge rates range from 4 to 27 mm/y, indicating a vertical movement of these nitrate pulses toward the water table over multi-decadal timescales. These profiles are sampled from dune crests, away from high concentrations of animals and without termite mounds. Given low-density animal grazing is unlikely to contribute consistent spot-scale nitrate over decades, these profiles give an initial estimate of naturally-produced concentrations. This insight is important for the management of the Stampriet Basin and wider Kalahari groundwater. This study expands our knowledge about elevated nitrate in dryland USZs, demonstrating that it can occur as pulses, probably in response to transient vegetation cover and that it is not limited to long-residence time USZs with very limited downward moisture flux (recharge).
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Musy, S., & Purtschert, R. (2023). Reviewing 39Ar and 37Ar underground production in shallow depths with implications for groundwater dating. Science of The Total Environment, 884, 163868.
Abstract: Argon-37 (37Ar) and Argon-39 (39Ar) are used for groundwater dating on timescales from weeks to centuries. For both isotopes, the quantification of underground sources is essential to accurately infer water residence times from sampled dissolved activities. Subsurface production resulting from interactions with neutrons from the natural radioactivity in rocks and with primary cosmogenic neutrons has been known for a long time. More recently, the capture of slow negative muons and reactions with muon-induced neutrons were documented for 39Ar subsurface production in the context of underground particle detectors (e.g. for Dark Matter research). However, the contribution from these particles was never considered for groundwater dating applications. Here, we reevaluate the importance of all potential depth-related production channels at depth ranges relevant for 39Ar groundwater dating [0 − 200 meters below the surface (m.b.s)]. The production of radioargon by muon-induced processes is considered in this depth range for the first time. The uncertainty on the total depth-dependent production rate is estimated with Monte Carlo simulations assuming a uniform distribution of the parameter uncertainties. This work aims to provide a comprehensive framework for interpreting 39Ar activities in terms of groundwater residence times and for exposure age dating of rocks. The production of 37Ar is also addressed since this isotope is relevant as a proxy for 39Ar production, for the timing of river-groundwater exchanges, and in the context of on-site inspections (OSI) within the verification framework of the Comprehensive Nuclear-Test-Ban Treaty (CTBT). In this perspective, we provide an interactive web-based application for the calculation of 37Ar and 39Ar production rates in rocks.
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Heine, F., & Einsiedl, F. (2021). Groundwater dating with dissolved organic radiocarbon: A promising approach in carbonate aquifers. Applied Geochemistry, 125, 104827.
Abstract: A complete hydrogeological understanding of the deep Upper Jurassic carbonate aquifer in the South German Molasse Basin is essential for the future development of this important drinking water resource and geothermally used system. Water chemistry data, δ13CDIC, 14C of the dissolved inorganic carbon (14CDIC) and stable water isotope (δ18O and δD) measurements have been used to evaluate a promising groundwater dating approach with 14C of dissolved organic carbon (14CDOC). The pre-concentration of dissolved organic matter (DOM) was performed by the easy applicable solid phase extraction (SPE) with a styrene-divinylbenzene copolymer sorbent (PPL). Based on the sampling campaign of seven groundwater wells conducted between 2017 and 2019, it was shown that the groundwater is mainly of Ca–HCO3 type with some evidence of ion exchange between Ca2+ and Na+ at two of the investigated wells. The δD values ranged from −89.4‰ to −70.9‰ while δ18O values varied between −12.5‰ and −9.8‰. The obtained stable water isotope signatures indicated that the groundwater is of meteoric origin and was recharged during warm climate (Holocene), intermediate climate and cold climate (Pleistocene) infiltration conditions. The measured 14CDOC activities varied from 5.7 pmC to 51.1 pmC and the calculated piston-flow water ages (ORAs) ranged from 4200 years to 25,248 years using an initial 14C0DOC of 85 pmC. The calculated ORAs showed a very good correlation to the infiltration temperature-sensitive δ18O values which were affirmed with noble gas infiltration temperatures for two wells after Weise et al. (1991) and were also in good accordance with the atmospheric temperature record of the northern hemisphere from Dokken et al. (2015). The results reflect a consistent hydrogeological picture of the carbonate aquifer, which also supports the applicability of the SPE-PPL method for 14CDOC dating in groundwater with a low DOC content (<1 mg/l). In contrast, 14CDIC activities of 1.4 pmC to 21.3 pmC led to geochemically corrected piston-flow ages between 8057 years and >30,000 years and generally to an overestimation of the apparent water ages. This study gives insights into the promising approach of 14CDOC groundwater dating in carbonate aquifers with low DOC contents and allows future sustainable groundwater resource management of the investigated aquifer system.
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Musy, S., Meyzonnat, G., Barbecot, F., Hunkeler, D., Sültenfuss, J., Solomon, D. K., et al. (2021). In-situ sampling for krypton-85 groundwater dating. Journal of Hydrology X, 11, 100075.
Abstract: Krypton-85 and other radioactive noble gases are widely used for groundwater dating purposes. 85Kr analysis require large volumes of water to reach the analytical requirements. Conventionally, this water is pumped to the surface to be degassed with a gas extraction system. The large pumping rate may disturb the natural flow field and requires substantial field logistics. Hence, we propose a new in-situ degassing method, in which membrane contactors are used to degas the groundwater directly in the well and gas is collected at the surface. This way, field work is facilitated, groundwater system disturbance is minimized, and the gas sample is collected at a specific depth. We demonstrate the tightness of the system regarding atmospheric air contamination for a collection times of 24 h, which is sufficient for both low-level counting and laser-based counting methods for 85Kr. The minimal borehole diameter is 7.5 cm for the prototype presented in this research but can easily be reduced to smaller diameters. In a case study, we compare the results obtained with the new passive method with those from a conventional packer setup sampling. Additionally, 3H/3He samples were collected for both sampling regimes and the dating results were compared with those from 85Kr. A good agreement between tracer ages is demonstrated and the age stratigraphy is consistent with the expected age distribution for a porous unconfined aquifer. In addition, our study emphasizes the differences between the age information sampled with various methods. In conclusion, we demonstrate that the new in situ quasi-passive method provides a more representative age stratigraphy with depth in most cases.
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Romeo, N., Mabry, J., Hillegonds, D., Kainz, G., Jaklitsch, M., & Matsumoto, T. (2022). Developments of a field gas extraction device and krypton purification system for groundwater radio-krypton dating at the IAEA. Applied Radiation and Isotopes, 189, 110450.
Abstract: The long-lived radio-krypton isotope 81Kr (t1/2 = 2.29 × 105 yr) is an ideal tracer for old groundwater age dating in the range of 105–106 years which goes beyond the reach of radio-carbon (14C) age dating. Analytical breakthrough made over the last two decades in Atom Trap Trace Analysis (ATTA) has enabled the use of this isotope with extremely low abundance (81Kr/Kr = 6 × 10−13) to be used as a practical dating tool for very old groundwater. The International Atomic Energy Agency aims to provide this new isotope tool for better groundwater resource management of Member States and developed a field sampling device to collect dissolved gas samples from groundwater and a system to separate and purify trace amounts of krypton from the gas samples for the ATTA analysis. The design, setup and performances of our sampling and purification systems are described here. Our system can produce a high purity aliquot of about 5 μL of krypton from 5 L of air sample (recovery yield of >90%). The samples made by our system were confirmed to be acceptable for the ATTA analysis.
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