Evaluating the impact of muon-induced cosmogenic 39Ar and 37Ar underground production on groundwater dating with field observations and numerical modeling.

Musy, Stephanie; Hinsby, Klaus; Troldborg, Lars; Delottier, Hugo; Guillon, Sophie; Brunner, Philip; Purtschert, Roland (2023). Evaluating the impact of muon-induced cosmogenic 39Ar and 37Ar underground production on groundwater dating with field observations and numerical modeling. The Science of the total environment, 903, p. 166588. Elsevier 10.1016/j.scitotenv.2023.166588

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Groundwater dating by radioactive cosmogenic tracers such as 39Ar relies on the decay rate from a known initial atmospheric activity (100%modern). Thereby, it is assumed that cosmogenic 39Ar production in the subsurface is negligible at depths below the water table and that contributions from natural rock radioactivity are minor or missing. Here we present 39Ar data from aquifers located in quaternary glacial sediments and tertiary limestones in Denmark, which unequivocally demonstrate that cosmogenic production can induce considerable age biases. 39Ar values larger than 100%modern are observed at relatively shallow groundwater depths in non-radiogenic rocks. These activities are compared to calculations based on previously assessed depth-dependent production rates in rocks and realistic estimates of the emanated fractions to the water phase. The water residence time distribution with depth, which was determined by numerical flow modeling and particle tracking, underpinned the significance of muon-induced 39Ar production. The short-lived isotope 37Ar is produced by similar processes as 39Ar and demonstrated its usefulness as an indicator of local underground production in an aquifer. The significance of cosmogenic underground production in other possible recharge scenarios was then assessed by explicitly simulating the radioargon accumulation and decay in a 2D synthetical numerical model. These simulations demonstrated that underground production is negligible when the water infiltrates freely in a porous aquifer. However, in the presence of a confining layer impeding the infiltration at shallow depths (<30 m), as is the case in our study site in Denmark for instance, over-modern 39Ar activities (>100%modern) may occur. The age concluded from the dissolved activities is then possibly biased towards young values. Special attention should thus be paid to the recharge rates when using 39Ar for dating groundwater. 37Ar activities provide complementary information about the strength and mechanisms of underground production.

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