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

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.