Quantification of ³⁷Ar emanation fractions from irradiated natural rock samples and field applications

Underground-produced ³⁷Ar can be used for underground nuclear explosions (UNE) detection and for groundwater dating. The quantification of the emanation, that is the fraction of activity produced in the rock that escapes to the pore space, is essential for predicting the background activity expected in natural environments. We propose an experiment in which artificial CaCO₃ powder and natural rock particles are irradiated with neutrons in a routinely operated medical cyclotron, whose energy spectrum is experimentally measured. The produced activity was quantified and compared with the emanated activity to determine the emanating fraction. The results showed consistent and reproducible patterns with a dominance of the recoil process at small scales (<2 mm). We observed emanation values ≤1% with a dependency on the grain size and the inner geometry of particles. Soil weathering and the presence of water increased the recoil emanation. The atoms produced that were instantaneously recoiled in the intra- or inter-granular pore space left macroscopic samples by diffusion on timescales of days to weeks (D_eff = 10^-12 - 10^-16 m² s^-1). This diffusive transport determines the activity that prevails in the fluid-filled pore space accessible for groundwater or soil gas sampling.