Helium incorporation and diffusion in polycrystalline olivine

Helium is a key tracer of mantle geochemical and isotopic heterogeneities and can constrain our understanding of mantle geodynamics. Nevertheless, the mechanisms of helium storage and transport in mantle minerals remain poorly understood. Polycrystalline olivine was doped with helium at high temperature (1050 ± 25 °C) and high pressure (0.30 ± 0.01 GPa), followed by step heating extraction experiments to investigate helium storage and diffusion in Earth's upper mantle. We also tested the effect of heterogeneous initial concentrations on the extracted diffusivities, and demonstrate the robustness of diffusion parameters obtained in this study. Our results show that two diffusion processes are acting in polycrystalline olivine: (i) a high temperature process with high activation energy (Ea) where diffusion is only controlled by lattice diffusion, and (ii) a lower temperature process with lower Ea where diffusion is controlled by both grain boundary and lattice diffusion. These two diffusion processes are separated by a transition temperature that depends on the depletion of helium hosted in grain boundaries, i.e., the amount of helium stored at grain boundaries and the temperature and duration of the step heating sequence. Our results confirm that grain boundaries can represent a significant storage site for He. Moreover, we report two different populations of diffusion parameters in the lattice diffusion field, which are interpreted as diffusion in interstitials (Ea = 95 ± 15 kJ·mol−1 and log(D0) = −8.26 ± 2.13) and Mg vacancies (Ea = 168 ± 19 kJ·mol−1 and log(D0) = −3.59 ± 2.12). Similar diffusion parameters populations are observed in literature data after reprocessing the diffusivities. Furthermore, we determine grain boundary diffusion parameters: Ea = 57 ± 14 kJ·mol−1 and log(D0) = −9.20 ± 0.99. Applying these results to the upper mantle reveals that an important amount of He can be stored at grain boundaries for typical mantle grain size (22% for a grain size of 1 mm) and that most helium can be stored at grain boundaries for relatively small grain sizes (≤290 μm and ≤10 μm for segregation factors of 1/10−5 and 1/0.0025, respectively). As a consequence, bulk diffusivities can be significantly higher than lattice diffusivities. Although our study cannot be applied directly to the lower mantle, the similar storage sites and diffusion mechanisms are expected in lower mantle silicates if high pressure does not inhibit diffusion.