Simulations and Experiments Reveal Effect of Nanopores on Helium Diffusion in Quartz

Abstract:

The diffusion properties of noble gases in minerals are widely utilized to reconstruct the thermal histories of rocks. Here, we combine density functional theory (DFT) calculations with laboratory experiments to investigate controls on helium diffusion in quartz. DFT calculations for perfect α-quartz predict substantially lower activation energies and frequency factors for helium diffusion than observed in laboratory experiments, especially in the [001] direction. These results imply that no helium could be retained in quartz at Earth surface temperatures, which conflicts with observations of partial cosmogenic 3He retention over geologic timescales. Here, we implement a model of helium diffusion in α-quartz modulated by nanopore defects that disrupt energetically-favorable diffusion pathways. In this model, we find that laboratory-determined diffusivities can be most closely reproduced when a helium atom encounters ~1-10 nanopore sites per million interstitial sites. The results of our model indicate that diffusion of helium in natural quartz, like other noble gases in other minerals, can be significantly modulated by defects.