First-Principles Calculations of the Diffusivity of Interstitial Helium in Alpha-U Considering Anisotropy, Isotope Effects, and Quantum Effects

Abstract

The interstitial migration of helium in alpha-U, which is planned to be used as a tritium storage material for nuclear fusion reactors and as a metallic fuel for advanced nuclear reactors, is studied by first-principles calculations. First, all migration paths are identified using the nudged elastic band method, and the migration barrier is determined for each path considering the thermal expansion of the lattice. In addition, the jump attempt frequencies are determined by applying harmonic transition state theory coupled with vibration analysis. Subsequently, the diffusion coefficient is evaluated numerically by kinetic Monte Carlo calculations using the determined migration barriers and jump attempt frequencies for all migration paths. Diffusion in the [010]-direction is found to be the most unlikely until sufficiently high temperature, while [001]-diffusion is the most dominant diffusion direction through the whole temperature range. The isotope effect, which is important because the beta decay of tritium produces helium-3, is not large and approaches the classical limit as the temperature increases. The quantum tunneling crossover temperature is computed to be approximately 100 K for helium-3 and 86 K for helium-4, which ensures the validity of the present calculation results over a wide temperature range. The diffusion coefficients are obtained as D=(9.67×10−4)×exp(−0.202eVkT)cm2/s for helium-3 and D=(8.48×10−4)×exp(−0.201eVkT)cm2/s for helium-4 over a temperature range from 200 to 900 K.