Energetic landscape and diffusion of He in α-Fe grain boundaries from first principles

Combined density functional theory and empirical-potential calculations are performed to investigate the lowest-energy sites and migration mechanisms of He in various α-Fe grain boundaries (GBs). Before the defect calculations, we show that structural optimizations, including simulated annealing and atom removal, are crucial for locating the stable GB structure in a given temperature regime. Then, the He formation energies for all the substitutional and interstitial sites in two different GBs are evaluated, showing a strong He segregation tendency. At variance with the bulk Fe case, the formation energy of an interstitial He is either lower than or similar to that of a substitutional He in the GBs. Finally, both static and dynamic barriers for interstitial He diffusion in the GBs are determined. Although the diffusion details and precise paths are GB dependent, some common features are identified: (1) The He atom always remains confined to the GB region while diffusing; (2) the He diffusion is highly anisotropic along the GBs; (3) the GB diffusion of an interstitial He atom is found to be always slower than its bulk diffusion, but it can still be faster than the bulk diffusion of a substitutional He.