DOI: 10.57760/sciencedb.03823
title: Influence of irradiation-induced point defects on the dissolution and diffusion properties of hydrogen in α-Al2O3: a first-principles study
title: Influence of irradiation-induced point defects on the dissolution and diffusion properties of hydrogen in α-Al2O3: a first-principles study

description: Alpha-alumina (α-Al2O3) is considered to be an ideal candidate material for the tritium permeation barrier (TPB) with excellent tritium resistance properties. However, in a fusion reactor, the irradiation-induced defects could sum up on fabrication-induced defects so to reduce drastically the barrier performance. The underlying mechanism is still not settled. In this paper, the first-principles density functional theory (DFT) approach is used to explore the influence of irradiation-induced point defects on the dissolution and diffusion properties of hydrogen (H) in α-Al2O3. [H+− V−3Al]and [H+ − V0O] defects have much lower formation energies at EG/2 in both Al-rich and O-rich growth environments that H atoms are easily captured by vacancy-type irradiation-induced point defects. As a result, higher H retention can be expected, which is consistent with the experimental results. Moreover, by calculating several different diffusion pathways of H-defect complexes and the corresponding diffusion coefficient, it can be inferred that H atoms and vacancy-type point defects can hardly diffuse as a bound entity. Therefore, isolated vacancy-type irradiation-induced point defects can trap multiple H atoms to form H-defect complexes and impede the diffusion process of H, which can enhance the efficiency of protection against H permeation through α-Al2O3 TPB. However, the minimum diffusion barrier for OiH− migration to the first nearest neighbor O interstitial site is 0.44 eV, which is so low that OiH− can migrate quickly at room temperature. This fast diffusion pathway for H could be the underlying mechanism for the low efficiency in preventing H permeation through irradiated α-Al2O3. Our results provide a sound theoretical explanation for recent experimental results of H permeation in α-Al2O3 under irradiation environment.
description: Alpha-alumina (α-Al2O3) is considered to be an ideal candidate material for the tritium permeation barrier (TPB) with excellent tritium resistance properties. However, in a fusion reactor, the irradiation-induced defects could sum up on fabrication-induced defects so to reduce drastically the barrier performance. The underlying mechanism is still not settled. In this paper, the first-principles density functional theory (DFT) approach is used to explore the influence of irradiation-induced point defects on the dissolution and diffusion properties of hydrogen (H) in α-Al2O3. [H+− V−3Al]and [H+ − V0O] defects have much lower formation energies at EG/2 in both Al-rich and O-rich growth environments that H atoms are easily captured by vacancy-type irradiation-induced point defects. As a result, higher H retention can be expected, which is consistent with the experimental results. Moreover, by calculating several different diffusion pathways of H-defect complexes and the corresponding diffusion coefficient, it can be inferred that H atoms and vacancy-type point defects can hardly diffuse as a bound entity. Therefore, isolated vacancy-type irradiation-induced point defects can trap multiple H atoms to form H-defect complexes and impede the diffusion process of H, which can enhance the efficiency of protection against H permeation through α-Al2O3 TPB. However, the minimum diffusion barrier for OiH− migration to the first nearest neighbor O interstitial site is 0.44 eV, which is so low that OiH− can migrate quickly at room temperature. This fast diffusion pathway for H could be the underlying mechanism for the low efficiency in preventing H permeation through irradiated α-Al2O3. Our results provide a sound theoretical explanation for recent experimental results of H permeation in α-Al2O3 under irradiation environment.