Unveiling the origin of diffusion suppression of hydrogen isotopes at the {\alpha}-Al2O3(0001)/{\alpha}-Cr2O3(0001) interfaces

TL;DR

This study uses first-principles calculations to reveal that interfaces between { extalpha}-Al2O3 and { extalpha}-Cr2O3 create chemical bonds and defect sites that trap hydrogen isotopes, significantly reducing their diffusion and permeation.

Contribution

It provides a detailed atomic-level understanding of how interfaces suppress hydrogen isotope diffusion, highlighting the role of chemical bonding and vacancies.

Findings

Hydrogen isotopes form stable O-H covalent bonds near interfaces.

Diffusion barriers are higher at sites adjacent to interfaces.

Interfaces enhance oxygen vacancies, further inhibiting permeation.

Abstract

It has been reported that the {\alpha}-Al2O3, a promising tritium permeation barrier material for a fusion reactor, can be grown at low temperatures on the {\alpha}-Cr2O3 template, and that {\alpha}-Al2O3/{\alpha}-Cr2O3 composite films have more efficiently suppress the hydrogen isotope permeation than the single {\alpha}-Al2O3 film. In this study, we investigated the diffusion properties of hydrogen isotopes at the {\alpha}-Al2O3(0001)/{\alpha}-Cr2O3(0001) interfaces using first-principles calculations based on density functional theory. In the {\alpha}-Al2O3 region near the interfaces, O-H covalent bonds, which are not observed in the bulk {\alpha}-Al2O3, are formed, and hydrogen isotopes become stable. Such chemical bonds induced by the interfaces are the origin of hydrogen isotope trapping and result in a larger diffusion barrier than in the {\alpha}-Al2O3 and the {\alpha}-Cr2O3. It was also found that the suppression of hydrogen isotope diffusion does not occur at the interface site but at sites adjacent to the interfaces. In addition, the interface enhances the oxygen vacancies, which may also suppress hydrogen isotope permeation.