Hydrogen and vacancy clustering in zirconium

TL;DR

This study uses ab initio simulations to explore how hydrogen influences vacancy cluster stability in zirconium, revealing hydrogen's strong binding to small clusters and its role in reducing stacking fault energies, which affects irradiation behavior.

Contribution

It provides new insights into hydrogen-vacancy interactions in zirconium, combining atomistic simulations and thermodynamic modeling to explain experimental observations.

Findings

Hydrogen strongly binds to small vacancy clusters.

Hydrogen enrichment reduces stacking fault energies.

Vacancy loops in basal planes trap more hydrogen, stabilizing them.

Abstract

The effect of solute hydrogen on the stability of vacancy clusters in hexagonal closed packed zirconium is investigated with an ab initio approach, including contributions of H vibrations. Atomistic simulations within the density functional theory evidence a strong binding of H to small vacancy clusters. The hydrogen effect on large vacancy loops is modeled through its interaction with the stacking faults. A thermodynamic modeling of H segregation on the various faults, relying on ab initio binding energies, shows that these faults are enriched in H, leading to a decrease of the stacking fault energies. This is consistent with the trapping of H by vacancy loops observed experimentally. The stronger trapping, and thus the stronger stabilization, is obtained for vacancy loops lying in the basal planes, i.e. the loops responsible for the breakaway growth observed under high irradiation dose.