Hydrogen bubble nucleation by self-clustering: Density Functional Theory and statistical models studies using tungsten as a model system

TL;DR

This study combines first-principles calculations and statistical models to reveal how hydrogen self-clusters form and lead to bubble nucleation in tungsten, providing insights into plasma-induced damage mechanisms.

Contribution

It demonstrates that hydrogen self-clusters become energetically favorable with increasing size and predicts conditions for bubble formation, advancing understanding of hydrogen behavior in tungsten.

Findings

Hydrogen self-clusters are more stable as they grow larger.

Hydrogen forms platelet-like structures along {100} planes.

Predicted hydrogen concentrations for bubble formation match experimental data.

Abstract

Low-energy hydrogen irradiation is known to induce bubble formation in tungsten, while its atomistic mechanisms remain little understood. Using first-principles calculations and statistical models, we studied the self-clustering behavior of hydrogen in tungsten. Unlike previous speculations that hydrogen self-clusters are energetically unstable owing to the general repulsion between two hydrogens, we demonstrated that hydrogen self-cluster becomes more favorable as the cluster size increases. We found that hydrogen atoms would form two-dimensional platelet-like structures along {100} planes. These hydrogen self-clustering behaviors can be quantitative understood by the competition between long-ranged elastic attraction and local electronic repulsion. Further statistical analysis showed that there exists a critical hydrogen concentration above which hydrogen self-clusters are thermodynamically stable and kinetically feasible. Based on this critical hydrogen concentration, the plasma loading conditions under which hydrogen self-clusters form were predicted. Our predictions showed excellent agreement with experimental results of hydrogen bubble formation in tungsten exposed to low-energy hydrogen irradiation. Finally, we proposed a possible mechanism for the hydrogen bubble nucleation via hydrogen self-clustering. This work provides mechanistic insights and quantitative models towards understanding of plasma-induced hydrogen bubble formation in plasma-facing tungsten.