Machine Learning Potentials for Hydrogen Absorption in TiCr$_2$ Laves Phases

Fuente: arXiv
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Autori principali: Kumar, Pranav, Körmann, Fritz, Grabowski, Blazej, Ikeda, Yuji
Natura: Preprint
Pubblicazione: 2025
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author Kumar, Pranav
Körmann, Fritz
Grabowski, Blazej
Ikeda, Yuji
author_facet Kumar, Pranav
Körmann, Fritz
Grabowski, Blazej
Ikeda, Yuji
contents The energetics of hydrogen absorption in C15 cubic and C14 hexagonal TiCr$_2$H$_x$ Laves phases is investigated for $0 < x \le 6$ with density functional theory (DFT) and machine learning interatomic potentials (MLIPs). The MLIPs are trained with configurations generated through a series of active-learning schemes. Basin-hopping Monte Carlo (BHMC) simulations based on the MLIPs predict minimum-energy hydrogen configurations, along with enthalpies of formation and hydrogen orderings. The obtained phase transformations at 0 K agree well with the experiments at low temperatures. The hydrogen solubility limits in the low-concentration $α$ phases at 0 K are predicted to be $x = 1.0$ and $x = 1.5$ for the C15 and the C14 phases, respectively. At these concentrations, C15 TiCr$_2$H shows the $Cc$ monoclinic symmetry, while C14 TiCr$_2$H$_{1.5}$ shows the $Ama2$ orthorhombic symmetry, both of which have not been reported for this system. The first and the second hydride phases, i.e., $β$ and $β'$, at 0 K are found around $x = 3$ and $x = 4$, respectively, for both the C15 and the C14 phases. In the second-hydride $β'$ phases, C15 TiCr$_2$H$_4$ shows the $I4_1/a$ tetragonal symmetry, while C14 TiCr$_2$H$_4$ shows the $R\bar3c$ rhombohedral symmetry. Hydrogen repulsion are found to extend to edge-sharing interstices, affecting the hydrogen ordering. Furthermore, the $6h_2$ A$_2$B$_2$ interstices are found to be energetically substantially more preferable for C14 TiCr$_2$H$_x$ than the other A$_2$B$_2$ interstices at low hydrogen concentrations, influencing the hydrogen-occupation trend.
format Preprint
id arxiv_https___arxiv_org_abs_2503_22824
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Machine Learning Potentials for Hydrogen Absorption in TiCr$_2$ Laves Phases
Kumar, Pranav
Körmann, Fritz
Grabowski, Blazej
Ikeda, Yuji
Materials Science
The energetics of hydrogen absorption in C15 cubic and C14 hexagonal TiCr$_2$H$_x$ Laves phases is investigated for $0 < x \le 6$ with density functional theory (DFT) and machine learning interatomic potentials (MLIPs). The MLIPs are trained with configurations generated through a series of active-learning schemes. Basin-hopping Monte Carlo (BHMC) simulations based on the MLIPs predict minimum-energy hydrogen configurations, along with enthalpies of formation and hydrogen orderings. The obtained phase transformations at 0 K agree well with the experiments at low temperatures. The hydrogen solubility limits in the low-concentration $α$ phases at 0 K are predicted to be $x = 1.0$ and $x = 1.5$ for the C15 and the C14 phases, respectively. At these concentrations, C15 TiCr$_2$H shows the $Cc$ monoclinic symmetry, while C14 TiCr$_2$H$_{1.5}$ shows the $Ama2$ orthorhombic symmetry, both of which have not been reported for this system. The first and the second hydride phases, i.e., $β$ and $β'$, at 0 K are found around $x = 3$ and $x = 4$, respectively, for both the C15 and the C14 phases. In the second-hydride $β'$ phases, C15 TiCr$_2$H$_4$ shows the $I4_1/a$ tetragonal symmetry, while C14 TiCr$_2$H$_4$ shows the $R\bar3c$ rhombohedral symmetry. Hydrogen repulsion are found to extend to edge-sharing interstices, affecting the hydrogen ordering. Furthermore, the $6h_2$ A$_2$B$_2$ interstices are found to be energetically substantially more preferable for C14 TiCr$_2$H$_x$ than the other A$_2$B$_2$ interstices at low hydrogen concentrations, influencing the hydrogen-occupation trend.
title Machine Learning Potentials for Hydrogen Absorption in TiCr$_2$ Laves Phases
topic Materials Science
url https://arxiv.org/abs/2503.22824