A reactive molecular dynamics model for uranium/hydrogen containing systems

Uranium-based materials are valuable assets in the energy, medical, and military industries. However, understanding their sensitivity to hydrogen embrittlement is particularly challenging due to the toxicity of uranium and the computationally expensive nature of quantum-based methods generally requi...

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Bibliographic Details
Published in:The Journal of chemical physics 2024-03, Vol.160 (9)
Main Authors: Soshnikov, Artem, Lindsey, Rebecca, Kulkarni, Ambarish, Goldman, Nir
Format: Article
Language:English
Subjects:
Actinides
Chebyshev approximation
Computational efficiency
computational models
CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
corrosion
Density Functional Theory
Diffusion barriers
embrittlement
Free energy
Heat of formation
hydriding
Hydrogen
Hydrogen embrittlement
INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Interaction models
Interstitials
machine learning
MATERIALS SCIENCE
Molecular dynamics
Quantum theory
Temperature dependence
Uranium
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Summary:Uranium-based materials are valuable assets in the energy, medical, and military industries. However, understanding their sensitivity to hydrogen embrittlement is particularly challenging due to the toxicity of uranium and the computationally expensive nature of quantum-based methods generally required to study such processes. In this regard, we have developed a Chebyshev Interaction Model for Efficient Simulation (ChIMES) that can be employed to compute energies and forces of U and UH3 bulk structures with vacancies and hydrogen interstitials with accuracy similar to that of Density Functional Theory (DFT) while yielding linear scaling and orders of magnitude improvement in computational efficiency. We show that the bulk structural parameters, uranium and hydrogen vacancy formation energies, and diffusion barriers predicted by the ChIMES potential are in strong agreement with the reference DFT data. We then use ChIMES to conduct molecular dynamics simulations of the temperature-dependent diffusion of a hydrogen interstitial and determine the corresponding diffusion activation energy. Our model has particular significance in studies of actinides and other high-Z materials, where there is a strong need for computationally efficient methods to bridge length and time scales between experiments and quantum theory.
ISSN:0021-9606
1089-7690
DOI:10.1063/5.0183610