A reactive molecular dynamics model for uranium/hydrogen containing systems

Soshnikov, Artem; Lindsey, Rebecca; Kulkarni, Ambarish; Goldman, Nir

doi:10.1063/5.0183610

Title: A reactive molecular dynamics model for uranium/hydrogen containing systems

Journal Article · 07 March 2024 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/5.0183610 · OSTI ID:2375948

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Univ. of California, Davis, CA (United States)
Univ. of Michigan, Ann Arbor, MI (United States)
Univ. of California, Davis, CA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

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. Here, 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.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 2375948

Report Number(s):: LLNL-JRNL-855941; 1085155

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 9 Vol. 160; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Title: A reactive molecular dynamics model for uranium/hydrogen containing systems

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