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Quantum Accurate Prediction of Plutonium–Plutonium Dihydride Phase Equilibrium Using a Spin-Lattice Model

preprint
submitted on 12.03.2020 and posted on 13.03.2020 by Ryan Gotchy Mullen, Nir Goldman

Plutonium-based materials are vital for use as nuclear fuels and as portable power sources for space vehicles. However, elucidating their sensitivity to hydriding corrosion represents an extreme challenge due to the toxicity of Pu as well as its anomalous magnetic properties. In this work, we develop a spin-lattice model of plutonium–plutonium dihydride (Pu–PuH2) phase equilibrium that retains the accuracy of density functional theory (DFT) while yielding many orders of magnitude improvement in computational efficiency. Using Monte Carlo and free energy sampling algorithms, we compute a number of Pu–PuH2 equilibrium properties that are difficult to probe experimentally, including equilibrium pressures and phase compositions at room temperature and the PuH2 heat of formation. Our method will have particular impact on these types of materials studies, where there is a strong need for computationally efficient approaches to bridge time and length scale gaps between quantum calculations and experiments.

History

Email Address of Submitting Author

mullen10@llnl.gov

Institution

Lawrence Livermore National Laboratory

Country

United States

ORCID For Submitting Author

0000-0002-2099-6955

Declaration of Conflict of Interest

No conflict of interest.

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