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

submitted on 12.03.2020, 22:50 and posted on 13.03.2020, 12:56 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.


Email Address of Submitting Author


Lawrence Livermore National Laboratory


United States

ORCID For Submitting Author


Declaration of Conflict of Interest

No conflict of interest.