Development and application of a uranium mononitride (UN) potential: Thermomechanical properties and Xe diffusion

Kocevski, Vancho; Cooper, Michael William Donald; Claisse, Antoine; Andersson, Anders David Ragnar

doi:10.1016/j.jnucmat.2022.153553

Development and application of a uranium mononitride (UN) potential: Thermomechanical properties and Xe diffusion

Journal Article · Wed Feb 02 00:00:00 EST 2022 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2022.153553· OSTI ID:1845260

Kocevski, Vancho ^[1]; ^[1]; Claisse, Antoine ^[2]; ^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Westinghouse Electric Sweden, Vasteras (Sweden)

We report that atomic-scale modeling of thermophysical and defect properties of uranium mononitride (UN) plays an important role in establishing a better understanding and improved models of UN fuel performance. Having an accurate interatomic potential is crucial for generating reliable data at finite temperatures using molecular dynamic simulations. We report a new interatomic potential for UN, based on a combination of many-body and pairwise interactions, a simple form that we later show could be easily adapted to include Xe-U and Xe-N interactions, i.e., generating a U-N-Xe interatomic potential. The potential was fitted to experimental thermal expansion and single crystal elastic constants, as well as Frenkel, Schottky, anti-Schottky, and antisite pair reaction energies from density functional theory (DFT) calculations. Using the potential, we successfully reproduced experimental lattice parameters, thermal expansion, single crystal elastic constants, and temperature dependent heat capacity. The potential also performs reasonably well in reproducing the energy of the aforementioned stoichiometric defect reactions and defect migration barriers calculated using DFT. However, the potential underestimates the energy difference between the tetrahedral and dumbbell uranium interstitials, and a more complex potential form might be needed to overcome this issue. The potential was also used to predict UN single crystal elastic constants and elastic properties at different temperatures, showing that UN becomes softer and more compressible with increasing temperature. We also compare our potential against literature data from previous empirical potentials, demonstrating similar or better behavior depending on the property of interest. To enable the simulation of Xe in UN a Buckingham potential has been fitted to DFT-derived Xe incorporation energies. The potential was then used to determine the activation energy for Xe diffusion due to various Xe-containing defects, with {XeU : VU} exhibiting the lowest activation energy.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

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

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1845260

Report Number(s):: LA-UR-21-28424

Journal Information:: Journal of Nuclear Materials, Journal Name: Journal of Nuclear Materials Vol. 562; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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