An improved interatomic potential for xenon in UO2: a combined density functional theory/genetic algorithm approach

J Phys Condens Matter. 2014 Mar 12;26(10):105501. doi: 10.1088/0953-8984/26/10/105501. Epub 2014 Feb 19.

Abstract

We have created an improved xenon interatomic potential for use with existing UO2 potentials. This potential was fit to density functional theory calculations with the Hubbard U correction (DFT + U) using a genetic algorithm approach called iterative potential refinement (IPR). We examine the defect energetics of the IPR-fitted xenon interatomic potential as well as other, previously published xenon potentials. We compare these potentials to DFT + U derived energetics for a series of xenon defects in a variety of incorporation sites (large, intermediate, and small vacant sites). We find the existing xenon potentials overestimate the energy needed to add a xenon atom to a wide set of defect sites representing a range of incorporation sites, including failing to correctly rank the energetics of the small incorporation site defects (xenon in an interstitial and xenon in a uranium site neighboring uranium in an interstitial). These failures are due to problematic descriptions of Xe-O and/or Xe-U interactions of the previous xenon potentials. These failures are corrected by our newly created xenon potential: our IPR-generated potential gives good agreement with DFT + U calculations to which it was not fitted, such as xenon in an interstitial (small incorporation site) and xenon in a double Schottky defect cluster (large incorporation site). Finally, we note that IPR is very flexible and can be applied to a wide variety of potential forms and materials systems, including metals and EAM potentials.

Publication types

  • Comparative Study

MeSH terms

  • Algorithms*
  • Computer Simulation
  • Models, Chemical*
  • Models, Molecular*
  • Quantum Theory*
  • Uranium Compounds / chemistry*
  • Xenon / chemistry*

Substances

  • Uranium Compounds
  • Xenon
  • uranium oxide