First-principles study of noble gas impurities and defects in UO 2

Alexander E. Thompson*, C. Wolverton

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

70 Scopus citations


We performed a series of density functional theory + U (DFT + U) calculations to explore the energetics of various defects in UO2, i.e., noble gases (He, Ne, Ar, Kr, Xe), Schottky defects, and the interaction between these defects. We found the following: (1) collinear antiferromagnetic UO2 has an energy-lowering distortion of the oxygen sublattice from ideal fluorite positions; (2) DFT + U qualitatively affects the formation volume of Schottky defect clusters in UO2 (without U the formation volume is negative, but including U the formation volume is positive); (3) the configuration of the Schottky defect cluster is dictated by a competition between electrostatic and surface energy effects; (4) the incorporation energy of inserting noble gas atoms into an interstitial site has a strong dependence on the volume of the noble gas atom, corresponding to the strain it causes in the interstitial site, from He (0.98 eV) to Xe (9.73 eV); (5) the energetics of each of the noble gas atoms incorporated in Schottky defects show strong favorable binding, due to strain relief associated with moving the noble gas atom from the highly strained interstitial position into the vacant space of the Schottky defect; and (6) for argon, krypton, and xenon, the binding energy of a noble gas impurity with the Schottky defect is larger than the formation energy of a Schottky defect, thereby making the formation of Schottky defects thermodynamically favorable in the presence of these large impurities.

Original languageEnglish (US)
Article number134111
JournalPhysical Review B - Condensed Matter and Materials Physics
Issue number13
StatePublished - Oct 21 2011

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Condensed Matter Physics


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