Development of Xe and Kr empirical potentials for CeO2, ThO2, UO2 and PuO2, combining DFT with high temperature MD

M. W.D. Cooper, N. Kuganathan, P. A. Burr, M. J.D. Rushton, R. W. Grimes, C. R. Stanek, D. A. Andersson

Research output: Contribution to journalArticle

13 Citations (Scopus)

Abstract

The development of embedded atom method (EAM) many-body potentials for actinide oxides and associated mixed oxide (MOX) systems has motivated the development of a complementary parameter set for gas-actinide and gas-oxygen interactions. A comprehensive set of density functional theory (DFT) calculations were used to study Xe and Kr incorporation at a number of sites in CeO2, ThO2, UO2 and PuO2. These structures were used to fit a potential, which was used to generate molecular dynamics (MD) configurations incorporating Xe and Kr at 300 K, 1500 K, 3000 K and 5000 K. Subsequent matching to the forces predicted by DFT for these MD configurations was used to refine the potential set. This fitting approach ensured weighted fitting to configurations that are thermodynamically significant over a broad temperature range, while avoiding computationally expensive DFT-MD calculations. The resultant gas potentials were validated against DFT trapping energies and are suitable for simulating combinations of Xe and Kr in solid solutions of CeO2, ThO2, UO2 and PuO2, providing a powerful tool for the atomistic simulation of conventional nuclear reactor fuel UO2 as well as advanced MOX fuels.

Original languageEnglish
Article number405401
JournalJournal of Physics Condensed Matter
Volume28
Issue number40
DOIs
Publication statusPublished - 23 Aug 2016
Externally publishedYes

Fingerprint

Density functional theory
Molecular dynamics
Actinoid Series Elements
molecular dynamics
density functional theory
nuclear fuels
Gases
Actinides
mixed oxides
Oxides
configurations
gases
Mixed oxide fuels
Temperature
embedded atom method
nuclear reactors
Nuclear reactors
Solid solutions
solid solutions
trapping

Keywords

  • atomic interactions
  • empirical potentials
  • fission gas
  • molecular dynamics
  • nuclear fuel

ASJC Scopus subject areas

  • Materials Science(all)
  • Condensed Matter Physics

Cite this

Development of Xe and Kr empirical potentials for CeO2, ThO2, UO2 and PuO2, combining DFT with high temperature MD. / Cooper, M. W.D.; Kuganathan, N.; Burr, P. A.; Rushton, M. J.D.; Grimes, R. W.; Stanek, C. R.; Andersson, D. A.

In: Journal of Physics Condensed Matter, Vol. 28, No. 40, 405401, 23.08.2016.

Research output: Contribution to journalArticle

Cooper, M. W.D. ; Kuganathan, N. ; Burr, P. A. ; Rushton, M. J.D. ; Grimes, R. W. ; Stanek, C. R. ; Andersson, D. A. / Development of Xe and Kr empirical potentials for CeO2, ThO2, UO2 and PuO2, combining DFT with high temperature MD. In: Journal of Physics Condensed Matter. 2016 ; Vol. 28, No. 40.
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