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

Abstract

In this study, 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.

Authors:
 [1];  [2];  [3];  [2];  [2];  [1];  [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Imperial College London, London (United Kingdom)
  3. Univ. of New South Wales, Sydney, NSW (Australia)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1325651
Alternate Identifier(s):
OSTI ID: 1306679
Report Number(s):
LA-UR-16-22766
Journal ID: ISSN 0953-8984; TRN: US1700096
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physics. Condensed Matter
Additional Journal Information:
Journal Volume: 28; Journal Issue: 40; Journal ID: ISSN 0953-8984
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; molecular dynamics; empirical potentials; atomic interactions; fission gas; nuclear fuel

Citation Formats

Cooper, M. W. D., Kuganathan, N., Burr, P. A., Rushton, M. J. D., Grimes, R. W., Stanek, C. R., and Andersson, D. A. Development of Xe and Kr empirical potentials for CeO2, ThO2, UO2 and PuO2, combining DFT with high temperature MD. United States: N. p., 2016. Web. https://doi.org/10.1088/0953-8984/28/40/405401.
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. United States. https://doi.org/10.1088/0953-8984/28/40/405401
Cooper, M. W. D., Kuganathan, N., Burr, P. A., Rushton, M. J. D., Grimes, R. W., Stanek, C. R., and Andersson, D. A. Tue . "Development of Xe and Kr empirical potentials for CeO2, ThO2, UO2 and PuO2, combining DFT with high temperature MD". United States. https://doi.org/10.1088/0953-8984/28/40/405401. https://www.osti.gov/servlets/purl/1325651.
@article{osti_1325651,
title = {Development of Xe and Kr empirical potentials for CeO2, ThO2, UO2 and PuO2, combining DFT with high temperature MD},
author = {Cooper, M. W. D. and Kuganathan, N. and Burr, P. A. and Rushton, M. J. D. and Grimes, R. W. and Stanek, C. R. and Andersson, D. A.},
abstractNote = {In this study, 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.},
doi = {10.1088/0953-8984/28/40/405401},
journal = {Journal of Physics. Condensed Matter},
number = 40,
volume = 28,
place = {United States},
year = {2016},
month = {8}
}

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Works referenced in this record:

Thermophysical properties and oxygen transport in the (U ,Pu1−)O2 lattice
journal, June 2015


Gallium Removal from Weapons-Grade Plutonium and Cerium Oxide Surrogate by a Thermal Technique
journal, January 1999

  • Park, YoungSoo; Kolman, David G.; Ziraffe, Hisham
  • MRS Proceedings, Vol. 556
  • DOI: 10.1557/proc-556-129

A new empirical potential for simulating the formation of defects and their mobility in uranium dioxide
journal, January 2003


Molecular dynamics study on planar clustering of xenon in UO2
journal, June 2008


Predicting the probability for fission gas resolution into uranium dioxide
journal, July 2009


Thermophysical and anion diffusion properties of (U x ,Th 1− x )O 2
journal, November 2014

  • Cooper, Michael W. D.; Murphy, Samuel T.; Fossati, Paul C. M.
  • Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 470, Issue 2171
  • DOI: 10.1098/rspa.2014.0427

Fission Gas Release during Post Irradiation Annealing of BWR Fuels
journal, November 1990


Stability of oxygen point defects in UO 2 by first-principles DFT + U calculations: Occupation matrix control and Jahn-Teller distortion
journal, July 2010


Nuclear Fuels: Present and Future
journal, February 2009


Fast Parallel Algorithms for Short-Range Molecular Dynamics
journal, March 1995


GULP: A computer program for the symmetry-adapted simulation of solids
journal, January 1997

  • Gale, Julian D.
  • Journal of the Chemical Society, Faraday Transactions, Vol. 93, Issue 4
  • DOI: 10.1039/a606455h

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


Molecular dynamics simulation of intragranular Xe bubble re-solution in UO2
journal, July 2009


Mechanical and electronic properties of CeO 2 , ThO 2 , and ( Ce , Th ) O 2 alloys
journal, July 2009


The diffusion coefficients of gaseous and volatile species during the irradiation of uranium dioxide
journal, June 1982


An Evaluation of the Thermophysical Properties of Stoichiometric CeO 2 in Comparison to UO 2 and PuO 2
journal, August 2014

  • Nelson, Andrew T.; Rittman, Dylan R.; White, Joshua T.
  • Journal of the American Ceramic Society, Vol. 97, Issue 11
  • DOI: 10.1111/jace.13170

Opportunities for Advanced Ceramics and Composites in the Nuclear Sector
journal, June 2013

  • Lee, William Edward; Gilbert, Matthew; Murphy, Samuel Thomas
  • Journal of the American Ceramic Society, Vol. 96, Issue 7
  • DOI: 10.1111/jace.12406

Diatomic Molecules According to the Wave Mechanics. II. Vibrational Levels
journal, July 1929


LDA+U study of Pu and PuO2 on ground state with spin–orbital coupling
journal, August 2012


Nuclear fuels – Present and future
journal, May 2009


A new fission-gas release model
journal, August 1983


Atomistic study of stability of xenon nanoclusters in uranium oxide
journal, May 2010


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


First-principles study of noble gas impurities and defects in UO 2
journal, October 2011


Embedded-atom method: Derivation and application to impurities, surfaces, and other defects in metals
journal, June 1984


The van der Waals potentials between all the rare gas atoms from He to Rn
journal, March 2003

  • Tang, K. T.; Toennies, J. P.
  • The Journal of Chemical Physics, Vol. 118, Issue 11
  • DOI: 10.1063/1.1543944

Development of a multiscale thermal conductivity model for fission gas in UO2
journal, February 2016


Method for locating low-energy solutions within DFT + U
journal, November 2010


Interplay of defect cluster and the stability of xenon in uranium dioxide from density functional calculations
journal, September 2010


Advances in first-principles modelling of point defects in UO 2 : f electron correlations and the issue of local energy minima
journal, July 2013


Thermodynamics of fission products in UO 2 ± x
journal, October 2009


Density-functional theory and strong interactions: Orbital ordering in Mott-Hubbard insulators
journal, August 1995


Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/physrevlett.77.3865

Segregation of xenon to dislocations and grain boundaries in uranium dioxide
journal, November 2011


The distribution of intragranular fission gas bubbles in UO2 during irradiation
journal, February 1971


Analysis of Intrinsic Defects in CeO 2 Using a Koopmans-Like GGA+ U Approach
journal, November 2011

  • Keating, Patrick R. L.; Scanlon, David O.; Morgan, Benjamin J.
  • The Journal of Physical Chemistry C, Vol. 116, Issue 3
  • DOI: 10.1021/jp2080034

Fission Gas Diffusion in Uranium Dioxide
journal, December 1978

  • Catlow, C. R. A.
  • Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 364, Issue 1719
  • DOI: 10.1098/rspa.1978.0213

Semiempirical GGA-type density functional constructed with a long-range dispersion correction
journal, January 2006

  • Grimme, Stefan
  • Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799
  • DOI: 10.1002/jcc.20495

U and Xe transport in UO 2 ± x : Density functional theory calculations
journal, August 2011


Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976


Gas release mechanisms in UO 2 —a critical review
journal, January 1980


DL_POLY_3: new dimensions in molecular dynamics simulations via massive parallelism
journal, January 2006

  • Todorov, Ilian T.; Smith, William; Trachenko, Kostya
  • Journal of Materials Chemistry, Vol. 16, Issue 20, p. 1911-1918
  • DOI: 10.1039/b517931a

Die Berechnung optischer und elektrostatischer Gitterpotentiale
journal, January 1921


Classical molecular dynamics simulation of UO2 to predict thermophysical properties
journal, October 2003


Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998

  • Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
  • Physical Review B, Vol. 57, Issue 3, p. 1505-1509
  • DOI: 10.1103/physrevb.57.1505

Gallium Removal from Weapons-Grade Plutonium and Cerium Oxide Surrogate by a Thermal Technique
journal, January 1999

  • Park, YoungSoo; Kolman, David G.; Ziraffe, Hisham
  • MRS Proceedings, Vol. 556
  • DOI: 10.1557/PROC-556-129

Segregation of xenon to dislocations and grain boundaries in uranium dioxide
journal, November 2011


U and Xe transport in UO 2 ± x : Density functional theory calculations
journal, August 2011


Embedded-atom method: Derivation and application to impurities, surfaces, and other defects in metals
journal, June 1984


Diatomic Molecules According to the Wave Mechanics. II. Vibrational Levels
journal, July 1929


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Density-functional theory and strong interactions: Orbital ordering in Mott-Hubbard insulators
journal, August 1995


Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998

  • Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
  • Physical Review B, Vol. 57, Issue 3, p. 1505-1509
  • DOI: 10.1103/PhysRevB.57.1505

Mechanical and electronic properties of CeO 2 , ThO 2 , and ( Ce , Th ) O 2 alloys
journal, July 2009


Stability of oxygen point defects in UO 2 by first-principles DFT + U calculations: Occupation matrix control and Jahn-Teller distortion
journal, July 2010


Method for locating low-energy solutions within DFT + U
journal, November 2010


Interplay of defect cluster and the stability of xenon in uranium dioxide from density functional calculations
journal, September 2010


First-principles study of noble gas impurities and defects in UO 2
journal, October 2011


Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976


Atomistic study of stability of xenon nanoclusters in uranium oxide
journal, May 2010


Classical molecular dynamics simulation of UO2 to predict thermophysical properties
journal, October 2003


    Works referencing / citing this record:

    A tungsten-rhenium interatomic potential for point defect studies
    journal, May 2018

    • Setyawan, Wahyu; Gao, Ning; Kurtz, Richard J.
    • Journal of Applied Physics, Vol. 123, Issue 20
    • DOI: 10.1063/1.5030113

    Atomistic model of xenon gas bubble re-solution rate due to thermal spike in uranium oxide
    journal, August 2018

    • Setyawan, Wahyu; Cooper, Michael W. D.; Roche, Kenneth J.
    • Journal of Applied Physics, Vol. 124, Issue 7
    • DOI: 10.1063/1.5042770