Density functional theory calculations of the thermodynamic and kinetic properties of point defects in β -U
Abstract
Density functional theory (DFT) calculations of the thermodynamic and kinetic properties of point defects in the β phase of uranium are reported. Defect energies and entropies were calculated using 2 x 2 x 2 supercells and the Generalized Gradient Approximation (GGA) of Perdew-Burke-Ernzerhof (PBE) for the exchange-correlation potential. Due to computational cost, calculations of the vibrational properties governing entropies were performed by only displacing atoms within (roughly) the 3rd or 4th nearest neighbor shell of the defect, which implicitly assumes that atoms beyond this distance are unaffected by the defect. Migration barriers were estimated by nudged elastic band (NEB) calculations. The low symmetry of the β-U phase (the unit cell is tetragonal and contains 30 atoms) results in many point defect configurations and even more migration pathways. A connectivity map, starting from the most stable point defects, was developed in order to identify the rate-limiting step controlling the net diffusion rate in each crystallographic direction. The uranium self-diffusivity tensor was calculated by combining the defect formation energies, entropies, migration barriers and attempt frequencies. The fastest diffusion rate was determined to be a vacancy mechanism in the z crystallographic direction. The predicted uranium self-diffusivity for this mechanism agrees well with availablemore »
- Authors:
-
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Univ. of Wisconsin, Madison, WI (United States)
- North Carolina State University, Raleigh, NC (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE), Nuclear Energy Advanced Modeling and Simulation (NEAMS); USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1998113
- Report Number(s):
- LA-UR-21-22460
Journal ID: ISSN 0022-3115; TRN: US2405354
- Grant/Contract Number:
- 89233218CNA000001
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Nuclear Materials
- Additional Journal Information:
- Journal Volume: 557; Journal ID: ISSN 0022-3115
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; nuclear fuel; Uranium; DFT; diffusion
Citation Formats
Andersson, David Anders, Matthews, Christopher, Zhang, Yongfeng, and Beeler, Benjamin. Density functional theory calculations of the thermodynamic and kinetic properties of point defects in β-U. United States: N. p., 2021.
Web. doi:10.1016/j.jnucmat.2021.153238.
Andersson, David Anders, Matthews, Christopher, Zhang, Yongfeng, & Beeler, Benjamin. Density functional theory calculations of the thermodynamic and kinetic properties of point defects in β-U. United States. https://doi.org/10.1016/j.jnucmat.2021.153238
Andersson, David Anders, Matthews, Christopher, Zhang, Yongfeng, and Beeler, Benjamin. Fri .
"Density functional theory calculations of the thermodynamic and kinetic properties of point defects in β-U". United States. https://doi.org/10.1016/j.jnucmat.2021.153238. https://www.osti.gov/servlets/purl/1998113.
@article{osti_1998113,
title = {Density functional theory calculations of the thermodynamic and kinetic properties of point defects in β-U},
author = {Andersson, David Anders and Matthews, Christopher and Zhang, Yongfeng and Beeler, Benjamin},
abstractNote = {Density functional theory (DFT) calculations of the thermodynamic and kinetic properties of point defects in the β phase of uranium are reported. Defect energies and entropies were calculated using 2 x 2 x 2 supercells and the Generalized Gradient Approximation (GGA) of Perdew-Burke-Ernzerhof (PBE) for the exchange-correlation potential. Due to computational cost, calculations of the vibrational properties governing entropies were performed by only displacing atoms within (roughly) the 3rd or 4th nearest neighbor shell of the defect, which implicitly assumes that atoms beyond this distance are unaffected by the defect. Migration barriers were estimated by nudged elastic band (NEB) calculations. The low symmetry of the β-U phase (the unit cell is tetragonal and contains 30 atoms) results in many point defect configurations and even more migration pathways. A connectivity map, starting from the most stable point defects, was developed in order to identify the rate-limiting step controlling the net diffusion rate in each crystallographic direction. The uranium self-diffusivity tensor was calculated by combining the defect formation energies, entropies, migration barriers and attempt frequencies. The fastest diffusion rate was determined to be a vacancy mechanism in the z crystallographic direction. The predicted uranium self-diffusivity for this mechanism agrees well with available experimental data. Finally, the diffusion mechanisms and rates identified in this study will inform fuel performance models of swelling and gas evolution.},
doi = {10.1016/j.jnucmat.2021.153238},
journal = {Journal of Nuclear Materials},
number = ,
volume = 557,
place = {United States},
year = {Fri Aug 13 00:00:00 EDT 2021},
month = {Fri Aug 13 00:00:00 EDT 2021}
}
Works referenced in this record:
Metallic fuels for advanced reactors
journal, July 2009
- Carmack, W. J.; Porter, D. L.; Chang, Y. I.
- Journal of Nuclear Materials, Vol. 392, Issue 2
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
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Ab initio molecular dynamics investigation of point defects in -U
journal, March 2021
- Beeler, Benjamin; Andersson, David; Jiang, Chao
- Journal of Nuclear Materials, Vol. 545
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
journal, July 1996
- Kresse, G.; Furthmüller, J.
- Computational Materials Science, Vol. 6, Issue 1, p. 15-50
Structure, formation energies and elastic constants of uranium metal investigated by first principles calculations
journal, March 2012
- Li, J. H.; Ren, Q. B.; Lu, C. H.
- Journal of Alloys and Compounds, Vol. 516
KineCluE: A kinetic cluster expansion code to compute transport coefficients beyond the dilute limit
journal, February 2020
- Schuler, Thomas; Messina, Luca; Nastar, Maylise
- Computational Materials Science, Vol. 172
Special points for Brillouin-zone integrations
journal, June 1976
- Monkhorst, Hendrik J.; Pack, James D.
- Physical Review B, Vol. 13, Issue 12, p. 5188-5192
Vacancy Formation Enthalpy in Polycrystalline Depleted Uranium
journal, June 2013
- Lund, K. R.; Lynn, K. G.; Weber, M. H.
- Journal of Physics: Conference Series, Vol. 443
Ab initio molecular dynamics for open-shell transition metals
journal, November 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 48, Issue 17
High-temperature and high-pressure phase transitions in uranium
journal, February 2017
- Bouchet, J.; Bottin, F.
- Physical Review B, Vol. 95, Issue 5
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Calculation of point-defect entropy in metals
journal, November 2001
- Mishin, Yuri; S⊘rensen, Mads R.; Voter, Arthur F.
- Philosophical Magazine A, Vol. 81, Issue 11
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Abaissement des coefficients d'autodiffusion de l'uranium en phase γ par des additions de molybdene, de zirconium ou de niobium
journal, May 1962
- Adda, Y.; Kirianenko, A.
- Journal of Nuclear Materials, Vol. 6, Issue 1
Cluster dynamics simulation of uranium self-diffusion during irradiation in UO2
journal, December 2019
- Matthews, Christopher; Perriot, Romain; Cooper, Michael W. D.
- Journal of Nuclear Materials, Vol. 527
First-principles elastic and structural properties of uranium metal
journal, August 2002
- Söderlind, Per
- Physical Review B, Vol. 66, Issue 8
Atomistic properties of γ uranium
journal, February 2012
- Beeler, Benjamin; Deo, Chaitanya; Baskes, Michael
- Journal of Physics: Condensed Matter, Vol. 24, Issue 7
The structure of β-uranium
journal, September 1971
- Donohue, J.; Einspahr, H.
- Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 27, Issue 9
Investigation of vacancy formation and phase transformations in uranium by positron annihilation
journal, February 1980
- Matter, H.; Winter, J.; Triftshäuser, W.
- Journal of Nuclear Materials, Vol. 88, Issue 2-3
First principles calculations of the structure and elastic constants of α, β and γ uranium
journal, February 2013
- Beeler, Benjamin; Deo, Chaitanya; Baskes, Michael
- Journal of Nuclear Materials, Vol. 433, Issue 1-3
First principles calculations for defects in U
journal, November 2010
- Beeler, B.; Good, B.; Rashkeev, S.
- Journal of Physics: Condensed Matter, Vol. 22, Issue 50
Metallic fast reactor fuels
journal, January 1997
- Hofman, G. L.; Walters, L. C.; Bauer, T. H.
- Progress in Nuclear Energy, Vol. 31, Issue 1-2
Comment on “Correlation and relativistic effects in U metal and U-Zr alloy: Validation of ab initio approaches”
journal, October 2014
- Söderlind, P.; Landa, A.; Turchi, P. E. A.
- Physical Review B, Vol. 90, Issue 15
Correlation and relativistic effects in U metal and U-Zr alloy: Validation of ab initio approaches
journal, December 2013
- Xie, Wei; Xiong, Wei; Marianetti, Chris A.
- Physical Review B, Vol. 88, Issue 23
Coefficient de diffusion du fer dans l'uranium en phase α a 645 °C
journal, June 1972
- Stelly, M.; Servant, J. M.
- Journal of Nuclear Materials, Vol. 43, Issue 3
A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000
- Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes
- The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904
Etude de l'autodiffusion de l'uranium en phase β
journal, October 1959
- Adda, Y.; Kirianenko, A.; Mairy, C.
- Journal of Nuclear Materials, Vol. 1, Issue 3
Etude de l'autodiffusion de l'uranium en phase γ
journal, July 1959
- Adda, Y.; Kirianenko, A.
- Journal of Nuclear Materials, Vol. 1, Issue 2
Frequency factors and isotope effects in solid state rate processes
journal, January 1957
- Vineyard, George H.
- Journal of Physics and Chemistry of Solids, Vol. 3, Issue 1-2
Cluster dynamics simulation of xenon diffusion during irradiation in UO2
journal, November 2020
- Matthews, Christopher; Perriot, Romain; Cooper, M. W. D.
- Journal of Nuclear Materials, Vol. 540
Automatic numerical evaluation of vacancy-mediated transport for arbitrary crystals: Onsager coefficients in the dilute limit using a Green function approach
journal, June 2017
- Trinkle, Dallas R.
- Philosophical Magazine, Vol. 97, Issue 28
First-principles study of diffusion of interstitial and vacancy in α U–Zr
journal, May 2011
- Huang, Gui-Yang; Wirth, Brian D.
- Journal of Physics: Condensed Matter, Vol. 23, Issue 20
First-principles calculations of the stability and incorporation of helium, xenon and krypton in uranium
journal, June 2012
- Beeler, B.; Good, B.; Rashkeev, S.
- Journal of Nuclear Materials, Vol. 425, Issue 1-3
Thermodynamic stabilization of alloys: Effect of Mo content and temperature
journal, May 2020
- Castellano, Aloïs; Bottin, François; Dorado, Boris
- Physical Review B, Vol. 101, Issue 18
Swelling behavior of U-Pu-Zr fuel
journal, February 1990
- Hofman, Gerard L.; Pahl, R. G.; Lahm, C. E.
- Metallurgical Transactions A, Vol. 21, Issue 2