Determination of Thermal Expansion, Defect Formation Energy, and Defect-Induced Strain of α-U Via ab Initio Molecular Dynamics
Abstract
Uranium (U) is often alloyed with molybdenum (Mo) or zirconium (Zr) in order to stabilize its high-temperature body-centered cubic phase for use in nuclear reactors. However, in all metallic fuel forms, the α phase of U remains in some fraction. This phase decomposition due to temperature or compositional variance can play an outsized role on fuel performance and microstructural evolution. Relatively little is known about fundamental point defect properties in α -U at non-zero temperatures, from either computational or experimental studies. This work performs the first thorough evaluation of the α phase of U via ab initio molecular dynamics (AIMD). A number of thermophysical properties are calculated as a function of temperature, including equilibrium lattice parameters, thermal expansion, and heat capacity. These results indicate a two-region behavior, with the transition at 400 K. The thermal expansion/contraction in the a / b direction occurs rapidly from 100 up to 400 K, after which a more linear and gradual change in the lattice constant takes place. The volumetric expansion matches experiments quantitatively, but the individual lattice constant expansion only matches experiments qualitatively. Point defect formation energies and induced lattice strains are also determined as a function of temperature, providing insight on defect populations andmore »
- Authors:
- Publication Date:
- Research Org.:
- Idaho National Laboratory (INL), Idaho Falls, ID (United States)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
- OSTI Identifier:
- 1787674
- Alternate Identifier(s):
- OSTI ID: 2222434
- Report Number(s):
- INL/JOU-22-68788-Revision-0
Journal ID: ISSN 2296-8016; 661387
- Grant/Contract Number:
- AC07-05ID14517
- Resource Type:
- Published Article
- Journal Name:
- Frontiers in Materials
- Additional Journal Information:
- Journal Name: Frontiers in Materials Journal Volume: 8; Journal ID: ISSN 2296-8016
- Publisher:
- Frontiers Media SA
- Country of Publication:
- Switzerland
- Language:
- English
- Subject:
- 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; 36 MATERIALS SCIENCE; alpha uranium; ab initio molecular dynamics; point defects; lattice strain; fuel swelling
Citation Formats
Beeler, Benjamin, Mahbuba, Khadija, Wang, Yuhao, and Jokisaari, Andrea. Determination of Thermal Expansion, Defect Formation Energy, and Defect-Induced Strain of α-U Via ab Initio Molecular Dynamics. Switzerland: N. p., 2021.
Web. doi:10.3389/fmats.2021.661387.
Beeler, Benjamin, Mahbuba, Khadija, Wang, Yuhao, & Jokisaari, Andrea. Determination of Thermal Expansion, Defect Formation Energy, and Defect-Induced Strain of α-U Via ab Initio Molecular Dynamics. Switzerland. https://doi.org/10.3389/fmats.2021.661387
Beeler, Benjamin, Mahbuba, Khadija, Wang, Yuhao, and Jokisaari, Andrea. Thu .
"Determination of Thermal Expansion, Defect Formation Energy, and Defect-Induced Strain of α-U Via ab Initio Molecular Dynamics". Switzerland. https://doi.org/10.3389/fmats.2021.661387.
@article{osti_1787674,
title = {Determination of Thermal Expansion, Defect Formation Energy, and Defect-Induced Strain of α-U Via ab Initio Molecular Dynamics},
author = {Beeler, Benjamin and Mahbuba, Khadija and Wang, Yuhao and Jokisaari, Andrea},
abstractNote = {Uranium (U) is often alloyed with molybdenum (Mo) or zirconium (Zr) in order to stabilize its high-temperature body-centered cubic phase for use in nuclear reactors. However, in all metallic fuel forms, the α phase of U remains in some fraction. This phase decomposition due to temperature or compositional variance can play an outsized role on fuel performance and microstructural evolution. Relatively little is known about fundamental point defect properties in α -U at non-zero temperatures, from either computational or experimental studies. This work performs the first thorough evaluation of the α phase of U via ab initio molecular dynamics (AIMD). A number of thermophysical properties are calculated as a function of temperature, including equilibrium lattice parameters, thermal expansion, and heat capacity. These results indicate a two-region behavior, with the transition at 400 K. The thermal expansion/contraction in the a / b direction occurs rapidly from 100 up to 400 K, after which a more linear and gradual change in the lattice constant takes place. The volumetric expansion matches experiments quantitatively, but the individual lattice constant expansion only matches experiments qualitatively. Point defect formation energies and induced lattice strains are also determined as a function of temperature, providing insight on defect populations and the fundamentals of irradiation growth in α -U. Interstitials induce significantly more strain than vacancies, and the nature of that strain is highly dependent on the individual lattice directions. The direction of point defect-induced lattice strain is contrary to the irradiation growth behavior of α -U. This work shows that isolated point defects cannot be the primary driving force responsible for the significant irradiation-induced growth of α -U observed experimentally.},
doi = {10.3389/fmats.2021.661387},
journal = {Frontiers in Materials},
number = ,
volume = 8,
place = {Switzerland},
year = {Thu Jun 10 00:00:00 EDT 2021},
month = {Thu Jun 10 00:00:00 EDT 2021}
}
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Works referenced in this record:
Length and electrical resistivity changes of neutron irradiated uranium
journal, September 1968
- Loomis, B. A.; Gerber, S. B.
- Philosophical Magazine, Vol. 18, Issue 153
Adiabatic Elastic Moduli of Single Crystal Alpha‐Uranium
journal, October 1958
- Fisher, E. S.; McSkimin, H. J.
- Journal of Applied Physics, Vol. 29, Issue 10
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
The Thermodynamic Properties of the f-Elements and Their Compounds. I. The Lanthanide and Actinide Metals
journal, December 2010
- Konings, Rudy J. M.; Beneš, Ondrej
- Journal of Physical and Chemical Reference Data, Vol. 39, Issue 4
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
Irradiation-induced internal stresses in polycrystalline -uranium: a mesoscale mechanical approach
journal, April 2020
- Jokisaari, A. M.
- Computational Materials Science, Vol. 176
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
First-principles study of bubble nucleation and growth behaviors in α U–Zr
journal, September 2012
- Huang, Gui-Yang; Wirth, B. D.
- Journal of Physics: Condensed Matter, Vol. 24, Issue 41
Enthalpy of uranium to 1500 K by drop calorimetry
journal, July 1976
- Marchidan, D. I.; Ciopec, M.
- The Journal of Chemical Thermodynamics, Vol. 8, Issue 7
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
Lattice dynamics simulation using machine learning interatomic potentials
journal, February 2020
- Ladygin, V. V.; Korotaev, P. Yu.; Yanilkin, A. V.
- Computational Materials Science, Vol. 172
Generalized Gradient Approximation Made Simple [Phys. Rev. Lett. 77, 3865 (1996)]
journal, February 1997
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 78, Issue 7
Quantum mechanical calculations of uranium phases and niobium defects in γ-uranium
journal, March 2008
- Xiang, Shikai; Huang, Hanchen; Hsiung, L. M.
- Journal of Nuclear Materials, Vol. 375, Issue 1
Theory of the crystal structures of cerium and the light actinides
journal, November 1998
- Soderlind, Per
- Advances in Physics, Vol. 47, Issue 6
Dissociation of NaCl in water from ab initio molecular dynamics simulations
journal, March 2010
- Timko, Jeff; Bucher, Denis; Kuyucak, Serdar
- The Journal of Chemical Physics, Vol. 132, Issue 11