Establishing the temperature and orientation dependence of the threshold displacement energy in ThO2 via molecular dynamics simulations

Yu, Lin-Chieh; Zhou, Shuxiang; Jin, Miaomiao; Khafizov, Marat; Hurley, David H.; Zhang, Yongfeng

doi:10.1016/j.nme.2024.101774

Establishing the temperature and orientation dependence of the threshold displacement energy in ThO₂ via molecular dynamics simulations

Journal Article · Sun Oct 20 00:00:00 EDT 2024 · Nuclear Materials and Energy

DOI:https://doi.org/10.1016/j.nme.2024.101774· OSTI ID:2474353

^[1]; ^[2]; ^[3]; ^[4]; ^[2]; ^[1]

Univ. of Wisconsin, Madison, WI (United States)
Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Pennsylvania State Univ., University Park, PA (United States)
The Ohio State Univ., Columbus, OH (United States)

ThO₂ is a promising fuel for next-generation nuclear reactors. As a critical quantity measuring its radiation tolerance, the dependence of the threshold displacement energy on temperature and crystal orientation in ThO₂ is unclear and established using comprehensive molecular dynamics simulations in this work. For both Th and O primary knock-on atoms (PKAs), the thresholds, denoted as $$E_d^{Th}$$ and $$E_d^O$$, respectively, are calculated using two different interatomic potentials. Similar temperature and orientation dependence are observed, albeit with some quantitative differences. While on average over all orientations, higher energy is required for Th PKAs than O PKAs to displace atoms, the polar-averaged $$E_d^{Th}$$ is significantly lower than that for $$E_d^O$$. Further, $$E_d^{Th}$$ and $$E_d^O$$ show different crystal orientation dependence and temperature dependence. Notably, the cubic symmetry in the fluorite structure is followed by $$E_d^{Th}$$ but does not hold for $$E_d^O$$ because of the existence of two sublattices. The much higher average $$E_d^O$$ and $$E_d^{Th}$$ and their different temperature dependence are interpreted by the distinct recombination rates of Th and O Frenkel pairs in thermal spikes, resulting from the substantially lower migration barriers of O vacancies and interstitials. The recombination of O vacancies and interstitials, both of which are charged, is further enhanced by the Coulomb interaction at small Frenkel pair separations. The new findings are discussed for their generality in fluorite-structured oxides by comparing the results in ThO₂ and UO₂.

View Journal Article

Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: USDOE; USDOE Office of Nuclear Energy (NE); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC07-05ID14517

OSTI ID:: 2474353

Alternate ID(s):: OSTI ID: 2570601

Report Number(s):: INL/JOU--24-76199-Rev000

Journal Information:: Nuclear Materials and Energy, Journal Name: Nuclear Materials and Energy Vol. 41; ISSN 2352-1791

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (64)

Fast Parallel Algorithms for Short-Range Molecular Dynamics Plimpton, Steve Journal of Computational Physics, Vol. 117, Issue 1 https://doi.org/10.1006/jcph.1995.1039	journal	March 1995
The Stopping and Range of Ions in Matter Ziegler, James F.; Biersack, Jochen P. Treatise on Heavy-Ion Science https://doi.org/10.1007/978-1-4615-8103-1_3	book	January 1985
The calculated defect structure of thoria Colbourn, E. A.; Mackrodt, W. C. Journal of Nuclear Materials, Vol. 118, Issue 1 https://doi.org/10.1016/0022-3115(83)90178-2	journal	August 1983
High voltage electron microscope observations of UO2 Soullard, J. Journal of Nuclear Materials, Vol. 135, Issue 2-3 https://doi.org/10.1016/0022-3115(85)90077-7	journal	October 1985
A proposed method of calculating displacement dose rates Norgett, M. J.; Robinson, M. T.; Torrens, I. M. Nuclear Engineering and Design, Vol. 33, Issue 1 https://doi.org/10.1016/0029-5493(75)90035-7	journal	August 1975
Primary Radiation Damage Formation Stoller, R. E. Comprehensive Nuclear Materials https://doi.org/10.1016/B978-0-08-056033-5.00027-6	book	January 2012
Fuel Performance of Light Water Reactors (Uranium Oxide and MOX) Baron, D. D.; Hallstadius, L. Comprehensive Nuclear Materials, p. 481-514 https://doi.org/10.1016/B978-0-08-056033-5.00040-9	book	January 2012
Electron irradiation of single crystal thorium dioxide and electron transfer reactions Griffiths, Trevor R.; Dixon, James Inorganica Chimica Acta, Vol. 300-302 https://doi.org/10.1016/S0020-1693(99)00597-6	journal	April 2000
Defect production in ceramics Zinkle, S. J.; Kinoshita, C. Journal of Nuclear Materials, Vol. 251 https://doi.org/10.1016/S0022-3115(97)00224-9	journal	November 1997
Displacement threshold energies in β-SiC Devanathan, R.; Diaz de la Rubia, T.; Weber, W. J. Journal of Nuclear Materials, Vol. 253, Issue 1-3 https://doi.org/10.1016/S0022-3115(97)00304-8	journal	March 1998
The high burn-up structure in nuclear fuel Rondinella, Vincenzo V.; Wiss, Thierry Materials Today, Vol. 13, Issue 12 https://doi.org/10.1016/S1369-7021(10)70221-2	journal	December 2010
Defect energetics and Xe diffusion in UO2 and ThO2 Yun, Younsuk; Oppeneer, Peter M.; Kim, Hanchul Acta Materialia, Vol. 57, Issue 5 https://doi.org/10.1016/j.actamat.2008.12.010	journal	March 2009
Stability and migration of charged oxygen interstitials in ThO2 and CeO2 Xiao, H. Y.; Zhang, Y.; Weber, W. J. Acta Materialia, Vol. 61, Issue 20 https://doi.org/10.1016/j.actamat.2013.09.001	journal	December 2013
An integrated experimental and computational investigation of defect and microstructural effects on thermal transport in thorium dioxide Dennett, Cody A.; Deskins, W. Ryan; Khafizov, Marat Acta Materialia, Vol. 213 https://doi.org/10.1016/j.actamat.2021.116934	journal	July 2021
Preferential Cu precipitation at extended defects in bcc Fe: An atomistic study Zhang, Yongfeng; Millett, Paul C.; Tonks, Michael R. Computational Materials Science, Vol. 101 https://doi.org/10.1016/j.commatsci.2015.01.041	journal	April 2015
Primary radiation damage on displacement cascades in UO2, ThO2 and (U0.5Th0.5)O2 Rahman, M. J.; Cooper, M. W. D.; Szpunar, B. Computational Materials Science, Vol. 154 https://doi.org/10.1016/j.commatsci.2018.08.024	journal	November 2018
Calculation of the threshold displacement energies in UO2 using ionic potentials Meis, C.; Chartier, A. Journal of Nuclear Materials, Vol. 341, Issue 1 https://doi.org/10.1016/j.jnucmat.2005.01.001	journal	May 2005
Trapping and diffusion of fission products in ThO2 and CeO2 Xiao, H. Y.; Zhang, Y.; Weber, W. J. Journal of Nuclear Materials, Vol. 414, Issue 3 https://doi.org/10.1016/j.jnucmat.2011.05.037	journal	July 2011
Effects of the short-range repulsive potential on cascade damage in iron Byggmästar, J.; Granberg, F.; Nordlund, K. Journal of Nuclear Materials, Vol. 508 https://doi.org/10.1016/j.jnucmat.2018.06.005	journal	September 2018
Primary radiation damage: A review of current understanding and models Nordlund, Kai; Zinkle, Steven J.; Sand, Andrea E. Journal of Nuclear Materials, Vol. 512 https://doi.org/10.1016/j.jnucmat.2018.10.027	journal	December 2018
Atomistic modeling of out-of-pile xenon diffusion by vacancy clusters in UO2 Perriot, Romain; Matthews, Christopher; Cooper, Michael W. D. Journal of Nuclear Materials, Vol. 520 https://doi.org/10.1016/j.jnucmat.2019.03.050	journal	July 2019
Calculation of threshold displacement energies in UO2 Dacus, Benjamin; Beeler, Benjamin; Schwen, Daniel Journal of Nuclear Materials, Vol. 520 https://doi.org/10.1016/j.jnucmat.2019.04.002	journal	July 2019
Thermal and diffusional properties of (Th,Np)O2 and (U,Np)O2 mixed oxides Ghosh, P. S.; Arya, A.; Kuganathan, N. Journal of Nuclear Materials, Vol. 521 https://doi.org/10.1016/j.jnucmat.2019.04.039	journal	August 2019
An AIMD+U simulation of low-energy displacement events in UO2 Jiang, Ming; Gong, Hengfeng; Zhou, Birong Journal of Nuclear Materials, Vol. 540 https://doi.org/10.1016/j.jnucmat.2020.152379	journal	November 2020
SRIM – The stopping and range of ions in matter (2010) Ziegler, James F.; Ziegler, M. D.; Biersack, J. P. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 268, Issue 11-12 https://doi.org/10.1016/j.nimb.2010.02.091	journal	June 2010
Displacement threshold and Frenkel pair formation energy in ionic systems Kittiratanawasin, L.; Smith, Roger; Uberuaga, B. P. Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 268, Issue 19 https://doi.org/10.1016/j.nimb.2010.04.024	journal	October 2010
Raman and photoluminescence evaluation of ion-induced damage uniformity in ThO2 Rickert, Karl; Prusnick, Timothy A.; Hunt, Eric Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 515 https://doi.org/10.1016/j.nimb.2022.01.011	journal	March 2022
Unraveling small-scale defects in irradiated ThO2 using kinetic Monte Carlo simulations Jiang, Chao; He, Lingfeng; Dennett, Cody A. Scripta Materialia, Vol. 214 https://doi.org/10.1016/j.scriptamat.2022.114684	journal	June 2022
Point defects and non-stoichiometry in thoria Murphy, S. T.; Cooper, M. W. D.; Grimes, R. W. Solid State Ionics, Vol. 267 https://doi.org/10.1016/j.ssi.2014.09.017	journal	December 2014
Thermal Energy Transport in Oxide Nuclear Fuel Hurley, David H.; El-Azab, Anter; Bryan, Matthew S. Chemical Reviews, Vol. 122, Issue 3 https://doi.org/10.1021/acs.chemrev.1c00262	journal	December 2021
Oxygen Vacancy Formation and Migration in Ce _x Th _{1– x} O ₂ Solid Solution Xiao, H. Y.; Weber, W. J. The Journal of Physical Chemistry B, Vol. 115, Issue 20 https://doi.org/10.1021/jp202016s	journal	May 2011
Thermophysical properties and oxygen transport in (Thx,Pu1−x)O2 Galvin, C. O. T.; Cooper, M. W. D.; Rushton, M. J. D. Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep36024	journal	October 2016
Theoretical investigation of thermodynamic stability and mobility of the oxygen vacancy in ThO ₂ –UO ₂ solid solutions Liu, B.; Aidhy, D. S.; Zhang, Y. Phys. Chem. Chem. Phys., Vol. 16, Issue 46 https://doi.org/10.1039/C4CP03660C	journal	January 2014
Structural dynamics of Schottky and Frenkel defects in ThO₂: a density-functional theory study Moxon, Samuel; Skelton, Jonathan; Tse, Joshua S. Journal of Materials Chemistry A, Vol. 10, Issue 4 https://doi.org/10.1039/D1TA10072F	journal	January 2022
Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points Henkelman, Graeme; Jónsson, Hannes The Journal of Chemical Physics, Vol. 113, Issue 22 https://doi.org/10.1063/1.1323224	journal	December 2000
A climbing image nudged elastic band method for finding saddle points and minimum energy paths Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904 https://doi.org/10.1063/1.1329672	journal	December 2000
The influence of lattice defects, recombination, and clustering on thermal transport in single crystal thorium dioxide Dennett, Cody A.; Hua, Zilong; Khanolkar, Amey APL Materials, Vol. 8, Issue 11 https://doi.org/10.1063/5.0025384	journal	November 2020
Thermal conductivity of ThO ₂ : Effect of point defect disorder Deskins, W. Ryan; Hamed, Ahmed; Kumagai, Tomohisa Journal of Applied Physics, Vol. 129, Issue 7 https://doi.org/10.1063/5.0038117	journal	February 2021
A first-principles investigation of point defect structure and energetics in ThO2 Singh, Maniesha; Kumagai, Tomohisa; El-Azab, Anter Journal of Applied Physics, Vol. 132, Issue 13 https://doi.org/10.1063/5.0087369	journal	October 2022
Etude du ralentissement des ions dans une cible diatomique: II—calcul du nombre d'atomes deplacés Soullard, J.; Alamo, Et A. Radiation Effects, Vol. 38, Issue 3-4 https://doi.org/10.1080/00337577808233221	journal	January 1978
The threshold energy for atom displacement in irradiated copper studied by high-voltage electron microscopy Urban, K.; Yoshida, N. Philosophical Magazine A, Vol. 44, Issue 5 https://doi.org/10.1080/01418618108235802	journal	November 1981
Molecular dynamics studies of displacement cascades in the uranium dioxide matrix Van Brutzel, L.; Delaye, J. -M.; Ghaleb, D. Philosophical Magazine, Vol. 83, Issue 36 https://doi.org/10.1080/14786430310001616081	journal	December 2003
The Displacement of Atoms in Solids by Radiation Kinchin, G. H.; Pease, R. S. Reports on Progress in Physics, Vol. 18, Issue 1 https://doi.org/10.1088/0034-4885/18/1/301	journal	January 1955
Thermal Conductivity of Some Alkali Halides Containing F Centers Walker, Charles T. Physical Review, Vol. 132, Issue 5 https://doi.org/10.1103/PhysRev.132.1963	journal	December 1963
F Centers in Thorium Oxide Neeley, V. I.; Gruber, J. B.; Gray, W. J. Physical Review, Vol. 158, Issue 3 https://doi.org/10.1103/PhysRev.158.809	journal	June 1967
Diatomic Molecules According to the Wave Mechanics. II. Vibrational Levels Morse, Philip M. Physical Review, Vol. 34, Issue 1 https://doi.org/10.1103/PhysRev.34.57	journal	July 1929
Embedded-atom method: Derivation and application to impurities, surfaces, and other defects in metals Daw, Murray S.; Baskes, M. I. Physical Review B, Vol. 29, Issue 12 https://doi.org/10.1103/PhysRevB.29.6443	journal	June 1984
Defect production in collision cascades in elemental semiconductors and fcc metals Nordlund, K.; Ghaly, M.; Averback, R. S. Physical Review B, Vol. 57, Issue 13 https://doi.org/10.1103/PhysRevB.57.7556	journal	April 1998
Basic mechanisms of Frenkel pair recombinations in UO 2 fluorite structure calculated by molecular dynamics simulations Van Brutzel, L.; Chartier, A.; Crocombette, J. P. Physical Review B, Vol. 78, Issue 2 https://doi.org/10.1103/PhysRevB.78.024111	journal	July 2008
Charge states of point defects in uranium oxide calculated with a local hybrid functional for correlated electrons Crocombette, Jean-Paul; Torumba, Doru; Chartier, Alain Physical Review B, Vol. 83, Issue 18 https://doi.org/10.1103/PhysRevB.83.184107	journal	May 2011
Systematic calculation of threshold displacement energies: Case study in rutile Robinson, M.; Marks, N. A.; Whittle, K. R. Physical Review B, Vol. 85, Issue 10 https://doi.org/10.1103/PhysRevB.85.104105	journal	March 2012
Influence of charge states on energies of point defects and clusters in uranium dioxide Crocombette, Jean-Paul Physical Review B, Vol. 85, Issue 14 https://doi.org/10.1103/PhysRevB.85.144101	journal	April 2012
First-principles calculations of uranium diffusion in uranium dioxide Dorado, Boris; Andersson, David A.; Stanek, Christopher R. Physical Review B, Vol. 86, Issue 3 https://doi.org/10.1103/PhysRevB.86.035110	journal	July 2012
Ab initio molecular dynamics simulations of low-energy recoil events in ThO 2 , CeO 2 , and ZrO 2 Xiao, H. Y.; Zhang, Y.; Weber, W. J. Physical Review B, Vol. 86, Issue 5 https://doi.org/10.1103/PhysRevB.86.054109	journal	August 2012
Sensitivity of the threshold displacement energy to temperature and time Robinson, M.; Marks, N. A.; Lumpkin, G. R. Physical Review B, Vol. 86, Issue 13 https://doi.org/10.1103/PhysRevB.86.134105	journal	October 2012
F center in lithium fluoride revisited: Comparison of solid-state physics and quantum-chemistry approaches Karsai, Ferenc; Tiwald, Paul; Laskowski, Robert Physical Review B, Vol. 89, Issue 12 https://doi.org/10.1103/PhysRevB.89.125429	journal	March 2014
Importance of elastic finite-size effects: Neutral defects in ionic compounds Burr, P. A.; Cooper, M. W. D. Physical Review B, Vol. 96, Issue 9 https://doi.org/10.1103/PhysRevB.96.094107	journal	September 2017
Atomistic simulation of displacement damage and effective nonionizing energy loss in InAs Chen, Nanjun; Huang, Danhong; Heller, Eric R. Physical Review Materials, Vol. 5, Issue 3 https://doi.org/10.1103/PhysRevMaterials.5.033603	journal	March 2021
Anisotropy of electron radiation damage in metal crystals Vajda, Peter Reviews of Modern Physics, Vol. 49, Issue 3 https://doi.org/10.1103/RevModPhys.49.481	journal	July 1977
Opportunities for Advanced Ceramics and Composites in the Nuclear Sector Lee, William Edward; Gilbert, Matthew; Murphy, Samuel Thomas Journal of the American Ceramic Society, Vol. 96, Issue 7 https://doi.org/10.1111/jace.12406	journal	June 2013
Calculation of diffusion coefficients of defects and ions in UO2 Kuksin, A. Yu.; Smirnova, D. E. Physics of the Solid State, Vol. 56, Issue 6 https://doi.org/10.1134/S1063783414060201	journal	June 2014
Atomistic Study for the Tantalum and Tantalum–Tungsten Alloy Threshold Displacement Energy under Local Strain Bany Salman, Mohammad; Park, Minkyu; Banisalman, Mosab Jaser International Journal of Molecular Sciences, Vol. 24, Issue 4 https://doi.org/10.3390/ijms24043289	journal	February 2023
Influence of Elevated Temperature on Color Centers in LiF Crystals and Their Photoluminescence Sankowska, Małgorzata; Bilski, Pawel; Marczewska, Barbara Materials, Vol. 16, Issue 4 https://doi.org/10.3390/ma16041489	journal	February 2023
Fast Anion Defect Recovery through Superionic-Type Hopping Displacements in UO₂Following Radiation Annamareddy, Ajay; Eapen, Jacob Defect and Diffusion Forum, Vol. 375 https://doi.org/10.4028/www.scientific.net/DDF.375.43	journal	May 2017

Similar Records

Computer simulations of low energy displacement cascades in a face centered cubic lattice. [25 to 200 eV, Frenkel pairs, kinetics, COMENT, stability]

Conference · Wed Sep 01 00:00:00 EDT 1976 · OSTI ID:7226073

Basic mechanisms of Frenkel pair recombinations in UO{sub 2} fluorite structure calculated by molecular dynamics simulations

Journal Article · Tue Jul 01 00:00:00 EDT 2008 · Physical Review. B, Condensed Matter and Materials Physics · OSTI ID:21143584

Related Subjects

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS
Coulomb interaction
Molecular Dynamics
Orientation dependence
Temperature dependence
ThO2
Threshold Displacement Energy
thorium dioxide

Establishing the temperature and orientation dependence of the threshold displacement energy in ThO2 via molecular dynamics simulations

Citation Formats

References (64)

Similar Records

Related Subjects

Establishing the temperature and orientation dependence of the threshold displacement energy in ThO₂ via molecular dynamics simulations