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

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...

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Main Authors: Lin-Chieh Yu, Shuxiang Zhou, Miaomiao Jin, Marat Khafizov, David Hurley, Yongfeng Zhang
Format: Article
Language:English
Published: Elsevier 2024-12-01
Series:Nuclear Materials and Energy
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Online Access:http://www.sciencedirect.com/science/article/pii/S2352179124001972
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author Lin-Chieh Yu
Shuxiang Zhou
Miaomiao Jin
Marat Khafizov
David Hurley
Yongfeng Zhang
author_facet Lin-Chieh Yu
Shuxiang Zhou
Miaomiao Jin
Marat Khafizov
David Hurley
Yongfeng Zhang
author_sort Lin-Chieh Yu
collection DOAJ
description 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 EdTh and EdO, 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 EdTh is significantly lower than that for EdO. Further, EdTh and EdO show different crystal orientation dependence and temperature dependence. Notably, the cubic symmetry in the fluorite structure is followed by EdTh, but does not hold for EdO because of the existence of two sublattices. The much higher average EdO than EdTh 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.
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spelling doaj-art-096b42e221a045e68bd4d5a8b07792532024-12-21T04:28:22ZengElsevierNuclear Materials and Energy2352-17912024-12-0141101774Establishing the temperature and orientation dependence of the threshold displacement energy in ThO2 via molecular dynamics simulationsLin-Chieh Yu0Shuxiang Zhou1Miaomiao Jin2Marat Khafizov3David Hurley4Yongfeng Zhang5Department of Material Science and Engineering, University of Wisconsin-Madison, Madison, WI 53706, USA; Department of Nuclear Engineering and Engineering Physics, University of Wisconsin-Madison, Madison, WI 53706, USAIdaho National Laboratory, Idaho Falls, ID 83415, USADepartment of Nuclear Engineering, The Pennsylvania State University, University Park, PA 16802, USADepartment of Mechanical and Aerospace Engineering, The Ohio State University, Columbus, OH 43210, USAIdaho National Laboratory, Idaho Falls, ID 83415, USADepartment of Nuclear Engineering and Engineering Physics, University of Wisconsin-Madison, Madison, WI 53706, USA; Corresponding author.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 EdTh and EdO, 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 EdTh is significantly lower than that for EdO. Further, EdTh and EdO show different crystal orientation dependence and temperature dependence. Notably, the cubic symmetry in the fluorite structure is followed by EdTh, but does not hold for EdO because of the existence of two sublattices. The much higher average EdO than EdTh 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.http://www.sciencedirect.com/science/article/pii/S2352179124001972ThO2Threshold displacement energyMolecular dynamicsTemperature dependenceOrientation dependenceCoulomb interaction
spellingShingle Lin-Chieh Yu
Shuxiang Zhou
Miaomiao Jin
Marat Khafizov
David Hurley
Yongfeng Zhang
Establishing the temperature and orientation dependence of the threshold displacement energy in ThO2 via molecular dynamics simulations
Nuclear Materials and Energy
ThO2
Threshold displacement energy
Molecular dynamics
Temperature dependence
Orientation dependence
Coulomb interaction
title Establishing the temperature and orientation dependence of the threshold displacement energy in ThO2 via molecular dynamics simulations
title_full Establishing the temperature and orientation dependence of the threshold displacement energy in ThO2 via molecular dynamics simulations
title_fullStr Establishing the temperature and orientation dependence of the threshold displacement energy in ThO2 via molecular dynamics simulations
title_full_unstemmed Establishing the temperature and orientation dependence of the threshold displacement energy in ThO2 via molecular dynamics simulations
title_short Establishing the temperature and orientation dependence of the threshold displacement energy in ThO2 via molecular dynamics simulations
title_sort establishing the temperature and orientation dependence of the threshold displacement energy in tho2 via molecular dynamics simulations
topic ThO2
Threshold displacement energy
Molecular dynamics
Temperature dependence
Orientation dependence
Coulomb interaction
url http://www.sciencedirect.com/science/article/pii/S2352179124001972
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