A Comparative Study of Electron Radiation Responses of Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> and La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>: An <i>ab</i><i>initio</i> Molecular Dynamics Study

A Comparative Study of Electron Radiation Responses of Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> and La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>: An <i>ab</i><i>initio</i> Molecular Dynamics Study

In this study, the response of Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> and La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> to electronic radiation is simulated, employing an <i>ab initio</i> molecular dynamics method. It...

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Main Authors: Shounuo Zhang, Menglu Li, Haiyan Xiao, Zijiang Liu, Xiaotao Zu
Format: Article
Language:English
Published: MDPI AG 2021-03-01
Series:Materials
Subjects:
pyrochlores
electron radiation
structural amorphization
<i>ab initio</i> molecular dynamics simulations
Online Access:https://www.mdpi.com/1996-1944/14/6/1516
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author Shounuo Zhang
Menglu Li
Haiyan Xiao
Zijiang Liu
Xiaotao Zu
author_facet Shounuo Zhang
Menglu Li
Haiyan Xiao
Zijiang Liu
Xiaotao Zu
author_sort Shounuo Zhang
collection DOAJ
description In this study, the response of Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> and La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> to electronic radiation is simulated, employing an <i>ab initio</i> molecular dynamics method. It is shown that Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> undergoes a crystalline-to-amorphous structural transition with 0.3% electronic excitation, while for La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>, the structural amorphization occurs with 1.2% electronic excitation. During the microstructural evolution, the anion disorder further drives cation disorder and eventually results in the structural amorphization of Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> and La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>. The difference in responses to electron radiation between Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> and La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> mainly results from the strong correlation effects between Pu 5<i>f</i> electrons and the smaller band gap of Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>. These results suggest that Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> is less resistant to amorphization under local ionization rates that produce a low level of electronic excitation, since the level of the concentration of excited electrons is relatively low in Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>. The presented results will advance the understanding of the radiation damage effects of zirconate pyrochlores.
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spelling doaj.art-61af5222c49941c1924418b89052c0e12023-11-21T11:15:49ZengMDPI AGMaterials1996-19442021-03-01146151610.3390/ma14061516A Comparative Study of Electron Radiation Responses of Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> and La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>: An <i>ab</i><i>initio</i> Molecular Dynamics StudyShounuo Zhang0Menglu Li1Haiyan Xiao2Zijiang Liu3Xiaotao Zu4School of Physics, University of Electronic Science and Technology of China, Chengdu 610054, ChinaSchool of Physics, University of Electronic Science and Technology of China, Chengdu 610054, ChinaSchool of Physics, University of Electronic Science and Technology of China, Chengdu 610054, ChinaDepartment of Physics, Lanzhou City University, Lanzhou 730070, ChinaSchool of Physics, University of Electronic Science and Technology of China, Chengdu 610054, ChinaIn this study, the response of Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> and La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> to electronic radiation is simulated, employing an <i>ab initio</i> molecular dynamics method. It is shown that Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> undergoes a crystalline-to-amorphous structural transition with 0.3% electronic excitation, while for La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>, the structural amorphization occurs with 1.2% electronic excitation. During the microstructural evolution, the anion disorder further drives cation disorder and eventually results in the structural amorphization of Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> and La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>. The difference in responses to electron radiation between Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> and La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> mainly results from the strong correlation effects between Pu 5<i>f</i> electrons and the smaller band gap of Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>. These results suggest that Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> is less resistant to amorphization under local ionization rates that produce a low level of electronic excitation, since the level of the concentration of excited electrons is relatively low in Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>. The presented results will advance the understanding of the radiation damage effects of zirconate pyrochlores.https://www.mdpi.com/1996-1944/14/6/1516pyrochloreselectron radiationstructural amorphization<i>ab initio</i> molecular dynamics simulations
spellingShingle Shounuo Zhang
Menglu Li
Haiyan Xiao
Zijiang Liu
Xiaotao Zu
A Comparative Study of Electron Radiation Responses of Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> and La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>: An <i>ab</i><i>initio</i> Molecular Dynamics Study
Materials
pyrochlores
electron radiation
structural amorphization
<i>ab initio</i> molecular dynamics simulations
title A Comparative Study of Electron Radiation Responses of Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> and La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>: An <i>ab</i><i>initio</i> Molecular Dynamics Study
title_full A Comparative Study of Electron Radiation Responses of Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> and La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>: An <i>ab</i><i>initio</i> Molecular Dynamics Study
title_fullStr A Comparative Study of Electron Radiation Responses of Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> and La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>: An <i>ab</i><i>initio</i> Molecular Dynamics Study
title_full_unstemmed A Comparative Study of Electron Radiation Responses of Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> and La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>: An <i>ab</i><i>initio</i> Molecular Dynamics Study
title_short A Comparative Study of Electron Radiation Responses of Pu<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub> and La<sub>2</sub>Zr<sub>2</sub>O<sub>7</sub>: An <i>ab</i><i>initio</i> Molecular Dynamics Study
title_sort comparative study of electron radiation responses of pu sub 2 sub zr sub 2 sub o sub 7 sub and la sub 2 sub zr sub 2 sub o sub 7 sub an i ab i i initio i molecular dynamics study
topic pyrochlores
electron radiation
structural amorphization
<i>ab initio</i> molecular dynamics simulations
url https://www.mdpi.com/1996-1944/14/6/1516
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