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Title: Ab initio molecular dynamics simulations of ion-solid interactions in zirconate pyrochlores

Abstract

In this paper, an ab initio molecular dynamics method is employed to study low energy recoil events in zirconate pyrochlores (A2Zr2O7, A = La, Nd and Sm). It shows that both cations and anions in Nd2Zr2O7 and Sm2Zr2O7 are generally more likely to be displaced than those in La2Zr2O7. The damage end states mainly consist of Frenkel pair defects, and the Frenkel pair formation energies in Nd2Zr2O7 and Sm2Zr2O7 are lower than those in La2Zr2O7. These results suggest that the order–disorder structural transition more easily occurs in Nd2Zr2O7 and Sm2Zr2O7 resulting in a defect-fluorite structure, which agrees well with experimental observations. Our calculations indicate that oxygen migration from 48f and 8b to 8a sites is dominant under low energy irradiation. A number of new defects, including four types of cation Frenkel pairs and six types of anion Frenkel pairs, are revealed by ab initio molecular dynamics simulations. The present findings may help to advance the fundamental understanding of the irradiation response behavior of zirconate pyrochlores.

Authors:
 [1];  [2];  [3];  [1]
+ Show Author Affiliations
  1. University of Electronic Science and Technology of China, Chengdu (China)
  2. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1265303
Alternate Identifier(s):
OSTI ID: 1250964
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Acta Materialia
Additional Journal Information:
Journal Volume: 87; Journal ID: ISSN 1359-6454
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; Computer simulation; Zirconate pyrochlores; Radiation effects; Charge transfer

Citation Formats

Xiao, Haiyan Y., Weber, William J., Zhang, Yanwen, and Zu, X. T. Ab initio molecular dynamics simulations of ion-solid interactions in zirconate pyrochlores. United States: N. p., 2015. Web. doi:10.1016/j.actamat.2015.01.019.
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Xiao, Haiyan Y., Weber, William J., Zhang, Yanwen, & Zu, X. T. Ab initio molecular dynamics simulations of ion-solid interactions in zirconate pyrochlores. United States. https://doi.org/10.1016/j.actamat.2015.01.019
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Xiao, Haiyan Y., Weber, William J., Zhang, Yanwen, and Zu, X. T. Sat . "Ab initio molecular dynamics simulations of ion-solid interactions in zirconate pyrochlores". United States. https://doi.org/10.1016/j.actamat.2015.01.019. https://www.osti.gov/servlets/purl/1265303.
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@article{osti_1265303,
title = {Ab initio molecular dynamics simulations of ion-solid interactions in zirconate pyrochlores},
author = {Xiao, Haiyan Y. and Weber, William J. and Zhang, Yanwen and Zu, X. T.},
abstractNote = {In this paper, an ab initio molecular dynamics method is employed to study low energy recoil events in zirconate pyrochlores (A2Zr2O7, A = La, Nd and Sm). It shows that both cations and anions in Nd2Zr2O7 and Sm2Zr2O7 are generally more likely to be displaced than those in La2Zr2O7. The damage end states mainly consist of Frenkel pair defects, and the Frenkel pair formation energies in Nd2Zr2O7 and Sm2Zr2O7 are lower than those in La2Zr2O7. These results suggest that the order–disorder structural transition more easily occurs in Nd2Zr2O7 and Sm2Zr2O7 resulting in a defect-fluorite structure, which agrees well with experimental observations. Our calculations indicate that oxygen migration from 48f and 8b to 8a sites is dominant under low energy irradiation. A number of new defects, including four types of cation Frenkel pairs and six types of anion Frenkel pairs, are revealed by ab initio molecular dynamics simulations. The present findings may help to advance the fundamental understanding of the irradiation response behavior of zirconate pyrochlores.},
doi = {10.1016/j.actamat.2015.01.019},
journal = {Acta Materialia},
number = ,
volume = 87,
place = {United States},
year = {Sat Jan 31 00:00:00 EST 2015},
month = {Sat Jan 31 00:00:00 EST 2015}
}
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https://doi.org/10.1016/j.actamat.2015.01.019
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    Works referencing / citing this record:

    Investigation of mechanical and thermal properties of rare earth pyrochlore oxides by first‐principles calculations
    journal, October 2018

    • Yang, Lan; Zhu, Changhua; Sheng, Ye
    • Journal of the American Ceramic Society
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    Composition‐dependent intrinsic defect structures in pyroclore RE 2 B 2 O 7 ( RE  = La, Nd, Gd; B  = Sn, Hf, Zr)
    journal, August 2019

    • Yang, Lan; Wang, Peiying; Zhang, Chengguan
    • Journal of the American Ceramic Society, Vol. 103, Issue 1
    • DOI: 10.1111/jace.16705

    Investigations of atomic disorder and grain growth kinetics in polycrystalline La2Zr2O7
    journal, May 2019

    Ab initio molecular dynamics simulation of low energy radiation responses of α-Al2O3
    journal, June 2017

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