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Title: Effect of structure and composition on the electronic excitation induced amorphization of La 2Ti 2-xZr xO 7 ceramics

Abstract

Understanding the response of ceramics operating in extreme environments is of interest for a variety of applications. Ab initio molecular dynamic simulations have been used to investigate the effect of structure and B-site (=Ti, Zr) cation composition of lanthanum-based oxides (La 2B 2O 7) on electronic-excitation-induced amorphization. We find that the amorphous transition in monoclinic layered perovskite La 2Ti 2O 7 occurs for a lower degree of electronic excitation than for cubic pyrochlore La 2Zr 2O 7. While every case the formation of O 2-like molecules drives the structure to an amorphous state, an analysis of the polyhedral connection network reveals that the rotation of TiO 6 octahedra in the monoclinic phase can promote such molecule formation, while such octahedral rotation is not possible in the cubic phase. However, once the symmetry of the cubic structure is broken by substituting Ti for Zr, it becomes less resistant to amorphization. A compound made of 50% Ti and 50% Zr (La 2TiZrO 7) is found to be more resistant in the monoclinic than in the cubic phase, which may be related to the lower bandgap of the cubic phase. These results illustrate the complex interplay of structure and composition in giving risemore » to the radiation resistance of these important functional materials.« less

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1542084
Report Number(s):
PNNL-SA-139722
Journal ID: ISSN 2045-2322
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 97 MATHEMATICS AND COMPUTING

Citation Formats

Sassi, Michel, Kaspar, Tiffany, Rosso, Kevin M., and Spurgeon, Steven R. Effect of structure and composition on the electronic excitation induced amorphization of La2Ti2-xZrxO7 ceramics. United States: N. p., 2019. Web. doi:10.1038/s41598-019-44621-5.
Sassi, Michel, Kaspar, Tiffany, Rosso, Kevin M., & Spurgeon, Steven R. Effect of structure and composition on the electronic excitation induced amorphization of La2Ti2-xZrxO7 ceramics. United States. doi:10.1038/s41598-019-44621-5.
Sassi, Michel, Kaspar, Tiffany, Rosso, Kevin M., and Spurgeon, Steven R. Mon . "Effect of structure and composition on the electronic excitation induced amorphization of La2Ti2-xZrxO7 ceramics". United States. doi:10.1038/s41598-019-44621-5. https://www.osti.gov/servlets/purl/1542084.
@article{osti_1542084,
title = {Effect of structure and composition on the electronic excitation induced amorphization of La2Ti2-xZrxO7 ceramics},
author = {Sassi, Michel and Kaspar, Tiffany and Rosso, Kevin M. and Spurgeon, Steven R.},
abstractNote = {Understanding the response of ceramics operating in extreme environments is of interest for a variety of applications. Ab initio molecular dynamic simulations have been used to investigate the effect of structure and B-site (=Ti, Zr) cation composition of lanthanum-based oxides (La2B2O7) on electronic-excitation-induced amorphization. We find that the amorphous transition in monoclinic layered perovskite La2Ti2O7 occurs for a lower degree of electronic excitation than for cubic pyrochlore La2Zr2O7. While every case the formation of O2-like molecules drives the structure to an amorphous state, an analysis of the polyhedral connection network reveals that the rotation of TiO6 octahedra in the monoclinic phase can promote such molecule formation, while such octahedral rotation is not possible in the cubic phase. However, once the symmetry of the cubic structure is broken by substituting Ti for Zr, it becomes less resistant to amorphization. A compound made of 50% Ti and 50% Zr (La2TiZrO7) is found to be more resistant in the monoclinic than in the cubic phase, which may be related to the lower bandgap of the cubic phase. These results illustrate the complex interplay of structure and composition in giving rise to the radiation resistance of these important functional materials.},
doi = {10.1038/s41598-019-44621-5},
journal = {Scientific Reports},
number = 1,
volume = 9,
place = {United States},
year = {2019},
month = {6}
}

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