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Title: Defects induced in cerium dioxide single crystals by electron irradiation

Abstract

In this work, Micro-Raman spectroscopy, X-band electron paramagnetic resonance (EPR) spectroscopy, and UV-visible optical absorption spectroscopy were used to study the damage production in cerium dioxide (CeO2) single crystals by electron irradiation for three energies (1.0, 1.4, and 2.5 MeV). The Raman-active T2g peak was left unchanged after 2.5-MeV electron irradiation at a high fluence. This shows that no structural modifications occurred for the cubic fluorite structure. UV-visible optical absorption spectra exhibited a characteristic sub band-gap tail for 1.4-MeV and 2.5-MeV energies, but not for 1.0 MeV. Narrow EPR lines were recorded near liquid-helium temperature after 2.5-MeV electron irradiation; whereas no such signal was found for the virgin un-irradiated crystal or after 1.0-MeV irradiation for the same fluence. The angular variation of these lines in the {111} plane revealed a weak g-factor anisotropy assigned to Ce3+ ions (with the 4f1 configuration) in a high-symmetry local environment. Finally, it is concluded that Ce3+ ions may be produced by a reduction resulting from the displacement damage process. However, no evidence of F+ or F0 center or hole center formation due to irradiation was found from the present EPR and optical absorption spectra.

Authors:
 [1];  [2];  [3];  [3];  [3];  [4];  [4]; ORCiD logo [5]
+ Show Author Affiliations
  1. DEN, Service de Recherches Metallurgiques Appliquees, CEA, Universite Paris-Saclay (France)
  2. DEN, Service de Recherches de Metallurgie Physique, CEA, Universite Paris-Saclay (France)
  3. Chimie Paris-Tech, PSL Research University, Institut de Recherche de Chimie-Paris (France); Sorbonne Universite, UPMC (France)
  4. Institut de Mineralogie, de Physique des Materiaux et Cosmochimie (IMPMC), Sorbonne Universites-UPMC Univ Paris (France). Museum National d Histoire Naturelle
  5. Univ. of Tennessee, Knoxville, TN (United States). Materials Science and Engineering; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE
OSTI Identifier:
1422581
Alternate Identifier(s):
OSTI ID: 1416844
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 123; Journal Issue: 2; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Cerium dioxide; electron irradiation; Raman spectroscopy; electron paramagnetic resonance spectroscopy; UV-visible optical absorption spectroscopy

Citation Formats

Costantini, Jean-Marc, Miro, Sandrine, Touati, Nadia, Binet, Laurent, Wallez, Gilles, Lelong, Gérald, Guillaumet, Maxime, and Weber, William J. Defects induced in cerium dioxide single crystals by electron irradiation. United States: N. p., 2018. Web. doi:10.1063/1.5007823.
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Costantini, Jean-Marc, Miro, Sandrine, Touati, Nadia, Binet, Laurent, Wallez, Gilles, Lelong, Gérald, Guillaumet, Maxime, & Weber, William J. Defects induced in cerium dioxide single crystals by electron irradiation. United States. https://doi.org/10.1063/1.5007823
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Costantini, Jean-Marc, Miro, Sandrine, Touati, Nadia, Binet, Laurent, Wallez, Gilles, Lelong, Gérald, Guillaumet, Maxime, and Weber, William J. Fri . "Defects induced in cerium dioxide single crystals by electron irradiation". United States. https://doi.org/10.1063/1.5007823. https://www.osti.gov/servlets/purl/1422581.
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@article{osti_1422581,
title = {Defects induced in cerium dioxide single crystals by electron irradiation},
author = {Costantini, Jean-Marc and Miro, Sandrine and Touati, Nadia and Binet, Laurent and Wallez, Gilles and Lelong, Gérald and Guillaumet, Maxime and Weber, William J.},
abstractNote = {In this work, Micro-Raman spectroscopy, X-band electron paramagnetic resonance (EPR) spectroscopy, and UV-visible optical absorption spectroscopy were used to study the damage production in cerium dioxide (CeO2) single crystals by electron irradiation for three energies (1.0, 1.4, and 2.5 MeV). The Raman-active T2g peak was left unchanged after 2.5-MeV electron irradiation at a high fluence. This shows that no structural modifications occurred for the cubic fluorite structure. UV-visible optical absorption spectra exhibited a characteristic sub band-gap tail for 1.4-MeV and 2.5-MeV energies, but not for 1.0 MeV. Narrow EPR lines were recorded near liquid-helium temperature after 2.5-MeV electron irradiation; whereas no such signal was found for the virgin un-irradiated crystal or after 1.0-MeV irradiation for the same fluence. The angular variation of these lines in the {111} plane revealed a weak g-factor anisotropy assigned to Ce3+ ions (with the 4f1 configuration) in a high-symmetry local environment. Finally, it is concluded that Ce3+ ions may be produced by a reduction resulting from the displacement damage process. However, no evidence of F+ or F0 center or hole center formation due to irradiation was found from the present EPR and optical absorption spectra.},
doi = {10.1063/1.5007823},
journal = {Journal of Applied Physics},
number = 2,
volume = 123,
place = {United States},
year = {Fri Jan 12 00:00:00 EST 2018},
month = {Fri Jan 12 00:00:00 EST 2018}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1063/1.5007823
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Cited by: 11 works
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Figures / Tables:

Table I Table I: Electron irradiation features for CeO2 (mass density = 7.215 g cm-3) with mean ionization energy I = 407.6 eV: incident energy (E), total inelastic stopping power (−dE/dx)inel, and CSDA range (R) computed with the ESTAR code, maximum recoil energy (Tmax) of Ce and O atoms in the primarymore » electron-nuclei collisions, maximum number of displaced Ce and O atoms (Nmax) per Ce and O recoiling atoms in secondary nuclei-nuclei collisions (i.e. Ce → Ce, O → Ce, Ce → O, and O → O cascade contributions) above the threshold displacement energy (Ed) for Ce (Ed = 45 eV) and O| (Ed = 35 eV) atoms, total number of displaced Ce and O atoms (Ntot), and number of displaced O and Ce atoms in cascades (Ncasc) for a reference fluence of 5x1018 cm-2 in a single crystal of volume V = 5x10-4 cm3.« less
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    Works referencing / citing this record:

    Optical spectroscopy study of modifications induced in cerium dioxide by electron and ion irradiations
    journal, April 2019

    Investigation of the influence of irradiation with Fe +7 ions on structural properties of AlN ceramics
    journal, June 2018

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