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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 (CeO 2) single crystals by electron irradiation for three energies (1.0, 1.4, and 2.5 MeV). The Raman-active T 2g 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 Ce 3+ ions (with the 4f 1 configuration) in a high-symmetry local environment. Finally, it is concluded that Ce 3+ ions may be produced by a reduction resulting from the displacement damage process. However, no evidence of F + or F 0 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]
  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:
Journal Article: 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.
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. doi:10.1063/1.5007823.
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. doi:10.1063/1.5007823. https://www.osti.gov/servlets/purl/1422581.
@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},
issn = {0021-8979},
number = 2,
volume = 123,
place = {United States},
year = {2018},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
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Cited by: 3 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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    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.