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Title: Damage evolution of ion irradiated defected-fluorite La 2 Zr 2 O 7 epitaxial thin films

Abstract

Pyrochlore-structure oxides, A2B2O7, may exhibit remarkable radiation tolerance due to the ease with which they can accommodate disorder by transitioning to a defected fluorite structure. In this paper, the mechanism of defect formation was explored by evaluating the radiation damage behavior of high quality epitaxial La2Zr2O7 thin films with the defected fluorite structure, irradiated with 1 MeV Zr+ at doses up to 10 displacements per atom (dpa). The level of film damage was evaluated as a function of dose by Rutherford backscattering spectrometry in the channeling geometry (RBS/c) and scanning transmission electron microscopy (STEM). At lower doses, the surface of the La2Zr2O7 film amorphized, and the amorphous fraction as a function of dose fit well to a stimulated amorphization model. As the dose increased, the surface amorphization slowed, and amorphization appeared at the interface. Even at a dose of 10 dpa, the core of the film remained crystalline, despite the prediction of amorphization from the model. To inform future ab initio simulations of La2Zr2O7, the bandgap of a thick La2Zr2O7 film was measured to be indirect at 4.96 eV, with a direct transition at 5.60 eV.

Authors:
; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER)
OSTI Identifier:
1342222
Alternate Identifier(s):
OSTI ID: 1550599
Report Number(s):
PNNL-SA-121946
Journal ID: ISSN 1359-6454; PII: S1359645417300228; TRN: US1700529
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Acta Materialia
Additional Journal Information:
Journal Volume: 130; Journal Issue: C; Journal ID: ISSN 1359-6454
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; crystalline oxides; ion irradiation; structural disordering; STEM HAADF

Citation Formats

Kaspar, Tiffany C., Gigax, Jonathan G., Shao, Lin, Bowden, Mark E., Varga, Tamas, Shutthanandan, Vaithiyalingam, Spurgeon, Steven R., Yan, Pengfei, Wang, Chongmin, Ramuhalli, Pradeep, and Henager, Charles H. Damage evolution of ion irradiated defected-fluorite La 2 Zr 2 O 7 epitaxial thin films. United States: N. p., 2017. Web. doi:10.1016/j.actamat.2017.01.012.
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Kaspar, Tiffany C., Gigax, Jonathan G., Shao, Lin, Bowden, Mark E., Varga, Tamas, Shutthanandan, Vaithiyalingam, Spurgeon, Steven R., Yan, Pengfei, Wang, Chongmin, Ramuhalli, Pradeep, & Henager, Charles H. Damage evolution of ion irradiated defected-fluorite La 2 Zr 2 O 7 epitaxial thin films. United States. https://doi.org/10.1016/j.actamat.2017.01.012
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Kaspar, Tiffany C., Gigax, Jonathan G., Shao, Lin, Bowden, Mark E., Varga, Tamas, Shutthanandan, Vaithiyalingam, Spurgeon, Steven R., Yan, Pengfei, Wang, Chongmin, Ramuhalli, Pradeep, and Henager, Charles H. Mon . "Damage evolution of ion irradiated defected-fluorite La 2 Zr 2 O 7 epitaxial thin films". United States. https://doi.org/10.1016/j.actamat.2017.01.012. https://www.osti.gov/servlets/purl/1342222.
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@article{osti_1342222,
title = {Damage evolution of ion irradiated defected-fluorite La 2 Zr 2 O 7 epitaxial thin films},
author = {Kaspar, Tiffany C. and Gigax, Jonathan G. and Shao, Lin and Bowden, Mark E. and Varga, Tamas and Shutthanandan, Vaithiyalingam and Spurgeon, Steven R. and Yan, Pengfei and Wang, Chongmin and Ramuhalli, Pradeep and Henager, Charles H.},
abstractNote = {Pyrochlore-structure oxides, A2B2O7, may exhibit remarkable radiation tolerance due to the ease with which they can accommodate disorder by transitioning to a defected fluorite structure. In this paper, the mechanism of defect formation was explored by evaluating the radiation damage behavior of high quality epitaxial La2Zr2O7 thin films with the defected fluorite structure, irradiated with 1 MeV Zr+ at doses up to 10 displacements per atom (dpa). The level of film damage was evaluated as a function of dose by Rutherford backscattering spectrometry in the channeling geometry (RBS/c) and scanning transmission electron microscopy (STEM). At lower doses, the surface of the La2Zr2O7 film amorphized, and the amorphous fraction as a function of dose fit well to a stimulated amorphization model. As the dose increased, the surface amorphization slowed, and amorphization appeared at the interface. Even at a dose of 10 dpa, the core of the film remained crystalline, despite the prediction of amorphization from the model. To inform future ab initio simulations of La2Zr2O7, the bandgap of a thick La2Zr2O7 film was measured to be indirect at 4.96 eV, with a direct transition at 5.60 eV.},
doi = {10.1016/j.actamat.2017.01.012},
journal = {Acta Materialia},
number = C,
volume = 130,
place = {United States},
year = {Mon May 01 00:00:00 EDT 2017},
month = {Mon May 01 00:00:00 EDT 2017}
}
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https://doi.org/10.1016/j.actamat.2017.01.012
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    Works referencing / citing this record:

    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

    Modulating the thermal conductivity of La 2 Zr 2 O 7 by Thorium (Th) doping: an ab initio study
    journal, September 2019

    Theoretical investigations of electronic and thermodynamic properties of Ce doped La 2 Zr 2 O 7 pyrochlore
    journal, May 2019

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