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Title: Colossal oxygen vacancy formation at a fluorite-bixbyite interface

Abstract

Oxygen vacancies in complex oxides are indispensable for information and energy technologies. There are several means to create oxygen vacancies in bulk materials. However, the use of ionic interfaces to create oxygen vacancies has not been fully explored. As such, we report an oxide nanobrush architecture designed to create high-density interfacial oxygen vacancies. An atomically well-defined (111) heterointerface between the fluorite CeO2 and the bixbyite Y2O3 is found to induce a charge modulation between Y3+ and Ce4+ ions enabled by the chemical valence mismatch between the two elements. Local structure and chemical analyses, along with theoretical calculations, suggest that more than 10% of oxygen atoms are spontaneously removed without deteriorating the lattice structure. Our fluorite–bixbyite nanobrush provides an excellent platform for the rational design of interfacial oxide architectures to precisely create, control, and transport oxygen vacancies critical for developing ionotronic and memristive devices for advanced energy and neuromorphic computing technologies.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [2];  [3]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [4];  [4];  [5];  [1]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
  3. Univ. of South Carolina, Columbia, SC (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1615212
Alternate Identifier(s):
OSTI ID: 1765587
Grant/Contract Number:  
AC05-00OR22725; AC02-05CH11231; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 11; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Electronic devices; Materials for energy and catalysis; Nanoscale materials; Surfaces, interfaces and thin films

Citation Formats

Lee, Dongkyu, Gao, Xiang, Sun, Lixin, Jee, Youngseok, Poplawsky, Jonathan, Farmer, Thomas O., Fan, Lisha, Guo, Er-Jia, Lu, Qiyang, Heller, William T., Choi, Yongseong, Haskel, Daniel, Fitzsimmons, Michael R., Chisholm, Matthew F., Huang, Kevin, Yildiz, Bilge, and Lee, Ho Nyung. Colossal oxygen vacancy formation at a fluorite-bixbyite interface. United States: N. p., 2020. Web. doi:10.1038/s41467-020-15153-8.
Lee, Dongkyu, Gao, Xiang, Sun, Lixin, Jee, Youngseok, Poplawsky, Jonathan, Farmer, Thomas O., Fan, Lisha, Guo, Er-Jia, Lu, Qiyang, Heller, William T., Choi, Yongseong, Haskel, Daniel, Fitzsimmons, Michael R., Chisholm, Matthew F., Huang, Kevin, Yildiz, Bilge, & Lee, Ho Nyung. Colossal oxygen vacancy formation at a fluorite-bixbyite interface. United States. doi:https://doi.org/10.1038/s41467-020-15153-8
Lee, Dongkyu, Gao, Xiang, Sun, Lixin, Jee, Youngseok, Poplawsky, Jonathan, Farmer, Thomas O., Fan, Lisha, Guo, Er-Jia, Lu, Qiyang, Heller, William T., Choi, Yongseong, Haskel, Daniel, Fitzsimmons, Michael R., Chisholm, Matthew F., Huang, Kevin, Yildiz, Bilge, and Lee, Ho Nyung. Fri . "Colossal oxygen vacancy formation at a fluorite-bixbyite interface". United States. doi:https://doi.org/10.1038/s41467-020-15153-8. https://www.osti.gov/servlets/purl/1615212.
@article{osti_1615212,
title = {Colossal oxygen vacancy formation at a fluorite-bixbyite interface},
author = {Lee, Dongkyu and Gao, Xiang and Sun, Lixin and Jee, Youngseok and Poplawsky, Jonathan and Farmer, Thomas O. and Fan, Lisha and Guo, Er-Jia and Lu, Qiyang and Heller, William T. and Choi, Yongseong and Haskel, Daniel and Fitzsimmons, Michael R. and Chisholm, Matthew F. and Huang, Kevin and Yildiz, Bilge and Lee, Ho Nyung},
abstractNote = {Oxygen vacancies in complex oxides are indispensable for information and energy technologies. There are several means to create oxygen vacancies in bulk materials. However, the use of ionic interfaces to create oxygen vacancies has not been fully explored. As such, we report an oxide nanobrush architecture designed to create high-density interfacial oxygen vacancies. An atomically well-defined (111) heterointerface between the fluorite CeO2 and the bixbyite Y2O3 is found to induce a charge modulation between Y3+ and Ce4+ ions enabled by the chemical valence mismatch between the two elements. Local structure and chemical analyses, along with theoretical calculations, suggest that more than 10% of oxygen atoms are spontaneously removed without deteriorating the lattice structure. Our fluorite–bixbyite nanobrush provides an excellent platform for the rational design of interfacial oxide architectures to precisely create, control, and transport oxygen vacancies critical for developing ionotronic and memristive devices for advanced energy and neuromorphic computing technologies.},
doi = {10.1038/s41467-020-15153-8},
journal = {Nature Communications},
number = 1,
volume = 11,
place = {United States},
year = {2020},
month = {3}
}

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