Colossal oxygen vacancy formation at a fluorite-bixbyite interface

Dongkyu Lee, Xiang Gao, Lixin Sun, Youngseok Jee, Jonathan Poplawsky, Thomas O. Farmer, Lisha Fan, Er-Jia Guo, Qiyang Lu, William T. Heller, Yongseong Choi, Daniel Haskel, Michael R. Fitzsimmons, Matthew F. Chisholm, Kevin Huang, Bilge Yildiz and Ho Nyung Lee ()
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Dongkyu Lee: Oak Ridge National Laboratory
Xiang Gao: Oak Ridge National Laboratory
Lixin Sun: Massachusetts Institute of Technology
Youngseok Jee: University of South Carolina
Jonathan Poplawsky: Oak Ridge National Laboratory
Thomas O. Farmer: Oak Ridge National Laboratory
Lisha Fan: Oak Ridge National Laboratory
Er-Jia Guo: Oak Ridge National Laboratory
Qiyang Lu: Massachusetts Institute of Technology
William T. Heller: Oak Ridge National Laboratory
Yongseong Choi: Argonne National Laboratory
Daniel Haskel: Argonne National Laboratory
Michael R. Fitzsimmons: Oak Ridge National Laboratory
Matthew F. Chisholm: Oak Ridge National Laboratory
Kevin Huang: University of South Carolina
Bilge Yildiz: Massachusetts Institute of Technology
Ho Nyung Lee: Oak Ridge National Laboratory

Nature Communications, 2020, vol. 11, issue 1, 1-7

Abstract: 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. Herein, 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.

Date: 2020
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DOI: 10.1038/s41467-020-15153-8

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