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; Ho Nyung Lee

doi:10.1038/s41467-020-15153-8

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, Ho Nyung Lee

Research output: Contribution to journal › Article › peer-review

78 Scopus citations

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.

Original language	English
Article number	1371
Journal	Nature Communications
Volume	11
Issue number	1
DOIs	https://doi.org/10.1038/s41467-020-15153-8
State	Published - Dec 1 2020

Funding

The authors are grateful for helpful discussions with S.M. Haile, J. Maier, and H.L. Tuller. This work was supported by the US Department of Energy (DOE), Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. A portion of this research used resources at the Center for Nanophase Materials Sciences (STEM and APT) and the Spallation Neutron Source (SANS), which are U.S. DOE Office of Science User Facilities operated by Oak Ridge National Laboratory. Theoretical calculations used resources at the National Energy Research Scientific Computing Center, a U.S. DOE Office of Science User Facility operated under Contract No. DE-AC02-05CH11231. X-ray absorption fine structure work used resources of the Advanced Photon Source, a U.S. DOE Office of Science User Facility operated for the U.S. DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357.

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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. 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.",

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AU - Choi, Yongseong

AU - Haskel, Daniel

AU - Fitzsimmons, Michael R.

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Colossal oxygen vacancy formation at a fluorite-bixbyite interface

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