Nanoscale Control of Oxygen Defects and Metal–Insulator Transition in Epitaxial Vanadium Dioxides
Abstract
Strongly correlated vanadium dioxide (VO2) is one of the most promising materials that exhibits a temperature-driven, metal insulator transition (MIT) near room temperature. The ability to manipulate the MIT at nanoscale offers both insight into understanding the energetics of phase transition and a promising potential for nanoelectronic devices. In this work, we study nanoscale electrochemical modifications of the MIT in epitaxial VO2 thin films using a combined approach with scanning probe microscopy (SPM) and theoretical calculations. We find that applying electric voltages of different polarity through an SPM tip locally changes the contact potential difference and conductivity on the surface of VO2 by modulating the oxygen stoichiometry. We observed nearly 2 orders of magnitude change in resistance between positive and negative biased-tip written areas of the film, demonstrating the electric field modulated MIT behavior at the nanoscale. Density functional theory calculations, benchmarked against more accurate many-body quantum Monte Carlo calculations, provide information on the formation energetics of oxygen defects that can be further manipulated by strain. This study highlights the crucial role of oxygen vacancies in controlling the MIT in epitaxial VO2 thin films, useful for developing advanced electronic and iontronic devices.
- Authors:
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- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1462904
- Alternate Identifier(s):
- OSTI ID: 1466361
- Grant/Contract Number:
- AC05-00OR22725; AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Nano
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 7; Journal ID: ISSN 1936-0851
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; density functional theory; metal−insulator transition; oxygen vacancy; quantum Monte Carlo; scanning probe microscopy; vanadium dioxide
Citation Formats
Sharma, Yogesh, Balachandran, Janakiraman, Sohn, Changhee, Krogel, Jaron T., Ganesh, Panchapakesan, Collins, Liam F., Ievlev, Anton V., Li, Qian, Gao, Xiang, Balke, Nina, Ovchinnikova, Olga S., Kalinin, Sergei V., Heinonen, Olle, and Lee, Ho Nyung. Nanoscale Control of Oxygen Defects and Metal–Insulator Transition in Epitaxial Vanadium Dioxides. United States: N. p., 2018.
Web. doi:10.1021/acsnano.8b03031.
Sharma, Yogesh, Balachandran, Janakiraman, Sohn, Changhee, Krogel, Jaron T., Ganesh, Panchapakesan, Collins, Liam F., Ievlev, Anton V., Li, Qian, Gao, Xiang, Balke, Nina, Ovchinnikova, Olga S., Kalinin, Sergei V., Heinonen, Olle, & Lee, Ho Nyung. Nanoscale Control of Oxygen Defects and Metal–Insulator Transition in Epitaxial Vanadium Dioxides. United States. https://doi.org/10.1021/acsnano.8b03031
Sharma, Yogesh, Balachandran, Janakiraman, Sohn, Changhee, Krogel, Jaron T., Ganesh, Panchapakesan, Collins, Liam F., Ievlev, Anton V., Li, Qian, Gao, Xiang, Balke, Nina, Ovchinnikova, Olga S., Kalinin, Sergei V., Heinonen, Olle, and Lee, Ho Nyung. Fri .
"Nanoscale Control of Oxygen Defects and Metal–Insulator Transition in Epitaxial Vanadium Dioxides". United States. https://doi.org/10.1021/acsnano.8b03031. https://www.osti.gov/servlets/purl/1462904.
@article{osti_1462904,
title = {Nanoscale Control of Oxygen Defects and Metal–Insulator Transition in Epitaxial Vanadium Dioxides},
author = {Sharma, Yogesh and Balachandran, Janakiraman and Sohn, Changhee and Krogel, Jaron T. and Ganesh, Panchapakesan and Collins, Liam F. and Ievlev, Anton V. and Li, Qian and Gao, Xiang and Balke, Nina and Ovchinnikova, Olga S. and Kalinin, Sergei V. and Heinonen, Olle and Lee, Ho Nyung},
abstractNote = {Strongly correlated vanadium dioxide (VO2) is one of the most promising materials that exhibits a temperature-driven, metal insulator transition (MIT) near room temperature. The ability to manipulate the MIT at nanoscale offers both insight into understanding the energetics of phase transition and a promising potential for nanoelectronic devices. In this work, we study nanoscale electrochemical modifications of the MIT in epitaxial VO2 thin films using a combined approach with scanning probe microscopy (SPM) and theoretical calculations. We find that applying electric voltages of different polarity through an SPM tip locally changes the contact potential difference and conductivity on the surface of VO2 by modulating the oxygen stoichiometry. We observed nearly 2 orders of magnitude change in resistance between positive and negative biased-tip written areas of the film, demonstrating the electric field modulated MIT behavior at the nanoscale. Density functional theory calculations, benchmarked against more accurate many-body quantum Monte Carlo calculations, provide information on the formation energetics of oxygen defects that can be further manipulated by strain. This study highlights the crucial role of oxygen vacancies in controlling the MIT in epitaxial VO2 thin films, useful for developing advanced electronic and iontronic devices.},
doi = {10.1021/acsnano.8b03031},
journal = {ACS Nano},
number = 7,
volume = 12,
place = {United States},
year = {Fri Jun 15 00:00:00 EDT 2018},
month = {Fri Jun 15 00:00:00 EDT 2018}
}
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