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Title: Nanoscale Control of Oxygen Defects and Metal–Insulator Transition in Epitaxial Vanadium Dioxides

Abstract

Strongly correlated vanadium dioxide (VO 2) 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 VO 2 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 VO 2 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. In conclusion, this study highlights the crucial role of oxygen vacancies in controlling the MIT in epitaxial VO 2 thin films, useful for developing advanced electronic and iontronic devices.

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
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. 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, and Lee, Ho Nyung. Fri . "Nanoscale Control of Oxygen Defects and Metal–Insulator Transition in Epitaxial Vanadium Dioxides". United States. doi: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. In conclusion, 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 = {2018},
month = {6}
}

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