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

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

doi:10.1021/acsnano.8b03031

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

Journal Article · Fri Jun 15 00:00:00 EDT 2018 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.8b03031· OSTI ID:1462904

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^[1]; Sohn, Changhee ^[1];

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Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)

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.

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Research Organization:: 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 Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; AC02-06CH11357

OSTI ID:: 1462904

Alternate ID(s):: OSTI ID: 1466361

Journal Information:: ACS Nano, Vol. 12, Issue 7; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 34 works

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

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