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

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

^[1]; ^[1]; Sohn, Changhee ^[1]; ^[1]; ^[1]; ^[1]; ^[1]; ^[1]; Gao, Xiang ^[1]; ^[1]; ^[1]; ^[1]; ^[2]; ^[1]

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. 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.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1462904

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

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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

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