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Evolution of Metallicity in Vanadium Dioxide by Creation of Oxygen Vacancies

Zhen Zhang1, Fan Zuo1, Chenghao Wan2, Aveek Dutta3, Jongbum Kim3, Jura Rensberg4, Ronny Nawrodt4, Helen Hejin Park5,9, Thomas J. Larrabee5,8 et al.

Xiaofei Guan6, You Zhou7, S. M. Prokes5, Carsten Ronning4, Vladimir M. Shalaev3, Alexandra Boltasseva3, Mikhail A. Kats2, and Shriram Ramanathan1,*

  • 1School of Materials Engineering, Purdue University, West Lafayette, Indiana 47907, USA
  • 2Department of Electrical and Computer Engineering, Department of Materials Science and Engineering, University of Wisconsin-Madison, Madison, Wisconsin 53706, USA
  • 3School of Electrical and Computer Engineering and Birck Nanotechnology Center, Purdue University, West Lafayette, Indiana 47907, USA
  • 4Institute for Solid State Physics, Friedrich Schiller University Jena, 07743 Jena, Germany
  • 5United States Naval Research Laboratory, Washington, D.C. 20375, USA
  • 6John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, USA
  • 7Department of Chemistry and Chemical Biology, Harvard University, Cambridge, Massachusetts 02138, USA
  • 8National Research Council Research Associate at the Naval Research Laboratory, Washington, D.C. 20375, USA
  • 9American Society for Engineering Education Research Associate at the Naval Research Laboratory, Washington, D.C. 20375, USA

  • *Shriram@purdue.edu
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Phys. Rev. Applied 7, 034008 – Published 10 March, 2017

DOI: https://doi.org/10.1103/PhysRevApplied.7.034008

Abstract

Tuning of the electronic state of correlated materials is key to their eventual use in advanced electronics and photonics. The prototypical correlated oxide (VO2) is insulating at room temperature and transforms to a metallic state when heated to 67 °C (340 K). We report the emergence of a metallic state that is preserved down to 1.8 K by annealing thin films of VO2 at an ultralow oxygen partial pressure (PO2∼10−24  atm). The films can be reverted back to their original state by annealing in oxygen, and this process can be iterated multiple times. The metallic phase created by oxygen deficiency has a tetragonal rutile structure and contains a large number of oxygen vacancies far beyond the solubility at equilibrium (greater than approximately 50 times). The oxygen starvation reduces the oxidation state of vanadium from V4+ to V3+ and leads to the metallization. The extent of resistance reduction (concurrent with tuning of optical properties) can be controlled by the time-temperature envelope of the annealing conditions since the process is diffusionally driven. This experimental platform, which can extensively tune oxygen vacancies in correlated oxides, provides an approach to study emergent phases and defect-mediated adaptive electronic and structural phase boundary crossovers.

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Phys. Rev. Applied 7, 034008– Published 10 March, 2017
  • Received 2 November 2016
Article part of CHORUS

© 2017 American Physical Society

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