DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Competing phases in epitaxial vanadium dioxide at nanoscale

Abstract

Phase competition in correlated oxides offers tantalizing opportunities as many intriguing physical phenomena occur near the phase transitions. Owing to a sharp metal-insulator transition (MIT) near room temperature, the correlated vanadium dioxide (VO2) exhibits a strong competition between insulating and metallic phases, which is important for practical applications. However, the phase boundary undergoes a strong modification when strain is involved, yielding complex phase transitions. Here, we report the emergence of nanoscale M2 phase domains in VO2 epitaxial films under anisotropic strain relaxation. The competing phases of the films are imaged by multilength-scale probes, detecting the structural and electrical properties in individual local domains. Competing evolution of the M1 and M2 phases indicates the critical role of lattice-strain on both the stability of the M2 Mott phase and the energetics of the MIT in VO2 films. This study demonstrates how strain engineering can be utilized to design phase states, which allow deliberate control of MIT behavior at the nanoscale in epitaxial VO2 films.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; 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)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE
OSTI Identifier:
1561644
Alternate Identifier(s):
OSTI ID: 1559361
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
APL Materials
Additional Journal Information:
Journal Volume: 7; Journal Issue: 8; Journal ID: ISSN 2166-532X
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Sharma, Yogesh, Holt, Martin V., Laanait, Nouamane, Gao, Xiang, Ivanov, Ilia N., Collins, Liam, Sohn, Changhee, Liao, Zhaoliang, Skoropata, Elizabeth, Kalinin, Sergei V., Balke, Nina, Eres, Gyula, Ward, Thomas Z., and Lee, Ho Nyung. Competing phases in epitaxial vanadium dioxide at nanoscale. United States: N. p., 2019. Web. doi:10.1063/1.5115784.
Sharma, Yogesh, Holt, Martin V., Laanait, Nouamane, Gao, Xiang, Ivanov, Ilia N., Collins, Liam, Sohn, Changhee, Liao, Zhaoliang, Skoropata, Elizabeth, Kalinin, Sergei V., Balke, Nina, Eres, Gyula, Ward, Thomas Z., & Lee, Ho Nyung. Competing phases in epitaxial vanadium dioxide at nanoscale. United States. https://doi.org/10.1063/1.5115784
Sharma, Yogesh, Holt, Martin V., Laanait, Nouamane, Gao, Xiang, Ivanov, Ilia N., Collins, Liam, Sohn, Changhee, Liao, Zhaoliang, Skoropata, Elizabeth, Kalinin, Sergei V., Balke, Nina, Eres, Gyula, Ward, Thomas Z., and Lee, Ho Nyung. Thu . "Competing phases in epitaxial vanadium dioxide at nanoscale". United States. https://doi.org/10.1063/1.5115784. https://www.osti.gov/servlets/purl/1561644.
@article{osti_1561644,
title = {Competing phases in epitaxial vanadium dioxide at nanoscale},
author = {Sharma, Yogesh and Holt, Martin V. and Laanait, Nouamane and Gao, Xiang and Ivanov, Ilia N. and Collins, Liam and Sohn, Changhee and Liao, Zhaoliang and Skoropata, Elizabeth and Kalinin, Sergei V. and Balke, Nina and Eres, Gyula and Ward, Thomas Z. and Lee, Ho Nyung},
abstractNote = {Phase competition in correlated oxides offers tantalizing opportunities as many intriguing physical phenomena occur near the phase transitions. Owing to a sharp metal-insulator transition (MIT) near room temperature, the correlated vanadium dioxide (VO2) exhibits a strong competition between insulating and metallic phases, which is important for practical applications. However, the phase boundary undergoes a strong modification when strain is involved, yielding complex phase transitions. Here, we report the emergence of nanoscale M2 phase domains in VO2 epitaxial films under anisotropic strain relaxation. The competing phases of the films are imaged by multilength-scale probes, detecting the structural and electrical properties in individual local domains. Competing evolution of the M1 and M2 phases indicates the critical role of lattice-strain on both the stability of the M2 Mott phase and the energetics of the MIT in VO2 films. This study demonstrates how strain engineering can be utilized to design phase states, which allow deliberate control of MIT behavior at the nanoscale in epitaxial VO2 films.},
doi = {10.1063/1.5115784},
journal = {APL Materials},
number = 8,
volume = 7,
place = {United States},
year = {2019},
month = {8}
}

Works referenced in this record:

Sharpened VO 2 Phase Transition via Controlled Release of Epitaxial Strain
journal, August 2017


A hard X-ray nanoprobe beamline for nanoscale microscopy
journal, September 2012

  • Winarski, Robert P.; Holt, Martin V.; Rose, Volker
  • Journal of Synchrotron Radiation, Vol. 19, Issue 6
  • DOI: 10.1107/s0909049512036783

A robot-based detector manipulator system for a hard X-ray nanoprobe instrument
journal, November 2007

  • Shu, D.; Maser, J.; Holt, M.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 582, Issue 1
  • DOI: 10.1016/j.nima.2007.08.097

Phase transition in bulk single crystals and thin films of V O 2 by nanoscale infrared spectroscopy and imaging
journal, June 2015


Direct evidence of M 2 phase during the monoclinic-tetragonal (rutile) phase transition of W-doped VO 2 nanowires
journal, January 2017

  • Asayesh-Ardakani, Hasti; Yao, Wentao; Nie, Anmin
  • Applied Physics Letters, Vol. 110, Issue 5
  • DOI: 10.1063/1.4975210

Role of microstructures on the M1-M2 phase transition in epitaxial VO2 thin films
journal, May 2014

  • Ji, Yanda; Zhang, Yin; Gao, Min
  • Scientific Reports, Vol. 4, Issue 1
  • DOI: 10.1038/srep04854

Transport properties of ultra-thin VO 2 films on (001) TiO 2 grown by reactive molecular-beam epitaxy
journal, October 2015

  • Paik, Hanjong; Moyer, Jarrett A.; Spila, Timothy
  • Applied Physics Letters, Vol. 107, Issue 16
  • DOI: 10.1063/1.4932123

Nanoscale Control of Oxygen Defects and Metal–Insulator Transition in Epitaxial Vanadium Dioxides
journal, June 2018

  • Sharma, Yogesh; Balachandran, Janakiraman; Sohn, Changhee
  • ACS Nano, Vol. 12, Issue 7
  • DOI: 10.1021/acsnano.8b03031

Doping-Based Stabilization of the M2 Phase in Free-Standing VO 2 Nanostructures at Room Temperature
journal, February 2012

  • Strelcov, Evgheni; Tselev, Alexander; Ivanov, Ilia
  • Nano Letters, Vol. 12, Issue 12
  • DOI: 10.1021/nl303065h

Symmetry Relationship and Strain-Induced Transitions between Insulating M1 and M2 and Metallic R phases of Vanadium Dioxide
journal, November 2010

  • Tselev, A.; Luk’yanchuk, I. A.; Ivanov, I. N.
  • Nano Letters, Vol. 10, Issue 11
  • DOI: 10.1021/nl1020443

Strain engineering and one-dimensional organization of metal–insulator domains in single-crystal vanadium dioxide beams
journal, September 2009


Appearance of large crystalline domains in VO 2 films grown on sapphire (001) and their phase transition characteristics
journal, June 2015

  • Azhan, Nurul Hanis; Su, Kui; Okimura, Kunio
  • Journal of Applied Physics, Vol. 117, Issue 24
  • DOI: 10.1063/1.4923223

Strain-induced metal–insulator phase coexistence in perovskite manganites
journal, March 2004


Anisotropic Electronic State via Spontaneous Phase Separation in Strained Vanadium Dioxide Films
journal, August 2013


Local Temperature Redistribution and Structural Transition During Joule-Heating-Driven Conductance Switching in VO 2
journal, July 2013

  • Kumar, Suhas; Pickett, Matthew D.; Strachan, John Paul
  • Advanced Materials, Vol. 25, Issue 42
  • DOI: 10.1002/adma.201302046

Large epitaxial bi-axial strain induces a Mott-like phase transition in VO 2
journal, August 2014

  • Kittiwatanakul, Salinporn; Wolf, Stuart A.; Lu, Jiwei
  • Applied Physics Letters, Vol. 105, Issue 7
  • DOI: 10.1063/1.4893326

Terahertz-field-induced insulator-to-metal transition in vanadium dioxide metamaterial
journal, July 2012

  • Liu, Mengkun; Hwang, Harold Y.; Tao, Hu
  • Nature, Vol. 487, Issue 7407
  • DOI: 10.1038/nature11231

Control of the metal–insulator transition in vanadium dioxide by modifying orbital occupancy
journal, September 2013

  • Aetukuri, Nagaphani B.; Gray, Alexander X.; Drouard, Marc
  • Nature Physics, Vol. 9, Issue 10
  • DOI: 10.1038/nphys2733

Imaging nanoscale lattice variations by machine learning of x-ray diffraction microscopy data
journal, August 2016


Mott Transition in VO2 Revealed by Infrared Spectroscopy and Nano-Imaging
journal, December 2007


Oxide Electronics Utilizing Ultrafast Metal-Insulator Transitions
journal, August 2011


Isostructural metal-insulator transition in VO 2
journal, November 2018


Reducing orbital occupancy in VO 2 suppresses Mott physics while Peierls distortions persist
journal, August 2017


Stability of the M2 phase of vanadium dioxide induced by coherent epitaxial strain
journal, August 2016


Decoupling of Structural and Electronic Phase Transitions in VO 2
journal, October 2012


Modern Scattering‐Type Scanning Near‐Field Optical Microscopy for Advanced Material Research
journal, April 2019


Temperature-dependent Raman and ultraviolet photoelectron spectroscopy studies on phase transition behavior of VO 2 films with M1 and M2 phases
journal, April 2014

  • Okimura, Kunio; Hanis Azhan, Nurul; Hajiri, Tetsuya
  • Journal of Applied Physics, Vol. 115, Issue 15
  • DOI: 10.1063/1.4870868

Characterization of high-resolution diffractive X-ray optics by ptychographic coherent diffractive imaging
journal, January 2011

  • Vila-Comamala, Joan; Diaz, Ana; Guizar-Sicairos, Manuel
  • Optics Express, Vol. 19, Issue 22
  • DOI: 10.1364/oe.19.021333

Dimerization of a linear Heisenberg chain in the insulating phases of V 1 x Cr x O 2
journal, September 1974


Phase Separation Scenario for Manganese Oxides and Related Materials
journal, March 1999


Metal-Insulator Transition
journal, October 1968


Roles of strain and domain boundaries on the phase transition stability of VO 2 thin films
journal, October 2017

  • Jian, Jie; Chen, Aiping; Chen, Youxing
  • Applied Physics Letters, Vol. 111, Issue 15
  • DOI: 10.1063/1.4991882

Growth control of the oxidation state in vanadium oxide thin films
journal, December 2014

  • Lee, Shinbuhm; Meyer, Tricia L.; Park, Sungkyun
  • Applied Physics Letters, Vol. 105, Issue 22
  • DOI: 10.1063/1.4903348

Percolative phase separation underlies colossal magnetoresistance in mixed-valent manganites
journal, June 1999

  • Uehara, M.; Mori, S.; Chen, C. H.
  • Nature, Vol. 399, Issue 6736
  • DOI: 10.1038/21142

A photoinduced metal-like phase of monoclinic VO 2 revealed by ultrafast electron diffraction
journal, October 2014

  • Morrison, Vance R.; Chatelain, Robert. P.; Tiwari, Kunal L.
  • Science, Vol. 346, Issue 6208
  • DOI: 10.1126/science.1253779

Metallization of vanadium dioxide driven by large phonon entropy
journal, November 2014

  • Budai, John D.; Hong, Jiawang; Manley, Michael E.
  • Nature, Vol. 515, Issue 7528
  • DOI: 10.1038/nature13865

Metal-insulator transitions
journal, October 1998

  • Imada, Masatoshi; Fujimori, Atsushi; Tokura, Yoshinori
  • Reviews of Modern Physics, Vol. 70, Issue 4, p. 1039-1263
  • DOI: 10.1103/revmodphys.70.1039

Sequential Electronic and Structural Transitions in VO 2 Observed Using X-ray Absorption Spectromicroscopy
journal, October 2014

  • Kumar, Suhas; Strachan, John Paul; Pickett, Matthew D.
  • Advanced Materials, Vol. 26, Issue 44
  • DOI: 10.1002/adma.201402404

Extended Mapping and Exploration of the Vanadium Dioxide Stress-Temperature Phase Diagram
journal, July 2010


Persistent Electrochemical Performance in Epitaxial VO 2 (B)
journal, March 2017


Nano-optical Investigations of the Metal−Insulator Phase Behavior of Individual VO 2 Microcrystals
journal, May 2010

  • Jones, Andrew C.; Berweger, Samuel; Wei, Jiang
  • Nano Letters, Vol. 10, Issue 5
  • DOI: 10.1021/nl903765h

Stress relaxation effect on transport properties of strained vanadium dioxide epitaxial thin films
journal, November 2006


Epitaxial stabilization and phase instability of VO2 polymorphs
journal, January 2016

  • Lee, Shinbuhm; Ivanov, Ilia N.; Keum, Jong K.
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep19621

Textured metastable VO 2 (B) thin films on SrTiO 3 substrates with significantly enhanced conductivity
journal, February 2014

  • Chen, Aiping; Bi, Zhenxing; Zhang, Wenrui
  • Applied Physics Letters, Vol. 104, Issue 7
  • DOI: 10.1063/1.4865898

Direct Correlation of Structural Domain Formation with the Metal Insulator Transition in a VO 2 Nanobeam
journal, December 2009

  • Zhang, Shixiong; Chou, Jung Yen; Lauhon, Lincoln J.
  • Nano Letters, Vol. 9, Issue 12
  • DOI: 10.1021/nl9028973

Measurement of a solid-state triple point at the metal–insulator transition in VO2
journal, August 2013

  • Park, Jae Hyung; Coy, Jim M.; Kasirga, T. Serkan
  • Nature, Vol. 500, Issue 7463
  • DOI: 10.1038/nature12425

Mott Memory and Neuromorphic Devices
journal, August 2015


Nanoscale imaging of the electronic and structural transitions in vanadium dioxide
journal, April 2011


VO 2 : Peierls or Mott-Hubbard? A view from band theory
journal, May 1994

  • Wentzcovitch, Renata M.; Schulz, Werner W.; Allen, Philip B.
  • Physical Review Letters, Vol. 72, Issue 21
  • DOI: 10.1103/physrevlett.72.3389

Oxides Which Show a Metal-to-Insulator Transition at the Neel Temperature
journal, July 1959


Spatially Inhomogeneous Metal-Insulator Transition in Doped Manganites
journal, September 1999


Inhomogeneity of the ultrafast insulator-to-metal transition dynamics of VO2
journal, April 2015

  • O’Callahan, Brian T.; Jones, Andrew C.; Hyung Park, Jae
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms7849

Highly repeatable nanoscale phase coexistence in vanadium dioxide films
journal, February 2018


Strain and temperature dependence of the insulating phases of VO 2 near the metal-insulator transition
journal, January 2012


The two components of the crystallographic transition in VO2
journal, November 1971


Direct Observation of Decoupled Structural and Electronic Transitions and an Ambient Pressure Monocliniclike Metallic Phase of VO 2
journal, November 2014


Full-field X-ray reflection microscopy of epitaxial thin-films
journal, October 2014

  • Laanait, Nouamane; Zhang, Zhan; Schlepütz, Christian M.
  • Journal of Synchrotron Radiation, Vol. 21, Issue 6
  • DOI: 10.1107/s1600577514016555

Mechanics and Dynamics of the Strain-Induced M1–M2 Structural Phase Transition in Individual VO 2 Nanowires
journal, August 2011


Comment on "V O 2 : Peierls or Mott-Hubbard? A View from Band Theory"
journal, November 1994


Metal-insulator transitions
journal, June 1991


Scalable radiative thermal logic gates based on nanoparticle networks
journal, February 2020


Inhomogeneity of the ultrafast insulator-to-metal transition dynamics of VO2
text, January 2015

  • T., O'Callahan, Brian; Jae, Hyung Park,; H., Cobden, David
  • The University of North Carolina at Chapel Hill University Libraries
  • DOI: 10.17615/9cck-6p65

Mott transition in VO2 revealed by infrared spectroscopy and nano-imaging
text, January 2008


Nanoscale imaging of the electronic and structural transitions in vanadium dioxide
text, January 2011


Measurement of a solid-state triple point at the metal-insulator transition in VO2
text, January 2013


Epitaxial stabilization and phase instability of VO2 polymorphs
preprint, January 2015