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Title: Evidence of a second-order Peierls-driven metal-insulator transition in crystalline NbO 2

Abstract

The metal-insulator transition of NbO 2 is thought to be important for the functioning of recent niobium oxide-based memristor devices, and is often described as a Mott transition in these contexts. Yet, the actual transition mechanism remains unclear, as current devices actually employ electroformed NbO x that may be inherently different to crystalline NbO 2 . We report on our synchrotron x-ray spectroscopy and density-functional-theory study of crystalline, epitaxial NbO 2 thin films grown by pulsed laser deposition and molecular beam epitaxy across the metal-insulator transition at ~ 810°C . The observed spectral changes reveal a second-order Peierls transition driven by a weakening of Nb dimerization without significant electron correlations, further supported by our density-functional-theory modeling. Our findings suggest that employing crystalline NbO 2 as an active layer in memristor devices may facilitate analog control of the resistivity, whereby Joule-heating can modulate Nb-Nb dimer distance and consequently control the opening of a pseudogap.

Authors:
 [1];  [1];  [1];  [2];  [1];  [1];  [1];  [3];  [4];  [4];  [5];  [5];  [5];  [6];  [7];  [8];  [9];  [6];  [1];  [3] more »;  [1] « less
  1. State Univ. of New York, Binghamton, NY (United States)
  2. Imperial College, London (United Kingdom)
  3. Georgia Inst. of Technology, Atlanta, GA (United States)
  4. Leibniz Inst. for Crystal Growth (IKZ), Berlin (Germany)
  5. Univ. of Liverpool (United Kingdom)
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  7. Science and Technology Facilities Council (STFC), Harwell Campus, Oxford (United Kingdom). Diamond Light Source, Ltd.
  8. Argonne National Lab. (ANL), Lemont, IL (United States)
  9. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; Engineering and Physical Sciences Research Council (EPSRC); US Air Force Office of Scientific Research (AFOSR); Air Force Research Laboratory (AFRL), Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF); Imperial College London; Diamond Light Source, UK; Leibniz Institute for Crystal Growth (IKZ); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
OSTI Identifier:
1547289
Alternate Identifier(s):
OSTI ID: 1546445; OSTI ID: 1560150; OSTI ID: 1601203
Report Number(s):
BNL-211927-2019-JAAM
Journal ID: ISSN 2475-9953; PRMHAR
Grant/Contract Number:  
SC0012704; AC02-06CH11357; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 3; Journal Issue: 7; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Wahila, Matthew J., Paez, Galo, Singh, Christopher N., Regoutz, Anna, Sallis, Shawn, Zuba, Mateusz J., Rana, Jatinkumar, Tellekamp, M. Brooks, Boschker, Jos E., Markurt, Toni, Swallow, Jack E. N., Jones, Leanne A. H., Veal, Tim D., Yang, Wanli, Lee, Tien-Lin, Rodolakis, Fanny, Sadowski, Jerzy T., Prendergast, David, Lee, Wei-Cheng, Doolittle, W. Alan, and Piper, Louis F. J. Evidence of a second-order Peierls-driven metal-insulator transition in crystalline NbO2. United States: N. p., 2019. Web. doi:10.1103/PhysRevMaterials.3.074602.
Wahila, Matthew J., Paez, Galo, Singh, Christopher N., Regoutz, Anna, Sallis, Shawn, Zuba, Mateusz J., Rana, Jatinkumar, Tellekamp, M. Brooks, Boschker, Jos E., Markurt, Toni, Swallow, Jack E. N., Jones, Leanne A. H., Veal, Tim D., Yang, Wanli, Lee, Tien-Lin, Rodolakis, Fanny, Sadowski, Jerzy T., Prendergast, David, Lee, Wei-Cheng, Doolittle, W. Alan, & Piper, Louis F. J. Evidence of a second-order Peierls-driven metal-insulator transition in crystalline NbO2. United States. doi:10.1103/PhysRevMaterials.3.074602.
Wahila, Matthew J., Paez, Galo, Singh, Christopher N., Regoutz, Anna, Sallis, Shawn, Zuba, Mateusz J., Rana, Jatinkumar, Tellekamp, M. Brooks, Boschker, Jos E., Markurt, Toni, Swallow, Jack E. N., Jones, Leanne A. H., Veal, Tim D., Yang, Wanli, Lee, Tien-Lin, Rodolakis, Fanny, Sadowski, Jerzy T., Prendergast, David, Lee, Wei-Cheng, Doolittle, W. Alan, and Piper, Louis F. J. Tue . "Evidence of a second-order Peierls-driven metal-insulator transition in crystalline NbO2". United States. doi:10.1103/PhysRevMaterials.3.074602. https://www.osti.gov/servlets/purl/1547289.
@article{osti_1547289,
title = {Evidence of a second-order Peierls-driven metal-insulator transition in crystalline NbO2},
author = {Wahila, Matthew J. and Paez, Galo and Singh, Christopher N. and Regoutz, Anna and Sallis, Shawn and Zuba, Mateusz J. and Rana, Jatinkumar and Tellekamp, M. Brooks and Boschker, Jos E. and Markurt, Toni and Swallow, Jack E. N. and Jones, Leanne A. H. and Veal, Tim D. and Yang, Wanli and Lee, Tien-Lin and Rodolakis, Fanny and Sadowski, Jerzy T. and Prendergast, David and Lee, Wei-Cheng and Doolittle, W. Alan and Piper, Louis F. J.},
abstractNote = {The metal-insulator transition of NbO2 is thought to be important for the functioning of recent niobium oxide-based memristor devices, and is often described as a Mott transition in these contexts. Yet, the actual transition mechanism remains unclear, as current devices actually employ electroformed NbOx that may be inherently different to crystalline NbO2. We report on our synchrotron x-ray spectroscopy and density-functional-theory study of crystalline, epitaxial NbO2 thin films grown by pulsed laser deposition and molecular beam epitaxy across the metal-insulator transition at ~ 810°C . The observed spectral changes reveal a second-order Peierls transition driven by a weakening of Nb dimerization without significant electron correlations, further supported by our density-functional-theory modeling. Our findings suggest that employing crystalline NbO2 as an active layer in memristor devices may facilitate analog control of the resistivity, whereby Joule-heating can modulate Nb-Nb dimer distance and consequently control the opening of a pseudogap.},
doi = {10.1103/PhysRevMaterials.3.074602},
journal = {Physical Review Materials},
number = 7,
volume = 3,
place = {United States},
year = {2019},
month = {7}
}

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The metal-insulator transition of NbO 2 : An embedded Peierls instability
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Chaotic dynamics in nanoscale NbO2 Mott memristors for analogue computing
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Tuning a strain-induced orbital selective Mott transition in epitaxial VO 2
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Scalable Memdiodes Exhibiting Rectification and Hysteresis for Neuromorphic Computing
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    Works referencing / citing this record:

    Mott Memory and Neuromorphic Devices
    journal, August 2015


    Uniform second Li ion intercalation in solid state ϵ-LiVOPO4
    journal, August 2016

    • Wangoh, Linda W.; Sallis, Shawn; Wiaderek, Kamila M.
    • Applied Physics Letters, Vol. 109, Issue 5
    • DOI: 10.1063/1.4960452

    Dynamic electronic correlation effects in NbO 2 as compared to VO 2
    journal, November 2017


    Real-space multiple-scattering calculation and interpretation of x-ray-absorption near-edge structure
    journal, September 1998


    Chaotic dynamics in nanoscale NbO2 Mott memristors for analogue computing
    journal, August 2017

    • Kumar, Suhas; Strachan, John Paul; Williams, R. Stanley
    • Nature, Vol. 548, Issue 7667
    • DOI: 10.1038/nature23307

    Electronic and optical properties of NbO2
    journal, December 2014

    • O'Hara, Andrew; Nunley, Timothy N.; Posadas, Agham B.
    • Journal of Applied Physics, Vol. 116, Issue 21
    • DOI: 10.1063/1.4903067

    NbO x based oscillation neuron for neuromorphic computing
    journal, September 2017

    • Gao, Ligang; Chen, Pai-Yu; Yu, Shimeng
    • Applied Physics Letters, Vol. 111, Issue 10
    • DOI: 10.1063/1.4991917

    Physical origins of current and temperature controlled negative differential resistances in NbO2
    journal, September 2017


    Measurement & Minimization of Mount Induced Strain on Double Crystal Monochromator Crystals
    journal, March 2013


    Tuning a strain-induced orbital selective Mott transition in epitaxial VO 2
    journal, June 2016


    A scalable neuristor built with Mott memristors
    journal, December 2012

    • Pickett, Matthew D.; Medeiros-Ribeiro, Gilberto; Williams, R. Stanley
    • Nature Materials, Vol. 12, Issue 2
    • DOI: 10.1038/nmat3510

    Cooperative effects of strain and electron correlation in epitaxial VO 2 and NbO 2
    journal, February 2019

    • Lee, Wei-Cheng; Wahila, Matthew J.; Mukherjee, Shantanu
    • Journal of Applied Physics, Vol. 125, Issue 8
    • DOI: 10.1063/1.5052636

    Generalized Gradient Approximation Made Simple
    journal, October 1996

    • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
    • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
    • DOI: 10.1103/physrevlett.77.3865

    Sub-100 fJ and sub-nanosecond thermally driven threshold switching in niobium oxide crosspoint nanodevices
    journal, May 2012


    Accurate X-Ray Spectral Predictions: An Advanced Self-Consistent-Field Approach Inspired by Many-Body Perturbation Theory
    journal, March 2017


    Scalable Memdiodes Exhibiting Rectification and Hysteresis for Neuromorphic Computing
    journal, August 2018


    Molecular Beam Epitaxy of lithium niobium oxide multifunctional materials
    journal, April 2017


    ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
    journal, June 2005


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


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


    Electrical Properties of Semiconducting NbO 2
    journal, April 1985

    • Sakai, Yoshio; Tsuda, Nobuo; Sakata, Tamio
    • Journal of the Physical Society of Japan, Vol. 54, Issue 4
    • DOI: 10.1143/jpsj.54.1514

    Nature of the metal-insulator transition in Nb O 2
    journal, March 2015


    Transfer of Spectral Weight and Symmetry across the Metal-Insulator Transition in VO 2
    journal, September 2006


    Transient dynamics of NbO x threshold switches explained by Poole-Frenkel based thermal feedback mechanism
    journal, May 2018

    • Wang, Ziwen; Kumar, Suhas; Nishi, Yoshio
    • Applied Physics Letters, Vol. 112, Issue 19
    • DOI: 10.1063/1.5027152

    Nature of the Metal Insulator Transition in Ultrathin Epitaxial Vanadium Dioxide
    journal, September 2013

    • Quackenbush, N. F.; Tashman, J. W.; Mundy, J. A.
    • Nano Letters, Vol. 13, Issue 10
    • DOI: 10.1021/nl402716d

    Orbital-Assisted Metal-Insulator Transition in VO 2
    journal, November 2005


    The metal-insulator transition of NbO 2 : An embedded Peierls instability
    journal, June 2002


    Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set
    journal, July 1996


    Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
    journal, October 1996


    IFEFFIT  : interactive XAFS analysis and FEFF fitting
    journal, March 2001