Insulating phases of vanadium dioxide are Mott-Hubbard insulators

Huffman, T. J.; Hendriks, C.; Walter, E. J.; Yoon, Joonseok; Ju, Honglyoul; Smith, R.; Carr, G. L.; Krakauer, H.; Qazilbash, M. M.

doi:10.1103/PhysRevB.95.075125

Title: Insulating phases of vanadium dioxide are Mott-Hubbard insulators

Journal Article · Tue Feb 14 23:00:00 EST 2017 · Physical Review B

DOI: https://doi.org/10.1103/PhysRevB.95.075125 · OSTI ID:1376670

Huffman, T. J. ^[1]; Hendriks, C. ^[1]; Walter, E. J. ^[1]; Yoon, Joonseok ^[2]; Ju, Honglyoul ^[2]; Smith, R. ^[3]; Carr, G. L. ^[3]; Krakauer, H. ^[1]; Qazilbash, M. M. ^[1]

College of William and Mary, Williamsburg, VA (United States)
Yonsei Univ., Seoul (Republic of Korea)
Brookhaven National Lab. (BNL), Upton, NY (United States)

Here, we present comprehensive broadband optical spectroscopy data on two insulating phases of vanadium dioxide (VO₂): monoclinic M₂ and triclinic. The main result of our work is that the energy gap and the electronic structure are essentially unaltered by the first-order structural phase transition between the M₂ and triclinic phases. Moreover, the optical interband features in the M₂ and triclinic phases are remarkably similar to those observed in the well-studied monoclinic M₁ insulating phase of VO₂. As the energy gap is insensitive to the different lattice structures of the three insulating phases, we rule out vanadium-vanadium pairing (the Peierls component) as the dominant contributor to the opening of the gap. Rather, the energy gap arises primarily from intra-atomic Coulomb correlations.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

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

OSTI ID:: 1376670

Report Number(s):: BNL--114002-2017-JA

Journal Information:: Physical Review B, Journal Name: Physical Review B Journal Issue: 7 Vol. 95; ISSN 2469-9950; ISSN PRBMDO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (61)

Observation of insulating-insulating monoclinic structural transition in macro-sized VO2 single crystals Mun, Bongjin Simon; Chen, Kai; Leem, Youngchul physica status solidi (RRL) - Rapid Research Letters, Vol. 5, Issue 3 https://doi.org/10.1002/pssr.201105011	journal	January 2011
Observation of insulating-insulating monoclinic structural transition in macro-sized VO ₂ single crystals [Phys. Status Solidi RRL 5 , No. 3, R107-R109 (2011)] : Observation of insulating-insulating monoclinic structural transition in macro-sized VO2 single crystals [Phys. Status Solidi RRL 5, No. 3, R107-R109 Mun, Bongjin Simon; Chen, Kai; Leem, Youngchul physica status solidi (RRL) - Rapid Research Letters, Vol. 9, Issue 3 https://doi.org/10.1002/pssr.201510046	journal	February 2015
Metal-insulator transitions Paesler, Michael Journal of Non-Crystalline Solids, Vol. 130, Issue 1 https://doi.org/10.1016/0022-3093(91)90162-y	journal	June 1991
Structural aspects of the metal-insulator transitions in V0.985Al0.015O2 Ghedira, M.; Vincent, H.; Marezio, M. Journal of Solid State Chemistry, Vol. 22, Issue 4 https://doi.org/10.1016/0022-4596(77)90020-2	journal	December 1977
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Ultrafast dynamics during the photoinduced phase transition in VO2 Wegkamp, Daniel; Stähler, Julia Progress in Surface Science, Vol. 90, Issue 4 https://doi.org/10.1016/j.progsurf.2015.10.001	journal	December 2015
Extended Mapping and Exploration of the Vanadium Dioxide Stress-Temperature Phase Diagram Cao, J.; Gu, Y.; Fan, W. Nano Letters, Vol. 10, Issue 7 https://doi.org/10.1021/nl101457k	journal	July 2010
Doping-Based Stabilization of the M2 Phase in Free-Standing VO ₂ Nanostructures at Room Temperature Strelcov, Evgheni; Tselev, Alexander; Ivanov, Ilia Nano Letters, Vol. 12, Issue 12 https://doi.org/10.1021/nl303065h	journal	February 2012
Metallization of vanadium dioxide driven by large phonon entropy Budai, John D.; Hong, Jiawang; Manley, Michael E. Nature, Vol. 515, Issue 7528 https://doi.org/10.1038/nature13865	journal	November 2014
Inhomogeneity of the ultrafast insulator-to-metal transition dynamics of VO2 O’Callahan, Brian T.; Jones, Andrew C.; Hyung Park, Jae Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms7849	journal	April 2015
Reducing Dzyaloshinskii-Moriya interaction and field-free spin-orbit torque switching in synthetic antiferromagnets Chen, Ruyi; Cui, Qirui; Liao, Liyang Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-23414-3	journal	May 2021
High-resolution X-ray luminescence extension imaging Ou, Xiangyu; Qin, Xian; Huang, Bolong Nature, Vol. 590, Issue 7846 https://doi.org/10.1038/s41586-021-03251-6	journal	February 2021
Scalable radiative thermal logic gates based on nanoparticle networks Kathmann, Christoph; Reina, Marta; Messina, Riccardo Scientific Reports, Vol. 10, Issue 1 https://doi.org/10.1038/s41598-020-60603-4	journal	February 2020
Resolution limits for infrared microspectroscopy explored with synchrotron radiation Carr, G. L. Review of Scientific Instruments, Vol. 72, Issue 3 https://doi.org/10.1063/1.1347965	journal	January 2001
Hybrid functionals based on a screened Coulomb potential Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias The Journal of Chemical Physics, Vol. 118, Issue 18 https://doi.org/10.1063/1.1564060	journal	May 2003
Erratum: “Hybrid functionals based on a screened Coulomb potential” [J. Chem. Phys. 118, 8207 (2003)] Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias The Journal of Chemical Physics, Vol. 124, Issue 21 https://doi.org/10.1063/1.2204597	journal	June 2006
Physical properties of V _{1− x} Ti _x O ₂ (0 < x < 0.187) single crystals Kong, Tai; Masters, Morgan W.; Bud’ko, Sergey L. APL Materials, Vol. 3, Issue 4 https://doi.org/10.1063/1.4908245	journal	April 2015
Cation disproportionation and pairing in the insulating T phase of V _0.985 Al _0.15 O ₂ Ghedira, M.; Chenavas, J.; Marezio, M. Journal of Physics C: Solid State Physics, Vol. 10, Issue 11 https://doi.org/10.1088/0022-3719/10/11/007	journal	June 1977
Electron spin resonance in V _1-x Cr _x O ₂ D'Haenens, J. P.; Kaplan, D.; Merenda, P. Journal of Physics C: Solid State Physics, Vol. 8, Issue 14 https://doi.org/10.1088/0022-3719/8/14/009	journal	July 1975
Optical properties across the insulator to metal transitions in vanadium oxide compounds Perucchi, A.; Baldassarre, L.; Postorino, P. Journal of Physics: Condensed Matter, Vol. 21, Issue 32 https://doi.org/10.1088/0953-8984/21/32/323202	journal	July 2009
Hybrid functionals applied to perovskites Franchini, Cesare Journal of Physics: Condensed Matter, Vol. 26, Issue 25 https://doi.org/10.1088/0953-8984/26/25/253202	journal	May 2014
Optical Properties of V O 2 between 0.25 and 5 eV Verleur, Hans W.; Barker, A. S.; Berglund, C. N. Physical Review, Vol. 172, Issue 3 https://doi.org/10.1103/PhysRev.172.788	journal	August 1968
Dimerization of a linear Heisenberg chain in the insulating phases of V 1 − x Cr x O 2 Pouget, J. P.; Launois, H.; Rice, T. M. Physical Review B, Vol. 10, Issue 5 https://doi.org/10.1103/PhysRevB.10.1801	journal	September 1974
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Structural Aspects of the Metal-Insulator Transitions in Cr-Doped V O 2 Marezio, M.; McWhan, D. B.; Remeika, J. P. Physical Review B, Vol. 5, Issue 7 https://doi.org/10.1103/PhysRevB.5.2541	journal	April 1972
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Role of electron-electron and electron-phonon interaction effects in the optical conductivity of VO 2 Okazaki, K.; Sugai, S.; Muraoka, Y. Physical Review B, Vol. 73, Issue 16 https://doi.org/10.1103/PhysRevB.73.165116	journal	April 2006
Electrodynamics of the vanadium oxides V O 2 and V 2 O 3 Qazilbash, M. M.; Schafgans, A. A.; Burch, K. S. Physical Review B, Vol. 77, Issue 11 https://doi.org/10.1103/PhysRevB.77.115121	journal	March 2008
Optical properties of V 1 − x Cr x O 2 compounds under high pressure Marini, C.; Arcangeletti, E.; Di Castro, D. Physical Review B, Vol. 77, Issue 23 https://doi.org/10.1103/PhysRevB.77.235111	journal	June 2008
Photoemission evidence for a Mott-Hubbard metal-insulator transition in VO 2 Eguchi, R.; Taguchi, M.; Matsunami, M. Physical Review B, Vol. 78, Issue 7 https://doi.org/10.1103/PhysRevB.78.075115	journal	August 2008
Optical properties of correlated materials: Generalized Peierls approach and its application to VO 2 Tomczak, Jan M.; Biermann, Silke Physical Review B, Vol. 80, Issue 8 https://doi.org/10.1103/PhysRevB.80.085117	journal	August 2009
Nonpercolative metal-insulator transition in VO 2 single crystals Mun, Bongjin Simon; Chen, Kai; Yoon, Joonseok Physical Review B, Vol. 84, Issue 11 https://doi.org/10.1103/PhysRevB.84.113109	journal	September 2011
Screened hybrid functional applied to 3 d 0 → 3 d 8 transition-metal perovskites La M O 3 ( M = Sc–Cu): Influence of the exchange mixing parameter on the structural, electronic, and magnetic properties He, Jiangang; Franchini, Cesare Physical Review B, Vol. 86, Issue 23 https://doi.org/10.1103/PhysRevB.86.235117	journal	December 2012
Temperature dependence of the optical properties of VO 2 deposited on sapphire with different orientations Nazari, M.; Zhao, Y.; Kuryatkov, V. V. Physical Review B, Vol. 87, Issue 3 https://doi.org/10.1103/PhysRevB.87.035142	journal	January 2013
Anisotropic infrared response of vanadium dioxide microcrystals Huffman, T. J.; Xu, Peng; Qazilbash, M. M. Physical Review B, Vol. 87, Issue 11 https://doi.org/10.1103/PhysRevB.87.115121	journal	March 2013
Theoretical unification of hybrid-DFT and DFT + U methods for the treatment of localized orbitals Ivády, Viktor; Armiento, Rickard; Szász, Krisztián Physical Review B, Vol. 90, Issue 3 https://doi.org/10.1103/PhysRevB.90.035146	journal	July 2014
Electron-hole interactions in correlated electron materials: Optical properties of vanadium dioxide from first principles Gatti, Matteo; Sottile, Francesco; Reining, Lucia Physical Review B, Vol. 91, Issue 19 https://doi.org/10.1103/PhysRevB.91.195137	journal	May 2015
Modification of electronic structure in compressively strained vanadium dioxide films Huffman, T. J.; Xu, Peng; Hollingshad, A. J. Physical Review B, Vol. 91, Issue 20 https://doi.org/10.1103/PhysRevB.91.205140	journal	May 2015
Tunneling breakdown of a strongly correlated insulating state in V O 2 induced by intense multiterahertz excitation Mayer, B.; Schmidt, C.; Grupp, A. Physical Review B, Vol. 91, Issue 23 https://doi.org/10.1103/PhysRevB.91.235113	journal	June 2015
Stability of the M2 phase of vanadium dioxide induced by coherent epitaxial strain Quackenbush, N. F.; Paik, H.; Wahila, M. J. Physical Review B, Vol. 94, Issue 8 https://doi.org/10.1103/PhysRevB.94.085105	journal	August 2016
VO 2 : A Novel View from Band Theory Eyert, V. Physical Review Letters, Vol. 107, Issue 1 https://doi.org/10.1103/PhysRevLett.107.016401	journal	June 2011
Vanadium Dioxide: A Peierls-Mott Insulator Stable against Disorder Weber, Cédric; O’Regan, David D.; Hine, Nicholas D. M. Physical Review Letters, Vol. 108, Issue 25 https://doi.org/10.1103/PhysRevLett.108.256402	journal	June 2012
Instantaneous Band Gap Collapse in Photoexcited Monoclinic VO 2 due to Photocarrier Doping Wegkamp, Daniel; Herzog, Marc; Xian, Lede Physical Review Letters, Vol. 113, Issue 21 https://doi.org/10.1103/PhysRevLett.113.216401	journal	November 2014
Computation of the Correlated Metal-Insulator Transition in Vanadium Dioxide from First Principles Zheng, Huihuo; Wagner, Lucas K. Physical Review Letters, Vol. 114, Issue 17 https://doi.org/10.1103/PhysRevLett.114.176401	journal	April 2015
Correlation-Driven Insulator-Metal Transition in Near-Ideal Vanadium Dioxide Films Gray, A. X.; Jeong, J.; Aetukuri, N. P. Physical Review Letters, Vol. 116, Issue 11 https://doi.org/10.1103/PhysRevLett.116.116403	journal	March 2016
Metal-Insulator Transition in VO 2 : A DFT + DMFT Perspective Brito, W. H.; Aguiar, M. C. O.; Haule, K. Physical Review Letters, Vol. 117, Issue 5 https://doi.org/10.1103/PhysRevLett.117.056402	journal	July 2016
Electron Localization Induced by Uniaxial Stress in Pure V O 2 Pouget, J. P.; Launois, H.; D'Haenens, J. P. Physical Review Letters, Vol. 35, Issue 13 https://doi.org/10.1103/PhysRevLett.35.873	journal	September 1975
Comment on "V O 2 : Peierls or Mott-Hubbard? A View from Band Theory" Rice, T. M.; Launois, H.; Pouget, J. P. Physical Review Letters, Vol. 73, Issue 22 https://doi.org/10.1103/PhysRevLett.73.3042	journal	November 1994
Orbital-Assisted Metal-Insulator Transition in VO 2 Haverkort, M. W.; Hu, Z.; Tanaka, A. Physical Review Letters, Vol. 95, Issue 19 https://doi.org/10.1103/PhysRevLett.95.196404	journal	November 2005
Transfer of Spectral Weight and Symmetry across the Metal-Insulator Transition in VO 2 Koethe, T. C.; Hu, Z.; Haverkort, M. W. Physical Review Letters, Vol. 97, Issue 11 https://doi.org/10.1103/PhysRevLett.97.116402	journal	September 2006
Metal-insulator transitions Imada, Masatoshi; Fujimori, Atsushi; Tokura, Yoshinori Reviews of Modern Physics, Vol. 70, Issue 4, p. 1039-1263 https://doi.org/10.1103/RevModPhys.70.1039	journal	October 1998
Electrodynamics of correlated electron materials Basov, D. N.; Averitt, Richard D.; van der Marel, Dirk Reviews of Modern Physics, Vol. 83, Issue 2 https://doi.org/10.1103/RevModPhys.83.471	journal	June 2011
Optical Properties of V O 2 between 0.25 and 5 eV Verleur, Hans W.; Barker, A. S.; Berglund, C. N. Reviews of Modern Physics, Vol. 40, Issue 4 https://doi.org/10.1103/revmodphys.40.737	journal	October 1968
Twinning in Cr-doped VO ₂ Marezio, M.; Dernier, P. D.; Santoro, A. Acta Crystallographica Section A, Vol. 29, Issue 6 https://doi.org/10.1107/S0567739473001592	journal	November 1973
Mott Transition in VO2 Revealed by Infrared Spectroscopy and Nano-Imaging Qazilbash, M. M.; Brehm, M.; Chae, B. -G. Science, Vol. 318, Issue 5857 https://doi.org/10.1126/science.1150124	journal	December 2007
A photoinduced metal-like phase of monoclinic VO ₂ revealed by ultrafast electron diffraction Morrison, Vance R.; Chatelain, Robert. P.; Tiwari, Kunal L. Science, Vol. 346, Issue 6208 https://doi.org/10.1126/science.1253779	journal	October 2014
Inhomogeneity of the ultrafast insulator-to-metal transition dynamics of VO2 T., O'Callahan, Brian; Jae, Hyung Park,; H., Cobden, David The University of North Carolina at Chapel Hill University Libraries https://doi.org/10.17615/9cck-6p65	text	January 2015
Mott transition in VO2 revealed by infrared spectroscopy and nano-imaging Qazilbash, M. M.; Brehm, M.; Chae, Byung-Gyu arXiv https://doi.org/10.48550/arxiv.0801.1171	text	January 2008
Computation of the correlated metal-insulator transition in vanadium dioxide from first principles Zheng, Huihuo; Wagner, Lucas K. arXiv https://doi.org/10.48550/arxiv.1310.1066	text	January 2013
Theoretical unification of hybrid-DFT and DFT+U methods for the treatment of localized orbitals Ivády, Viktor; Armiento, Rickard; Szász, Krisztián arXiv https://doi.org/10.48550/arxiv.1406.2944	text	January 2014

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Microscopic nature of the asymmetric hysteresis in the insulator-metal transition of VO ₂ revealed by spectroscopic ellipsometry Voloshenko, Ievgen; Kuhl, Florian; Gompf, Bruno Applied Physics Letters, Vol. 113, Issue 20 https://doi.org/10.1063/1.5055296	journal	November 2018
How optical excitation controls the structure and properties of vanadium dioxide Otto, Martin R.; René de Cotret, Laurent P.; Valverde-Chavez, David A. Proceedings of the National Academy of Sciences, Vol. 116, Issue 2 https://doi.org/10.1073/pnas.1808414115	journal	December 2018
Ultrafast response of photoexcited carriers in VO ₂ at high-pressure Braun, Johannes M.; Schneider, Harald; Helm, Manfred New Journal of Physics, Vol. 20, Issue 8 https://doi.org/10.1088/1367-2630/aad4ef	journal	August 2018
Insulator-metal transitions in the T phase Cr-doped and M 1 phase undoped VO 2 thin films Majid, S. S.; Shukla, D. K.; Rahman, F. Physical Review B, Vol. 98, Issue 7 https://doi.org/10.1103/physrevb.98.075152	journal	August 2018
Electronic structure of metallic and insulating phases of vanadium dioxide and its oxide alloys Lu, Haichang; Guo, Yuzheng; Robertson, John Physical Review Materials, Vol. 3, Issue 9 https://doi.org/10.1103/physrevmaterials.3.094603	journal	September 2019
Modification of the Properties of Vanadium Oxide Thin Films by Plasma-Immersion Ion Implantation Burdyukh, Sergey; Berezina, Olga; Pergament, Alexander Advances in Condensed Matter Physics, Vol. 2018 https://doi.org/10.1155/2018/9789370	journal	January 2018
Electronic structure of metallic and insulating phases of vanadium dioxide and its oxide alloys Lu, Haichang; Guo, Yuzheng; Robertson, John American Physical Society (APS) https://doi.org/10.17863/cam.45834	journalarticle	January 2019
How optical excitation controls the structure and properties of vanadium dioxide Otto, Martin R.; de Cotret, Laurent P. René; Valverde-Chavez, David A. arXiv https://doi.org/10.48550/arxiv.1805.01430	text	January 2018

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