Basic aspects of the metal–insulator transition in vanadium dioxide VO$_{2}$: a critical review

Jean-Paul Pouget

doi:10.5802/crphys.74

Article de recherche

Basic aspects of the metal–insulator transition in vanadium dioxide VO

_{2}

: a critical review
[Aspects principaux de la transition métal–isolant du dioxyde de vanadium VO

_{2}

: une revue critique]

Jean-Paul Pouget ¹

¹ Laboratoire de physique des solides, CNRS UMR 8502, Université Paris-Sud, Université Paris-Saclay, 91405 Orsay, France

Comptes Rendus. Physique, Volume 22 (2021) no. 1, pp. 37-87.

Abstract (VO)
Résumé

Vanadium dioxide exhibits a first order metal to insulator transition (MIT) at 340 K ( $T_{MI}$ ) from a rutile (R) structure to a monoclinic ( $M_{1}$ ) structure. The mechanism of this transition interpreted as due either to a Peierls instability or to a Mott–Hubbard instability is controversial since half a century. However, in the last twenty years the study of chemical and physical properties of ${VO}_{2}$ and of its alloys, benefits of a renewed interest due to possible applications coming from the realization of devices made of thin films. We describe in this review the structural, electronic and magnetic properties of the different metallic (R) and insulating ( $M_{1}$ , T, $M_{2}$ ) phases of ${VO}_{2}$ , of its solid solutions and under constraint. We present in a synthetic manner the various phase diagrams and their symmetry analysis. This work allows us to revisit older interpretation and to emphasize in particular the combined role of electron–electron interactions in the various phase of ${VO}_{2}$ and of structural fluctuations in the MIT mechanism. In this framework we show that the phase transition is surprisingly announced by anisotropic one-dimensional (1D) structural fluctuations revealing chain like correlations between the V due to an incipient instability of the rutile structure. This leads to an unexpected critical dynamics of the order–disorder (or relaxation) type. We describe how the two-dimensional (2D) coupling between these 1D fluctuations, locally forming uniform $V^{4 +}$ zig-zag chains and V–V pairs, stabilizes the $M_{2}$ and $M_{1}$ insulating phases. These phases exhibit a 1D electronic anisotropy where substantial electron–electron correlations conduct to a spin–charge decoupling. The spin-Peierls ground state of $M_{1}$ is analyzed via a mechanism of dimerization, in the T phase, of the spin 1/2 $V^{4 +}$ zig-zag Heisenberg chains formed in the $M_{2}$ phase. This review summarizes in a critical manner the main results of the large literature on fundamental aspects of the MIT of ${VO}_{2}$ . It is completed by unpublished old results. Interpretations are also placed in a large conceptual frame which is also relevant to interpret physical properties of other classes of materials.

Le dioxyde de vanadium présente une transition métal–isolant (TMI) du premier ordre à 340 K ( $= T_{MI}$ ) d’une structure rutile (R) à une structure monoclinique ( $M_{1}$ ). Le mécanisme de cette transition interprétée comme étant due soit à une instabilité de Peierls soit à une instabilité de Mott–Hubbard reste très controversé depuis près d’un demi-siècle. Cependant depuis une vingtaine d’années l’étude des propriétés chimiques et physiques de ${VO}_{2}$ et de ses alliages suscite un renouveau d’intérêt par la possibilité d’applications provenant de l’obtention de dispositifs s’appuyant sur la réalisation de films minces. Nous décrivons dans cette revue les propriétés structurales, électroniques et magnétiques des différentes phases métallique (R) et isolantes ( $M_{1}$ , T et $M_{2}$ ) de ${VO}_{2}$ , de ses solutions solides et des modifications sous contrainte. Nous présentons de façon synthétique les divers diagrammes de phase et leur analyse par symétrie. Ce travail conduit à relativiser certaines interprétations du passé et à souligner en particulier le rôle particulièrement important des interactions électron–électron dans les différentes phases de ${VO}_{2}$ et des fluctuations structurales dans le mécanisme de la TMI. Dans ce cadre nous montrons que la transition de phase est annoncée de façon surprenante par des corrélations structurales d’anisotropie unidimensionnelle (1D) révélant un ordre local en chaine du V issu d’une instabilité sous-jacente de la structure rutile. A celles-ci correspond une dynamique critique inattendue de type relaxation (ou ordre-désordre). Nous décrivons comment le couplage bidimensionnel (2D) de ces fluctuations 1D forme localement des chaines zig-zag de $V^{4 +}$ et des paires V–V, conduisant aux phases isolantes $M_{2}$ et $M_{1}$ . Ces phases présentent une forte anisotropie électronique avec de substantielles corrélations électron–électron conduisant à un découplage spin–charge. Le fondamental de type spin-Peierls de la phase $M_{1}$ est analysé à partir d’un mécanisme de dimérisation, en phase T, des chaines d’Heisenberg de spin 1/2 formées par les zig-zags de $V^{4 +}$ dans la phase $M_{2}$ . Cette revue résume de façon critique les résultats principaux de l’abondante littérature concernant les aspects fondamentaux de la TMI de ${VO}_{2}$ . Elle est complétée par d’anciens résultats jamais publiés. Les interprétations proposées se placent dans un cadre conceptuel relativement large se révélant pertinent pour l’interprétation des propriétés physiques d’autres classes de matériaux.

Reçu le : 2020-11-28
Révisé le : 2021-02-25
Accepté le : 2021-04-20
Publié le : 2021-06-11

DOI : 10.5802/crphys.74

Keywords: Vanadium dioxide, Metal–insulator transition, Mott–Hubbard charge localization, Spin-Peierls and Peierls transitions, Chain-like structural instability, Electron–phonon coupling
Mots-clés : Dioxyde de vanadium, Transition métal–isolant, Localisation de charge de Mott–Hubbard, Transitions de Peierls et de spin-Peierls, Instabilités structurales corrélées à une dimension, Couplage électron–phonon

Affiliations des auteurs :

Jean-Paul Pouget ¹

¹ Laboratoire de physique des solides, CNRS UMR 8502, Université Paris-Sud, Université Paris-Saclay, 91405 Orsay, France

Licence :

CC-BY 4.0

Droits d'auteur : Les auteurs conservent leurs droits

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Jean-Paul Pouget. Basic aspects of the metal–insulator transition in vanadium dioxide VO$_{2}$: a critical review. Comptes Rendus. Physique, Volume 22 (2021) no. 1, pp. 37-87. doi : 10.5802/crphys.74. https://comptes-rendus.academie-sciences.fr/physique/articles/10.5802/crphys.74/

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Zhuoqun Fang; Alexandre Zimmers; Ke Li; Dongjiu Zhang; Tianyu Lan; Baoquan Sun; Laurent Billot; Lionel Aigouy; Zhuoying Chen Hybrid Plasmonic Nanorods/VO2 Photodetectors Sensitive to Short‐Wave Infrared Photons with Fast Response, Advanced Electronic Materials (2025) | DOI:10.1002/aelm.202500172
Larisa Patlagan; George M. Reisner; Bertina Fisher Revealing Resistive Switching of Phase Transitions in an Al‐Doped Single Crystal of VO2 by DC and Pulsed Electrical Measurements, Advanced Physics Research, Volume 4 (2025) no. 2 | DOI:10.1002/apxr.202400112
Feng-Wu Guo; Wen-Hao Liu; Zhi Wang; Shu-Shen Li; Lin-Wang Wang; Jun-Wei Luo Photoinduced hidden monoclinic metallic phase of VO2 driven by local nucleation, Nature Communications, Volume 16 (2025) no. 1 | DOI:10.1038/s41467-024-55760-3
Achyut Tiwari; Bruno Gompf; Savita Priya; Dieter Schweitzer; Reizo Kato; Koichi Hiraki; Martin Dressel Nature of electronic phase transitions in substituted α−(BEDT−TTF)2I3 studied by generalized ellipsometry, Physical Review B, Volume 111 (2025) no. 19 | DOI:10.1103/physrevb.111.195142
Swayam Prakash Sahoo; Matthieu Bugnet; Ingrid Cañero Infante; Victor Pierron; Laurence Méchin; Rebecca Cervasio; Pierre Hemme; Jean‐Blaise Brubach; Pascale Roy; Luc G. Fréchette; Anne D. Lamirand; Bertrand Vilquin Low Hysteresis Vanadium Dioxide Integrated on Silicon Using Complementary Metal‐Oxide Semiconductor Compatible Oxide Buffer Layer, Small Science, Volume 5 (2025) no. 2 | DOI:10.1002/smsc.202400398
Mansoor A. Najeeb; Ahmed H. Mokhtar; David A. Serban; Daniel G. Porter; Stephen Collins; Alessandro Bombardi; Marcus C. Newton Three‐Dimensional Imaging of the Structural Phase Transition in a Single Vanadium Dioxide Nanocrystal, physica status solidi (a), Volume 222 (2025) no. 3 | DOI:10.1002/pssa.202400503
Masoud Ahmadi; Atul Atul; Sytze de Graaf; Ewout van der Veer; Ansgar Meise; Amir Hossein Tavabi; Marc Heggen; Rafal E. Dunin-Borkowski; Majid Ahmadi; Bart J. Kooi Atomically Resolved Phase Coexistence in VO2 Thin Films, ACS Nano, Volume 18 (2024) no. 21, p. 13496 | DOI:10.1021/acsnano.3c10745
Xuanchi Zhou; Haifan Li; Yongjie Jiao; Guowei Zhou; Huihui Ji; Yong Jiang; Xiaohong Xu Hydrogen‐Associated Multiple Electronic Phase Transitions for d‐Orbital Transitional Metal Oxides: Progress, Application, and Beyond, Advanced Functional Materials, Volume 34 (2024) no. 28 | DOI:10.1002/adfm.202316536
A.J. Santos; N. Martin; J.J. Jiménez; R. García; F.M. Morales Enhancing luminous transmittance and hysteresis width of VO2-based thermochromic coatings by combining GLAD and RGPP approaches, Construction and Building Materials, Volume 419 (2024), p. 135472 | DOI:10.1016/j.conbuildmat.2024.135472
Andrzej Grzechnik; B. Viliam Hakala; Sophia Kurig; Nicolas Walte; Noriyoshi Tsujino; Sho Kakizawa; Yuji Higo; Dejan Zagorac; Jelena Zagorac; Richard Dronskowski; J. Christian Schön; Karen Friese Structures, Phase Stability, Amorphization, and Decomposition of V6O13 at High Pressures and Temperatures: Synthesis of Rutile-Related V0.92O2, Crystal Growth Design, Volume 24 (2024) no. 13, p. 5582 | DOI:10.1021/acs.cgd.4c00363
Florian Kuhl; Hao Lu; Martin Becker; Limei Chen; Yonghui Zheng; Angelika Polity; Zaoli Zhang; Yunbin He; Peter J. Klar Raman scattering of TixV1‐xO2 thin films on (110) rutile TiO2 in the low and high temperature phase adjacent to the metal–insulator transition, Journal of Raman Spectroscopy, Volume 55 (2024) no. 8, p. 923 | DOI:10.1002/jrs.6684
Mahmoud Darwish; Yana Zhabura; László Pohl Recent Advances of VO2 in Sensors and Actuators, Nanomaterials, Volume 14 (2024) no. 7, p. 582 | DOI:10.3390/nano14070582
L. Patlagan; G. M. Reisner; B. Fisher Two insulator-insulator transitions in Al-doped VO 2 single crystals, Phase Transitions, Volume 97 (2024) no. 11-12, p. 780 | DOI:10.1080/01411594.2024.2445670
Akash Kumar Singh; H K Singh; P K Siwach Effect of Ar pressure on phase transition characteristics and charge transport mechanism in VO2 films grown by RF sputtering of V2O5, Physica Scripta, Volume 99 (2024) no. 5, p. 055939 | DOI:10.1088/1402-4896/ad3692
Shunsuke Kitou; Akitoshi Nakano; Masato Imaizumi; Yuiga Nakamura; Ichiro Terasaki; Taka-hisa Arima Molecular orbital formation and metastable short-range ordered structure in VO2, Physical Review B, Volume 109 (2024) no. 10 | DOI:10.1103/physrevb.109.l100101
Carl Willem Rischau; Artem Korshunov; Volodymyr Multian; Sara A. Lopez-Paz; Chubin Huang; Lucia Varbaro; Jérémie Teyssier; Yoav Kalcheim; Stefano Gariglio; Alexei Bosak; Jean-Marc Triscone; Javier del Valle Anomalous temperature dependence of phonon lifetimes in metallic VO2, Physical Review B, Volume 109 (2024) no. 9 | DOI:10.1103/physrevb.109.094122
Peter Mlkvik; Maximilian E. Merkel; Nicola A. Spaldin; Claude Ederer Single-site DFT+DMFT for vanadium dioxide using bond-centered orbitals, Physical Review Research, Volume 6 (2024) no. 3 | DOI:10.1103/physrevresearch.6.033122
Jean-Paul Pouget; Enric Canadell Structural approach to charge density waves in low-dimensional systems: electronic instability and chemical bonding, Reports on Progress in Physics, Volume 87 (2024) no. 2, p. 026501 | DOI:10.1088/1361-6633/ad124f
Yubo Zhang; Da Ke; Junxiong Wu; Chutong Zhang; Lin Hou; Baichen Lin; Zuhuang Chen; John P. Perdew; Jianwei Sun Challenges for density functional theory in simulating metal–metal singlet bonding: A case study of dimerized VO2, The Journal of Chemical Physics, Volume 160 (2024) no. 13 | DOI:10.1063/5.0180315
Yuta Ochiai; Masami Kawahara; Tsuyoshi Samura; Takashi Tachiki; Takashi Uchida Evaluation of V₁_-xCr_xO₂ Thin Films Fabricated by MOD, IEEJ Transactions on Fundamentals and Materials, Volume 143 (2023) no. 3, p. 91 | DOI:10.1541/ieejfms.143.91
Haitao Zong; Shiqi Zhang; Linyan Bian; Houchang Chen; Zhiguo Liu; Bai Sun; Wentao Qiao; Lingling Yan; Qiang Hu; Ming Li Preparation and characterization of VO2/Cu-Zr NPs/VO2 composite films with enhanced thermochromic properties, Journal of Alloys and Compounds, Volume 967 (2023), p. 171654 | DOI:10.1016/j.jallcom.2023.171654
Larisa Patlagan; Idan Sthzeglowski; George M. Reisner; Bertina Fisher Non-thermal to thermal electric field effects induced by DC and current pulses in pure and doped VO2 single crystals, Journal of Applied Physics, Volume 133 (2023) no. 23 | DOI:10.1063/5.0142659
Elena Solana-Madruga; Olivier Mentré; Eugenia P. Arévalo-López; Dmitry Khalyavin; Francois Fauth; Alexandr Missiul; Angel M. Arévalo-López High-pressure ilmenite-type MnVO3: crystal and spin structures in the itinerant-localized regimes, Journal of Materials Chemistry C, Volume 11 (2023) no. 27, p. 9238 | DOI:10.1039/d3tc01541f
P. Bouvier; L. Bussmann; D. Machon; I. Breslavetz; G. Garbarino; P. Strobel; V. Dmitriev VO2 under hydrostatic pressure: Isostructural phase transition close to a critical endpoint, Physical Review B, Volume 108 (2023) no. 14 | DOI:10.1103/physrevb.108.144106
Sergio Conejeros; Pere Alemany; Enric Canadell Insulator-to-metal transition in low-dimensional NbS3 under pressure, Physical Review B, Volume 108 (2023) no. 21 | DOI:10.1103/physrevb.108.214109
Berenike Stahl; Thomas Bredow Exploiting Phase Transitions in Catalysis: Adsorption of CO on doped VO2‐Polymorphs, ChemPhysChem, Volume 23 (2022) no. 20 | DOI:10.1002/cphc.202200131
Yasuhiro H. Matsuda; Yuji Muraoka; Daisuke Nakamura; Akihiko Ikeda; Yuto Ishii; Xu-Guang Zhou; Hironobu Sawabe; Shojiro Takeyama Magnetic-Field-Induced Insulator Metal Transition of W-doped VO2 Observed by Electromagnetic Flux Compression at ISSP, Journal of the Physical Society of Japan, Volume 91 (2022) no. 10 | DOI:10.7566/jpsj.91.101008
Jinshi Zhao; Danke Chen; Chenyang Hao; Wei Mi; Liwei Zhou The optimization and role of Ti surface doping in thermochromic VO2 film, Optical Materials, Volume 133 (2022), p. 112960 | DOI:10.1016/j.optmat.2022.112960
Peter Mlkvik; Claude Ederer; Nicola A. Spaldin Influence of germanium substitution on the structural and electronic stability of the competing vanadium dioxide phases, Physical Review Research, Volume 4 (2022) no. 4 | DOI:10.1103/physrevresearch.4.043129
Hao-Wen Liu; Wen-Hao Liu; Zhao-Jun Suo; Zhi Wang; Jun-Wei Luo; Shu-Shen Li; Lin-Wang Wang Unifying the order and disorder dynamics in photoexcited VO2, Proceedings of the National Academy of Sciences, Volume 119 (2022) no. 28 | DOI:10.1073/pnas.2122534119
Haitao Zong; Jiangbin Wu; Daiqi Zhou; Yuehong Yin; Lingling Yan; Ming Li; Wentao Qiao; Qiang Hu; Yuanjun Yang Realization of high luminous transmittance and solar modulation ability of VO2 films by multistep deposition and in-situ annealing method, Surfaces and Interfaces, Volume 30 (2022), p. 101882 | DOI:10.1016/j.surfin.2022.101882
Top B. Rawot Chhetri; Tyra C. Douglas; Matthew A. Davenport; Stephan Rosenkranz; Raymond Osborn; Matthew J. Krogstad; Jared M. Allred Geometric Frustration Suppresses Long-Range Structural Distortions in NbxV1–xO2, The Journal of Physical Chemistry C, Volume 126 (2022) no. 4, p. 2049 | DOI:10.1021/acs.jpcc.1c08392
Laura Rodríguez; Felip Sandiumenge; Carles Frontera; José Manuel Caicedo; Jessica Padilla; Gustau Catalán; José Santiso Strong strain gradients and phase coexistence at the metal-insulator transition in VO2 epitaxial films, Acta Materialia, Volume 220 (2021), p. 117336 | DOI:10.1016/j.actamat.2021.117336
Bogdan Guster; Miguel Pruneda; Pablo Ordejón; Enric Canadell; Jean-Paul Pouget Basic aspects of the charge density wave instability of transition metal trichalcogenides NbSe3 and monoclinic-TaS3, Journal of Physics: Condensed Matter, Volume 33 (2021) no. 48, p. 485401 | DOI:10.1088/1361-648x/ac238a
A.J. Santos; B. Lacroix; M. Domínguez; R. García; N. Martin; F.M. Morales Controlled grain-size thermochromic VO2 coatings by the fast oxidation of sputtered vanadium or vanadium oxide films deposited at glancing angles, Surfaces and Interfaces, Volume 27 (2021), p. 101581 | DOI:10.1016/j.surfin.2021.101581

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