Decoupled few-femtosecond phase transitions in vanadium dioxide

Christian Brahms (), Lin Zhang, Xiao Shen, Utso Bhattacharya, Maria Recasens, Johann Osmond, Tobias Grass, Ravindra W. Chhajlany, Kent A. Hallman, Richard F. Haglund, Sokrates T. Pantelides, Maciej Lewenstein, John C. Travers and Allan S. Johnson ()
Additional contact information
Christian Brahms: Heriot-Watt University
Lin Zhang: The Barcelona Institute of Science and Technology
Xiao Shen: University of Memphis
Utso Bhattacharya: The Barcelona Institute of Science and Technology
Maria Recasens: The Barcelona Institute of Science and Technology
Johann Osmond: The Barcelona Institute of Science and Technology
Tobias Grass: DIPC - Donostia International Physics Center
Ravindra W. Chhajlany: Adam Mickiewicz University
Kent A. Hallman: Vanderbilt University
Richard F. Haglund: Vanderbilt University
Sokrates T. Pantelides: Vanderbilt University
Maciej Lewenstein: The Barcelona Institute of Science and Technology
John C. Travers: Heriot-Watt University
Allan S. Johnson: IMDEA Nanoscience

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract The nature of the insulator-to-metal phase transition in vanadium dioxide (VO2) is one of the longest-standing problems in condensed-matter physics. Ultrafast spectroscopy has long promised to determine whether the transition is primarily driven by the electronic or structural degree of freedom, but measurements to date have been stymied by their sensitivity to only one of these components and/or their limited temporal resolution. Here we use ultra-broadband few-femtosecond pump-probe spectroscopy to resolve the electronic and structural phase transitions in VO2 at their fundamental time scales. Our experiments show that the system transforms into a bad-metallic phase within 10 fs after photoexcitation, but requires another 100 fs to complete the transition, during which we observe electronic oscillations and a partial re-opening of the bandgap, signalling a transient semi-metallic state. Comparisons with tensor-network simulations and density-functional theory calculations show these features result from an unexpectedly fast structural transition, in which the vanadium dimers separate and untwist with two different timescales. Our results resolve the structural and electronic nature of the light-induced phase transition in VO2 and establish ultra-broadband few-femtosecond spectroscopy as a powerful tool for studying quantum materials out of equilibrium.

Date: 2025
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DOI: 10.1038/s41467-025-58895-z

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