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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 VO<jats:sub>2</jats:sub> 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 VO<jats:sub>2</jats:sub> and establish ultra-broadband few-femtosecond spectroscopy as a powerful tool for studying quantum materials out of equilibrium.</jats:p>"],"publicationDate":"2025-04-19","publisher":"Springer Science and Business Media LLC","embargoEndDate":"2025-05-02","sources":["Crossref","Nat Commun","reponame:Repositorio Institucional del Instituto Madrileño de Estudios Avanzados en Nanociencia","instname:Instituto Madrileño de Estudios Avanzados en Nanociencia (IMDEA Nanociencia)","Nature Communications, Vol 16, Iss 1, Pp 1-10 (2025)","Nature Communications, 16 (1)","arXiv - under review at Nature Physics","arXiv.org"],"formats":["application/pdf","application/application/pdf"],"contributors":["000000041762408X","School of Engineering and Physical Sciences, Heriot-Watt University, Edinburgh, United Kingdom; ICFO - Institut de Ciencies Fotoniques, The Barcelona Institute of 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