Switching speed limits in electrically driven VO2 structural Mott–Peierls transition

Mott materials are archetypal quantum systems actively explored as next-generation electronic and photonic platforms, with potential applications spanning non-Von Neumann computing, robotics, energy storage, and microwave technologies. Among these, vanadium dioxide (VO₂) has emerged as one of the most intensively studied compounds, owing to its sharp, near-room-temperature insulator-to-metal phase transition. VO₂ also serves as a benchmark system for testing cutting-edge theories and experimental techniques. Here, we directly visualize the electrically driven transition dynamics in VO₂ using a microwave-driven, frequency-tunable pulsed transmission electron microscope that combines nanometer spatial and picosecond temporal resolution. Under high-frequency (MHz-GHz) excitation, we capture the ultrafast nucleation, propagation, and dissolution of metallic domains within an operating device over millions of reversible cycles. We observe the ultrafast formation of consistent metallic nuclei beneath the electrodes, followed by the propagation of a structural phase front at 4.54 nm/ns. Our experiments show that phonon-mediated structural recovery ultimately limits reversible switching of VO₂ at GHz frequencies, and that a tunable regime for reversible operation spans from kHz to GHz through device engineering. Beyond VO₂, our approach provides a powerful framework for probing non-equilibrium structural transformations in correlated and functional materials under realistic electrical stimuli.