S. Ito, M. Schüler, M. Meierhofer, S. Schlauderer, J. Freudenstein, J. Reimann, D. Afanasiev, K. A. Kokh, O. E. Tereshchenko, J. Güdde, M. A. Sentef, U. Höfer & R. Huber

Nature  616, 696–701 (2023)

Strong light fields have created opportunities to tailor novel functionalities of solids. Floquet–Bloch states can form under periodic driving of electrons and enable exotic quantum phases. On subcycle timescales, lightwaves can simultaneously drive intraband currents and interband transitions, which enable high-harmonic generation and pave the way towards ultrafast electronics. Yet, the interplay of intraband and interband excitations and their relation to Floquet physics have been key open questions as dynamical aspects of Floquet states have remained elusive. Here we provide this link by visualizing the ultrafast build-up of Floquet–Bloch bands with time-resolved and angle-resolved photoemission spectroscopy. We drive surface states on a topological insulator with mid-infrared fields—strong enough for high-harmonic generation—and directly monitor the transient band structure with subcycle time resolution. Starting with strong intraband currents, we observe how Floquet sidebands emerge within a single optical cycle; intraband acceleration simultaneously proceeds in multiple sidebands until high-energy electrons scatter into bulk states and dissipation destroys the Floquet bands. Quantum non-equilibrium calculations explain the simultaneous occurrence of Floquet states with intraband and interband dynamics. Our joint experiment and theory study provides a direct time-domain view of Floquet physics and explores the fundamental frontiers of ultrafast band-structure engineering.