Evidence for a structurally-driven insulator-to-metal transition in VO2: A view from the ultrafast timescale

We apply ultrafast spectroscopy to establish a time-domain hierarchy between structural and electronic effects in a strongly correlated electron system. We discuss the case of the model system VO2, a prototypical nonmagnetic compound that exhibits cell doubling, charge localization, and a metal-insulator transition below 340 K. We initiate the formation of the metallic phase by prompt hole photo-doping into the valence band of the low-T insulator. The insulator-to-metal transition is, however, delayed with respect to hole injection, exhibiting a bottleneck time scale, associated with the phonon connecting the two crystallographic phases. This structural bottleneck is observed despite faster depletion of the d bands and is indicative of important bandlike character for this controversial insulator.