Ultrafast Charge Carrier Dynamics in Vanadium Dioxide, VO2: Nonequilibrium Contributions to the Photoinduced Phase Transitions

band gap (0.6-0.92 eV), we note that numerous optical features do not correspond to the first-order phase transition. Previous studies indeed induced such a phase transition, but they relied on fluences at least an order of magnitude higher, leading to temperature increases well above the transition threshold (340 K). Instead, for excitation fluences that correspond to lattice temperatures only in slight excess of the phase transition (absolute temperatures < 500 K), we find that the marked changes in optical properties are dominated by a shift in the electronic density of states/Fermi level. We find that this effect is a lattice-driven process and does not occur until sufficient energy has been transferred from the excited electrons into the phonon subsystem.