Instantaneous band gap collapse in photoexcited monoclinic VO2 due to photocarrier doping

Phys Rev Lett. 2014 Nov 21;113(21):216401. doi: 10.1103/PhysRevLett.113.216401. Epub 2014 Nov 17.

Abstract

Using femtosecond time-resolved photoelectron spectroscopy we demonstrate that photoexcitation transforms monoclinic VO2 quasi-instantaneously into a metal. Thereby, we exclude an 80 fs structural bottleneck for the photoinduced electronic phase transition of VO2. First-principles many-body perturbation theory calculations reveal a high sensitivity of the VO2 band gap to variations of the dynamically screened Coulomb interaction, supporting a fully electronically driven isostructural insulator-to-metal transition. We thus conclude that the ultrafast band structure renormalization is caused by photoexcitation of carriers from localized V 3d valence states, strongly changing the screening before significant hot-carrier relaxation or ionic motion has occurred.

Publication types

  • Research Support, Non-U.S. Gov't
  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Models, Chemical*
  • Oxides / chemistry*
  • Phase Transition
  • Photochemical Processes
  • Photoelectron Spectroscopy / methods
  • Vanadium Compounds / chemistry*

Substances

  • Oxides
  • Vanadium Compounds
  • vanadium dioxide