Instantaneous Band Gap Collapse in Photoexcited Monoclinic VO2 due to 
Photocarrier Doping

Wegkamp, Daniel; Herzog, Marc; Xian, Lede; Gatti, Matteo; Cudazzo, Pierluigi; McGahan, Christina L.; Marvel, Robert E.; Haglund, Richard F.; Rubio, Angel; Wolf, Martin; Stähler, Julia

doi:10.1103/PhysRevLett.113.216401

Item

ITEM ACTIONSEXPORT

Add to Basket

Local TagsRelease HistoryDetailsSummary

Released

Journal Article

Instantaneous Band Gap Collapse in Photoexcited Monoclinic VO₂ due to Photocarrier Doping

MPS-Authors

/persons/resource/persons22225

Wegkamp, Daniel
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons81237

Herzog, Marc
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22028

Rubio, Angel
Nano-Bio Spectroscopy group, Universidad del País Vasco CFM CSIC-UPV/EHU-MPC & DIPC;
European Theoretical Spectroscopy Facility (ETSF);
Theory, Fritz Haber Institute, Max Planck Society;
Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;

/persons/resource/persons22250

Wolf, Martin
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22128

Stähler, Julia
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

External Resource

http://dx.doi.org/10.1103/PhysRevLett.113.216401
(Publisher version)

http://arxiv.org/abs/1408.3209
(Preprint)

Fulltext (restricted access)

There are currently no full texts shared for your IP range.

Fulltext (public)

1408.3209.pdf
(Preprint), 637KB

Supplementary Material (public)

There is no public supplementary material available

Citation

Wegkamp, D., Herzog, M., Xian, L., Gatti, M., Cudazzo, P., McGahan, C. L., et al. (2014). Instantaneous Band Gap Collapse in Photoexcited Monoclinic VO₂ due to Photocarrier Doping. Physical Review Letters, 113(21): 216401. doi:10.1103/PhysRevLett.113.216401.

Cite as: https://hdl.handle.net/11858/00-001M-0000-0024-B307-6

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.