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

Daniel Wegkamp, Marc Herzog, Lede Xian, Matteo Gatti, Pierluigi Cudazzo, Christina L. McGahan, Robert E. Marvel, Richard F. Haglund, Jr., Angel Rubio, Martin Wolf, and Julia Stähler
Phys. Rev. Lett. 113, 216401 – Published 17 November 2014
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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.

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  • Received 15 July 2014

DOI:https://doi.org/10.1103/PhysRevLett.113.216401

© 2014 American Physical Society

Authors & Affiliations

Daniel Wegkamp1, Marc Herzog1, Lede Xian2,3, Matteo Gatti4,3,5, Pierluigi Cudazzo2,3, Christina L. McGahan6, Robert E. Marvel6, Richard F. Haglund, Jr.6, Angel Rubio2,7,3,1, Martin Wolf1, and Julia Stähler1,*

  • 1Fritz-Haber-Institut der Max-Planck-Gesellschaft, Abteilung Physikalische Chemie, Faradayweg 4-6, 14195 Berlin, Germany
  • 2Nano-Bio Spectroscopy group, Universidad del País Vasco CFM CSIC-UPV/EHU-MPC & DIPC, 20018 San Sebastián, Spain
  • 3European Theoretical Spectroscopy Facility (ETSF)
  • 4Laboratoire des Solides Irradiés, École Polytechnique, CNRS-CEA/DSM, F-91128 Palaiseau, France
  • 5Synchrotron SOLEIL, L’Orme des Merisiers, Saint-Aubin, BP 48, F-91192 Gif-sur-Yvette, France
  • 6Department of Physics and Astronomy and Interdisciplinary Materials Science Program, Vanderbilt University, Nashville, Tennessee 37235-1807, USA
  • 7Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, 22761 Hamburg, Germany

  • *staehler@fhi-berlin.mpg.de

See Also

Direct Observation of Decoupled Structural and Electronic Transitions and an Ambient Pressure Monocliniclike Metallic Phase of VO2

J. Laverock, S. Kittiwatanakul, A. A. Zakharov, Y. R. Niu, B. Chen, S. A. Wolf, J. W. Lu, and K. E. Smith
Phys. Rev. Lett. 113, 216402 (2014)

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Vol. 113, Iss. 21 — 21 November 2014

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