Ultrafast Triggering of Insulator-Metal Transition in Two-Dimensional VSe2

Deepnarayan Biswas, Alfred J.H. Jones, Paulina Majchrzak, Byoung Ki Choi, Tsung Han Lee, Klara Volckaert, Jiagui Feng, Igor Marković, Federico Andreatta, Chang Jong Kang, Hyuk Jin Kim, In Hak Lee, Chris Jozwiak, Eli Rotenberg, Aaron Bostwick, Charlotte E. Sanders, Yu Zhang, Gabriel Karras, Richard T. Chapman, Adam S. WyattEmma Springate, Jill A. Miwa, Philip Hofmann, Phil D.C. King, Young Jun Chang, Nicola Lanatà, Søren Ulstrup*

*Corresponding author for this work

Research output: Contribution to journalLetterpeer-review

9 Citations (Scopus)

Abstract

The transition-metal dichalcogenide VSe2 exhibits an increased charge density wave transition temperature and an emerging insulating phase when thinned to a single layer. Here, we investigate the interplay of electronic and lattice degrees of freedom that underpin these phases in single-layer VSe2 using ultrafast pump-probe photoemission spectroscopy. In the insulating state, we observe a light-induced closure of the energy gap, which we disentangle from the ensuing hot carrier dynamics by fitting a model spectral function to the time-dependent photoemission intensity. This procedure leads to an estimated time scale of 480 fs for the closure of the gap, which suggests that the phase transition in single-layer VSe2 is driven by electron-lattice interactions rather than by Mott-like electronic effects. The ultrafast optical switching of these interactions in SL VSe2 demonstrates the potential for controlling phase transitions in 2D materials with light.

Original languageEnglish
Pages (from-to)1968-1975
Number of pages8
JournalNano Letters
Volume21
Issue number5
Early online date18 Feb 2021
DOIs
Publication statusPublished - 10 Mar 2021

Bibliographical note

Funding Information:
We thank Phil Rice, Alistair Cox, and David Rose for technical support during the Artemis beamtime. We gratefully acknowledge funding from VILLUM FONDEN through the Young Investigator Program (15375) and the Centre of Excellence for Dirac Materials (11744), the Danish Council for Independent Research, Natural Sciences, under the Sapere Aude program (DFF-9064-00057B and DFF-6108-00409), and the Aarhus University Research Foundation. This work is also supported by National Research Foundation (NRF) grants funded by the Korean government (NRF-2020R1A2C200373211 and 2019K1A3A7A09033389) and by the International Max Planck Research School for Chemistry and Physics of Quantum Materials (IMPRS-CPQM). The authors also acknowledge The Royal Society and The Leverhulme Trust. Access to the Artemis Facility was funded by STFC. The Advanced Light Source is supported by the Director, Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under contract no. DE-AC02-05CH11231. The research data supporting this publication can be accessed at Ref. .

Publisher Copyright:
© 2021 American Chemical Society.

Keywords

  • charge density wave
  • metal-insulator transition
  • Single-layer VSe
  • time- and angle-resolved photoemission spectroscopy
  • ultrafast dynamics

ASJC Scopus subject areas

  • Bioengineering
  • General Chemistry
  • General Materials Science
  • Condensed Matter Physics
  • Mechanical Engineering

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