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Title: Tracking the insulator-to-metal phase transition in VO2 with few-femtosecond extreme UV transient absorption spectroscopy

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
 [1];  [2];  [1];  [1];  [2];  [3];  [4];  [5];  [6]
  1. Univ. of California, Berkeley, CA (United States). Department of Chemistry
  2. Univ. of California, Berkeley, CA (United States). Department of Chemistry and Department of Physics
  3. Vanderbilt Univ., Nashville, TN (United States). Interdisciplinary Materials Science Program
  4. Vanderbilt Univ., Nashville, TN (United States). Interdisciplinary Materials Science Program and Department of Physics and Astronomy
  5. Univ. of California, Berkeley, CA (United States). Department of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
  6. Univ. of California, Berkeley, CA (United States). Department of Chemistry and Department of Physics; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division

We present coulomb correlations can manifest in exotic properties in solids, but how these properties can be accessed and ultimately manipulated in real time is not well understood. The insulator-to-metal phase transition in vanadium dioxide (VO2) is a canonical example of such correlations. Here, few-femtosecond extreme UV transient absorption spectroscopy (FXTAS) at the vanadium M2,3 edge is used to track the insulator-to-metal phase transition in VO2 . This technique allows observation of the bulk material in real time, follows the photoexcitation process in both the insulating and metallic phases, probes the subsequent relaxation in the metallic phase, and measures the phase-transition dynamics in the insulating phase. An understanding of the VO2 absorption spectrum in the extreme UV is developed using atomic cluster model calculations, revealing V3+/d2 character of the vanadium center. We find that the insulator-to-metal phase transition occurs on a timescale of 26 ± 6 fs and leaves the system in a long-lived excited state of the metallic phase, driven by a change in orbital occupation. Potential interpretations based on electronic screening effects and lattice dynamics are discussed. A Mott–Hubbard-type mechanism is favored, as the observed timescales and d2 nature of the vanadium metal centers are inconsistent with a Peierls driving force. In conclusion, the findings provide a combined experimental and theoretical roadmap for using time-resolved extreme UV spectroscopy to investigate nonequilibrium dynamics in strongly correlated materials.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
AC02-05CH11231; AC03-76SF00098
OSTI ID:
1426733
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Vol. 114, Issue 36; ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 88 works
Citation information provided by
Web of Science

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  • Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 377, Issue 2145 https://doi.org/10.1098/rsta.2017.0463
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Multiscale time-dependent density functional theory for a unified description of ultrafast dynamics: Pulsed light, electron, and lattice motions in crystalline solids journal June 2019
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