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

Jager, Marieke F.; Ott, Christian; Kraus, Peter M.; Kaplan, Christopher J.; Pouse, Winston; Marvel, Robert E.; Haglund, Richard F.; Neumark, Daniel M.; Leone, Stephen R.

doi:10.1073/pnas.1707602114

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

Journal Article · Mon Aug 21 00:00:00 EDT 2017 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1707602114· OSTI ID:1426733

Jager, Marieke F. ^[1]; Ott, Christian ^[2]; Kraus, Peter M. ^[1]; Kaplan, Christopher J. ^[1]; Pouse, Winston ^[2]; Marvel, Robert E. ^[3]; Haglund, Richard F. ^[4]; Neumark, Daniel M. ^[5]; Leone, Stephen R. ^[6]

Univ. of California, Berkeley, CA (United States). Department of Chemistry
Univ. of California, Berkeley, CA (United States). Department of Chemistry and Department of Physics
Vanderbilt Univ., Nashville, TN (United States). Interdisciplinary Materials Science Program
Vanderbilt Univ., Nashville, TN (United States). Interdisciplinary Materials Science Program and Department of Physics and Astronomy
Univ. of California, Berkeley, CA (United States). Department of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Chemical Sciences Division
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 M_2,3 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.

View Accepted Manuscript (DOE)

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, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 36 Vol. 114; ISSN 0027-8424

Publisher:: National Academy of Sciences, Washington, DC (United States)Copyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

36 MATERIALS SCIENCE
71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
extreme UV
insulator-to-metal transition
ultrafast dynamics
vanadium dioxide