Tracking the insulator-to-metal phase transition in VO 2 with few-femtosecond extreme UV transient absorption spectroscopy
Open accessAbstract
Significance: An insulator-to-metal phase transition is a process that changes a solid material from being electrically nonconductive to being conductive. The phase transition in vanadium dioxide is a well-studied example where the process can occur in less than a picosecond, making it exciting for ultrafast electronic switches. This paper measures a record speed for the phase transition of 26 fs into a long-lived excited state of the metal that persists out to >60 ps. The extreme UV absorption spectrum of the material is also measured and (together with the ultrafast timescale) belies a structural mechanism that has long been deliberated. The measured femtosecond timescale provides fundamental insight into the electronic speed limits of these complex phenomena.
The claims and statistics of this paper haven’t been checked yet.
Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.
Integrity signals
Registry
Cites
Statistics
Claims the paper makes
The claims and statistics of this paper haven’t been checked yet.
Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.
Claims other papers make about this one
Each is checked against this paper’s own text: does it say what the citing paper says it does?
In solids, excitations across band gaps in basic semiconductors allow mechanisms and timescales to be established for insulator-to-metal transitions.
“allowing mechanisms and timescales to be established for insulator-to-metal transitions [219].”
From Roadmap of ultrafast x-ray atomic and molecular physics (2018) · cites this paper as [219]
Self-check
Percentages, sums and reported differences re-computed from the paper’s own numbers.
The self-check needs the paper’s full text.
Cites
Imada, M., Fujimori, A., & Tokura, Y. (1998) · Reviews of Modern Physics · doi:10.1103/revmodphys.70.1039 · Cited by 7,565 · see citing works
Henke, B. L., Gullikson, E. M., & Davis, J. C. (1993) · Atomic Data and Nuclear Data Tables · doi:10.1006/adnd.1993.1013 · Cited by 6,313 · see citing works
Femtosecond Structural Dynamics in VO2 during an Ultrafast Solid-Solid Phase Transition
Cavalleri, A., Tóth, C., Siders, C. W., et al. (2001) · Physical Review Letters · doi:10.1103/physrevlett.87.237401 · Cited by 1,283 · see citing works
Attosecond spectroscopy in condensed matter
Cavalieri, A. L., Müller, N., Uphues, T., Yakovlev, V. S., Baltuška, A., Horvath, B., Schmidt, B., Blümel, L., Holzwarth, R., Hendel, S., et al. (2007) · Nature · doi:10.1038/nature06229 · Cited by 1,113 · see citing works
Oxide Electronics Utilizing Ultrafast Metal-Insulator Transitions
Yang, Z., Ko, C., & Ramanathan, S. (2011) · Annual Review of Materials Research · doi:10.1146/annurev-matsci-062910-100347 · Cited by 1,026 · see citing works
Theory for displacive excitation of coherent phonons
Zeiger, H. J., Vidal, J., Cheng, T. K., Ippen, E. P., Dresselhaus, G., & Dresselhaus, M. S. (1992) · Physical review. B, Condensed matter · doi:10.1103/physrevb.45.768 · Cited by 997 · see citing works
Multiplet effects in X-ray spectroscopy
de Groot, F. M. F. (2004) · Coordination Chemistry Reviews · doi:10.1016/j.ccr.2004.03.018 · Cited by 799 · see citing works
The CTM4XAS program for EELS and XAS spectral shape analysis of transition metal L edges
Stavitski, E., & de Groot, F. M. F. (2010) · Micron · doi:10.1016/j.micron.2010.06.005 · Cited by 744 · see citing works
Linking high harmonics from gases and solids
Vampa, G., Hammond, T. J., Thiré, N., Schmidt, B. E., Légaré, F., McDonald, C., Brabec, T., & Corkum, P. B. (2015) · Nature · doi:10.1038/nature14517 · Cited by 734 · see citing works
Dynamical Singlets and Correlation-Assisted Peierls Transition in V O 2
Biermann, S., Poteryaev, A. I., Lichtenstein, A. I., et al. (2005) · Physical Review Letters · doi:10.1103/physrevlett.94.026404 · Cited by 715 · see citing works
Cavalleri, A., Dekorsy, T., Chong, H., et al. (2004) · Physical Review B · doi:10.1103/physrevb.70.161102 · Cited by 710 · see citing works
VO 2 : Peierls or Mott-Hubbard? A view from band theory
Wentzcovitch, R. M. M., Schulz, W., & Allen, P. B. (1994) · Physical Review Letters · doi:10.1103/physrevlett.72.3389 · Cited by 672 · see citing works
A photoinduced metal-like phase of monoclinic VO 2 revealed by ultrafast electron diffraction
Morrison, V. R., Chatelain, R. P., Tiwari, K. L., et al. (2014) · Science · doi:10.1126/science.1253779 · Cited by 608 · see citing works
Controlling dielectrics with the electric field of light
Schultze, M., Bothschafter, E. M., Sommer, A., Holzner, S., Schweinberger, W., Fiess, M., Hofstetter, M., Kienberger, R., Apalkov, V., Yakovlev, V. S., et al. (2013) · Nature · doi:10.1038/nature11720 · Cited by 604 · see citing works
Control of the metal–insulator transition in vanadium dioxide by modifying orbital occupancy
Aetukuri, N. P. B., Gray, A. X., Drouard, M., Cossale, M., Li, G., Reid, A. H., Kukreja, R., Ohldag, H., Jenkins, C., Arenholz, E., et al. (2013) · Nature Physics · doi:10.1038/nphys2733 · Cited by 589 · see citing works
Electronic Properties of V O2 near the Semiconductor-Metal Transition
BERGLUND, C. N., & Guggenheim, H. J. (1969) · Physical Review · doi:10.1103/physrev.185.1022 · Cited by 585 · see citing works
4D Visualization of Transitional Structures in Phase Transformations by Electron Diffraction
Baum, P., Yang, D., & Zewail, A. H. (2007) · Science · doi:10.1126/science.1147724 · Cited by 574 · see citing works
Attosecond band-gap dynamics in silicon
Schultze, M., Ramasesha, K., Pemmaraju, C. D., Sato, S. A., Whitmore, D., Gandman, A., Prell, J. S., Borja, L. J., Prendergast, D., Yabana, K., et al. (2014) · Science · doi:10.1126/science.1260311 · Cited by 553 · see citing works
Self-citationLorentz Meets Fano in Spectral Line Shapes: A Universal Phase and Its Laser Control
Ott, C., Kaldun, A., Raith, P., Meyer, K., Laux, M., Evers, J., Keitel, C. H., Greene, C. H., & Pfeifer, T. (2013) · Science · doi:10.1126/science.1234407 · Cited by 518 · see citing works
Self-citationON THE TRANSITION TO METALLIC CONDUCTION IN SEMICONDUCTORS
Mott, N. F. (1956) · Canadian Journal of Physics · doi:10.1139/p56-151 · Cited by 510 · see citing works
Attosecond metrology: from electron capture to future signal processing
Krausz, F., & Stockman, M. I. (2014) · Nature Photonics · doi:10.1038/nphoton.2014.28 · Cited by 485 · see citing works
Shin, S., Suga, S., Taniguchi, M., et al. (1990) · Physical review. B, Condensed matter · doi:10.1103/physrevb.41.4993 · Cited by 448 · see citing works
Kübler, C., Ehrke, H., Huber, R., et al. (2007) · Physical Review Letters · doi:10.1103/physrevlett.99.116401 · Cited by 444 · see citing works
Orbital-Assisted Metal-Insulator Transition in VO2
Haverkort, M. W., Hu, Z., Tanaka, A., et al. (2005) · Physical Review Letters · doi:10.1103/physrevlett.95.196404 · Cited by 405 · see citing works
Suh, J. Y., López, R., Feldman, L. C., et al. (2004) · Journal of Applied Physics · doi:10.1063/1.1762995 · Cited by 367 · see citing works
Brassard, D., Fourmaux, S., Jean-Jacques, M., et al. (2005) · Applied Physics Letters · doi:10.1063/1.2001139 · Cited by 354 · see citing works
Metallization of vanadium dioxide driven by large phonon entropy
Budai, J. D., Hong, J., Manley, M. E., et al. (2014) · Nature · doi:10.1038/nature13865 · Cited by 345 · see citing works
The 2016 oxide electronic materials and oxide interfaces roadmap
Lorenz, M., Rao, M. S. R., Venkatesan, T., Fortunato, E. M. C., Barquinha, P. M. C., Branquinho, R., Salgueiro, D., Martins, R., Carlos, E., Liu, A., et al. (2016) · Journal of Physics D Applied Physics · doi:10.1088/0022-3727/49/43/433001 · Cited by 312 · see citing works
Synthesis of vanadium dioxide thin films and nanoparticles
Nag, J., & Haglund, R. F. (2008) · Journal of Physics Condensed Matter · doi:10.1088/0953-8984/20/26/264016 · Cited by 286 · see citing works
Self-citationBand-Selective Measurements of Electron Dynamics in VO2 Using Femtosecond Near-Edge X-Ray Absorption
Cavalleri, A., Rini, M., Chong, H., Fourmaux, S., Glover, T. E., Heimann, P., Kieffer, J. C., & Schoenlein, R. W. (2005) · Physical Review Letters · doi:10.1103/physrevlett.95.067405 · Cited by 279 · see citing works
Femtosecond laser excitation of the semiconductor-metal phase transition in VO2
Becker, M. F., Buckman, A. B., Walser, R. M., et al. (1994) · Applied Physics Letters · doi:10.1063/1.112974 · Cited by 267 · see citing works
Attosecond dynamical Franz-Keldysh effect in polycrystalline diamond
Lucchini, M., Sato, S. A., Ludwig, A., Herrmann, J., Volkov, M., Kasmi, L., Shinohara, Y., Yabana, K., Gallmann, L., & Keller, U. (2016) · Science · doi:10.1126/science.aag1268 · Cited by 266 · see citing works
Instantaneous Band Gap Collapse in Photoexcited Monoclinic VO2 due to Photocarrier Doping
Wegkamp, D., Herzog, M., Xian, L., Gatti, M., Cudazzo, P., McGahan, C., Marvel, R. E., Haglund, R. F., Rubio, Á., Wolf, M., et al. (2014) · Physical Review Letters · doi:10.1103/physrevlett.113.216401 · Cited by 258 · see citing works
Self-citationSchilbe, P. (2002) · Physica B Condensed Matter · doi:10.1016/s0921-4526(02)00584-7 · Cited by 256 · see citing works
Ultrafast changes in lattice symmetry probed by coherent phonons
Wall, S., Wegkamp, D., Foglia, L., Appavoo, K., Nag, J., Haglund, R. F., Stähler, J., & Wolf, M. (2012) · Nature Communications · doi:10.1038/ncomms1719 · Cited by 245 · see citing works
Self-citationDirect time-domain observation of attosecond final-state lifetimes in photoemission from solids
Tao, Z., Chen, C., Szilvási, T., Keller, M., Mavrikakis, M., Kapteyn, H., & Murnane, M. (2016) · Science · doi:10.1126/science.aaf6793 · Cited by 241 · see citing works
Characterization of broadband few-cycle laser pulses with the d-scan technique
Miranda, M., Arnold, C. L., Fordell, T., Silva, F., Alonso, B., Weigand, R., L’Huillier, A., & Crespo, H. (2012) · Optics Express · doi:10.1364/oe.20.018732 · Cited by 237 · see citing works
Appavoo, K., Lei, D. Y., Sonnefraud, Y., et al. (2012) · Nano Letters · doi:10.1021/nl203782y · Cited by 231 · see citing works
Real-Time Probing of Electron Dynamics Using Attosecond Time-Resolved Spectroscopy
Ramasesha, K., Leone, S. R., & Neumark, D. M. (2016) · Annual Review of Physical Chemistry · doi:10.1146/annurev-physchem-040215-112025 · Cited by 225 · see citing works
Self-citationMore Surprises in Theoretical Physics
Peierls, R. E. (1992) · Princeton University Press eBooks · doi:10.1515/9780691214320 · Cited by 222 · see citing works
Electronic structure of 3d-transition-metal oxides: on-site Coulomb repulsion versus covalency
Zimmermann, R. T., STEINER, P. R., Claessen, R., et al. (1999) · Journal of Physics Condensed Matter · doi:10.1088/0953-8984/11/7/002 · Cited by 221 · see citing works
Inhomogeneity of the ultrafast insulator-to-metal transition dynamics of VO2
O’Callahan, B. T., Jones, A. C., Park, J. H., et al. (2015) · Nature Communications · doi:10.1038/ncomms7849 · Cited by 202 · see citing works
Vanadium Dioxide: A Peierls-Mott Insulator Stable against Disorder
Weber, C., O’Regan, D. D., Hine, N. D. M., et al. (2012) · Physical Review Letters · doi:10.1103/physrevlett.108.256402 · Cited by 201 · see citing works
Strong hybridization in vanadium oxides: evidence from photoemission and absorption spectroscopy
Zimmermann, R. T., Claessen, R., Reinert, F., et al. (1998) · Journal of Physics Condensed Matter · doi:10.1088/0953-8984/10/25/018 · Cited by 188 · see citing works
Ultrafast dynamics during the photoinduced phase transition in VO2
Wegkamp, D., & Stähler, J. (2015) · Progress in Surface Science · doi:10.1016/j.progsurf.2015.10.001 · Cited by 152 · see citing works
Petahertz optical drive with wide-bandgap semiconductor
Mashiko, H., Oguri, K., Yamaguchi, T., Suda, A., & Gotoh, H. (2016) · Nature Physics · doi:10.1038/nphys3711 · Cited by 143 · see citing works
How optical excitation controls the structure and properties of vanadium dioxide
Otto, M. R., de Cotret, L. P. R., Valverde-Chávez, D. A., et al. (2018) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1808414115 · Cited by 141 · see citing works
More Surprises in Theoretical Physics
PEIERLS, R. (2020) · Princeton University Press eBooks · doi:10.2307/j.ctv10crg2s · Cited by 127 · see citing works
Ultrafast Nanoimaging of the Photoinduced Phase Transition Dynamics in VO2
Dönges, S. A., Khatib, O., O’Callahan, B. T., Atkin, J. M., Park, J. H., Cobden, D. H., & Raschke, M. B. (2016) · Nano Letters · doi:10.1021/acs.nanolett.5b05313 · Cited by 117 · see citing works
Davis, L. C., & Feldkamp, L. A. (1978) · Physical Review A · doi:10.1103/physreva.17.2012 · Cited by 115 · see citing works
Gurvitch, M., Luryi, S., Polyakov, A., et al. (2007) · Journal of Applied Physics · doi:10.1063/1.2764245 · Cited by 103 · see citing works
Wall, S., Foglia, L., Wegkamp, D., et al. (2013) · Physical Review B · doi:10.1103/physrevb.87.115126 · Cited by 97 · see citing works
Interaction of many discrete states with many continua
Davis, L. C., & Feldkamp, L. A. (1977) · Physical review. B, Solid state · doi:10.1103/physrevb.15.2961 · Cited by 97 · see citing works
Theory of X-Ray Photoemission and X-Ray Emission Spectra in Mn Compounds
Taguchi, M., Uozumi, T., & Kotani, A. (1997) · Journal of the Physical Society of Japan · doi:10.1143/jpsj.66.247 · Cited by 95 · see citing works
Schulz, K., Domke, M., Püttner, R., et al. (1996) · Physical Review A · doi:10.1103/physreva.54.3095 · Cited by 92 · see citing works
Cavalleri, A., Chong, H., Fourmaux, S., et al. (2004) · Physical Review B · doi:10.1103/physrevb.69.153106 · Cited by 89 · see citing works
Correlation-Driven Insulator-Metal Transition in Near-Ideal Vanadium Dioxide Films
Gray, A. X., Jeong, J., Aetukuri, N. P. B., et al. (2016) · Physical Review Letters · doi:10.1103/physrevlett.116.116403 · Cited by 86 · see citing works
Hole-lattice coupling and photoinduced insulator-metal transition in VO 2
Yuan, X. F., Zhang, W., & Zhang, P. (2013) · Physical Review B · doi:10.1103/physrevb.88.035119 · Cited by 81 · see citing works
Insulating phases of vanadium dioxide are Mott-Hubbard insulators
Huffman, T. J., Hendriks, C., Walter, E. J., et al. (2017) · Physical review. B./Physical review. B · doi:10.1103/physrevb.95.075125 · Cited by 78 · see citing works
Ultrafast evolution and transient phases of a prototype out-of-equilibrium Mott–Hubbard material
Lantz, G., Mansart, B., Grieger, D., et al. (2017) · Nature Communications · doi:10.1038/ncomms13917 · Cited by 75 · see citing works
M2,3absorption spectroscopy of 3d transition-metal compounds
van der Laan, G. (1991) · Journal of Physics Condensed Matter · doi:10.1088/0953-8984/3/38/016 · Cited by 55 · see citing works
THz Transmittance and Electrical Properties Tuning across IMT in Vanadium Dioxide Films by Al Doping
Wu, X., Wu, Z., Ji, C., et al. (2016) · ACS Applied Materials & Interfaces · doi:10.1021/acsami.5b12417 · Cited by 54 · see citing works
∼8 keV photoemission of the metal–insulator transition system VO2
Suga, S., Sekiyama, A., Imada, S., et al. (2009) · New Journal of Physics · doi:10.1088/1367-2630/11/10/103015 · Cited by 42 · see citing works
Bound states and critical behavior of the Yukawa potential
Li, Y., Luo, X.-Q., & Kröger, H. (2006) · doi:10.1007/s11433-004-0020-5 · Cited by 37 · see citing works
Experimental study of resonant photoemission in the metals V, Cr, Mn and Co
Kaurila, T., Väyrynen, J. P., & Isokallio, M. (1997) · Journal of Physics Condensed Matter · doi:10.1088/0953-8984/9/31/007 · Cited by 30 · see citing works
Autoionization in bulk, multilayer, and monolayer Cr
Bader, S. D., Zajac, G. W., Arko, A. J., et al. (1986) · Physical review. B, Condensed matter · doi:10.1103/physrevb.33.3636 · Cited by 22 · see citing works
In situ characterization of few-cycle laser pulses in transient absorption spectroscopy
Blättermann, A., Ott, C., Kaldun, A., Ding, T., Stooß, V., Laux, M., Rebholz, M., & Pfeifer, T. (2015) · Optics Letters · doi:10.1364/ol.40.003464 · Cited by 22 · see citing works
Self-citationWu, X., Wu, Z., Ji, C., et al. (2016) · Optical Materials Express · doi:10.1364/ome.6.003500 · Cited by 19 · see citing works
Slowdown of the Electronic Relaxation Close to the Mott Transition
Sayyad, S., & ECKSTEIN, M. C. (2016) · Physical Review Letters · doi:10.1103/physrevlett.117.096403 · Cited by 18 · see citing works
Flagged first, then by citations
Research works printed but not linked: 1
- Nag J (2011) The solid-solid phase transition in vanadium dioxide thin films: Synthesis, physics and applications (PhD dissertation, Vanderbilt University, Nashville, TN). Available at etd.library.vanderbilt.edu/available/etd-04202011-182358/. Accessed August 8, 2017.
Cited by
Sorted by citations
Roadmap of ultrafast x-ray atomic and molecular physics
Young, L., Ueda, K., Gühr, M., Bucksbaum, P. H., Simon, M., Mukamel, S., Rohringer, N., Prince, K. C., Masciovecchio, C., Meyer, M., et al. (2018) · Journal of Physics B: Atomic, Molecular and Optical Physics · doi:10.1088/1361-6455/aa9735 · Cited by 337 · see citing works
Self-citation
- Authors
- Jager, M. F., Ott, C., Kraus, P. M., Kaplan, C. J., Pouse, W., Marvel, R. E., Haglund, R. F., Neumark, D. M., & Leone, S. R.
- Affiliations
- University of California, Berkeley (US)
- Vanderbilt University (US)
- Lawrence Berkeley National Laboratory (US)
- Corresponding author
- Neumark, Daniel M.
- ORCID
- Venue
- Proceedings of the National Academy of Sciences
- Publisher
- National Academy of Sciences
- Published
- 2017-08-21
- Volume
- 114
- Issue
- 36
- Pages
- 9558-9563
- ISSN
- 0027-8424 (ISSN-L)
- 1091-6490
- PMC
- PMC5594684
- OpenAlex
- W2749580185
- Cited by
- 164
- References
- 69
- Citations by year
- 2026: 11 · 2025: 18 · 2024: 16 · 2023: 16 · 2022: 23 · 2021: 24 · 2020: 28 · 2019: 14 · 2018: 14
- FWCI
- 8.75
- Type
- journal article
- Language
- en
- Open access
- bronze
- doi.org
- Locations
- Proceedings of the National Academy of Sciences (publishedVersion)
- Europe PMC (PubMed Central) (publishedVersion)
- PubMed Central (publishedVersion)
- PubMed (publishedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- eScholarship (California Digital Library) (submittedVersion)
- Max Planck Digital Library (submittedVersion)
- MPG.PuRe (Max Planck Society) (submittedVersion)
- Funders
- DOD | Defense Advanced Research Projects Agency (W31P4Q-13-1-0017)
- DOD | USAF | AFMC | Air Force Office of Scientific Research (FA9550-15-1-0037)
- W. M. Keck Foundation (DE-AC03-76SF00098)
- National Science Foundation (DMR-1207507)
- Topics
- Physical Sciences › Materials Science › Polymers and Plastics › Transition Metal Oxide Nanomaterials
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Laser-Matter Interactions and Applications
- Physical Sciences › Materials Science › Materials Chemistry › Phase-change materials and chalcogenides
- Keywords
- vanadium dioxide, metal-insulator transition, phase transition dynamics
About these checks
Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.
Statistics and arithmetic are recomputed, not judged.
Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.
What counts as a claim ›How we measure confidence ›How we check this ›
Are you an author, or do you see a problem with this page? Request a review
