skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Ultrafast disordering of vanadium dimers in photoexcited VO 2

Abstract

Many ultrafast solid phase transitions are treated as chemical reactions that transform the structures between two different unit cells along a reaction coordinate, but this neglects the role of disorder. Although ultrafast diffraction provides insights into atomic dynamics during such transformations, diffraction alone probes an averaged unit cell and is less sensitive to randomness in the transition pathway. Using total scattering of femtosecond x-ray pulses, we show that atomic disordering in photoexcited vanadium dioxide (VO 2 ) is central to the transition mechanism and that, after photoexcitation, the system explores a large volume of phase space on a time scale comparable to that of a single phonon oscillation. These results overturn the current understanding of an archetypal ultrafast phase transition and provide new microscopic insights into rapid evolution toward equilibrium in photoexcited matter.

Authors:
ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ORCiD logo; ; ORCiD logo; ; ORCiD logo; ORCiD logo;
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); SLAC National Accelerator Lab., Menlo Park, CA (United States); Duke Univ., Durham, NC (United States); Barcelona Inst. of Science and Technology (Spain); Japan Synchrotron Radiation Research Inst., Hyogo (Japan)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Ministry of Economy and Business (MINECO) (Spain); Ramón y Cajal programme (Spain); European Regional Development Fund (ERDF); European Union (EU); Japan Synchrotron Radiation Research Inst. (JASRI)
OSTI Identifier:
1480375
Alternate Identifier(s):
OSTI ID: 1481692; OSTI ID: 1490850; OSTI ID: 1508593
Grant/Contract Number:  
AC02-76SF00515; SC0016166; AC02-05CH11231; AC05-00OR22725; SEV-2015-0522; RYC-2013-14838; FIS2015-67898-P; 758461; 2016A8008
Resource Type:
Published Article
Journal Name:
Science
Additional Journal Information:
Journal Name: Science Journal Volume: 362 Journal Issue: 6414; Journal ID: ISSN 0036-8075
Publisher:
American Association for the Advancement of Science (AAAS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Wall, Simon, Yang, Shan, Vidas, Luciana, Chollet, Matthieu, Glownia, James M., Kozina, Michael, Katayama, Tetsuo, Henighan, Thomas, Jiang, Mason, Miller, Timothy A., Reis, David A., Boatner, Lynn A., Delaire, Olivier, and Trigo, Mariano. Ultrafast disordering of vanadium dimers in photoexcited VO 2. United States: N. p., 2018. Web. doi:10.1126/science.aau3873.
Wall, Simon, Yang, Shan, Vidas, Luciana, Chollet, Matthieu, Glownia, James M., Kozina, Michael, Katayama, Tetsuo, Henighan, Thomas, Jiang, Mason, Miller, Timothy A., Reis, David A., Boatner, Lynn A., Delaire, Olivier, & Trigo, Mariano. Ultrafast disordering of vanadium dimers in photoexcited VO 2. United States. doi:10.1126/science.aau3873.
Wall, Simon, Yang, Shan, Vidas, Luciana, Chollet, Matthieu, Glownia, James M., Kozina, Michael, Katayama, Tetsuo, Henighan, Thomas, Jiang, Mason, Miller, Timothy A., Reis, David A., Boatner, Lynn A., Delaire, Olivier, and Trigo, Mariano. Thu . "Ultrafast disordering of vanadium dimers in photoexcited VO 2". United States. doi:10.1126/science.aau3873.
@article{osti_1480375,
title = {Ultrafast disordering of vanadium dimers in photoexcited VO 2},
author = {Wall, Simon and Yang, Shan and Vidas, Luciana and Chollet, Matthieu and Glownia, James M. and Kozina, Michael and Katayama, Tetsuo and Henighan, Thomas and Jiang, Mason and Miller, Timothy A. and Reis, David A. and Boatner, Lynn A. and Delaire, Olivier and Trigo, Mariano},
abstractNote = {Many ultrafast solid phase transitions are treated as chemical reactions that transform the structures between two different unit cells along a reaction coordinate, but this neglects the role of disorder. Although ultrafast diffraction provides insights into atomic dynamics during such transformations, diffraction alone probes an averaged unit cell and is less sensitive to randomness in the transition pathway. Using total scattering of femtosecond x-ray pulses, we show that atomic disordering in photoexcited vanadium dioxide (VO 2 ) is central to the transition mechanism and that, after photoexcitation, the system explores a large volume of phase space on a time scale comparable to that of a single phonon oscillation. These results overturn the current understanding of an archetypal ultrafast phase transition and provide new microscopic insights into rapid evolution toward equilibrium in photoexcited matter.},
doi = {10.1126/science.aau3873},
journal = {Science},
number = 6414,
volume = 362,
place = {United States},
year = {2018},
month = {11}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1126/science.aau3873

Citation Metrics:
Cited by: 13 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Symmetry Considerations and the Vanadium Dioxide Phase Transition
journal, March 1970


Diffuse x-ray scattering due to the lattice instability near the metal-semiconductor transition in V O 2
journal, March 1978


Electronic structure and lattice instability of metallic V O 2
journal, October 1977


Towards properties on demand in quantum materials
journal, October 2017

  • Basov, D. N.; Averitt, R. D.; Hsieh, D.
  • Nature Materials, Vol. 16, Issue 11
  • DOI: 10.1038/nmat5017

Atomic-Scale Visualization of Inertial Dynamics
journal, April 2005


Projector augmented-wave method
journal, December 1994


Structural Aspects of the Metal-Insulator Transitions in Cr-Doped V O 2
journal, April 1972


A photoinduced metal-like phase of monoclinic VO 2 revealed by ultrafast electron diffraction
journal, October 2014

  • Morrison, Vance R.; Chatelain, Robert. P.; Tiwari, Kunal L.
  • Science, Vol. 346, Issue 6208
  • DOI: 10.1126/science.1253779

Coherent Structural Dynamics of a Prototypical Charge-Density-Wave-to-Metal Transition
journal, July 2014


Ultrafast changes in lattice symmetry probed by coherent phonons
journal, January 2012

  • Wall, S.; Wegkamp, D.; Foglia, L.
  • Nature Communications, Vol. 3, Issue 1
  • DOI: 10.1038/ncomms1719

Coherent Structural Dynamics and Electronic Correlations during an Ultrafast Insulator-to-Metal Phase Transition in VO 2
journal, September 2007


Transient photoinduced ‘hidden’ phase in a manganite
journal, January 2011

  • Ichikawa, Hirohiko; Nozawa, Shunsuke; Sato, Tokushi
  • Nature Materials, Vol. 10, Issue 2
  • DOI: 10.1038/nmat2929

Metallization of vanadium dioxide driven by large phonon entropy
journal, November 2014

  • Budai, John D.; Hong, Jiawang; Manley, Michael E.
  • Nature, Vol. 515, Issue 7528
  • DOI: 10.1038/nature13865

4D Visualization of Transitional Structures in Phase Transformations by Electron Diffraction
journal, November 2007


Fourier-transform inelastic X-ray scattering from time- and momentum-dependent phonon–phonon correlations
journal, October 2013

  • Trigo, M.; Fuchs, M.; Chen, J.
  • Nature Physics, Vol. 9, Issue 12
  • DOI: 10.1038/nphys2788

Temperature dependent effective potential method for accurate free energy calculations of solids
journal, March 2013


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


First principles phonon calculations in materials science
journal, November 2015


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Anomalously low electronic thermal conductivity in metallic vanadium dioxide
journal, January 2017


Theory of displacive phase transitions in minerals
journal, April 1997


Structural phase transitions. II. Static critical behaviour
journal, February 1980


Time-domain separation of optical properties from structural transitions in resonantly bonded materials
journal, July 2015

  • Waldecker, Lutz; Miller, Timothy A.; Rudé, Miquel
  • Nature Materials, Vol. 14, Issue 10
  • DOI: 10.1038/nmat4359

Brillouin-zone database on the Bilbao Crystallographic Server
journal, February 2014

  • Aroyo, Mois I.; Orobengoa, Danel; de la Flor, Gemma
  • Acta Crystallographica Section A Foundations and Advances, Vol. 70, Issue 2, p. 126-137
  • DOI: 10.1107/S205327331303091X

X-ray diffraction study of metallic V O 2
journal, July 1974


Characterization of structural dynamics of VO 2 thin film on c -Al 2 O 3 using in-air time-resolved x-ray diffraction
journal, October 2010


Coulomb correlations and orbital polarization in the metal-insulator transition of V O 2
journal, February 2005


Nonlinear lattice dynamics as a basis for enhanced superconductivity in YBa2Cu3O6.5
journal, December 2014


Hole-lattice coupling and photoinduced insulator-metal transition in VO 2
journal, July 2013


The X-ray Pump–Probe instrument at the Linac Coherent Light Source
journal, April 2015

  • Chollet, Matthieu; Alonso-Mori, Roberto; Cammarata, Marco
  • Journal of Synchrotron Radiation, Vol. 22, Issue 3
  • DOI: 10.1107/S1600577515005135

Ab initiomolecular dynamics for liquid metals
journal, January 1993


Optical Properties of V O 2 between 0.25 and 5 eV
journal, August 1968


Ferroelectric Soft Mode in a SrTiO 3 Thin Film Impulsively Driven to the Anharmonic Regime Using Intense Picosecond Terahertz Pulses
journal, February 2012


Structural phase transitions I. Landau theory
journal, February 1980


Nonlinear phononics as an ultrafast route to lattice control
journal, August 2011

  • Först, M.; Manzoni, C.; Kaiser, S.
  • Nature Physics, Vol. 7, Issue 11
  • DOI: 10.1038/nphys2055

Ultrafast Bond Softening in Bismuth: Mapping a Solid's Interatomic Potential with X-rays
journal, February 2007


Time-domain classification of charge-density-wave insulators
journal, January 2012

  • Hellmann, S.; Rohwer, T.; Kalläne, M.
  • Nature Communications, Vol. 3, Issue 1
  • DOI: 10.1038/ncomms2078

A Refinement of the Structure of VO2.
journal, January 1970


A time-dependent order parameter for ultrafast photoinduced phase transitions
journal, August 2014

  • Beaud, P.; Caviezel, A.; Mariager, S. O.
  • Nature Materials, Vol. 13, Issue 10
  • DOI: 10.1038/nmat4046

Evidence for a structurally-driven insulator-to-metal transition in VO 2 : A view from the ultrafast timescale
journal, October 2004


Distortion-triggered loss of long-range order in solids with bonding energy hierarchy
journal, March 2011

  • Kolobov, A. V.; Krbal, M.; Fons, P.
  • Nature Chemistry, Vol. 3, Issue 4
  • DOI: 10.1038/nchem.1007

Femtosecond Structural Dynamics in VO 2 during an Ultrafast Solid-Solid Phase Transition
journal, November 2001


n Moldyn: A program package for a neutron scattering oriented analysis of molecular dynamics simulations
journal, March 2003

  • Róg, T.; Murzyn, K.; Hinsen, K.
  • Journal of Computational Chemistry, Vol. 24, Issue 5
  • DOI: 10.1002/jcc.10243

    Works referencing / citing this record:

    Noise correlations in time- and angle-resolved photoemission spectroscopy
    journal, June 2019


    Noise correlations in time- and angle-resolved photoemission spectroscopy
    journal, June 2019