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Ultrafast disordering of vanadium dimers in photoexcited VO 2

Journal Article · · Science
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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.

Research Organization:
Barcelona Inst. of Science and Technology (Spain); Duke Univ., Durham, NC (United States); Japan Synchrotron Radiation Research Inst., Hyogo (Japan); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); SLAC National Accelerator Lab., Menlo Park, CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
European Regional Development Fund (ERDF); European Union (EU); Japan Synchrotron Radiation Research Inst. (JASRI); Ministry of Economy and Business (MINECO) (Spain); Ramón y Cajal programme (Spain); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-05CH11231; AC02-76SF00515; AC05-00OR22725; SC0016166
OSTI ID:
1480375
Alternate ID(s):
OSTI ID: 1508593
OSTI ID: 1481692
OSTI ID: 1490850
Journal Information:
Science, Journal Name: Science Journal Issue: 6414 Vol. 362; ISSN 0036-8075
Publisher:
American Association for the Advancement of Science (AAAS)Copyright Statement
Country of Publication:
United States
Language:
English

References (46)

n Moldyn: A program package for a neutron scattering oriented analysis of molecular dynamics simulations journal March 2003
X-Ray Diffraction Crystallography book January 2011
First principles phonon calculations in materials science journal November 2015
Metallization of vanadium dioxide driven by large phonon entropy journal November 2014
Nonlinear lattice dynamics as a basis for enhanced superconductivity in YBa2Cu3O6.5 journal December 2014
Distortion-triggered loss of long-range order in solids with bonding energy hierarchy journal March 2011
Ultrafast changes in lattice symmetry probed by coherent phonons journal January 2012
Time-domain classification of charge-density-wave insulators journal January 2012
Transient photoinduced ‘hidden’ phase in a manganite journal January 2011
A time-dependent order parameter for ultrafast photoinduced phase transitions journal August 2014
Time-domain separation of optical properties from structural transitions in resonantly bonded materials journal July 2015
Towards properties on demand in quantum materials journal October 2017
Nonlinear phononics as an ultrafast route to lattice control journal August 2011
Fourier-transform inelastic X-ray scattering from time- and momentum-dependent phonon–phonon correlations journal October 2013
Structural phase transitions I. Landau theory journal February 1980
Structural phase transitions. II. Static critical behaviour journal February 1980
Optical Properties of V O 2 between 0.25 and 5 eV journal August 1968
Symmetry Considerations and the Vanadium Dioxide Phase Transition journal March 1970
X-ray diffraction study of metallic V O 2 journal July 1974
Electronic structure and lattice instability of metallic V O 2 journal October 1977
Diffuse x-ray scattering due to the lattice instability near the metal-semiconductor transition in V O 2 journal March 1978
Lattice dynamics of oxides with rutile structure and instabilities at the metal-semiconductor phase transitions of NbO 2 and VO 2 journal April 1985
Ab initiomolecular dynamics for liquid metals journal January 1993
Structural Aspects of the Metal-Insulator Transitions in Cr-Doped V O 2 journal April 1972
Projector augmented-wave method journal December 1994
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
From ultrasoft pseudopotentials to the projector augmented-wave method journal January 1999
Evidence for a structurally-driven insulator-to-metal transition in VO 2 : A view from the ultrafast timescale journal October 2004
Coulomb correlations and orbital polarization in the metal-insulator transition of V O 2 journal February 2005
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
Temperature dependent effective potential method for accurate free energy calculations of solids journal March 2013
Hole-lattice coupling and photoinduced insulator-metal transition in VO 2 journal July 2013
Ferroelectric Soft Mode in a SrTiO 3 Thin Film Impulsively Driven to the Anharmonic Regime Using Intense Picosecond Terahertz Pulses journal February 2012
Coherent Structural Dynamics of a Prototypical Charge-Density-Wave-to-Metal Transition journal July 2014
Generalized Gradient Approximation Made Simple journal October 1996
Femtosecond Structural Dynamics in VO 2 during an Ultrafast Solid-Solid Phase Transition journal November 2001
Coherent Structural Dynamics and Electronic Correlations during an Ultrafast Insulator-to-Metal Phase Transition in VO 2 journal September 2007
The X-ray Pump–Probe instrument at the Linac Coherent Light Source journal April 2015
Brillouin-zone database on the Bilbao Crystallographic Server journal February 2014
Atomic-Scale Visualization of Inertial Dynamics journal April 2005
Ultrafast Bond Softening in Bismuth: Mapping a Solid's Interatomic Potential with X-rays journal February 2007
4D Visualization of Transitional Structures in Phase Transformations by Electron Diffraction journal November 2007
A photoinduced metal-like phase of monoclinic VO 2 revealed by ultrafast electron diffraction journal October 2014
Anomalously low electronic thermal conductivity in metallic vanadium dioxide journal January 2017
Theory of displacive phase transitions in minerals journal April 1997
A Refinement of the Structure of VO2. journal January 1970

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