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Title: Ultrafast disordering of vanadium dimers in photoexcited VO 2

Journal Article · · Science

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 (VO2) 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:
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 Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); 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)
Grant/Contract Number:
AC02-76SF00515; SC0016166; AC02-05CH11231; AC05-00OR22725; SEV-2015-0522; RYC-2013-14838; FIS2015-67898-P; 758461; 2016A8008
OSTI ID:
1480375
Alternate ID(s):
OSTI ID: 1481692; OSTI ID: 1490850; OSTI ID: 1508593
Journal Information:
Science, Journal Name: Science Vol. 362 Journal Issue: 6414; ISSN 0036-8075
Publisher:
American Association for the Advancement of Science (AAAS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 111 works
Citation information provided by
Web of Science

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Cited By (10)

Noise correlations in time- and angle-resolved photoemission spectroscopy journal June 2019
Van der Waals Heteroepitaxial VO 2 /Mica Films with Extremely Low Optical Trigger Threshold and Large THz Field Modulation Depth journal July 2019
A Room‐Temperature Verwey‐type Transition in Iron Oxide, Fe 5 O 6 journal January 2020
Strain engineering on the metal-insulator transition of VO 2 /TiO 2 epitaxial films dependent on the strain state of vanadium dimers journal December 2019
Tuning critical phase transition in VO 2 via interfacial control of normal and shear strain journal November 2019
How optical excitation controls the structure and properties of vanadium dioxide journal December 2018
Floquet-engineered light-cone spreading of correlations in a driven quantum chain journal October 2019
Origin of the transition entropy in vanadium dioxide journal February 2019
Electronic structure of metallic and insulating phases of vanadium dioxide and its oxide alloys journal September 2019
Pump–probe experimental methodology at the Linac Coherent Light Source journal April 2019

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