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Title: Ultrafast disordering of vanadium dimers in photoexcited VO 2

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 [1] ; ORCiD logo [2] ; ORCiD logo [1] ; ORCiD logo [3] ; ORCiD logo [3] ; ORCiD logo [4] ; ORCiD logo [5] ; ORCiD logo [4] ;  [4] ; ORCiD logo [1] ;  [6] ; ORCiD logo [7] ; ORCiD logo [8] ;  [9]
  1. Barcelona Inst. of Science and Technology (Spain). Inst. of Photonic Sciences (ICFO)
  2. Duke Univ., Durham, NC (United States). Dept. of Mechanical Engineering and Materials Science
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford PULSE Inst.
  5. Japan Synchrotron Radiation Research Inst., Hyogo (Japan)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford PULSE Inst. Stanford Inst. for Materials and Energy Sciences; Stanford Univ., CA (United States). Dept. of Applied Physics
  7. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
  8. Duke Univ., Durham, NC (United States). Dept. of Mechanical Engineering and Materials Science. Dept. of Physics
  9. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford PULSE Inst. Stanford Inst. for Materials and Energy Sciences
Publication Date:
Grant/Contract Number:
AC05-00OR22725; AC02-76SF00515; AC02-05CH11231; SC0016166; SEV-2015-0522; RYC-2013-14838; FIS2015-67898-P; 758461; 2016A8008
Type:
Published Article
Journal Name:
Science
Additional Journal Information:
Journal Volume: 362; Journal Issue: 6414; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); 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)
Country of Publication:
United States
Language:
English
OSTI Identifier:
1480375
Alternate Identifier(s):
OSTI ID: 1481692

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 VO2. United States: N. p., 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 VO2. 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. 2018. "Ultrafast disordering of vanadium dimers in photoexcited VO2". United States. doi:10.1126/science.aau3873.
@article{osti_1480375,
title = {Ultrafast disordering of vanadium dimers in photoexcited VO2},
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}
}

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