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 (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.
- Authors:
- 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); 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. https://doi.org/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. https://doi.org/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 (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.},
doi = {10.1126/science.aau3873},
journal = {Science},
number = 6414,
volume = 362,
place = {United States},
year = {Thu Nov 01 00:00:00 EDT 2018},
month = {Thu Nov 01 00:00:00 EDT 2018}
}
https://doi.org/10.1126/science.aau3873
Web of Science
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