4.5 Review

The ultrafast X-ray spectroscopic revolution in chemical dynamics

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NATURE REVIEWS CHEMISTRY
卷 2, 期 6, 页码 82-94

出版社

NATURE PUBLISHING GROUP
DOI: 10.1038/s41570-018-0008-8

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资金

  1. Air Force Office of Scientific Research (AFOSR) [FA9550-15-1-0037, FA9550-14-1-0154]
  2. Army Research Office (ARO) [WN911NF-14-1-0383]
  3. Office of Assistant Secretary of Defense for Research and Engineering through a National Security Science and Engineering Faculty Fellowship (NSSEFF)
  4. W. M. Keck Foundation
  5. Defense Advanced Research Projects Agency PULSE program [W31P4Q-13-1-0017]
  6. National Science Foundation (NSF) [CHE-1361226, CHE-1660417]
  7. Foundation Major Research Instrumentation (NSF MRI) [1624322]
  8. U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Atomic, Molecular and Optical Sciences Program
  9. Physical Chemistry of Inorganic Nanostructures Program [DE-AC02-05-CH11231]
  10. Swiss National Science Foundation [P2EZP2 165252, P300P2 174293]
  11. Humboldt Foundation
  12. Department of Energy, Office of Energy Efficiency and Renewable Energy (EERE) Postdoctoral Research Award under the EERE Solar Energy Technologies Office
  13. Swiss National Science Foundation (SNF) [P2EZP2_165252, P300P2_174293] Funding Source: Swiss National Science Foundation (SNF)
  14. Division Of Chemistry
  15. Direct For Mathematical & Physical Scien [1624322] Funding Source: National Science Foundation

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The past two decades have seen rapid developments in short-pulse X-ray sources, which have enabled the study of nuclear and electronic dynamics by ultrafast X-ray spectroscopies with unprecedented time resolution ranging from nanoseconds to attoseconds. In this Perspective, we discuss some of the major achievements in the study of nuclear and electronic dynamics with X-ray pulses produced by high-harmonic, free-electron-laser and synchrotron sources. The particular dynamic processes probed by X-ray radiation highlighted in this Perspective are electronic coherences on attosecond to femtosecond timescales, chemical reactions, such as dissociations, and pericyclic ring-openings, spin crossover dynamics, ligand-exchange dynamics and structural deformations in excited states. X-ray spectroscopic probing of chemical dynamics holds great promise for the future owing to the ongoing developments of new spectroscopies, such as four-wave mixing, and the continuous improvements in emerging laboratory-based, high-harmonic sources and large-scale, facility-based, free-electron lasers.

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