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Probing ultrafast dynamics during and after passing through conical intersections.

Shunsuke Adachi1, Tom Schatteburg, Alexander Humeniuk

  • 1Department of Chemistry, Graduate School of Science, Kyoto University, Kitashirakawa Oiwakecho, Sakyo-ku, Kyoto 606-8502, Japan. suzuki@kuchem.kyoto-u.ac.jp.

Physical Chemistry Chemical Physics : PCCP
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Summary
This summary is machine-generated.

Ultrafast dynamics of furan molecules were observed using time-resolved photoelectron spectroscopy. Most excited furan molecules return to the ground state, while a small fraction isomerizes via a ring-puckering conical intersection.

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Area of Science:

  • Chemical Physics
  • Molecular Dynamics
  • Spectroscopy

Background:

  • Conical intersections (CIs) are crucial for understanding photochemical reactions.
  • Furan's ππ* photoexcitation involves a significant ring-puckering conical intersection.

Purpose of the Study:

  • To investigate the ultrafast dynamics of furan following photoexcitation.
  • To elucidate the role of the ring-puckering conical intersection in furan's photochemical fate.

Main Methods:

  • Time-resolved photoelectron spectroscopy utilizing vacuum-ultraviolet (VUV) probe pulses.
  • Observation of molecular dynamics on femtosecond timescales.

Main Results:

  • The study successfully observed ultrafast dynamics of furan after excitation.
  • More than 90% of excited furan molecules returned to the ground state.
  • Approximately 10% of molecules underwent isomerization after traversing the ring-puckering CI.

Conclusions:

  • The ring-puckering conical intersection is a key pathway in furan photochemistry.
  • Furan exhibits efficient radiationless decay back to the ground state.
  • A minor but significant channel leads to isomer formation through the CI.