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Related Experiment Videos

Ultrafast [2 + 2]-cycloaddition in norbornadiene.

Werner Fuss1, Kumbil Kuttan Pushpa, Wolfram E Schmid

  • 1Max-Planck-Institut für Quantenoptik, D-85741, Garching, Germany.

Photochemical & Photobiological Sciences : Official Journal of the European Photochemistry Association and the European Society for Photobiology
|March 28, 2003
PubMed
Summary

Norbornadiene excitation at 200 nm populates pi(pi*) and Rydberg states. Ultrafast relaxation occurs through conical intersections, with Rydberg states merging into the pi(pi*) pathway within 420 fs.

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Area of Science:

  • Photochemistry
  • Physical Chemistry
  • Molecular Dynamics

Background:

  • Norbornadiene (bicyclo[2.2.1]hepta-2,5-diene) is a model system for studying photochemical reactions.
  • Understanding excited-state dynamics is crucial for controlling chemical transformations.

Purpose of the Study:

  • To investigate the initial excited states populated by 200 nm excitation of norbornadiene.
  • To elucidate the relaxation pathways and timescales of these excited states.
  • To explore the role of conical intersections in the deactivation process.

Main Methods:

  • Transient nonresonant ionization was used to monitor excited-state populations.
  • Time-resolved spectroscopy provided information on relaxation dynamics.
  • Theoretical calculations informed the understanding of conical intersections.

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Main Results:

  • Excitation at 200 nm populates both a second pi(pi*) state and a Rydberg state in parallel.
  • The pi(pi*) state population decays in multiple steps with time constants of 5, 31, and 55 fs.
  • The Rydberg state population converges to the pi(pi*) surface within 420 fs.
  • Conical intersections, particularly one involving symmetry breaking, facilitate rapid relaxation.

Conclusions:

  • Norbornadiene exhibits complex excited-state dynamics involving parallel relaxation pathways.
  • Conical intersections play a critical role in the efficient deactivation to the ground state.
  • The study provides insights into the ultrafast photochemical behavior of conjugated dienes.