Time-resolved photoelectron imaging of ultrafast S2 → S1 internal conversion through conical intersection in pyrazine

Yoshi Ichi Suzuki, Takao Fuji, Takuya Horio, Toshinori Suzuki

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76 Citations (Scopus)

Abstract

A nonadiabatic electronic transition through a conical intersection was studied by pump-probe photoelectron imaging spectroscopy with a 22 fs time resolution in the benchmark polyatomic molecule of pyrazine and deuterated pyrazine. The lifetimes of the S2 state of pyrazine and deuterated pyrazine were determined to be 22±3 fs by the global fitting of the time-energy maps of photoelectron kinetic energy (PKE) distributions. The lifetime of S3 was determined to be 40-43 fs. Two-dimensional maps of photoelectron distributions were obtained for time (t) and PKE, and individual PKE distributions upon ionization from S2 and S1 were extracted. Quantum beat with an approximately 50 fs period was observed after the S2 → S1 internal conversion, which was attributed to the totally symmetric vibration μ6a in S1.

Original languageEnglish
Article number174302
JournalJournal of Chemical Physics
Volume132
Issue number17
DOIs
Publication statusPublished - May 7 2010
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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