Picosecond time-resolved CARS spectroscopy of a mixed excited singlet state of diphenylhexatriene

Sebastian Wachsmann-Hogiu, W. Werncke, M. Pfeiffer, A. Lau, T. Steinke

Research output: Contribution to journalArticle

16 Scopus citations

Abstract

Time-resolved coherent antistokes Raman spectroscopy (CARS) spectra from an excited singlet state of diphenylhexatriene (DPH) are reported. As determined from the CARS measurements, the excited-state population increases on a sub-picosecond time scale after excitation in the 1Ag-1Bu absorption band. We observe two strongly upshifted and anomalously broadened resonances in the double-bond stretching region. According to our semi-empirical calculations of vibrational frequencies, they can be assigned to polyenic p-chain modes of the 1Bu and 2Ag states, respectively. Frequency shifts as well as broadenings are extremely solvent-dependent, indicating a strong influence on the excited-state conformations. Our time-resolved measurements support a mixed excited singlet state with drastically different geometries of the local minima.

Original languageEnglish (US)
Pages (from-to)8-16
Number of pages9
JournalChemical Physics Letters
Volume287
Issue number1-2
StatePublished - Apr 24 1998
Externally publishedYes

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Spectroscopy
  • Atomic and Molecular Physics, and Optics

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