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Rotamer-Specific Photoisomerization of Difluorostilbenes from Transient Absorption and Transient Raman Spectroscopy.

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Photoisomerization dynamics of difluorostilbenes were investigated using transient absorption and Raman spectroscopy. Differences in rotamer populations significantly impact excited-state decay pathways.

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Area of Science:

  • Photochemistry
  • Spectroscopy
  • Computational Chemistry

Background:

  • Photoisomerization is a fundamental photochemical process.
  • The conformational landscape of molecules influences their excited-state dynamics.
  • Fluorinated stilbenes are of interest due to their unique electronic properties.

Purpose of the Study:

  • To investigate the photoisomerization of 2,2'-, 3,3'-, and 4,4'-difluorostilbene (F2, F3, F4).
  • To elucidate the role of molecular conformation and rotamers in excited-state decay.
  • To correlate experimental spectroscopic data with theoretical calculations.

Main Methods:

  • Broadband transient absorption (TA) spectroscopy.
  • Femtosecond stimulated Raman (FSR) spectroscopy.
  • Density Functional Theory (DFT) and Time-Dependent DFT (TDDFT) calculations.

Main Results:

  • F2 and F3 exhibit complex biexponential excited-state decays due to multiple rotamers, unlike F4 which shows a monoexponential decay.
  • Decay times and rotamer populations were quantified and found to agree with theoretical predictions.
  • Pure rotamer spectra were extracted by global fitting of TA and FSR data.

Conclusions:

  • Molecular conformation and the presence of distinct rotamers critically influence the photoisomerization dynamics of difluorostilbenes.
  • Combined experimental and computational approaches provide detailed insights into excited-state processes.
  • The study successfully characterized the spectral properties of ground and excited states for different rotamers.