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Area of Science:

  • Photochemistry
  • Biophysics
  • Spectroscopy

Background:

  • All-trans-retinal (ATR) is essential for vision as the chromophore in photoreceptor proteins.
  • ATR's excited-state dynamics involve multiple electronic states (S2, S1, nπ*, ICT).
  • Distinguishing S1 and ICT lifetimes is challenging due to spectral overlaps, leading to competing hypotheses.

Purpose of the Study:

  • Investigate ATR's structural dynamics in different solvents.
  • Differentiate competing hypotheses on the intramolecular charge transfer (ICT) state's role.
  • Elucidate the influence of solvent properties on ATR photoisomerization pathways.

Main Methods:

  • Femtosecond stimulated Raman spectroscopy (FSRS).
  • Analysis of ATR in solvents with varying polarity and viscosity.

Main Results:

  • Identified two distinct photochemical pathways for ATR.
  • Solvent viscosity significantly affects isomerization in Channel 2 (via ICT), but not Channel 1 (via S1).
  • Isomerization in Channel 2 involves large-scale one-bond flip torsional motions.

Conclusions:

  • ATR isomerization mechanisms are solvent-dependent.
  • The ICT state plays a distinct role, influenced by solvent viscosity.
  • ATR isomerization differs from protein-bound rhodopsin's bicycle-pedal mechanism.