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Vibronic coherence evolution in multidimensional ultrafast photochemical processes.

James D Gaynor1, Jason Sandwisch1, Munira Khalil2

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Understanding ultrafast energy transfer in photoexcited molecules is key. Multidimensional electronic-vibrational spectroscopy reveals how vibronic couplings drive charge separation and coherence in transition metal complexes.

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Area of Science:

  • Physical Chemistry
  • Spectroscopy
  • Molecular Dynamics

Background:

  • Efficient energy transfer in photoexcited molecules relies on complex electronic, vibrational, and vibronic couplings.
  • Experimentally characterizing the time-evolving vibronic states governing these processes remains challenging.

Purpose of the Study:

  • To identify time-dependent excited state vibronic couplings in a photoexcited transition metal complex.
  • To elucidate the mechanisms of ultrafast intersystem crossing and subsequent relaxation.

Main Methods:

  • Utilized multidimensional electronic-vibrational spectroscopy.
  • Investigated couplings involving multiple electronic states and high/low-frequency vibrations.

Main Results:

  • Discovered an excited state vibronic mechanism driving long-lived charge separation (~600 fs).
  • Observed electronic delocalization via nonadiabatic internal conversion driven by a 50 cm⁻¹ coupling.
  • Characterized vibronic coherence transfer lasting ~1 picosecond.

Conclusions:

  • Multidimensional electronic-vibrational spectroscopy can elucidate complex, non-equilibrium energy and charge transfer mechanisms.
  • Detailed insights into molecular dynamics involving multiple coordinates were achieved.