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Charge Transfer Driven Structural Relaxation in a Push-Pull Azobenzene Dye-Semiconductor Complex.

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Photoexcited isomerization of para-Methyl Red differs in isolation versus on TiO2. On TiO2, electron transfer prevents isomerization, leading to vibronic relaxation instead.

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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Quantum Dynamics

Background:

  • Azo-compounds exhibit unique photoexcited structural dynamics.
  • These dynamics can be altered by forming charge transfer complexes, e.g., with semiconductor surfaces.
  • Understanding these changes is crucial for applications in photochromism and photocatalysis.

Purpose of the Study:

  • To investigate the photoexcited structural dynamics of para-Methyl Red (pMR).
  • To compare the dynamics of isolated pMR with its charge transfer complex on TiO2.
  • To elucidate the influence of electron transfer on isomerization pathways.

Main Methods:

  • Employed a quantum-classical self-consistent approach.
  • Integrated nonadiabatic excited-state electronic quantum dynamics with molecular mechanics.
  • Simulated pMR in the gas phase and on the anatase TiO2 (101) surface.

Main Results:

  • Isolated pMR undergoes trans-to-cis isomerization via a pedal-like torsion, similar to azobenzene.
  • In the pMR/TiO2 complex, photoexcitation leads to rapid electron injection into TiO2 (τ ≈ 5 fs).
  • No isomerization was observed in the pMR/TiO2 complex; instead, vibronic relaxation and hole wavepacket delocalization occurred.

Conclusions:

  • The pathway of photoexcited structural dynamics in azo-compounds is fundamentally altered by heterogeneous charge transfer complex formation.
  • Electron transfer to TiO2 effectively quenches the isomerization pathway of para-Methyl Red.
  • The study highlights the critical role of electron transfer dynamics in controlling molecular photoreactions at interfaces.