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Isotopic Effect in Double Proton Transfer Process of Porphycene Investigated by Enhanced QM/MM Method
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Theory for proton-coupled energy transfer.

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Proton-coupled energy transfer (PCEnT) involves energy and proton transfer. A new theory explains PCEnT rates, considering quantum proton motion and vibronic states, even for dark states.

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Area of Science:

  • Photochemistry and Photophysics
  • Quantum Mechanics
  • Chemical Kinetics

Background:

  • Proton-coupled energy transfer (PCEnT) links electronic excitation energy transfer with proton transfer.
  • Understanding PCEnT is crucial for designing novel photochemical systems.

Purpose of the Study:

  • Develop a general quantum mechanical theory for nonadiabatic PCEnT.
  • Derive an analytical expression for the PCEnT rate constant.
  • Investigate key features of PCEnT processes using model systems.

Main Methods:

  • Quantum mechanical treatment of the transferring hydrogen nucleus.
  • Description of PCEnT via nonadiabatic transitions between electron-proton vibronic states.
  • Derivation of a rate constant expression involving vibronic coupling and a spectral convolution integral.

Main Results:

  • The PCEnT rate constant is a sum over vibronic states, influenced by vibronic coupling and a spectral convolution integral.
  • Excited vibronic states can significantly contribute to the PCEnT rate.
  • Shared vibrational modes can modulate the PCEnT rate, and PCEnT can occur without spectral overlap.

Conclusions:

  • The developed theory provides a framework for interpreting experimental PCEnT data.
  • The theory highlights the importance of vibronic coupling and spectral convolution in PCEnT.
  • This work guides the design and discovery of new PCEnT systems.