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We developed a new model for resonance energy transfer (RET) that includes energy dissipation. This model accurately describes ultrafast energy transfer in the strong coupling regime, occurring before donor relaxation.

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Area of Science:

  • Chemical Physics
  • Quantum Mechanics
  • Spectroscopy

Background:

  • Resonance energy transfer (RET) describes energy transfer between molecules.
  • The Förster model applies to weak coupling, assuming donor relaxation before transfer.
  • A more general model is needed for strong coupling, incorporating energy dissipation.

Purpose of the Study:

  • To present a dynamical, nonadiabatic model for RET that includes energy relaxation.
  • To accurately describe RET in both weak and strong coupling regimes.
  • To model molecular vibrations and energy dissipation.

Main Methods:

  • Developed an essential state formalism for RET pairs.
  • Treated molecular vibrations nonadiachronously.
  • Incorporated energy dissipation using the Redfield formalism.
  • Validated the model on an isolated dye and a RET pair.

Main Results:

  • The model accurately describes energy dissipation in isolated molecules across different timescales (fs to ns).
  • In the weak coupling regime, energy transfer occurs after donor internal conversion, consistent with the Förster model.
  • In the strong coupling regime, ultrafast energy transfer is observed before donor relaxation is complete.

Conclusions:

  • The developed model provides a more general description of RET, applicable to strong coupling regimes.
  • It accurately captures the interplay between energy transfer and relaxation dynamics.
  • This work advances the understanding of energy transfer processes in molecular systems.