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We extended the monomer transition density approach for spin multiplicity-altering excitation energy transfer (EET). This method accurately calculates triplet-singlet coupling for systems like platinum complexes and fluorescein derivatives.

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Area of Science:

  • Quantum Chemistry
  • Photochemistry
  • Spectroscopy

Background:

  • Excitation energy transfer (EET) is crucial in photochemistry.
  • Spin multiplicity-altering EET, like triplet-singlet transfer, is challenging to model.
  • Accurate theoretical methods are needed to understand these processes.

Purpose of the Study:

  • To extend the monomer transition density approach for spin multiplicity-altering EET.
  • To develop a computationally feasible method for triplet-singlet coupling.
  • To validate the approach with a model system.

Main Methods:

  • Utilized complex-valued wave functions from DFT-based multireference spin-orbit coupling configuration interaction.
  • Generated one-particle transition density matrices for donor and acceptor molecules.
  • Contracted density matrices with two-electron integrals, leveraging symmetry relations.

Main Results:

  • Developed a computationally feasible method for triplet-singlet coupling calculations.
  • Applied the method to a platinum complex (AG97) and fluorescein (FITC) system.
  • Estimated a Förster radius of approximately 35 Å for the model system.
  • Found minimal error from the dipole approximation for separations near and beyond the Förster radius.

Conclusions:

  • The extended monomer transition density approach is effective for spin multiplicity-altering EET.
  • The method provides accurate estimations for Förster radius and coupling.
  • This work facilitates theoretical studies of complex photochemical processes.