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Carlos M Bustamante1, Esteban D Gadea1, Tchavdar N Todorov2

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This study models fluorescence with vibronic resolution. A semiclassical model (CEED) accurately predicts emission frequencies but fails to capture spectral amplitudes when de-excitation involves multiple states.

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Area of Science:

  • Quantum dynamics
  • Spectroscopy
  • Theoretical chemistry

Background:

  • Modeling real-time fluorescence with vibronic resolution is complex, requiring coupled quantum mechanics for light-matter interactions and phonons.
  • Decoupling internal conversion and radiative relaxation based on timescale differences simplifies modeling.

Purpose of the Study:

  • To simulate electron dynamics in fluorescence using a Redfield-derived master equation.
  • To evaluate the accuracy of the coherent electron electric-field dynamics (CEED) semiclassical model for the radiative stage of fluorescence.
  • To compare CEED results with full quantum electrodynamics (QED) for light-matter interaction modeling.

Main Methods:

  • Simulated electron dynamics using a master equation from the Redfield formalism.
  • Employed the coherent electron electric-field dynamics (CEED) semiclassical model for radiative relaxation.
  • Compared CEED predictions against full quantum electrodynamics (QED) calculations.

Main Results:

  • The CEED model accurately predicts emission frequencies, aligning with QED results.
  • CEED fails to reproduce correct spectral amplitudes during de-excitation to closely lying states.
  • This amplitude inaccuracy is attributed to the inherent mean-field nature of CEED.

Conclusions:

  • The CEED model offers accurate prediction of emission peak positions without prior Hamiltonian knowledge.
  • CEED's mean-field approximation limits its accuracy for spectral amplitudes in specific de-excitation scenarios.
  • This study highlights a critical limitation of CEED for light-matter interaction studies involving complex electronic states.