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We present a new theory for Stark fluorescence (SF) in molecular aggregates, revealing that charge-transfer (CT) states significantly alter SF spectra. This method simplifies calculations by focusing on one-exciton states.

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Area of Science:

  • * Physical Chemistry
  • * Spectroscopy
  • * Theoretical Chemistry

Background:

  • * Stark fluorescence (SF) is a sensitive probe of molecular electronic structure.
  • * Understanding SF in molecular aggregates requires accounting for excited state interactions.
  • * Charge-transfer (CT) states can significantly influence optical properties.

Purpose of the Study:

  • * To develop a theoretical framework for Stark fluorescence (SF) in molecular aggregates.
  • * To investigate the impact of excited state mixing, including charge-transfer (CT) states, on SF spectra.
  • * To provide a simplified approach for calculating SF response without needing two-exciton states.

Main Methods:

  • * Development of theory for SF incorporating excited state mixing (including CT states).
  • * Application of the sum-over-state approach and modified rotating wave approximation.
  • * Calculation of SF spectral profiles using standard and modified Redfield theories for lineshapes.

Main Results:

  • * The theory allows SF interpretation using only one-exciton state calculations.
  • * Charge-transfer (CT) states dramatically alter SF spectrum shape and amplitude.
  • * SF responses are more sensitive to exciton-CT mixing than Stark absorption.

Conclusions:

  • * The developed theory offers a simplified yet powerful tool for analyzing SF in molecular aggregates.
  • * Exciton-CT mixing plays a crucial role in shaping SF spectra, providing enhanced sensitivity.
  • * The Redfield picture's limitations include neglecting dynamic localization in mixed exciton-CT configurations.