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Unified theory of internal conversion and fluorescence under macroscopic quantum electrodynamics framework
Chih-En Shen1,2, Hung-Sheng Tsai1,2, Liang-Yan Hsu1,2,3
1Department of Chemistry, National Taiwan University, Taipei 10617, Taiwan.
The Journal of Chemical Physics
|November 6, 2025
Summary
This study unifies fluorescence and internal conversion (IC) using macroscopic quantum electrodynamics (QED). It reveals that radiative and non-radiative processes compete, with cavity loss influencing outcomes in photonic environments.
Area of Science:
- Quantum Chemistry
- Photochemistry
- Spectroscopy
Background:
- Understanding molecular photophysics requires accounting for both radiative and non-radiative decay pathways.
- Existing models often treat these processes separately, especially in complex photonic environments.
Purpose of the Study:
- To develop a unified first-principles theory for fluorescence and internal conversion (IC) within macroscopic quantum electrodynamics (QED).
- To investigate the interplay between radiative and non-radiative processes in engineered photonic systems.
Main Methods:
- Formulation of a unified theory based on macroscopic quantum electrodynamics (QED).
- First-principles simulations incorporating molecular properties and photonic environments.
- Analysis of radiative (fluorescence) and non-radiative (IC, QED-NAE) decay channels.
Main Results:
- Identified IC, fluorescence, and two quantum electrodynamic non-adiabatic emission (QED-NAE) channels as non-adiabatic processes.
- Validated established emitter-surface interaction models and quantified vibrational overlap contributions.
- Demonstrated that cavity loss dictates the competition between fluorescence and QED-NAE, favoring QED-NAE in low-loss cavities.
Conclusions:
- The unified QED framework provides a comprehensive description of photonic non-adiabatic phenomena.
- This work enables deeper investigation into electron-nucleus-photon and electron-nucleus-polariton interactions.
- Opens new avenues for designing photochemical processes by controlling radiative and non-radiative decay.
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