Interplay between static and dynamic disorder: Contrasting effects on dark state population inside a cavity.

Area of Science:

• Quantum Optics
• Physical Chemistry
• Spectroscopy

Background:

• Strong light-matter interactions in optical cavities are promising but affected by inherent molecular disorder.
• Realistic molecular systems, especially in solution, exhibit both static and dynamic disorder.

Purpose of the Study:

• To explore the steady-state optical response of molecular emitters in a lossy cavity under combined static and dynamic disorder.
• To analyze the interplay between disorder, dark states, and polariton states in strong coupling regimes.

Main Methods:

• Analysis of transmission spectra.
• Measurement of molecular energy change.
• Investigation of dark state population dynamics.

Main Results:

• Static and dynamic disorders have contrasting effects on dark state population.
• Rabi splitting shows inversion with increasing disorder, influenced by the interplay of both disorder types.
• A novel dark state-induced polariton linewidth narrowing mechanism was identified, distinct from motional narrowing.

Conclusions:

• Dark states play a critical role in modulating polariton properties under disorder.
• The findings provide mechanistic insights into strong light-matter interactions in disordered systems.
• Establishes a foundation for advancements in polariton chemistry and strong coupling spectroscopy.