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Disorder-Induced Spectral Splitting versus Rabi Splitting under Strong Light-Matter Coupling.
1Department of Chemistry and Biochemistry, University of Notre Dame, Indiana 46556, United States.
The Journal of Physical Chemistry Letters
|June 24, 2025
Summary
Strong disorder in light-matter interactions can mimic Rabi splitting, a hallmark of polariton formation. This study reveals a new mechanism for spectral splitting induced by dark modes, challenging conventional understanding.
Area of Science:
- Optics and Photonics
- Condensed Matter Physics
- Materials Science
Background:
- Strong light-matter coupling typically leads to Rabi splitting and polariton formation.
- Disorder effects are often treated as perturbative, not a dominant factor.
- Distinguishing between polaritons and disorder-induced phenomena can be challenging.
Purpose of the Study:
- Investigate the impact of strong disorder on light-matter interactions.
- Explore spectral splitting mechanisms beyond traditional Rabi splitting.
- Analyze disordered molecular ensembles near plasmonic nanostructures.
Main Methods:
- Developed a nonperturbative effective model.
- Employed classical electrodynamics simulations.
- Studied absorption spectra of disordered molecular ensembles coupled to plasmonic nanodisks.
Main Results:
- Strong disorder induces spectral splitting that resembles Rabi splitting.
- This splitting originates from dark modes, not polaritons.
- Demonstrated disorder-induced spectral splitting in absorption spectra.
Conclusions:
- Spectral splitting can arise from both polaritons (strong coupling) and dark modes (strong disorder).
- Distinguishing these phenomena solely from steady-state absorption spectra is problematic.
- Challenges the conventional association of Rabi splitting exclusively with polaritons.
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