Multiple interacting photonic modes in strongly coupled organic microcavities.

Area of Science:

• Quantum optics
• Molecular materials science
• Cavity quantum electrodynamics

Background:

• Room-temperature cavity quantum electrodynamics (CQED) with molecular materials is promising for controlling quantum degrees of freedom.
• Strong coupling in molecular ensembles typically necessitates high densities and field confinement, leading to disorder and structured photonic states.
• The impact of these complexities on CQED models developed for atoms and inorganic semiconductors is not fully understood.

Purpose of the Study:

• To investigate the conditions and limitations of strong light-matter coupling in molecular ensembles within optical cavities.
• To analyze the role of molecular disorder and multi-mode resonators in CQED.
• To determine if vacuum Rabi splitting is a sufficient indicator of coherent light-matter interaction in complex molecular systems.

Main Methods:

• Microscopic quantum description of molecular ensembles.
• Modeling within realistic multimode optical resonators.
• Analysis of linear spectroscopy and vacuum Rabi splitting.
• Investigation of photonic dissipation channels.

Main Results:

• Vacuum Rabi splitting is a necessary but not sufficient metric for strong light-matter coupling.
• In low-finesse, multi-mode cavities, molecular dipoles can hybridize with photonic dissipation.
• Vacuum-induced dissipative processes limit the achievable light-matter coherence.

Conclusions:

• Standard CQED metrics may be insufficient for molecular systems due to complexities like disorder and multi-mode effects.
• Dissipative processes arising from cavity modes can hinder the realization of robust quantum coherence.
• Further theoretical and experimental work is needed to fully understand and harness CQED in molecular materials.