Electrically Driven Single-Photon Superradiance from Molecular Chains in a Plasmonic Nanocavity

Area of Science:

• Quantum optics
• Molecular physics
• Plasmonics

Background:

• Superradiance describes collective spontaneous emission from quantum emitters.
• Understanding light-matter interactions at the nanoscale is crucial for quantum technologies.

Purpose of the Study:

• To demonstrate and investigate single-photon superradiance in engineered molecular chains.
• To explore the influence of plasmonic nanocavities on superradiant emission from molecular systems.

Main Methods:

• Fabrication of nonbonded zinc-phthalocyanine molecular chains (up to 12 molecules).
• Excitation via electron tunneling within a plasmonic nanocavity.
• Subnanometer resolved spectroscopic imaging and second-order photon correlation measurements.

Main Results:

• Demonstrated single-photon superradiance from molecular chains.
• Observed dumbbell-like patterns indicating coherent coupling in superradiant states.
• Showed nanocavity plasmons modify emission intensity and linewidth but not intrinsic coherence.

Conclusions:

• Plasmonic nanocavities can enhance and control light emission from molecular ensembles.
• The intrinsic coherence of superradiant states in molecular chains is independent of the nanocavity.
• Provides insights into collective optical properties of molecules and their interaction with nanoscale plasmons.