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Journal Article

Electrically driven single-photon superradiance from molecular chains in a plasmonic nanocavity


Sandoghdar,  Vahid
Sandoghdar Division, Max Planck Institute for the Science of Light, Max Planck Society;

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Luo, Y., Chen, G., Zhang, Y., Zhang, L., Yu, Y., Kong, F., et al. (2019). Electrically driven single-photon superradiance from molecular chains in a plasmonic nanocavity. Physical Review Letters, 122: 233901. doi:10.1103/PhysRevLett.122.233901.

Cite as: http://hdl.handle.net/21.11116/0000-0003-BAC6-C
We demonstrate single-photon superradiance from artificially constructed nonbonded zinc-phthalocyanine molecular chains of up to 12 molecules. We excite the system via electron tunneling in a plasmonic nanocavity and quantitatively investigate the interaction of the localized plasmon with single-exciton superradiant states resulting from dipole-dipole coupling. Dumbbell-like patterns obtained by subnanometer resolved spectroscopic imaging disclose the coherent nature of the coupling associated with superradiant states while second-order photon correlation measurements demonstrate single-photon emission. The combination of spatially resolved spectral measurements with theoretical considerations reveals that nanocavity plasmons dramatically modify the linewidth and intensity of emission from the molecular chains, but they do not dictate the intrinsic coherence of the superradiant states. Our studies shed light on the optical properties of molecular collective states and their interaction with nanoscopically localized plasmons.