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Title: Molecular Emission near Metal Interfaces: The Polaritonic Regime

Journal Article · · Journal of Physical Chemistry Letters

The strong coupling of a dense layer of molecular excitons with surface-plasmon modes in a metal gives rise to polaritons (hybrid light–matter states) called plexcitons. Surface plasmons cannot directly emit into (or be excited by) free-space photons due to the fact that energy and momentum conservation cannot be simultaneously satisfied in photoluminescence. Most plexcitons are also formally nonemissive, even though they can radiate via molecules upon localization due to disorder and decoherence. However, a fraction of them are bright even in the presence of such deleterious processes. Here in this Letter, we theoretically discuss the superradiant emission properties of these bright plexcitons, which belong to the upper energy branch and reveal huge photoluminescence enhancements compared to bare excitons, due to near-divergences in the density of photonic modes available to them. Our study generalizes the well-known problem of molecular emission next to a metal interface to the polaritonic regime.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); City Univ. of New York (CUNY), NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0001088; SC0017760
OSTI ID:
1566535
Journal Information:
Journal of Physical Chemistry Letters, Vol. 9, Issue 22; ISSN 1948-7185
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 16 works
Citation information provided by
Web of Science

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Cited By (2)

Light-emitting metasurfaces journal July 2019
Manipulating optical nonlinearities of molecular polaritons by delocalization journal September 2019