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Surface Science

Cooperative emission by two different atoms into surface plasmons

K.C. Liu, Thomas F. George

Published Dec 1, 1985• 4 citations
Publisher
DOI
10.1016/0039-6028(85)90705-8

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arXiv:1001.0422•Physical Review B•Aug 30, 2010•104 citations
We develop a theory of cooperative emission of light by an ensemble of emitters, such as fluorescing molecules or semiconductor quantum dots, located near a metal nanostructure supporting surface plasmon. The primary mechanism of cooperative emission in such systems is resonant energy transfer between emitters and plasmons rather than the Dicke radiative coupling between emitters. We identify two types of plasmonic coupling between the emitters, (i) plasmon-enhanced radiative coupling and (ii) plasmon-assisted nonradiative energy transfer, the competition between them governing the structure of system eigenstates. Specifically, when emitters are removed by more than several nm from the metal surface, the emission is dominated by three superradiant states with the same quantum yield as a single emitter, resulting in a drastic reduction of ensemble radiated energy, while at smaller distances cooperative behavior is destroyed by nonradiative transitions. The crossover between two regimes can be observed in distance dependence of ensemble quantum efficiency. Our numerical calculations incorporating direct and plasmon-assisted interactions between the emitters indicate that they do not destroy the plasmonic Dicke effect.
We develop a theory of cooperative emission of light by an ensemble of emitters, such as fluorescing molecules or semiconductor quantum dots, located near a metal nanostructure supporting surface plasmon. The primary mechanism of cooperative emission in such systems is resonant energy transfer between emitters and plasmons rather than the Dicke radiative coupling between emitters. We identify two types of plasmonic coupling between the emitters, (i) plasmon-enhanced radiative coupling and (ii) plasmon-assisted nonradiative energy transfer, the competition between them governing the structure of system eigenstates. Specifically, when emitters are removed by more than several nanometers from the metal surface, the emission is dominated by three superradiant states with the same quantum yield as a single emitter, resulting in a drastic reduction of ensemble radiated energy, while at smaller distances cooperative behavior is destroyed by nonradiative transitions. The crossover between two regimes can be observed in distance dependence of ensemble quantum efficiency. Our numerical calculations incorporating direct and plasmon-assisted interactions between the emitters indicate that they do not destroy the plasmonic Dicke effect.