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Physical Review Letters

Cooperative Emission of an Excited Molecular Monolayer into Surface Plasmons

R. Bonifacio, Hans Morawitz

Published Jun 28, 1976• 17 citations
Publisher

Abstract

We propose a new cooperative phenomenon: the conversion of the energy stored in a monolayer of fully excited molecules, located at a distance $D\ensuremath{\ll}{\ensuremath{\lambda}}_{f}$ (the fluorescence wave-length) from a metal or doped semiconductor, into the resonant surface-plasmon mode. The effect resembles Dicke's superradiance, with significant modifications---the coherent burst is a propagating surface-polariton mode.

DOI
10.1103/physrevlett.36.1559

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We propose a new cooperative phenomenon: the conversion of the energy stored in a monolayer of fully excited molecules, located at a distance D\ensuremath≪\ensuremathλfD\ensuremath{\ll}{\ensuremath{\lambda}}_{f}D\ensuremath≪\ensuremathλf​ (the fluorescence wave-length) from a metal or doped semiconductor, into the resonant surface-plasmon mode. The effect resembles Dicke's superradiance, with significant modifications---the coherent burst is a propagating surface-polariton mode.
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.
Surface plasmon polaritons are charge density waves of electrons in a metal, which are coupled to an electromagnetic field at a metal-dielectric interface. The electro- magnetic field associated with surface plasmons is confined, resulting in increased field intensities near the interface. Optical emitters placed near a metal film interact strongly with the surface plasmon modes present, not only modifying the radiation rates, but also the radiation profile. These emitters may be used to store and process information, and understanding their behaviour in the presence of a lossy metal film is important in determining the advantages and limitations of using surface plasmons. In this thesis, we wish to understand how we can optically control atoms by exploring two physical phenomena: first, the influence of surface plasmons on collective effects in an ensemble of emitters. Secondly, the single photon excitation of an emitter near a metal film. In the first case, we analyze the collective radiative behaviour of multiple classical emitters near a metal film that radiatively couple to the far-field through surface plasmon modes. We demonstrate that the contributions of dipolar image charges within the metal film significantly affect the cooperative emission of nearby sources, generating sub- and super-radiant emission that can be controlled with a suitably detuned external driving field. In the second case, we determine the excitation probability of an atom near a metal film by a single photon pulse that is time reversed. Using a quantum electro- dynamic description of absorbing dielectrics, we show that non-radiative decay will limit the excitation probability to about half of the maximum that could be achieved in the absence of losses.
Subradiant states of a finite subwavelength atomic chain in free space offer a powerful resource for photon storage. Yet their preparation and control remain challenging experimentally. A standard technique is to drive the atoms by a laser and observe the florescence light of the long-lived subradiant modes of excitation after the laser is switched off. However, these modes are highly degenerate and form an almost continuous band in the subradiant manifold. Here we propose a new method of exciting a given subradiant state by coupling atoms to a surface plasmon wave propagating along the interface with a metallic film. By controlling the chain/surface distance we may load, store and release photons in the atoms, making them a promising tool for future quantum memories.
Plasmonic superradiance originates from the plasmon mediated strong correlation that builds up between dipolar emitters coupled to a metal nanoparticle. This leads to a fast burst of emission so that plasmonic superradiance constitutes ultrafast and extremely bright optical nanosources of strong interest for integrated quantum nano-optics platforms. We elucidate the superradiance effect by establishing the dynamics of the system, including all features such as the orientation of the dipoles, their distance to the particle, and the number of active plasmon modes. We determine an optimal configuration for Purcell enhanced superradiance. We also show superradiance blockade at small distances.