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Plasmonic superradiance in metallo-dielectric nanohybrids

Pierre Fauché

Published Jan 1, 2016• 0 citations
Publisher

Abstract

Hybridization of quantum emitters and plasmonic nanostructures has attracted much attention over the last years, due to their potential use as plasmon-based nanolasersor to achieve long-range quantum bit entanglement. Recent theoretical studies suggest that the plasmonic field can induce efficient cross-talking between emitters and lead to the formation of collective superradiant states. In this thesis, we developed a theoretical modelable to analyse collective effects in large ensemble of dipoles coupled by an electromagnetic nanoresonator. We experimentally investigated the plasmon-mediated superradiance of organic emitters grafted at a well-controlled distance from a metal nanosphere at room temperature. We report on the measured decay rates of these hybrid structures at the ensemble and single object levels. We find that the decay rate increases i) with the number ofemitters and ii) as the spacing between the emitters and the metal core decreases, a direct and clear evidence of plasmonic superradiance. This trend was observed for two types of hybrid structures, differing both by the size of the metal core and the type of organic dye used as emitter. The observation of plasmonic superradiance at room temperature opens questions about the robustness of these collective states against decoherence mechanisms.This robustness is of major interest for potential applications of quantum systems at room temperature.

DOI
10.70675/a63d9ae9z2362z4096zb9cfz0ea687684461

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Hybridization of quantum emitters and plasmonic nanostructures has attracted much attention over the last years, due to their potential use as plasmon-based nanolasersor to achieve long-range quantum bit entanglement. Recent theoretical studies suggest that the plasmonic field can induce efficient cross-talking between emitters and lead to the formation of collective superradiant states. In this thesis, we developed a theoretical modelable to analyse collective effects in large ensemble of dipoles coupled by an electromagnetic nanoresonator. We experimentally investigated the plasmon-mediated superradiance of organic emitters grafted at a well-controlled distance from a metal nanosphere at room temperature. We report on the measured decay rates of these hybrid structures at the ensemble and single object levels. We find that the decay rate increases i) with the number ofemitters and ii) as the spacing between the emitters and the metal core decreases, a direct and clear evidence of plasmonic superradiance. This trend was observed for two types of hybrid structures, differing both by the size of the metal core and the type of organic dye used as emitter. The observation of plasmonic superradiance at room temperature opens questions about the robustness of these collective states against decoherence mechanisms.This robustness is of major interest for potential applications of quantum systems at room temperature.
Superradiance plasmonique dans des nanohybrides métallo-diélectriques Hybridization of quantum emitters and plasmonic nanostructures has attracted much attention over the last years, due to their potential use as plasmon-based nanolasersor to achieve long-range quantum bit entanglement. Recent theoretical studies suggest that the plasmonic field can induce efficient cross-talking between emitters and lead to the formation of collective superradiant states. In this thesis, we developed a theoretical modelable to analyse collective effects in large ensemble of dipoles coupled by an electromagnetic nanoresonator. We experimentally investigated the plasmon-mediated superradiance of organic emitters grafted at a well-controlled distance from a metal nanosphere at room temperature. We report on the measured decay rates of these hybrid structures at the ensemble and single object levels. We find that the decay rate increases i) with the number ofemitters and ii) as the spacing between the emitters and the metal core decreases, a direct and clear evidence of plasmonic superradiance. This trend was observed for two types of hybrid structures, differing both by the size of the metal core and the type of organic dye used as emitter. The observation of plasmonic superradiance at room temperature opens questions about the robustness of these collective states against decoherence mechanisms.This robustness is of major interest for potential applications of quantum systems at room temperature.
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.
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.
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.
We investigate the long-range coupling of individual atoms coupled to plasmon modes of metallic nanostructures. Placing a pair of emitters along a thin metallic wire, we observe a strong, wire- mediated long-range interaction between the emitters. As a result, super- and subradiance can occur over distances large compared to the resonant wavelength. The states with enhanced or suppressed decay rate are the symmetric or anti-symmetric single-excitation states. Coupling more atoms to a wire network with a nontrivial coupling topology leads to interesting entangled subradiant states of the system. A similar long-range superradiance effect can be observed when two emitters are coupled by a metamaterial slab (also known as a perfect lens) having a refractive index n=-1. Besides the modification of decay rates, dipole-dipole shifts enter due to the plasmon-mediated interaction. Based on the superradiance effect, we propose setups for building a two-qubit quantum phase gate for quantum emitters coupled by a nanowire and a perfect lens, respectively, where the qubits are strongly interacting and individually addressable at the same time.