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Superradiance and Quantum Electrodynamics in the Presence of Surface Plasmons

Jérémie Choquette

Published Jan 1, 2012• 0 citations
Publisher

Abstract

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.

DOI
10.11575/prism/27935

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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 theoretically characterize the collective radiative behavior of NNN classical emitters near an interface between different dielectrics that supports the transfer of surface plasmon modes into the far-field of electromagnetic radiation. The phenomena of superradiance and surface plasmons can be combined to amplify the emitted radiation intensity SSS as S=AN2S0S=A{N}^{2}{S}_{0}S=AN2S0​ compared to a single emitter's intensity S0{S}_{0}S0​ in free space. For a practical case study within the article A=240A=240A=240, compared to A=1A=1A=1 in free space. We furthermore demonstrate that there are collective modes for which the intensity of the emitted radiation is suppressed by 2 orders of magnitude despite their supperadiant emission characteristics. A method to control the emission characteristics of the system and to switch from super- to subradiant behavior with a suitably detuned external driving field is devised.
Plasmons on the surface of a metal increase the light intensity by several orders of magnitude. To quantify the consequences of this phenomenon in quantum processes, we calculate the excitation probability for atoms near the surface, which are excited by a single-photon pulse. Using quantum electrodynamics in the presence of absorbing dielectrics, we predict that nonradiative decay in the metal will limit the excitation probability to about one-half of the maximum that could be achieved in the absence of such losses.
We develop a microscopic quantum theory of surface plasmon polaritons valid for arbitrary metal-dielectric geometries. Our framework is based on the Power-Zienau-Woolley representation of quantum electrodynamics, which provides an optimal separation between electronic and photonic degrees of freedom and is therefore particularly well suited for constructing quantum descriptions of polaritonic excitations in strongly dispersive media. Within this formulation, the fundamental electronic oscillator is identified as the bulk plasmon mode, which is nonperturbatively coupled to the radiative continuum of free photon modes. This coupling induces a geometry-dependent renormalization of the bulk plasma frequency, giving rise to confined plasmonic resonances. As specific applications, we recover the localized surface plasmon modes of metallic nanoparticles, including radiative frequency shifts and decay, as well as the exact dispersion relation of propagating surface plasmon polaritons at planar interfaces. Our quantum treatment further reveals that light-matter interactions at metal-dielectric interfaces are inherently in the ultrastrong coupling regime. As a result, in the quasistatic limit, the system exhibits unconventional ground-state quantum fluctuations that can be controlled through the refractive index. These results open new intriguing perspectives in the field of quantum plasmonics.
Enabling the confinement of light to a scale far below the one of conventional optics, surface plasmon polaritons (SPPs) induced by an electromagnetic field in a metal-dielectric interface supply an ideal system to explore strong quantized light-matter coupling. The fast matter-SPP population exchange reported in previous works makes it a candidate for spin manipulation, but such reversible dynamics asymptotically vanishes accompanying the quantum matter relaxing completely to its ground state. Here, we study the exact dissipative dynamics of a quantum emitter (QE) coupled to SPPs. It is interesting to find that, qualitatively different from conventional findings, the QE can be partially stabilized in its excited state even in the presence of the lossy metal. Our analysis reveals that it is the formation of a QE-SPP bound state which results in such suppressed dissipation. Enriching the decoherence dynamics of the QE in the lossy medium, our result is helpful to understand QE-SPP interactions and apply plasmonic nanostructures in quantum devices.
An ensemble of atoms coupled to the radiation field exhibits collective behaviours when the interatomic separation is comparable to the wavelength of photons emitted by the atoms. The collective coupling of the atoms with the electromagnetic field gives rise to coherent exchange interactions between the atoms. In addition, the spontaneous decay of photons from the ensemble becomes a collective process that can happen at a much faster (superradiant) or slower (subradiant) rate than that of a single atom. These processes affect the way that fluorescence light is scattered from the system when it is driven by a laser. However, little is known about the response of a dense atomic gas beyond the linear regime of very weak driving, due to the involved complexity of the problem. The first part of this thesis investigates how the presence of strong laser driving affects properties of the far-field fluorescence light emitted by the ensemble, such as the power spectrum and second order coherence. Depending on the strength of the driving laser and the particular arrangement of the atoms, the laser can modify considerably how the collective behaviours of the atomic ensemble are manifested in the fluorescence. The relative strengths of the coherent interaction and collective decay process are intrinsically linked to the way that the atoms couple to the radiation field; one cannot be changed without modifying the other. Altering the environment by, for example, placing the atoms near a surface or a waveguide, can change this relation significantly from that for atoms in free space. Therefore, modified environments represent a platform for the generation of otherwise inaccessible regimes of collective behaviour, with potential applications in quantum state engineering. The second part of this thesis provides a numerical investigation into how the collective properties of a dense atomic system can be manipulated by placing the atoms close to planar surfaces or an optical nanofiber. These structures modify the light-matter coupling by altering the electric field experienced by the atoms. It is shown that surfaces of metallic and dielectric materials can be used to either enhance or suppress the collective behaviours, depending on the particular system arrangement. In particular, the coupling of atoms with bound surface modes, such as the surface plasmon polaritons that are formed at an air-metal interface, is demonstrated to have a strong effect on the interactions. An optical nanofiber supports a set of fundamental guided modes, that propagate along the fiber. If the atoms are suitably polarised, then they will emit primarily into the guided modes travelling in one direction. By calculating and analysing the collective decay states of a chain of atoms placed near a nanofiber, it is demonstrated that the atom-fiber coupling leads to the formation of a superradiant mode that is preserved at large atomic separations. The presence of chiral emission is shown to introduce phase gradients to the collective modes.
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.