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Physical Review A

Excitation of atoms by single-photon pulses in the presence of surface plasmons

Jérémie Choquette, Karl-Peter Marzlin

Published Jun 29, 2012• 5 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.85.063841

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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.
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 examine the quantum dynamics of surface plasmons weakly coupled to optical soliton photons in a metal-dielectric-nonlinear Kerr medium interface. We consider a photon-number-dependent coupling model which is a heuristic extension of the classical soliton excitation of surface plasmons in the quantum limit. The coupling coefficient additionally depends on the distance between the dielectric and the metal. We propose a practical scheme to control the number of surface plasmons using a Gaussian variation of the metal-dielectric spatial separation. Our numerical simulations show that the curvature of the Gaussian distance profile can be used for controlling the number of surface plasmons.
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.
Heralded single surface plasmon polaritons are excited using photons generated via spontaneous parametric down conversion. The mean excitation rates, intensity correlations, and Fock state populations are studied. The observed dependence of the second-order coherence in our experiment is consistent with a linear uncorrelated Markovian environment in the quantum regime. Our results provide important information about the effect of loss for assessing the potential of plasmonic waveguides for future nanophotonic circuitry in the quantum regime.
Quantum Sensing Laser light can induce electronic excitations on metal surfaces. These excitations, or plasmons, are sensitive to the surface environment and are now routinely used in chemical and biological sensing applications. Dowran et al. show that the sensitivity of these plasmonic sensors can be enhanced by using quantum states of light. They replace the laser light (used in the classical configuration) with quantum light, in this case a twin beam of entangled photons; one beam is used as a reference and the other to excite the surface plasmons. They find an appreciable sensitivity enhancement in the quantum configuration. Moreover, the reduced light intensity could also prove useful for the detection of light-sensitive chemical or biological samples. Optica 5 , 628 (2018).
We study theoretically the quantum optical properties of hybrid molecules composed of an individual quantum dot and a metallic nanoparticle. We calculate the resonance fluorescence of this hybrid system. Its incoherent part, the one arising from nonlinear quantum processes, results to be enhanced by more than two orders of magnitude as compared to that in the absence of the metallic nanoparticle. Scattering spectra at different excitation powers and nonperturbative calculations of intensity-field correlation functions show that this system can act as a nonlinear ultra-compact two-photon switch for incident photons, where the presence (or absence) of a single incident photon field is sufficient to allow (or prevent) the scattering of subsequent photons. We also find that a small frequency shift of the incident light field may cause changes in the intensity field correlation function of orders of magnitude.