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arXiv:2102.10832 · Physical review. B./Physical review. B

Quantum surface effects in strong coupling dynamics

Vasilios D. Karanikolas, Ioannis Thanopulos, Joel D. Cox, Takashi Kuroda, Jun-ichi Inoue, N. Asger Mortensen, Emmanuel Paspalakis, Christos Tserkezis

Published Nov 12, 2021• 22 citations
arXivHTMLPDF

Abstract

Plasmons in nanostructured metals are widely utilized to trigger strong light-matter interactions with quantum light sources. While the nonclassical behavior of such quantum emitters (QEs) is well understood in this context, the role of quantum and surface effects in the plasmonic resonator is usually neglected. Here, we combine the Green's tensor approach with the Feibelman $d$-parameter formalism to theoretically explore the influence of quantum surface effects in metal-dielectric layered nanostructures on the relaxation dynamics of a proximal two-level QE. Having identified electron spill-out as the dominant source of quantum effects in jellium-like metals, we focus our study on sodium. Our results reveal a clear splitting in the emission spectrum, indicative of having reached the strong coupling regime, and, more importantly, non-Markovian relaxation dynamics of the emitter. Our findings establish that strong light-matter coupling is not suppressed by the emergence of nonclassical surface effects in the optical response of the metal.

DOI
10.1103/physrevb.104.l201405

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Plasmons in nanostructured metals are widely utilized to trigger strong light-matter interactions with quantum light sources. While the nonclassical behavior of such quantum emitters (QEs) is well understood in this context, the role of quantum and surface effects in the plasmonic resonator is usually neglected. Here, we combine the Green's tensor approach with the Feibelman ddd-parameter formalism to theoretically explore the influence of quantum surface effects in metal-dielectric layered nanostructures on the relaxation dynamics of a proximal two-level QE. Having identified electron spill-out as the dominant source of quantum effects in jellium-like metals, we focus our study on sodium. Our results reveal a clear splitting in the emission spectrum, indicative of having reached the strong coupling regime, and, more importantly, non-Markovian relaxation dynamics of the emitter. Our findings establish that strong light-matter coupling is not suppressed by the emergence of nonclassical surface effects in the optical response of the metal.
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We investigate the quantum optical properties of strong light-matter interaction between a quantum emitter and a metallic nanoparticle beyond idealized structures with a smooth surface. Based on the local coupling strength and macroscopic Green's function, we derived an exact quantum optics approach to obtain the field enhancement and light-emission spectrum of a quantum emitter. Numerical simulations show that the surface roughness has a greater effect on the near-field than on the far-field, and slightly increases the vacuum Rabi splitting on average. Further, we verified that the near-field enhancement is mainly determined by the surface features of hot-spot area.
A bound state between a quantum emitter (QE) and surface plasmon polaritons (SPPs) can be formed, where the excited QE will not relax completely to its ground state and is partially stabilized in its excited state after a long time. We develop some theoretical methods for investigating this problem and show how to form such a bound state and its effect on the non-Markovian decay dynamics. We put forward an efficient numerical approach for calculating the analytical part of the self-energy for frequency below the lower energy threshold. We also propose an efficient formalism for obtaining the long-time value of the excited-state population without calculating the eigenfrequency of the bound state or performing a time evolution of the system, in which the probability amplitude for the excited state in the steady limit is equal to one minus the integral of the evolution spectrum over the positive frequency range. With the above two quantities obtained, we show that the non-Markovian decay dynamics of an initially excited QE can be efficiently obtained by the method based on the Green's function expression for the evolution operator when a bound state exists. A general criterion for identifying the existence of a bound state is presented. The performances of the above methods are numerically demonstrated for a QE located around a metal nanosphere and in a gap plasmonic nanocavity. Numerical results show that these methods work well and the QE becomes partially stabilized in its excited state at a long time for the transition dipole moment beyond its critical value. In addition, it is also found that this critical value is heavily dependent on the distance between the QE and the metal surface, but nearly independent on the size of the nanosphere or the rod. Our methods can be utilized to understand the suppressed decay dynamics for a QE in an open quantum system and provide a general picture on how to form such a bound state.
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 theoretically study the dissipative dynamics of a quantum emitter placed near the planar surface of a metal supporting surface-plasmon excitations. The emitter-metal coupling regime can be tuned by varying some control parameters such as the qubit-surface separation and/or the detuning between characteristic frequencies. By using a Green's-function approach jointly with a time-convolutionless master equation, we analyze the non-Markovian dissipative features on the qubit time evolution in two cases of interest: (i) an undriven qubit initially prepared in its excited state and (ii) the evolution toward a steady state for a system driven by a laser field. For weak to moderate qubit-metal coupling strength, and on time scales large compared to the surface plasmon oscillation time, a Markovian approximation for the master-equation results to be adequate to describe the qubit main optical properties: surface enhancements of rate emission, optical spectra, and time-dependent photon-photon correlation functions. The qubit decay shows a crossover passing from being purely dissipative for small qubit-surface distances to plasmon emission for larger separations.