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Scientific Reports

Influence of Surface Roughness on Strong Light-Matter Interaction of a Quantum Emitter-Metallic Nanoparticle System

Yuwei Lu, Lingyan Li, Jing-Feng Liu

Published May 1, 2018• 26 citations
Publisher

Abstract

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.

DOI
10.1038/s41598-018-25584-5

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•Jan 1, 2017•0 citations
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.
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.
ABSTRACT. We study theoretically the quantum optical properties of hybrid artificial molecules composed of an individual quantum emitter and a metallic nanoparticle. The coupling between the two systems can give rise to a Fano interference effect which strongly influences the quantum statistical properties of the scattered photons: a small frequency shift of the incident light field may cause changes in the intensity correlation function of the scattered field of orders of magnitude. The system opens a good perspective for applica-tions in active metamaterials and ultracompact single-photon devices. We also demonstrate with accurate scattering calculations that a system constituted by a single quantum emitter (a semiconductor quantum dot) placed in the gap between two metallic nanoparticles can display the vacuum Rabi splitting. 1.
We investigate excitation dynamics in the system of a quantum dipole emitter (QDE) coupled to a located nearby metal nanoparticle (MNP), which exhibits a dipolar localized surface plasmon (LSP) resonance at the frequency of the QDE radiative transition, in the presence of a strong external resonant electromagnetic field. Considering the QDE-field interactions in the regime of strong QDE-field coupling, we show that the feedback provided by the MNP on the QDE (due to the LSP excitation with the field generated by the dipole moment of the QDE transition) influences significantly the coherent process of Rabi oscillations, resulting in the occurrence of additional satellite frequencies in the radiation spectrum scattered by the QDE-MNP configuration. The relative ratio of high harmonics depends strongly on the QDE-MNP separation, an important characteristic feature that can be used for observing this effect and can be exploited, for example, for controlling distances at the nanoscale.
We propose a hybrid photonic-plasmonic resonant structure which consists of a metal nanoparticle (MNP) and a whispering-gallery-mode (WGM) microcavity. It is found that the hybrid mode enables a strong interaction between the light and matter, and the single-atom cooperativity is enhanced by more than two orders of magnitude compared to that in a bare WGM microcavity. This improvement originates from two aspects: the MNP offers a highly enhanced local field in the vicinity of an emitter, and, interestingly, the high-QQQ property of WGMs can be maintained in the presence of the MNP. Thus the present system has advantages over a single microcavity or a single MNP, and holds potential in quantum optics, nonlinear optics, and highly sensitive biosensing.
Quantum emitters near the surface of silver nanoparticles undergo Rabi oscillations in electronic population dynamics due to strong coupling with near-field multipole modes that are not radiative. Low-frequency nanoparticle dipole modes are radiative but do not couple strong enough to quantum emitters. These features limit the observation of strong coupling. Using macroscopic quantum electrodynamics theory within a Lorentzian pseudo-mode approximation for the non-Markovian interaction kernel, we demonstrate that by coating spherical silver nanoparticles with a thin molecular J-aggregate layer, the resulting core-shell plexciton resonance restructures the local electromagnetic vacuum at dipole-mode frequencies to enable Rabi oscillations for quantum emitters that otherwise would only undergo exponential population decay. Specifically, we show for quantum dot emitters in the near field of silver nanospheres of 20 nm radius, that weak-to-strong coupling crossovers can be induced using 2 nm J-aggregate shells. Our work demonstrates the potential of molecular aggregates to enable deep sub-wavelength structuring of the vacuum field for the observation of coherent quantum dynamics in optical nanocavities.