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Scientific Reports

Radiative coupling of two quantum emitters in arbitrary metallic nanostructures

JingFeng Liu, Gengyan Chen, Lingyan Li, Renming Liu, Wei Li, Guanghui Liu, Feng Wu, Yongzhu Chen

Published Apr 27, 2022• 8 citations
Publisher

Abstract

We propose a general formalism beyond Weisskopf-Wigner approximation to efficiently calculate the coupling matrix element, evolution spectrum and population evolution of two quantum emitters in arbitrary metallic nanostructures. We demonstrate this formalism to investigate the radiative coupling and decay dynamics of two quantum emitters embedded in the two hot spots of three silver nano-spheroids. The vacuum Rabi oscillation in population evolution and the anti-crossing behavior in evolution spectrum show strong radiative coupling is realized in this metallic nanostructure despite its strong plasmon damping. Our formalism can serve as a flexible and efficient calculation tool to investigate the distant coherent interaction in a large variety of metallic nanostructures, and may be further developed to handle the cases for multiple quantum emitters and arbitrary dielectric-metallic hybrid nanostructures.

DOI
10.1038/s41598-022-10624-y

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We propose a general formalism beyond Weisskopf-Wigner approximation to efficiently calculate the coupling matrix element, evolution spectrum and population evolution of two quantum emitters in arbitrary metallic nanostructures. We demonstrate this formalism to investigate the radiative coupling and decay dynamics of two quantum emitters embedded in the two hot spots of three silver nano-spheroids. The vacuum Rabi oscillation in population evolution and the anti-crossing behavior in evolution spectrum show strong radiative coupling is realized in this metallic nanostructure despite its strong plasmon damping. Our formalism can serve as a flexible and efficient calculation tool to investigate the distant coherent interaction in a large variety of metallic nanostructures, and may be further developed to handle the cases for multiple quantum emitters and arbitrary dielectric-metallic hybrid nanostructures.
Photon-mediated coherent interaction determines the decay dynamics of quantum emitters and facilitates on-chip quantum manipulation for quantum information processing. We derive a general formalism to efficiently and flexibly simulate the radiative coupling between two two-level quantum emitters in arbitrary dielectric nanostructures, based on which, the decay dynamics of the two quantum emitters can be obtained. We demonstrate this formalism to investigate the two quantum dots embedded in the photonic crystal L3 cavity. The anticrossing behavior in the evolution spectrum and the vacuum Rabi oscillation in the populations of the two quantum dots can be simulated in both zero and small dot-dot detuning case. Our formalism can serve as a flexible and efficient theoretical tool and may be further developed to handle the cases for different initial states, multiple quantum emitters, and arbitrary metallic nanostructures.
Abstract Strong radiative coupling realizes coherent exchange of single excitation between two quantum emitters, while their dipole orientation influences the coupling strength in anisotropic environments. We propose a silver nano-arc with arbitrary radian which can support two hot spots of electric field with radian-independent resonant wavelength. Two quantum emitters resonant with the cavity mode, embedded inside the two hot spots and oriented along the nano-arc axis, can realize strong radiative coupling, verified by the large splitting and anti-crossing behavior in the spectrum and the population oscillation in the time domain. All these signatures of strong radiative coupling are robust against the nano-arc’s curvature. Our work provides a flexible approach to realize strong radiative coupling between two quantum emitters with arbitrary mutual orientation and facilitates quantum information processing.
We present results on the controlled dynamics of an externally driven four-level quantum emitter coupled to a plasmonic metamaterial, specifically a periodic two-dimensional array of metal-coated dielectric nanospheres. For the study of the system's dynamics, we combine the density matrix approach for the quantum emitter with ab initio electromagnetic calculations for the plasmonic nanostructure. We then present results for the time evolution of the populations of the different levels of the quantum emitter in both the presence and the absence of the plasmonic nanostructure. The dependence of the population dynamics to different distances of the quantum emitter from the plasmonic nanostructure is also studied.
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.
It has been recently shown that the placement of a three-level V\mathsf{V}V-type quantum emitter in the proximity of metallic nanostructures can create dynamics similar to that of quantum interference in spontaneous emission. Here we continue this work and present results on the population dynamics of a three-level V-type quantum emitter for various initial conditions in the presence of a two-dimensional array of metal-coated dielectric nanospheres.
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.