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Physica Scripta

Strong radiative coupling between two quantum emitters with arbitrary mutual orientation via a silver nano-arc

Qingtai Xie, Jinpeng Wang, Jie Hong, Jing-Feng Liu, Guanghui Liu, Feng Wu, Yongzhu Chen, Gengyan Chen

Published Jul 16, 2024• 2 citations
Publisher

Abstract

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.

DOI
10.1088/1402-4896/ad63e0

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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 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.
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.
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 Quantum state control of two‐level emitters is fundamental for many information processing, metrology, and sensing applications. However, quantum‐coherent photonic control of solid‐state emitters has traditionally been limited to cryogenic environments, which are not compatible with implementation in scalable, broadly distributed technologies. In contrast, plasmonic nano‐cavities with deep sub‐wavelength mode volumes have recently emerged as a path toward room temperature quantum control. However, optimization, control, and modeling of the cavity mode volume are still in their infancy. Here recent demonstrations of plasmonic tip‐enhanced strong coupling (TESC) with a configurable nano‐tip cavity are extended to perform a systematic experimental investigation of the cavity‐emitter interaction strength and its dependence on tip position, augmented by modeling based on both classical electrodynamics and a quasinormal mode framework. Based on this work, a perspective for nano‐cavity optics is provided as a promising tool for room temperature control of quantum coherent interactions that could spark new innovations in fields from quantum information and quantum sensing to quantum chemistry and molecular opto‐mechanics.
The theoretical method to study strong coupling between an ensemble of quantum emitters (QEs) and surface plasmons excited by the nanoparticle cluster has been presented by using a rigorous first-principles electromagnetic Green's tensor technique. We have demonstrated that multi-qubit entanglements for two-level QEs can be produced at different coupling resonance frequencies, when they locate in the hot spots of the metallic nanoparticle cluster. The duration of quantum beats for such an entanglement can reach two orders longer than that for the entanglement in a photonic cavity. The phenomenon originates from collective coupling resonance excitation of the cluster. At the frequency of single scattering resonance, the entanglement cannot be produced although the single QE spontaneous decay rate is very big.
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.