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arXiv:2010.06405 · The Journal of Chemical Physics

Collective strong coupling in a plasmonic nanocavity

H. Varguet, A. A. Díaz-Valles, S. Guérin, Hans Rudolf Jauslin, Gérard Colas des Francs

Published Feb 23, 2021• 16 citations
arXivHTMLPDF

Abstract

Quantum plasmonics extends cavity quantum electrodynamics (cQED) concepts to the nanoscale, benefiting from the strongly subwavelength confinement of the plasmon modes supported by metal nanostructures. In this work, we describe in detail collective strong coupling to a plasmonic nanocavity. Similarities and differences to cQED are emphasized. We notably observe that the Rabi splitting can strongly deviate from the standard NeΔΩ1 law, where Ne is the number of emitters and ΔΩ1 is the Rabi splitting for a single emitter. In addition, we discuss the collective Lamb shift and the role of quantum corrections to the emission spectra.

DOI
10.1063/5.0033531

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Quantum plasmonics extends cavity quantum electrodynamics (cQED) concepts to the nanoscale, benefiting from the strongly subwavelength confinement of the plasmon modes supported by metal nanostructures. In this work, we describe in detail collective strong coupling to a plasmonic nanocavity. Similarities and differences to cQED are emphasized. We notably observe that the Rabi splitting can strongly deviate from the standard NeΔΩ1 law, where Ne is the number of emitters and ΔΩ1 is the Rabi splitting for a single emitter. In addition, we discuss the collective Lamb shift and the role of quantum corrections to the emission spectra.
The quantum control of emitters is a key issue for quantum information processing at the nanoscale. This generally necessitates the strong coupling of emitters to a high Q-cavity for efficient manipulation of the atoms and field dynamics (cavity quantum electrodynamics or cQED). Since almost a decade, strong efforts are put to transpose cQED concepts to plasmonics in order to profit of the strong mode confinement of surface plasmons polaritons. Despite the intrinsic presence of lossy channels leading to strong decoherence in plasmonics systems, it has been experimentally proven that it is possible to reach the strong coupling regim [1].
Abstract In the light–matter strong coupling regime, the excited state of quantum emitters is inextricably linked to a photonic mode, leading to hybrid states that are part light and part matter. Recently, there has been a huge effort to realize strong coupling with nanoplasmonics, since it provides a versatile environment to study and control molecules in ambient conditions. Among the most promising designs are plasmonic nanocavities that confine light to unprecedentedly small volumes. Such nanocavities, though, support multiple types of modes, with different field profiles and radiative decay rates (bright and dark modes). Here, we show theoretically that the different nature of these modes leads to mode beating within the nanocavity and the Rabi oscillations, which alters the spatiotemporal dynamics of the hybrid system. By specifically designing the illumination setup, we decompose and control the dark and bright plasmon mode excitation and therefore their coupling with quantum emitters. Hence, this work opens new routes for dynamically dressing emitters, to tailor their hybrid states with external radiation.
Summary form only given. The interaction strength of light and matter can be greatly influenced by altering the environment of the emitters and the electric field. In a photonic cavity the emitter-field coupling strength may become sufficiently large that the emitters and the field can exchange an excitation multiple times before it decays, giving rise to Rabi oscillations. In a passive cavity with one (several) two-level emitter(s), this manifests itself as a (collective) Rabi splitting of the transmissions spectrum [1-3], and it has recently been shown that incoherently pumped single emitters in cavities may exhibit Rabi splitting of the emission spectrum at large coupling strengths [4,5]. We present a fully analytical model describing a large collection of incoherently pumped two-level emitters in a single-mode cavity (e.g. quantum dots in a nano-cavity) and show that collective Rabi splitting of the emission spectrum can occur in these systems as well [6]. We derive a condition in terms of system parameters for the splitting to occur, and show that this is different from the condition typically associated with strong emitter-field coupling. Moreover, we show that the collective Rabi splitting decreases with increasing pump rate P, giving a transition from the strong-coupling regime to the weak-coupling regime, and possibly lasing at large P (Fig. 1(a)).
Controlling quantum emitters (atoms, molecules, quantum dots, etc.), light, and its interactionsis a key issue for implementing all-optical devices and information processing at thequantum level. This generally necessitates a strong coupling of emitters to photonic modes,as achieved by a high-Q cavity, for efficient manipulation of the atoms and field dynamicsthrough cavity quantum electrodynamics (cQED).The integration of the principles of quantum optics at the nanoscale in a plasmonic platformhas been envisioned, on the basis of a possible strong coupling between a quantum emitter andthe surface plasmon polaritons (SPPs) via their strong mode confinement. Recent progressshowed the possibility to reach such a strong coupling regime, allowing the development ofquantum plasmonics where a SPP mode takes the role of the cavity mode. However, its applicationappears notoriously limited in practical situations due to the intrinsic presence ofnumerous and lossy modes, which complicates the description and the interpretation of theinteraction, and introduces strong decoherence in the system, in particular for strong coupling.In this work, a detailed overview of quantum control applied to ion trapping, cQED, and plasmonics,is presented. The first part of the thesis is a study of adiabatic processes in trappedion systems and cQED:- We summarize quantum computation processes using quantum gates, and control usingadiabatic laser pulses with atomic systems.- We design arbitrary quantum gates with ions manipulated with laser pulses.- Models for cQED are derived and applied for the production of photon states leakingfrom a cavity.In the second part, we develop a formalism to describe the quantum dynamics of emitters closeto nanoscale structures, and numerics showing the strong coupling regime and the couplingof emitters via plasmon modes. More specifically:- We provide a general field quantization procedure for spherically layered systems.- Effective models using the field quantization are derived, and we show they are analogousto cQED models.- We describe the interaction of localized plasmons (LSPs) with quantum emitters.- The coupling/entanglement of emitters by adiabatic passage through lossy plasmonicmodes of a nanosphere is shown.
Rabi oscillations characterize light-matter hybridization in the waveguide quantum electrodynamics~(WQED) framework, with their associated decay rates reflecting excitation damping, yet their behavior remains unresolved when collective emitters are coupled to a collective waveguide mode. This scenario reveals a conceptually novel collective-light-collective-matter interaction, realizable when a timed-Dicke state~(TDS) of subwavelength emitters couples to a slow, delocalized surface-plasmon mode, forming a hybridized plasmon-polariton~(HPP). The HPP acquires its directionality from the TDS via momentum matching. It also exhibits plasmonic characteristics, with excitation frequencies following the surface-plasmon dispersion relation. We obtain a Rabi oscillation and a long-time decay that describe the HPP and use them to reveal weak- and strong-coupling regimes through the emergence of normal-mode splitting. By performing a finite-time Lyapunov-exponent analysis, we show that the HPP also exhibits instantaneous decay and identify three distinct decay regimes: early-time rapid, transient-time oscillatory, and long-time classical. Finally, by analyzing the emission spectrum, we observe an anticrossing of the peak doublets~(a feature also seen in cavity QED setups) which originates from quantum vacuum effects and the resulting non-Markovian HPP evolution in our WQED.
Abstract Quantum nanophotonics places nanoscale structuring in direct dialogue with photonic quantum information—compressing functionality to the few-nanometre, few-femtosecond frontier while retaining energy efficiency, speed and room-temperature operation. We highlight nanoplasmonic cavity-QED architectures in which extreme mode confinement delivers strong coupling under ambient conditions, enabling ultrafast single-photon emission and near-field multipartite entanglement using industry-grade near-field transducers that nanofocus guided light at practical efficiencies. We set these advances against the arc from early plasmonic cQED proposals and single-emitter Purcell studies to modern time-domain measurements that resolve sub-picosecond polariton/Rabi dynamics—establishing a clear route from concept to device. In parallel, we point to low-loss, high-index Mie resonators whose spectrally sharp electric and magnetic modes afford narrow-band coherent control, filtering and radiation-pattern engineering, and which naturally co-integrate in hybrid metal–dielectric stacks that combine ultrastrong local coupling with low-loss routing and storage. Finally, we discuss quantum nanoplasmonic coherent perfect absorption (qnCPA)—a waveguide-fed, non-perturbing protocol that selectively prepares and protects plasmon–emitter dressed states via dissipation-assisted, unidirectional feeding. Together with macroscopic QED and quantum quasinormal-mode quantization, which regularize open, lossy resonators and clarify when loss can be a resource, these developments chart robust, chip-scale routes to room-temperature quantum technologies.