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.
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.
Recent rapid advances in quantum nanoplasmonics offer the potential for accessing quantum phenomena at room temperature. Despite this, entangled states have not yet been realized, and remain an outstanding challenge. In this work, we demonstrate how entanglement emerges in plasmonic nanocavities, which are inherently multimode, and demonstrate the conditions necessary for entanglement to persist. We find that, in general, these conditions are broken due to coupling with multiple plasmonic modes of different parity. We address this challenge with a new nanocavity design that supports high selective coupling to a single mode, enabling the robust generation of persistent entanglement in nanoplasmonics. Our results open exciting prospects for leveraging simple plasmonic setups in ambient conditions for applications in quantum communication, sensing, and rapid quantum memories.
Plasmonic nanocavities are known for their extreme field enhancement and subwavelength light confinement in gaps of just a few nanometers. Pairing this with the ability to host quantum emitters, they form highly promising platforms to control or engineer quantum states at room temperature. Here, we use the lossy nature of plasmonic nanocavities to form subradiant entangled states between two or more quantum emitters, that persist for ∼ 100 times longer than the plasmonic excitation. We develop a theoretical description that directly links quantum variables to experimentally measurable quantities, such as the extinction cross section, and unlike previous studies includes plasmonic excitations necessary to resonantly form subradiant states. This work paves the way towards engineering quantum entangled states in ambient conditions with plasmonic nanocavities.
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.
The design and preparation of quantum states free from environmental decohering effects is critically important in the development of on-chip quantum systems with robustness. One promising strategy is to harness quantum state superposition to construct decoherence-free subspace (DFS), which is termed dark state. Typically, the excitation of dark states relies on anti-phase-matching on two qubits and the inter-qubit distance is of wavelength scale, which limits the development of compact quantum chips. In this work, we propose a hybrid plasmonic quantum emitter composed of strongly correlated quantum emitters intermediated by a plasmonic nanocavity. Through turning the plasmonic loss from drawback into advantage, we break the anti-phase-matching rule by rapidly decaying the superposed bright state and preparing a sub-100 nm dark state with decay rate reduced by 3 orders of magnitudes. More interestingly, the dark state can be optically switched to a single-photon emitter with enhanced brightness through photon-blockade, with the quantum second order correlation function at zero delay showing a wide range of tunability down to 0.02.
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.
Strong light–matter interaction is at the heart of modern quantum technological applications and is the basis for a wide range of rich optical phenomena. Coupling a single quantum emitter strongly with electromagnetic fields provides an unprecedented control over its quantum states and enables high-fidelity quantum operations. However, single-emitter strong coupling is exceptionally fragile and has been realized mostly at cryogenic temperatures. Recent experiments have, however, demonstrated that single-emitter strong coupling can be realized at room temperature by using plasmonic nanocavities that confine optical fields via surface plasmons strongly on metal surfaces and facilitate sub-picosecond light–matter interaction. Here, we outline recent theoretical developments and experimental demonstrations of room-temperature strong coupling in the plasmonic platform, from emitter ensembles down to the single emitter limit, before placing a focus on selective studies that explore and provide insight into applications of plexcitonic strong coupling including sensing of single biological molecules, qubit entanglement generation, and reconfigurable single-photon sources and provide an outline of research directions in quantum sensing, quantum information processing, and ultrafast spectroscopy.