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Plasmonic nanocavities enable access to the quantum properties of matter, but are often simplified to single mode models despite their complex multimode structure. Here, we show that off-resonant plasmonic modes in fact play a crucial role in strong coupling, and determine the onset of a novel collective interaction. Our analysis reveals that $n$ strongly coupled plasmonic modes, introduce up to $n(n+1)/2$ oscillation frequencies that depend on their coupling strengths and detunings from the quantum emitter. Furthermore, we identify three distinct regions as the coupling strength increases: (1) single mode, (2) multimode, and (3) collective multimode strong coupling. Our findings enhance the understanding of quantum dynamics in realistic plasmonic environments and demonstrate their potential to achieve ultra-fast energy transfer in light-driven quantum technologies., Comment: 7 pages, 3 figures more...

Multi-partite entanglement is fundamental to emerging quantum technologies such as quantum networks, which ultimately require devices with strong light-matter interactions and long coherence times. Here, we introduce nanobeam photonic crystal cavities combining both extreme quality factors ($\sim10^{7}$) with sub-wavelength field confinement to reach unprecedented light-matter interactions. Operating at $780$ nm, our devices are tailored for efficient coupling and entanglement with ultracold $^{87}$Rb atoms, a key ingredient in quantum networks due to their hyperfine structure. Our new designs also facilitate the precise optical trapping of atoms, and we demonstrate coherent entanglement generation between them, that is remarkably resilient to atomic displacements. These platforms can be easily scaled-up to extremely large quantum networks, for distributed quantum computing and future light-based quantum technologies., Comment: 23 pages, 5 figures more...

Recent rapid advances in quantum nanoplasmonics offer the potential for accessing quantum phenomena at room temperature. Despite this, entangled states have not yet been realised, and remain an outstanding challenge. In this work, we demonstrate how entanglement emerges in plasmonic nanocavities, which are inherently multi-mode, 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 subradiant 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., Comment: 25 pages, 4 figures more...

We present a comprehensive second quantization scheme for radiative photonic devices. We canonically quantize the continuum of photonic eigenmodes by transforming them into a discrete set of pseudomodes that provide a \textit{complete} and \textit{exact} description of quantum emitters interacting with electromagnetic environments. This method avoids all reservoir approximations, and offers new insights into quantum correlations, accurately capturing all non-Markovian dynamics. This method overcomes challenges in quantizing non-Hermitian systems and is applicable to diverse nanophotonic geometries. more...

Plasmonic nanocavities are known for their extreme field enhancement and sub-wavelength 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 sub-radiant entangled states between two or more quantum emitters, that persist for $\sim 100$ 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, for potential applications such as rapid quantum memories, quantum communications and sensors. more...

Plasmonic nanocavities form very robust sub-nanometer gaps between nanometallic structures and confine light in deep subwavelength volumes to enable unprecedented control on light-matter interactions. However, spherical nanoparticles acquire various polyhedral shapes during their synthesis, which has defining impact on controlling many light-matter interactions, such as photocatalytic reactions. Here, we focus on nanocavities made of three polyhedral nanoparticles (cuboctahedron, rhombicuboctahedron, decahedron) that commonly occur during the synthesis of spherical nanoparticles. Their photonic modes have a very intricate and rich optical behaviour, both in the near- and far-field. Through a recombination technique, we obtain the total far-field produced by a molecule placed within these nanocavities, to reveal how energy couples in and out of the system. This work paves the way towards understanding and controlling light-matter interactions, such as photocatalytic reactions and non-linear vibrational pumping, in such extreme environments. more...

Plasmonic nanoantennas have the ability to confine and enhance incident electromagnetic fields into very sub-wavelength volumes, while at the same time efficiently radiating energy to the far-field. These properties have allowed plasmonic nanoantennas to be extensively used for exciting quantum emitters-such as molecules and quantum dots-and also for the extraction of photons from them for measurements in the far-field. Due to electromagnetic reciprocity, it is expected that plasmonic nanoantennas radiate energy as efficiently as an external source can couple energy to them. In this paper, we adopt a multipole expansion (Mie theory) and numerical simulations to show that although reciprocity holds, certain plasmonic antennas radiate energy much more efficiently than one can couple energy into them. This work paves the way towards designing plasmonic antennas with specific properties for applications where the near-to-far-field relationship is of high significance, such as: surface-enhanced Raman spectroscopy, strong coupling at room temperature, and the engineering of quantum states in nanoplasmonic devices., Comment: 22 pages (1.5 linespacing), 6 figures more...

The use of nanoplasmonics to control light and heat close to the thermodynamic limit enables exciting opportunities in the field of plasmonic catalysis. The decay of plasmonic excitations creates highly nonequilibrium distributions of hot carriers that can initiate or catalyze reactions through both thermal and nonthermal pathways. In this Perspective, we present the current understanding in the field of plasmonic catalysis, capturing vibrant debates in the literature, and discuss future avenues of exploration to overcome critical bottlenecks. Our Perspective spans first-principles theory and computation of correlated and far-from-equilibrium light-matter interactions, synthesis of new nanoplasmonic hybrids, and new steady-state and ultrafast spectroscopic probes of interactions in plasmonic catalysis, recognizing the key contributions of each discipline in realizing the promise of plasmonic catalysis. We conclude with our vision for fundamental and technological advances in the field of plasmon-driven chemical reactions in the coming years. more...

In the past decade, advances in nanotechnology have led to the development of plasmonic nanocavities which facilitate light-matter strong coupling in ambient conditions. The most robust example is the nanoparticle-on-mirror (NPoM) structure whose geometry is controlled with subnanometer precision. The excited plasmons in such nanocavities are extremely sensitive to the exact morphology of the nanocavity, giving rise to unexpected optical behaviors. So far, most theoretical and experimental studies on such nanocavities have been based solely on their scattering and absorption properties. However, these methods do not provide a complete optical description of a NPoM. Here, the NPoM is treated as an open non-conservative system supporting a set of photonic quasinormal modes (QNMs). By investigating the morphology-dependent optical properties of nanocavities, we propose a simple yet comprehensive nomenclature based on spherical harmonics and report spectrally overlapping bright and dark nanogap eigenmodes. The near-field and far-field optical properties of NPoMs are explored and reveal intricate multi-modal interactions. more...

Fabricating nanocavities in which optically-active single quantum emitters are precisely positioned, is crucial for building nanophotonic devices. Here we show that self-assembly based on robust DNA-origami constructs can precisely position single molecules laterally within sub-5nm gaps between plasmonic substrates that support intense optical confinement. By placing single-molecules at the center of a nanocavity, we show modification of the plasmon cavity resonance before and after bleaching the chromophore, and obtain enhancements of $\geq4\times10^3$ with high quantum yield ($\geq50$%). By varying the lateral position of the molecule in the gap, we directly map the spatial profile of the local density of optical states with a resolution of $\pm1.5$ nm. Our approach introduces a straightforward non-invasive way to measure and quantify confined optical modes on the nanoscale. more...

An emitter in the vicinity of a metal nanostructure is quenched by its decay through non-radiative channels, leading to the belief in a zone of inactivity for emitters placed within $<$10nm of a plasmonic nanostructure. Here we demonstrate that in tightly-coupled plasmonic resonators forming nanocavities "quenching is quenched" due to plasmon mixing. Unlike isolated nanoparticles, plasmonic nanocavities show mode hybridization which massively enhances emitter excitation and decay via radiative channels. This creates ideal conditions for realizing single-molecule strong-coupling with plasmons, evident in dynamic Rabi-oscillations and experimentally confirmed by laterally dependent emitter placement through DNA-origami. more...

The near-field and far-field spectral response of plasmonic systems are often assumed to be identical, due to the lack of methods that can directly compare and correlate both responses under similar environmental conditions. We develop a widely-tuneable optical technique to probe the near-field resonances within individual plasmonic nanostructures that can be directly compared to the corresponding far-field response. In tightly-coupled nanoparticle-on-mirror constructs with nanometer-sized gaps we find >40meV blueshifts of the near-field compared to the dark-field scattering peak, which agrees with full electromagnetic simulations. Using a transformation optics approach, we show such shifts arise from the different spectral interference between different gap modes in the near- and far-field. The control and tuning of near-field and far-field responses demonstrated here is of paramount importance in the design of optical nanostructures for field-enhanced spectroscopy, as well as to control near-field activity monitored through the far-field of nano-optical devices., Comment: 4 figures more...

Recent advances in nano-fabrication techniques allow for the manufacture of optical metamaterials, bringing their unique and extra-ordinary properties to the visible regime and beyond. However, an analytical description of optical nano-plasmonic metamaterials is challenging due to the characteristic optical behaviour of metals. Here we present an analytical theory that allows to bring established microwave metamaterials models to optical wavelengths. This method is implemented for nano-scaled plasmonic wire-mesh and tri-helical metamaterials, and we obtain an accurate prediction for their dispersive behaviour at optical and near-IR wavelengths. more...