The extraordinary sensitivity of plasmonic sensors is well known in the optics and photonics community. These sensors exploit simultaneously the enhancement and the localization of electromagnetic fields close to the interface between a metal and a dielectric. This enables, for example, the design of integrated biochemical sensors at scales far below the diffraction limit. Despite their practical realization and successful commercialization, the sensitivity and associated precision of plasmonic sensors are starting to reach their fundamental classical limit given by quantum fluctuations of light -- known as the shot-noise limit. To improve the sensing performance of these sensors beyond the classical limit, quantum resources are increasingly being employed. This area of research has become known as `quantum plasmonic sensing' and it has experienced substantial activity in recent years for applications in chemical and biological sensing. This review aims to cover both plasmonic and quantum techniques for sensing, and shows how they have been merged to enhance the performance of plasmonic sensors beyond traditional methods. We discuss the general framework developed for quantum plasmonic sensing in recent years, covering the basic theory behind the advancements made, and describe the important works that made these advancements. We also describe several key works in detail, highlighting their motivation, the working principles behind them, and their future impact. The intention of the review is to set a foundation for a burgeoning field of research that is currently being explored out of intellectual curiosity and for a wide range of practical applications in biochemistry, medicine, and pharmaceutical research.
Quantum resources can enhance the sensitivity of a device beyond the classical shot noise limit and, as a result, revolutionize the field of metrology through the development of quantum-enhanced sensors. In particular, plasmonic sensors, which are widely used in biological and chemical sensing applications, offer a unique opportunity to bring such an enhancement to real-life devices. Here, we use bright entangled twin beams to enhance the sensitivity of a plasmonic sensor used to measure local changes in refractive index. We demonstrate a 56% quantum enhancement in the sensitivity of state-of-…
The measurement of parameters that describe kinetic processes is important in the study of molecular interactions. It enables a deeper understanding of the physical mechanisms underlying how different biological entities interact with each other, such as viruses with cells, vaccines with antibodies, or new drugs with specific diseases. In this work, we study theoretically the use of quantum sensing techniques for measuring the kinetic parameters of molecular interactions. The sensor we consider is a plasmonic resonance sensor -- a label-free photonic sensor that is one of the most widely used …
Reducing the noise below the shot-noise limit in sensing devices is one of the key promises of quantum technologies. Here, we study quantum plasmonic sensing based on an attenuated total reflection configuration with single photons as input. Our sensor is the Kretschmann configuration with a gold film, and a blood protein in an aqueous solution with different concentrations serves as an analyte. The estimation of the refractive index is performed using heralded single photons. We also determine the estimation error from a statistical analysis over a number of repetitions of identical and indep…
We investigate an array of metal nanoparticles as a channel for nanophotonic quantum communication and the generation of quantum plasmonic interference. We consider the transfer of quantum states, including single-qubits as plasmonic wavepackets, and highlight the necessity of a quantum mechanical description by comparing the predictions of quantum theory with those of classical electromagnetic theory. The effects of loss in the metal are included, thus putting our investigation into a practical setting and enabling the quantification of the performance of realistic nanoparticle arrays as plas…
We demonstrate `deterministic' launching of propagative quantum surface-plasmon polaritons at freely chosen positions on gold plasmonic receptacles. This is achieved by using as plasmon launcher a near-field scanning optical source made of a diamond nanocrystal with two Nitrogen-Vacancy color-center occupancy. Our demonstration relies on leakage-radiation microscopy of a thin homogeneous gold film and on near-field optical microscopy of a nanostructured thick gold film. Our work paves the way to future fundamental studies and applications in quantum plasmonics that require an accurate position…
Kinetic models are essential for describing how molecules interact in a variety of biochemical processes. The estimation of a model's kinetic parameters by experiment enables researchers to understand how pathogens, such as viruses, interact with other entities like antibodies and trial drugs. In this work, we report a simple proof-of-principle experiment that uses quantum sensing techniques to give a more precise estimation of kinetic parameters than is possible with a classical approach. The interaction we study is that of bovine serum albumin (BSA) binding to gold via an electrostatic mecha…
Strong coupling between a single quantum emitter and an electromagnetic mode is one of the key effects in quantum optics. In the cavity QED approach to plasmonics, strongly coupled systems are usually understood as single-transition emitters resonantly coupled to a single radiative plasmonic mode. However, plasmonic cavities also support non-radiative (or "dark") modes, which offer much higher coupling strengths. On the other hand, realistic quantum emitters often support multiple electronic transitions of various symmetry, which could overlap with higher order plasmonic transitions -- in the …
Quantum plasmonics experiments have on multiple occasions reported the observation of quantum coherence of discrete plasmons, which exhibit remarkable preservation of quantum interference visibility, a seemingly surprising feature for systems mixing light and matter with high ohmic losses during propagation. However, most experiments to date used essentially weakly-confined plasmons, which experience limited light-matter hybridization, thus limiting the potential for decoherence. Here, we report quantum coherence of plasmons near the surface plasmon polariton (SPP) resonance frequency, where p…
Quantum plasmonics is a rapidly growing field of research that involves the study of the quantum properties of light and its interaction with matter at the nanoscale. Here, surface plasmons - electromagnetic excitations coupled to electron charge density waves on metal-dielectric interfaces or localized on metallic nanostructures - enable the confinement of light to scales far below that of conventional optics. In this article we review recent progress in the experimental and theoretical investigation of the quantum properties of surface plasmons, their role in controlling light-matter interac…
We investigate the frontier between classical and quantum plasmonics in highly doped semiconductor layers. The choice of a semiconductor platform instead of metals for our study permits an accurate description of the quantum nature of the electrons constituting the plasmonic response, which is a crucial requirement for quantum plasmonics. Our quantum model allows us to calculate the collective plasmonic resonances from the electronic states determined by an arbitrary one-dimensional potential. Our approach is corroborated with experimental spectra, realized on a single quantum well, in which h…
Localized-surface plasmon resonance is of importance in both fundamental and applied physics for the subwavelength confinement of optical field, but realization of quantum coherent processes is confronted with challenges due to strong dissipation. Here we propose to engineer the electromagnetic environment of metallic nanoparticles (MNPs) using optical microcavities. An analytical quantum model is built to describe the MNP-microcavity interaction, revealing the significantly enhanced dipolar radiation and consequentially reduced Ohmic dissipation of the plasmonic modes. As a result, when inter…
Quantum plasmonic systems suffer from significant decoherence due to the intrinsically large dissipative and radiative dampings. Based on our quantum simulations via a quantum tensor network algorithm, we numerically demonstrate the mitigation of this restrictive drawback by hybridizing a plasmonic nanocavity with an emitter ensemble with inhomogeneously-broadened transition frequencies. By burning two narrow spectral holes in the spectral density of the emitter ensemble, the coherent time of Rabi oscillation for the hybrid system is increased tenfold. With the suppressed decoherence, we move …
We report direct evidence of the bosonic nature of surface plasmon polaritons (SPPs) in a scattering-based beamsplitter. A parametric down-conversion source is used to produce two indistinguishable photons, each of which is converted into a SPP on a metal-stripe waveguide and then made to interact through a semi-transparent Bragg mirror. In this plasmonic analog of the Hong-Ou-Mandel experiment, we measure a coincidence dip with a visibility of 72%, a key signature that SPPs are bosons and that quantum interference is clearly involved.
Plasmonic nano-structures provides an efficient way to control and enhance the radiative properties of quantum emitters. Coupling these structures to single defects in low-dimensional materials provides a particularly promising material platform to study emitter-plasmon interactions because these emitters are not embedded in a surrounding dielectric. They can therefore approach a near-field plasmonic mode to nanoscale distances, potentially enabling strong light-matter interactions. However, this coupling requires precise alignment of the emitters to the plasmonic mode of the structures, which…
For almost two decades, it has been believed that the quantum statistical properties of bosons are preserved in plasmonic systems. This idea has been stimulated by experimental work reporting the possibility of preserving nonclassical correlations in light-matter interactions mediated by scattering among photons and plasmons. Furthermore, it has been assumed that similar dynamics underlies the conservation of the quantum fluctuations that define the nature of light sources. Here, we demonstrate that quantum statistics are not always preserved in plasmonic systems and report the first observati…
We introduce a scheme for generating entanglement between two quantum dots using a plasmonic waveguide made from an array of metal nanoparticles. We show that the scheme is robust to loss, enabling it to work over long distance plasmonic nanoparticle arrays, as well as in the presence of other imperfections such as the detuning of the energy levels of the quantum dots. The scheme represents an alternative strategy to the previously introduced dissipative driven schemes for generating entanglement in plasmonic systems. Here, the entanglement is generated by using dipole-induced interference eff…
We report perfect two photon quantum interference with near-unity visibility in a resonant tunneling plasmonic structure in folded Kretschmann geometry. This is despite absorption-induced loss of unitarity in plasmonic systems. The effect is traced to perfect destructive interference between the squares of amplitude reflection and transmission coefficients. We further highlight yet another remarkable potential of coincidence measurements as a probe with better resolution as compared to standard spectroscopic techniques. The finer features show up in both angle resolved and frequency resolved s…
Photonic sensors have many applications in a range of physical settings, from measuring mechanical pressure in manufacturing to detecting protein concentration in biomedical samples. A variety of sensing approaches exist, and plasmonic systems in particular have received much attention due to their ability to confine light below the diffraction limit, greatly enhancing sensitivity. Recently, quantum techniques have been identified that can outperform classical sensing methods and achieve sensitivity below the so-called shot-noise limit. Despite this significant potential, the use of definite p…
We experimentally demonstrate the active control of a plasmonic metamaterial operating in the quantum regime. A two-dimensional metamaterial consisting of unit cells made from gold nanorods is investigated. Using an external laser we control the temperature of the metamaterial and carry out quantum process tomography on single-photon polarization-encoded qubits sent through, characterizing the metamaterial as a variable quantum channel. The overall polarization response can be tuned by up to 33% for particular nanorod dimensions. To explain the results, we develop a theoretical model and find …
Hybrid photonic-plasmonic nanostructures allow one to engineer coupling of quantum emitters and cavity modes accounting for the direct coherent and environment mediated dissipative pathways. Using generalized plasmonic Dicke model, we explore the non-equilibrium phase diagram with respect to these interactions. The analysis shows that their interplay results in the extension of the superradiant and regular lasing states to the dissipative coupling regime and an emergent lasing phase without population inversion having boundary with the superradiant and normal states. Calculated photon emission…
The strong interaction of individual quantum emitters with resonant cavities is of fundamental interest for understanding light matter interactions. Plasmonic cavities hold the promise of attaining the strong coupling regime even under ambient conditions and within subdiffraction volumes. Recent experiments revealed strong coupling between individual plasmonic structures and multiple organic molecules, but so far strong coupling at the limit of a single quantum emitter has not been reported. Here we demonstrate vacuum Rabi splitting, a manifestation of strong coupling, using silver bowtie plas…
We introduce a new paradigm: the chiral electromagnetic local density of states (LDOS) in a spiral plasmonic nanostructure. In both classical and quantum regimes, we reveal using scanning near-field optical microscopy (NSOM) in combination with spin analysis that a spiral cavity possesses spin-dependent local optical modes. We expect this work to lead to promising directions for future quantum plasmonic device development, highlighting the potentials of chirality in quantum information processing.
We report an experimental realisation of a quantum random number generator using a plasmonic beamsplitter. Free-space single photons are converted into propagating single surface plasmon polaritons on a gold stripe waveguide via a grating. The surface plasmons are then guided to a region where they are scattered into one of two possible outputs. The presence of a plasmonic excitation in a given output determines the value of a random bit generated from the quantum scattering process. Using a stream of single surface plasmons injected into the beamsplitter we achieve a quantum random number gen…
The control of quantum states of light at the nanoscale has become possible in recent years with the use of plasmonics. Here, many types of nanophotonic devices and applications have been suggested that take advantage of quantum optical effects, despite the inherent presence of loss. A key example is quantum plasmonic sensing, which provides sensitivity beyond the classical limit using entangled N00N states and their generalizations in a compact system operating below the diffraction limit. In this work, we experimentally demonstrate the excitation and propagation of a two-plasmon entangled N0…
Plasmonics is a rapidly emerging platform for quantum state engineering with the potential for building ultra-compact and hybrid optoelectronic devices. Recent experiments have shown that despite the presence of decoherence and loss, photon statistics and entanglement can be preserved in single plasmonic systems. This preserving ability should carry over to plasmonic metamaterials, whose properties are the result of many individual plasmonic systems acting collectively, and can be used to engineer optical states of light. Here, we report an experimental demonstration of quantum state filtering…
Quantum plasmonics lies at the intersection between nanophotonics and quantum optics. Genuine quantum effects can be observed with non-classical states such as Fock states and with entangled states. A N00N state combines both aspects: it is a quantum superposition state of a Fock state with N excitations in two spatial modes. Here we report the first observation of two-plasmon (N=2) N00N state interferences using a plasmonic beamsplitter etched on a planar interface between gold and air. We analyze in detail the role of losses at the beamsplitter and during the propagation along the metal/air …
In recent years the controlled coupling of single photon emitters to propagating surface plasmons has been intensely studied, which is fueled by the prospect of a giant photonic non-linearity on a nano-scaled platform. In this article we will review the recent progress on coupling single emitters to nano-wires towards the construction of a new platform for strong light-matter interaction. The control over such a platform might open new doors for quantum information processing and quantum sensing at the nanoscale, and for the study of fundamental physics in the ultra-strong coupling regime.
We present a self-consistent quantum optics approach to calculating the surface enhanced Raman spectrum of molecules coupled to arbitrarily shaped plasmonic systems. Our treatment is intuitive to use and provides fresh analytical insight into the physics of the Raman scattering near metallic surfaces and can be applied to a wide range of geometries including resonators, waveguides, as well as hybrid photonic-plasmonic systems. Our general theory demonstrates that the detected Raman spectrum originates from an interplay between nonlinear light generation and propagation. Counter intuitively, at…
We present a scheme to generate continuous variable bipartite entanglement between two optical modes in a hybrid optical-microwave-plasmonic graphene waveguide system. In this scheme, we exploit the interaction of two light fields coupled to the same microwave mode via Plasmonic Graphene Waveguide to generate two-mode squeezing, which can be used for continuous-variable quantum teleportation of the light signals over large distances. Furthermore, we study the teleportation fidelity of an unknown coherent state. The teleportation protocol is robust against the thermal noise associated with the …
Plasmonic superradiance originates from the plasmon mediated strong correlation that builds up between dipolar emitters coupled to a metal nanoparticle. This leads to a fast burst of emission so that plasmonic superradiance constitutes ultrafast and extremely bright optical nanosources of strong interest for integrated quantum nano-optics platforms. We elucidate the superradiance effect by establishing the dynamics of the system, including all features like the orientation of the dipoles, their distance to the particle and the number of active plasmon modes. We determine an optimal configurati…
A system of two or more quantum dots interacting with a dissipative plasmonic nanostructure is investigated in detail by using a cavity quantum electrodynamics approach with a model Hamiltonian. We focus on determining and understanding system configurations that generate multiple bipartite quantum entanglements between the occupation states of the quantum dots. These configurations include allowing for the quantum dots to be asymmetrically coupled to the plasmonic system. Analytical solution of a simplified limit for an arbitrary number of quantum dots and numerical simulations and optimizati…
We provide a critical analysis of some of the commonly used theoretical models to describe quantum plasmons. We summarize the standard approach based on a Fano diagonalization and we show explicit discrepancies in the obtained results by taking the limit of vanishing coupling between the electromagnetic field and the material medium. We then discuss the derivation of spontaneous emission in a plasmonic environment, which usually relies on a Green tensor and is based on an incomplete identity. The effect of the missing terms is calculated in a one-dimensional model.
Surface polaritons at a meta-material interface are proposed as qubits. The SP fields are shown to have low losses, subwavelength confinement and can demonstrate very small modal volume. These important properties are used to demonstatre interesting applications in quantum information, i.e., coherent control of weak fields and large Kerr nonlinearity at the low photon level.
Quantum emitters, such as q-dots and dye molecules, in the immediate vicinity of plasmonic nanostructures, resonantly excite surface plasmon-polaritons (SPPs) under incoherent pump. The efficiency in the excitation of SPPs increases as the number of the emitters, because the SPP field synchronizes emission of the coupled emitters, in analogy with the superadiance (SR) of coupled emitters in free space. Using fully quantum mechanical model for two emitters coupled to a single gold nanorod, we predict up to 15% increase in the emission yield of single emitter compared to only one emitter coupled…
Quantum plasmonics extends cavity quantum electrodynamics (cQED) concepts to the nanoscale, taking benefit 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 $\sqrt{N_e}ΔΩ_1$ law, where $N_e$ is the number of emitters and $ΔΩ_1$ the Rabi splitting for a single emitter. In addition, we discuss the collective Lamb shift and th…