When the surface plasmon resonance in a metal-nanoparticle chain is excited at one point, the response signal will generally decay down the chain due to absorption and radiation losses. The decay length is a key parameter in such plasmonic systems. By studying the plasmon lattice Green's function, we found that the decay length is generally governed by two exponential decay constants with phase factors corresponding to guided Bloch modes and one power-law decay with a phase factor corresponding to that of free space photons. The results show a high level of similarity between the absorptive and radiative decay channels. By analyzing the poles (and the corresponding residues) of the Green's function in a transformed complex reciprocal space, the dominant decay channel of the real-space Green's function is understood.
We consider a simple cubic array of metallic nanoparticles supporting extended collective plasmons that arise from the near-field dipolar interaction between localized surface plasmons in each nanoparticle. We develop a fully analytical quantum theory of the strong-coupling regime between these collective plasmons and photons resulting in plasmon polaritons in the nanoparticle array. Remarkably, we show that the polaritonic band gap and the dielectric function of the metamaterial can be significantly modulated by the polarization of light. We unveil how such an anisotropic behavior in the plas…
In a proposed book chapter surface plasmon polariton assisted optical switching in noble metal nanoparticle systems is discussed in the sub-band gap formalism.
We present a quantum mechanical approach to calculate broadening of plasmonic resonances in metallic nanostructures due to collisions of electrons with the surface of the structure. The approach is applicable if the characteristic size of the structure is much larger than the de Broglie electron wavelength in the metal. The approach can be used in studies of plasmonic properties of both single nanoparticles and arrays of nanoparticles.
Transport properties of a single plasmon interacting with a hybrid system composed of a semiconductor quantum dot (SQD) and a metal nanoparticle (MNP) coupled to one-dimensional surface plasmonic waveguide are investigated theoretically via the real-space approach. We considered that the MNP-SQD interaction leads to the formation of a hybrid exciton and the transmission and reflection of a single incident plasmon could be controlled by adjusting the frequency of the classical control field applied to the MNP-SQD hybrid nanosystem, the kinds of metallic nanoparticles and the background media, r…
We theoretically investigate plasmon polaritons in cubic lattices of spherical metallic nanoparticles. The nanoparticles, each supporting triply-degenerate localized surface plasmons, couple through the Coulomb dipole-dipole interaction, giving rise to collective plasmons that extend over the whole metamaterial. The latter hybridize with photons forming plasmon polaritons, which are the hybrid light-matter eigenmodes of the system. We derive general analytical expressions to evaluate both plasmon and plasmon-polariton dispersions, and the corresponding eigenstates. These are obtained within a …
For plasmonic nanoparticles, we investigate the influence of surface roughness inherent to top-down fabrication on the optical properties, and find that it has a surprisingly small influence on the position and width of the plasmon peaks. Our experimental observation is supported by simulations based on the boundary element method approach. Using a perturbation approach, suitable for metallic nanoparticles with a moderate degree of surface roughness, we demonstrate that the reason for this lies in motional narrowing where the plasmon averages over the random height fluctuations. Surface roughn…
We analyze the plasmonic modes of a metal nanoparticle circular array. Closed form solutions to the eigenmode problem are given. For each polarization, the plasmonic mode with the highest quality is found to be an antiphase mode. We found that the significant suppression in radiative loss can be understood as the cancellation of the dipolar radiation term in the radiative linewidth. The remaining finite radiative linewidth decreases exponentially as the number of particle increases.
We study the topological edge plasmon modes between two "diatomic" chains of identical plasmonic nanoparticles. Zak phase for longitudinal plasmon modes in each chain is calculated analytically by solutions of macroscopic Maxwell's equations for particles in quasi-static dipole approximation. This approximation provides a direct analogy with the Su-Schrieffer-Heeger model such that the eigenvalue is mapped to the frequency dependent inverse-polarizability of the nanoparticles. The edge state frequency is found to be the same as the single-particle resonance frequency, which is insensitive to t…
The optical properties of metallic tin nanoparticles embedded in silicon-based host materials were studied. Thin films containing the nanoparticles were produced using RF magnetron sputtering followed by ex situ heat treatment. Transmission electron microscopy was used to determine the nanoparticle shape and size distribution; spherical, metallic tin nanoparticles were always found. The presence of a localized surface plasmon resonance in the nanoparticles was observed when SiO2 and amorphous silicon were the host materials. Optical spectroscopy revealed that the localized surface plasmon reso…
We consider a two-dimensional honeycomb lattice of metallic nanoparticles, each supporting a localized surface plasmon, and study the quantum properties of the collective plasmons resulting from the near field dipolar interaction between the nanoparticles. We analytically investigate the dispersion, the effective Hamiltonian and the eigenstates of the collective plasmons for an arbitrary orientation of the individual dipole moments. When the polarization points close to the normal to the plane the spectrum presents Dirac cones, similar to those present in the electronic band structure of graph…
We study a bipartite linear chain constituted by spherical metallic nanoparticles, where each nanoparticle supports a localized surface plasmon. The near-field dipolar interaction between the localized surface plasmons gives rise to collective plasmons, which are extended over the whole nanoparticle array. We derive analytically the spectrum and the eigenstates of the collective plasmonic excitations. At the edge of the Brillouin zone, the spectrum is of a pseudorelativistic nature similar to that present in the electronic band structure of polyacetylene. We find the effective Dirac Hamiltonia…
We develop a quantum theory of plasmon polaritons in chains of metallic nanoparticles, describing both near- and far-field interparticle distances, by including plasmon-photon Umklapp processes. Taking into account the retardation effects of the long-range dipole-dipole interaction between the nanoparticles, which are induced by the coupling of the plasmonic degrees of freedom to the photonic continuum, we reveal the polaritonic nature of the normal modes of the system. We compute the dispersion relation and radiative linewidth, as well as the group velocities of the eigenmodes, and compare ou…
Plasmonic nanoarrays which support collective surface lattice resonances (SLRs) have become an exciting frontier in plasmonics. Compared with the localized surface plasmon resonance (LSPR) in individual particles, these collective modes have appealing advantages such as angle-dependent dispersions and much narrower linewidths. Here, we investigate systematically how the geometry of the lattice affects the SLRs supported by metallic nanoparticles. We present a general theoretical framework from which the various SLR modes of a given geometry can be straightforwardly obtained by a simple compari…
We investigate the collective plasmonic modes in a chain of metallic nanoparticles that are coupled by near-field interactions. The size- and momentum-dependent nonradiative Landau damping and radiative decay rates are calculated analytically within an open quantum system approach. These decay rates determine the excitation propagation along the chain. In particular, the behavior of the radiative decay rate as a function of the plasmon wavelength leads to a transition from an exponential decay of the collective excitation for short distances to an algebraic decay for large distances. Important…
We study theoretically "graphene-like" plasmonic metamaterials constituted by two-dimensional arrays of metallic nanoparticles, including perfect honeycomb structures with and without inversion symmetry, as well as generic bipartite lattices. The dipolar interactions between localised surface plasmons in different nanoparticles gives rise to collective plasmons that extend over the whole lattice. We study the band structure of collective plasmons and unveil its tunability with the orientation of the dipole moments associated with the localised surface plasmons. Depending on the dipole orientat…
Recent experiments have shown that spatial dispersion may have a conspicuous impact on the response of plasmonic structures. This suggests that in some cases the Drude model should be replaced by more advanced descriptions that take spatial dispersion into account, like the hydrodynamic model. Here we show that nonlocality in the metallic response affects surface plasmons propagating at the interface between a metal and a dielectric with high permittivity. As a direct consequence, any nanoparticle with a radius larger than 20 nm can be expected to be sensitive to spatial dispersion whatever it…
We present a simple model of collective plasmons in a dimerized chain of spherical metallic nanoparticles, an elementary example of a topologically nontrivial nanoplasmonic system. Taking into account long-range quasistatic dipolar interactions throughout the chain, we provide an exact analytical expression for the full quasistatic bandstructure of the collective plasmons. An explicit calculation of the Zak phase proves the robustness of the topological physics of the system against the inclusion of long-range Coulomb interactions, despite the broken chiral symmetry. Using an open quantum syst…
Crystals of plasmonic metal nanoparticles have intriguing optical properties. They reach the regimes of ultrastrong and deep strong light-matter coupling, where the photonic states need to be included in the simulation of material properties. We propose a quantum description of the plasmon polaritons in supercrystals that starts from the dipole and quadrupole excitations of the nanoparticle building blocks and their coupling to photons. Our model excellently reproduces results of finite difference time domain simulations. It provides detailed insight into the emergence of the polariton states.…
Hybrid systems of excitons strongly coupled to localized surface plasmons supported by metallic nanoparticles define a new approach to control light-matter interactions. Here, we report exciton-plasmon coupling in two-dimensional (2D) semiconductors, such as MoS2 and WS2, hybridized with silver nanoparticles. Prominent photoluminescence enhancement in monolayer MoS2 was observed with localized surface plasmon resonance (LSPR) tuned to the exciton resonance. By tuning the excitation energy, the contributions from near field enhancement and radiative emission rate enhancement via Purcell effect …
In electron energy-loss spectroscopy (EELS) of individual silver nanoparticles encapsulated in silicon nitride, we observe besides the usual dipole resonance an additional surface plasmon (SP) resonance corresponding to higher angular momenta. We even observe both resonances for nanoparticle radii as small as 4 nm, where previously only the dipole resonance was assumed to play a role. Electron beams positioned outside of the particles mostly excite the dipole mode, but the higher-order resonance can even dominate the dipole peak when exciting at the particle surface, the usual choice for maxim…
We develop a theory to model the interaction of graphene substrate with localized plasmon resonances in metallic nanoparticles. The influence of a graphene substrate on the surface plasmon resonances is described using an effective background permittivity that is derived from a pseudoparticle concept using the electrostatic method. For this purpose, the interaction of metal nanoparticle with graphene sheet is studied to obtain the optical spectrum of gold nanoparticles deposited on a graphene substrate. Then, we introduce a factor based on dipole approximation to predict the influence of the s…
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 predict the simultaneous occurrence of two fundamental phenomena for metal nanoparticles possessing sharp corners: First, the main plasmonic dipolar mode experiences strong red shift with decreasing corner curvature radius; its resonant frequency is controlled by the apex angle of the corner and the normalized (to the particle size) corner curvature. Second, the split-off plasmonic mode experiences strong localization at the corners. Altogether, this paves the way for tailoring of metal nano-structures providing wavelength-selective excitation of localized plasmons and a strong near-field e…
Hybridized energies in rectangular nanoparticles may display an unusual behaviour. In some cases, they get separated with increasing distance between the particles. In this note this phenomenon is explained by an analytic method.
We consider a chain of regularly-spaced spherical metallic nanoparticles, where each particle supports three degenerate localized surface plasmons. Due to the dipolar interaction between the nanoparticles, the localized plasmons couple to form extended collective modes. Using an open quantum system approach in which the collective plasmons are interacting with vacuum electromagnetic modes and which, importantly, readily incorporates retardation via the light-matter coupling, we analytically evaluate the resulting radiative frequency shifts of the plasmonic bandstructure. For subwavelength-size…
We have studied theoretically the exciton-plasmon coupling effects on the third-order optical nonlinearity of a coherently coupled hybrid system of a metal nanoparticle and a semiconductor quantum dot in the presence of a strong control field with a weak probe field.
Single-molecule surface enhanced Raman scattering (SM-SERS) is one of the vital applications of plasmonic nanoparticles. The SM-SERS sensitivity critically depends on plasmonic hot-spots created at the vicinity of such nanoparticles. In conventional fluid-phase SM-SERS experiments, plasmonic hot-spots are facilitated by chemical aggregation of nanoparticles. Such aggregation is usually irreversible, and hence, nanoparticles cannot be re-dispersed in the fluid for further use. Here, we show how to combine SM-SERS with plasmon-polariton assisted, reversible assembly of plasmonic nanoparticles at…
It is now well established that, due to excitation of localized surface plasmon resonances in plasmonic nanosystems, the electric field from an external irradiation source is greatly amplified in their vicinity. Surface plasmon mediated electric field amplification near plasmonic nanosystems is of vital importance for; light absorption enhancement of solar cells, molecular detection using surface enhanced Raman spectroscopy, proximity measurement of biological macromolecules such as proteins, lipids and nucleic acids using plasmon enhanced FRET, cancer therapy using photothermal effects, just …
Experimental evidence of mode-selective evanescent power coupling at telecommunication frequencies with efficiencies up to 75 % from a tapered optical fiber to a carefully designed metal nanoparticle plasmon waveguide is presented. The waveguide consists of a two-dimensional square lattice of lithographically defined Au nanoparticles on an optically thin silicon membrane. The dispersion and attenuation properties of the waveguide are analyzed using the fiber taper. The high efficiency of power transfer into these waveguides solves the coupling problem between conventional optics and plasmonic …
Sharp metal corners and tips support plasmons localized on the scale of the curvature radius -- superlocalized plasmons. We analyze plasmonic properties of nanoparticles with small and sharp corner- and tip-shaped surface perturbations in terms of hybridization of the superlocalized plasmons, which frequencies are determined by the perturbations shape, and the ordinary plasmons localized on the whole particle. When the frequency of a superlocalized plasmon gets close to that of the ordinary plasmon, their strong hybridization occurs and facilitates excitation of an optical hot-spot near the co…
We numerically investigate the optical response of slowly scaling linear chains of mismatched silver nanoparticles. Hybridized plasmon chain resonances manifest unusual local field distributions around the nanoparticles that result from symmetry breaking of the geometry. Importantly, we find localization patterns characterized by bright hot-spots alternated by what we term \textit{dark} spots. A dark spot is associated to dark plasmons that have collinear and antiparallel dipole moments along the chain. As a result, the field amplification in the dark interjunction gap is extinguished for inci…
The plasmon oscillations of a metallic triaxial ellipsoid nanoparticle have been studied within the framework of the quasistatic approximation. A general method has been proposed for finding the analytical expressions describing the potential and frequencies of the plasmon oscillations of an arbitrary multipolarity order. The analytical expressions have been derived for an electric potential and plasmon oscillation frequencies of the first 24 modes. Other higher orders plasmon modes are investigated numerically.
We investigate the dynamics of a plasmonic oscillation over a metal nanoparticle when it is strongly coupled to a quantum emitter (e.g. quantum dot, molecule). We simulate the density matrix evolution for a simple model; coupled classical--quantum oscillators system. We show that lifetime of the plasmonic oscillations can be increased several orders of magnitude, upto the decay time of the quantum emitter. This effect shows itself as the narrowing of the plasmon emission band in the spaser (surface plasmon amplification by stimulated emission of radiation) experiment [{\it Nature}, {\bf 2009},…
Plasmon-assisted hot carrier processes in metal nanoparticles can be described either classically or using the full strength of quantum mechanics. We reconfirm that from the practical applications point of view, when it comes to description of the decay of plasmons in nanoparticles, classical description is sufficiently adequate for all but the smallest of the nanoparticles. At the same time, the electron temperature rise in nanoparticles is discrete (quantized) and neglecting this fact can lead to significant underestimating of hot carrier assisted effects, such as photo-catalysis.
The optical response of metallic nanoparticle arrays is dominated by localized surface plasmon excitations and is the sum of individual particle contributions modified by inter-particle coupling depending on specific array geometry. Here we scrutinize how experimentally measured properties of large scale (30 mm$^{2}$) amorphous Au nanodisk arrays stem from single particle properties and their interaction. They give rise to a distinct oscillatory behavior of the plasmon peak position, full-width at half-maximum, and extinction efficiency which depends on the minimum particle center-to-center (C…
We investigate the scattering and absorption properties of anisotropic metal-dielectric core-shell nanoparticles. It is revealed that the radially anisotropic dielectric layer can accelerate the evanescent decay of the localized resonant surface modes, leading to Q-factor and absorption rate enhancement. Moreover, the absorption cross section can be maximized to reach the single resonance absorption limit. We further show that such artificial anisotropic cladding materials can be realized by isotropic layered structures, which may inspire many applications based on scattering and absorption of…
Chemiphores are entities, which exhibit wide-band light emission without any external light source but just due to the chemical reaction resulting in the chemiluminescence effect. Since the chemiphores usually have low quantum efficiency, chemiluminescence is a weak optical effect. We found that plasmonic nanoparticles can efficiently enhance the peculiar effect of chemiluminescence due to the acceleration of the radiative decay of the chemiphore excited state which, in turn, enlarges the chemiluminescence yield. Correspondingly, plasmonic nanoparticles are nanoparticles with sub-wavelength si…
We experimentally show how a single Ag nanoparticle (NP) coupled to an Ag nanowire (NW) can convert propagating surface plasmon polaritons to directional photons. By employing dual-excitation Fourier microscopy with spatially filtered collection-optics, we show single- and dual-directional out-coupling of light from NW-NP junction for plasmons excited through glass-substrate and air-superstrate. Furthermore, we show NW-NP junction can influence the directionality of molecular-fluorescence emission, thus functioning as an optical antenna. The results discussed herein may have implications in re…
Nanoparticles made of non-noble metals such as gallium have recently attracted significant attention due to promising applications in UV plasmonics. To date, experiments have mostly focused on solid and liquid pure gallium particles immobilized on solid substrates. However, for many applications, colloidal liquid-metal nanoparticle solutions are vital. Here, we experimentally demonstrate strong UV plasmonic resonances of eutectic gallium-indium (EGaIn) liquid-metal alloy nanoparticles suspended in ethanol. We rationalise experimental results through a theoretical model based on Mie theory. Our…
We present theoretical and experimental studies of the optical response of L-shaped silver nanoparticles. The scattering spectrum exhibits several plasmon resonances that depend sensitively on the polarization of the incident electromagnetic field. The physical origin of the resonances is traced to different plasmon phenomena. In particular, a high energy band with unusual properties is interpreted in terms of volume plasmon oscillations arising from the asymmetry of a nanoparticle.
In this work we use femtosecond laser pulses of 800 nm wavelength to excite and characterize the multiphoton luminescence emission of single gold nanoparticles. For excitation with 100 fs laser pulses we observe a two and three photon emission dominated by radiative electron hole pair recombination, while the emission is caused by radiative plasmon decay for excitation with 500 fs pulses. For single gold nanorods with different aspect ratios, we study the interplay between the particle plasmon and electron hole pairs, which enables us to develop a quantitative model to fully describe the two a…
This work studies the optical binding of a dimer composed by dielectric particles close to a graphene sheet. Using a rigorous electromagnetic method, we calculated the optical force acting on each nanoparticle. In addition, we deduced analytical expressions enabling to evaluate the contribution of graphene surface plasmons (GSPs) to optical binding. Our results show that surface plasmon on graphene excitations generate multiple equilibrium positions for which the distance between particles are tens of times smaller than the photon wavelength. Moreover, these positions can be dynamically contro…
Disorder-induced effects on plasmon coupling in chains of metallic nanoparticles are studied within a dipole model, by considering two types of disorder: fluctuations of the particles' shapes and fluctuations of their positions. Typical localization effects are found both in the eigenmodes and in the transport behavior of the system, and an estimate of the localization length is made. It is argued that chains with deliberately introduced disorder constitute promising systems for studying localization effects of electromagnetic waves at optical frequencies under well controllable and manipulabl…
We use ultrafast pump-probe transmission spectroscopy to measure the electronic relaxation time for electrons in cobalt nanoparticles embedded on glass substrate using femtosecond laser pulses. We found that the plasmon excitation is inhomogenously broadening with a fast excitation time of 23 fs. and a plasmonic relaxation time of 97fs. The femtosecond laser pulses used in this experiment were come from a Ti:Sapphire resonator that uses a self-mode-locking mechanism based on the nonlinear Kerr effect. The pulses were found to have repetition rate of 103.52MHz with a pulse width of 64.5 fs at F…
Metal-dielectric interfaces of various geometries are fundamental photonic material platforms for surface plasmons. Surface plasmon polaritons and localized surface plasmons are two surface plasmon modes that are excited on planar and curved metal-dielectric interfaces, respectively. Herein, we demonstrate in-situ formation of silver nanoparticles by diffusion at a planar interface between sputter-deposited silver and nitride dielectrics. In one step, we synthesize a nanostructure that exhibits both localized surface plasmon resonances at silver nanoparticles and surface plasmon resonances at …
Out-of-plane lattice plasmons (OLPs) supported by metallic nanoparticle arrays are promising for diverse applications due to their remarkably narrow linewidths and significant enhancement of local fields. Here we investigate the necessary conditions for metallic nanoparticle arrays to achieve OLPs. Our results show that, besides the prerequisites of large height, oblique incidence, and TM polarization, which have been pointed out by the literature; the array period should be properly designed within a limited range, the dielectric environment should be homogeneous, and the height and the angle…
We study modulational instability in nonlinear arrays of subwavelength metallic nanoparticles, and analyze numerically nonlinear scenarios of the instability development. We demonstrate that modulational instability can lead to the formation of regular periodic or quasi-periodic modulations of the polarization. We reveal that such nonlinear nanoparticle arrays can support long-lived standing and moving oscillating nonlinear localized modes - plasmon oscillons.
We present a rigorous theoretical model for the optical interaction between a nitrogen-vacancy (NV) centre in diamond and a plasmonic metal nanoparticle (MNP), accompanied by a computationally efficient procedure to solve the evolution. The proposed model enables us to successfully explain existing optical emission measurements of NV centres both in the presence and absence of a metal nanoparticle. We show that the NV-plasmon interaction provides a versatile new avenue to enhance and control the optical emission of an NV centre. Changes to the MNP type and size, NV-MNP centre separation, subme…
We derive envelope equations which generate the Maxwell-Lorentz model and describe the interaction of optical pulses with plasmonic oscillations in metal nanoparticle composites. A family of solitary wave solutions is found which is analogous to self-induced transparency in Maxwell-Bloch. The evolution of incident optical pulses is studied numerically as are the collision dynamics of the solitary waves. These simulations reveal that the collision dynamics vary from near perfectly elastic to highly radiative depending on the relative phase of the initial pulses.
Noble metal nanoparticles show specific optical properties due to the excitation of localized surface plasmons that make them attractive candidates for highly sensitive bionanosensors. The underlying physical principle is either an analyte-induced modification of the dielectric properties of the medium surrounding the nanoparticle or an increase of the excitation and emission rates of an optically active analyte by the resonantly enhanced plasmon field. Either way, besides the nanoparticle geometry the dielectric properties of the metal and nanoscale surface roughness play an important role fo…
Two-dimensional double nanoparticles (DNPs) arrays are demonstrated theoretically supporting the interaction of out-of-plane magnetic plasmons and in-plane lattice resonances, which can be achieved by tuning the nanoparticle height or the array period due to the height-dependent magnetic resonance and the periodicity-dependent lattice resonance. The interplay of the two plasmon modes can lead to a remarkable change in resonance lineshape and an improvement of magnetic field enhancement. Simultaneous electric field and magnetic field enhancements can be obtained in the gap regions between neigh…
Nanoscale phase-control is one of the most powerful approaches to specifically tailor electrical fields in modern nanophotonics. Especially the precise sub-wavelength assembly of many individual nano-building-blocks has given rise to exciting new materials as diverse as metamaterials, for miniaturizing optics, or 3D assembled plasmonic structures for biosensing applications. Despite its fundamental importance, the phase-response of individual nanostructures is experimentally extremely challenging to visualize. Here, we address this shortcoming and measure the quantitative scattering phase of d…
We theoretically study the characteristics of photoelectron emission in plasmonic nanoparticle arrays. Nanoparticles are partially embedded in a semiconductor, forming Schottky barriers at metal/semiconductor interfaces through which photoelectrons can tunnel from the nanoparticle into the semiconductor; photodetection in the infrared range, where photon energies are below the semiconductor band gap (insufficient for band-to-band absorption in semiconductor), is therefore possible. The nanoparticles are arranged in a sparse rectangular lattice so that the wavelength of the lattice-induced Rayl…
