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 different nanomaterials such as gold nanorods and spheres as well as dielectric nanoparticles. Beyond reporting spectrally resolved responses, with phase-changes close to pi when passing the particles' plasmon resonance, we devise a simple method for distinguishing different plasmonic and dielectric particles purely based on their phase behavior. Finally, we integrate this novel approach in a single-shot two-color scheme, capable of directly identifying different types of nanoparticles on one sample, from a single widefield image.
We analyze nonlinear effects in optically driven arrays of nonlinear metallic nanoparticles. We demonstrate that such plasmonic systems are characterized by a bistable response, and they can support the propagation of dissipative switching waves (or plasmonic kinks) connecting the states with different polarization. We study numerically the properties of such plasmonic kinks which are characterized by a subwavelength extent and a tunable velocity.
For all applications of plasmonics to technology it is required to tailor the resonance to the optical system in question. This chapter gives an understanding of the design considerations for nanoparticles needed to tune the resonance. First the basic concepts of plasmonics are reviewed with a focus on the physics of nanoparticles. An introduction to the finite element method is given with emphasis on the suitability of the method to nanoplasmonic device simulation. The effects of nanoparticle shape on the spectral position and lineshape of the plasmonic resonance are discussed including retar…
Efficient manipulation and long distance transport of single-photons is a key component in nanoscale quantum optics. In this letter, we study the emission properties of an individual light emitter placed into a nanofiber and coupled to a metallic nanoparticle. We find that plasmonic field enhancement together with the nanofiber optical confinement uniquely and synergistically contribute to an overall increase of emission rates as well as quantum yields.
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…
Photoelectric properties of metamaterials containing non-centrosymmetric, similarly oriented metallic nanoparticles embedded in a homogeneous semiconductor matrix are theoretically studied. Due to the asymmetric shape of the nanoparticle boundary, photoelectron emission acquires a preferred direction, resulting in a photocurrent flow in that direction when nanoparticles are uniformly illuminated by a homogeneous plane wave. This effect is a direct analogy of the photogalvanic (or bulk photovoltaic) effect known to exist in media with non-centrosymmetric crystal structure, such as doped lithium…
The strong-field control of plasmonic nanosystems opens up new perspectives for nonlinear plasmonic spectroscopy and petahertz electronics. Questions, however, remain regarding the nature of nonlinear light-matter interactions at sub-wavelength spatial and ultrafast temporal scales. Addressing this challenge, we investigated the strong-field control of the plasmonic response of Au nanoshells with a SiO$_2$ core to an intense laser pulse. We show that the photoelectron energy spectrum from these core-shell nanoparticles displays a striking transition between the weak and strong-field regime. Th…
Here we demonstrate the gas sensing ability of cavity-coupled metallic nanoparticle systems, comprising gold nanoparticles separated from a gold mirror with a polymer spacer. An increase in relative humidity (RH) causes the spacer to expand, which induces a significant reduction of nanoparticle scattering intensity, as the scattering is highly dependent on the cavity-nanoparticle coupling that closely relates to the nanoparticle-mirror distance. This lithography-free structure enables a remarkable averaging sensitivity at 0.12 dB/% RH and 0.25 dB/% RH over RH range (45-75%), possessing an esti…
We have used a gold nanohole array to trap single polystyrene nanoparticles, with a mean diameter of 30 nm, into separated hot spots located at connecting nanoslot regions. A high trap stiffness of approximately 0.85 fN/(nmmW) at a low incident laser intensity of ~0.51 mW/um2 at 980 nm was obtained. The experimental results were compared to the simulated trapping force and a reasonable match was achieved. This plasmonic array is useful for lab-on-a-chip applications and has particular appeal for trapping multiple nanoparticles with predefined separations or arranged in patterns in order to stu…
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.
In this work, we present a novel technique to directly measure the phase shift of the optical signal scattered by single plasmonic nanoparticles in a diffraction-limited laser focus. We accomplish this by equipping an inverted confocal microscope with a Michelson interferometer and scanning single nanoparticles through the focal volume while recording interferograms of the scattered and a reference wave for each pixel. For the experiments, lithographically prepared gold nanorods where used, since their plasmon resonances can be controlled via their aspect ratio. We have developed a theoretical…
We investigated the plasmonic modes in a two-dimensional quasicrystalline array of metal nanoparticles. The polarization of the modes is in the array plane. A simplified eigen-decomposition method is presented with the help of rotational symmetry. Two kinds of anti-phase ring modes with radial and tangential polarizations are of highest spatial localizations among all of plasmonic modes. For the leaky characteristic of the anti-phase ring modes, the highest fidelity mode is found to be tangential polarized mode in the quasicrystal array, whereas normal-to-plane polarized mode in the solo ring.…
Multiple surface plasmon-polariton (SPP) waves excited at the interface of a homogeneous isotropic metal and a chiral sculptured thin film (STF) impregnated with silver nanoparticles were theoretically assessed for the multiple-SPP-waves-based sensing of a fluid uniformly infiltrating the chiral STF. The Bruggemann homogenization formalism was used in two different modalities to determine the three principal relative permittivity scalars of the silver-nanoparticle-impregnated chiral STF infiltrated uniformly by the fluid. The dynamic sensitivity increased when silver nanoparticles were present…
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…
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 …
The excitation of plasmonic nanoparticles by ultrashort laser pulses sets in motion a complex ultrafast relaxation process involving the gradual re-equilibration of the system's electron gas, lattice and environment. One of the major hurdles in studying these processes is the lack of direct measurements of the dynamic temperature evolution of the system subcomponents. We measured the dynamic optical response of ensembles of plasmonic Au nanoparticles following ultrashort-pulse excitation and we compared it with the corresponding static optical response as a function of the increasing temperatu…
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…
Unidirectional backward and forward scattering of electromagnetic waves by nanoparticles are usually interpreted as the interference of conventional multipole moments (i.e., electric and magnetic dipole, electric quadrupole, etc.). The role of toroidal dipole moments in unidirectional scattering is generally overlooked. In this work, we investigate the unidirectional scattering for the system of three plasmonic nanospheres. It is found that the unidirectional backward scattering is caused by the interference between the toroidal dipole moment and other conventional multipole moments. Tunable p…
Coupling of light into a thin layer of high refractive index material by plasmonic nanoparticles has been widely studied for application in photovoltaic devices, such as thin-film solar cells. In numerous studies this coupling has been investigated through measurement of e.g. quantum efficiency or photocurrent enhancement. Here we present a direct optical measurement of light coupling into a waveguide by plasmonic nanoparticles. We investigate the coupling efficiency into the guided modes within the waveguide by illuminating the surface of a sample, consisting of a glass slide coated with a hi…
Over the last decade, plasmonic antireflecting nanostructures have been extensively studied to be utilized in various optical and optoelectronic systems such as lenses, solar cells, photodetectors, and others. The growing interest to all-dielectric photonics as an alternative optical technology along with plasmonics motivates us to compare antireflection properties of all-dielectric and plasmonic nanoparticle coatings based on silver and crystalline silicon. Our results of numerical simulations for periodic arrays of spherical nanoparticles on top of amorphous silicon show that both silicon an…
We propose to use collective lattice resonances in plasmonic nanoparticle arrays to enhance photoelectron emission in Schottky-barrier photodetectors and solar cells. We show that the interaction of lattice resonances (the Rayleigh anomaly) and individual particle excitations (localized surface plasmon resonances) leads to stronger local field enhancement and significant increase of the photocurrent compared to the case when only individual particle excitations are present. The results can be used to design new photodetectors with highly selective, tunable spectral response, able to detect pho…
Information on the polarization properties of scattered light from plasmonic systems are of paramount importance due to fundamental interest and potential applications. However, such studies are severely compromised due to the experimental difficulties in recording full polarization response of plasmonic nanostructures. Here, we report on a novel Mueller matrix spectroscopic system capable of acquiring complete polarization information from single isolated plasmonic nanoparticle/nanostructure. The outstanding issues pertaining to reliable measurements of full 4X4 spectroscopic scattering Muell…
Hybrid photonic-plasmonic cavities have emerged as a new platform to increase light-matter interaction capable to enhance the Purcell factor in a singular way not attainable with either photonic or plasmonic cavities separately. In the hybrid cavities proposed so far, mainly consisting of metallic bow-tie antennas, the plasmonic gap sizes defined by lithography in a repeatable way are limited to minimum values \approx 10 nm. Nanoparticle-on-a-mirror (NPoM) cavities are far superior to achieve the smallest possible mode volumes, as gaps smaller than 1 nm can be created. Here, we design a hybrid…
Optical manipulation has attracted remarkable interest owing to its versatile and non-invasive nature. However, conventional optical trapping remains inefficient for the nanoscopic world. The emergence of plasmonics in recent years has brought a revolutionary change in overcoming limitations due to diffraction and the requirements for high trapping laser powers. Among the near-field optical trapping cavity-based systems, Fano resonant optical tweezers have a robust trapping capability. In this work, we experimentally demonstrate sequential trapping of 20 nm particles through the use of metamat…
We demonstrate that the fluorescent emitters can increase light emission from the plasmonic nanostructures in turn. With the help of atomic force microscopy, a hybrid system consisting of a fluorescent nanodiamond and a gold nanoparticle was assembled step-by-step for in situ optical measurements. We found that the emission from the nanoparticle increased compared with that before coupling. The interaction between plasmonic nanostructures and fluorescent emitter was understood as an entity based on the concept of a quantized optical cavity by considering the nanodiamond and the nanoparticle as…
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…
Cascaded optical field enhancement (CFE) can be realized in some specially designed multiscale plasmonic nanostructures, where the generation of extremely strong field at nanoscale volume is crucial for many applications, for example, surface enhanced Raman spectroscopy (SERS). Here, we propose a strategy of realizing a high-quality plasmonic nanoparticle-in-cavity (PIC) nanoantenna array, where strong coupling between a nanoparticle dark mode with a high order nanocavity bright mode can produce Fano resonance at a target wavelength. The Fano resonance can effectively boost the CFE in the PIC,…
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…
We present an optical mode solver for a whispering gallery resonator coupled to an adjacent arbitrary shaped nano-particle that breaks the axial symmetry of the resonator. Such a hybrid resonator-nanoparticle is similar to what was recently used for bio-detection and for field enhancement. We demonstrate our solver by parametrically studying a toroid-nanoplasmonic device and get the optimal nano-plasmonic size for maximal enhancement. We investigate cases near a plasmonic resonance as well as far from a plasmonic resonance. Unlike common plasmons that typically benefit from working near their …
Cathodoluminescence spectroscopy has been performed on silver nanoparticles in a scanning electron microscopy setup. Peaks appearing in the visible range for particles fabricated on silicon substrate are shown to arrive from excitation of out of plane eigenmodes by the electron beam. Monochromatic emission maps have been shown to resolve spatial field variation of resonant plasmon mode on length scale smaller than 25nm. Finite-difference time-domain numerical simulations are performed for both the cases of light excitation and electron excitation. The results of radiative emission under electr…
Collective resonances in plasmonic nanoparticle arrays with electric dipole moment oriented along the lattice wave propagation are theoretically investigated. The role of electric quadrupole (EQ) and magnetic dipole (MD) moments of gold nanoparticles in the resonant features of the arrays is analyzed. We perform both semi-analytical calculations of coupled multipole equations and rigorous numerical simulations varying contributions of the electric and magnetic multipoles by changing particle size and shape (spheres and disks). The arrays in homogeneous and non-homogeneous environments are cons…
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.
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…
Self-assembled Plasmonic Nanoparticle Networks (PNN) composed of chains of 12-nm diameter crystalline gold nanoparticles exhibit a longitudinally coupled plasmon mode cen- tered at 700 nm. We have exploited this longitudinal absorption band to efficiently confine light fields and concentrate heat sources in the close vicinity of these plasmonic chain net- works. The mapping of the two phenomena on the same superstructures was performed by combining two-photon luminescence (TPL) and fluorescence polarization anisotropy (FPA) imaging techniques. Besides the light and heat concentration, we show …
Synthetic perovskites with photovoltaic properties open a new era in solar photovoltaics. Due to high optical absorption perovskite-based thin-film solar cells are usually considered as fully absorbing solar radiation on condition of ideal blooming. However, is it really so? The analysis of the literature data has shown that the absorbance of all photovoltaic pervoskites has the spectral hole at infrared frequencies where the solar radiation spectrum has a small local peak. This absorption dip results in the decrease of the optical efficiency of thin-film pervoskite solar cells by nearly 3% an…
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 demonstrate an electrically controlled coherent random lasing with silver nano-particles dispersed in a dye-doped nematic liquid crystal (NLC), in which external electric field dependent emission intensity and frequency-splitting are recorded. A modified rate equation model is proposed to interpret the observed coherent lasing, which is a manifestation of double enhancements, caused by the plasmon-polariton near-fields of Ag particles, on the population inversion of laser dye molecules and the optical energy density of lasing modes. The noticeable quenching of lasing resonances in a weak ap…
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.
The plasmon resonances (modes) of a metal nanostructure can be defined as a dipole, a quadrupole, or high-order modes depending on the surface charge distribution induced by the incident field. In a non-symmetrical environment or clusters, the modes can hybridize and exhibit different behavior and properties. In this work, we study experimentally and numerically the substrate-induced hybridization of plasmonic modes of a silver nanocylinder. The applications of plasmonic nanoparticles such as refractive index sensing and enhanced spectroscopies often rely on the sustained mode spectral positio…
We demonstrate tunable pulling and pushing optical forces on plasmonic nanostructures around Fano resonance. The plasmonic nanostructure containing a spherical core with optical gain and a metallic shell shows much larger optical pulling force than a pure gain sphere. One can obtain large field enhancement and giant pulling force at the emerged quadrupole mode. The introduction of optical pump compensate the dissipative loss from metal shell, thus enable the strong coupling between a narrow quadrupole mode and a board dipole mode, giving rise to Fano resonance. The giant negative forces origin…
We review the basic physics behind light interaction with plasmonic nanoparticles. The theoretical foundations of light scattering on one metallic particle (a plasmonic monomer) and two interacting particles (a plasmonic dimer) are systematically investigated. Expressions for effective particle susceptibility (polarizability) are derived, and applications of these results to plasmonic nanoantennas are outlined. In the long-wavelength limit, the effective macroscopic parameters of an array of plasmonic dimers are calculated. These parameters are attributable to an effective medium corresponding…
We investigated theoretically the exciton-plasmon coupling effects on the population dynamics and the absorption properties of a hybrid nanosystem composed of a metal nanoparticle (MNP) and a V-type three level semiconductor quantum dot (SQD), which are created by the interaction with the induced dipole moments in the SQD and the MNP, respectively. Excitons of the SQD and the plasmons of the MNP in such a hybrid nanosystem could be coupled strongly or weakly to demonstrate novel properties of the hybrid system. Our results show that the nonlinear optical response of the hybrid nanosystem can b…
We study the light scattering by plasmonic and dielectric symmetric trimers to investigate the existence of polarization-independent Fano resonances. Plasmonic hybridization theory is revealed to hide simple physics, and we instead provide a simplified model for hybridization to derive a plasmonic trimer's eigenmodes analytically. This approach is demonstrated to accurately recreate full wave simulations of plasmonic trimers and their Fano resonances. We are subsequently able to deduce the grounds for modal interference in plasmonic trimers and the related formation of Fano resonances. However…
The rapidly developing field of plasmonics can be roughly categorized into two branches: surface plasmon polaritons (SPPs) propagating in plasmonic waveguides and localized surface plasmons (LSPs) supported by scattering plasmonic particles. Investigations along these two directions usually employ quite different approaches and techniques, resulting in more or less a dogma that the two branches progress almost independently of each other, with few interactions. Here in this work we interpret LSPs from a Bohr model based geometric perspective relying on SPPs, thus establishing a connection betw…
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.
