Large scale simulations are performed by means of the transfer-matrix method to reveal optimal conditions for metal-dielectric core-shell particles to induce the largest fluorescence on their surfaces. With commonly used plasmonic cores (Au and Ag) and dielectric shells (SiO2, Al2O3, ZnO), optimal core and shell radii are determined to reach maximum fluorescence enhancement for each wavelength within 550~850 nm (Au core) and 390~500 nm (Ag core) bands, in both air and aqueous hosts. The peak value of the maximum achievable fluorescence enhancement factors of core-shell nanoparticles, taken over entire wavelength interval, increases with the shell refractive index and can reach values up to 9 and 70 for Au and Ag cores, within 600~700 nm and 400~450 nm wavelength ranges, respectively, which is much larger than that for corresponding homogeneous metal nanoparticles. Replacing air by an aqueous host has a dramatic effect of nearly halving the sizes of optimal core-shell configurations at the peak value of the maximum achievable fluorescence. In the case of Au cores,the fluorescence enhancements for wavelengths within the first near-infrared biological window (NIR-I) between 700 and 900 nm can be improved twofold compared to homogeneous Au particle when the shell refractive index ns > 2. As a rule of thumb, the wavelength region of optimal fluorescence (maximal nonradiative decay) turns out to be red-shifted (blue-shifted) by as much as 50 nm relative to the localized surface plasmon resonance wavelength of corresponding optimized core-shell particle. Our results provide important design rules and general guidelines for enabling versatile platforms for imaging, light source, and biological applications.
Contrary to a paradigm of metal-enhanced fluorescence, unusually thick dielectric coatings can be very favorable to achieve extreme values of averaged fluorescence enhancement factor $\bar F\gtrsim 3000$ for emitters located on the surface, or in the interior, of the shell of Au@dielectric spherical core-shell particles under realistic conditions, even for the emitters with 100% intrinsic quantum yield. Thick dielectric coatings facilitate high-quality transverse electric (TE) multipole ($\ell=7$) resonances which are shown as the major cause for the reported extraordinary values of $\bar F$.
We theoretically and numerically investigate metal enhanced fluorescence of plasmonic core-shell nanoparticles doped with rare earth (RE) ions. Particle shape and size are engineered to maximize the average enhancement factor (AEF) of the overall doped shell. We show that the highest enhancement (11 in the visible and 7 in the near-infrared) are achieved by tuning either the dipolar or quadrupolar particle resonance to the rare earth ions excitation wavelength. Additionally, the calculated AEFs are compared to experimental data reported in the literature, obtained in similar conditions (plasmo…
Localized electromagnetic modes and negligible Ohmic losses dictate the growing interest in subwavelength all-dielectric nanoparticles. Although an exhaustive volume of study dealt with interaction of all-dielectric nanostructures with free-space electromagnetic fields, their performance as integrated photonics elements remains untackled. We present an experimental study of optical coupling between a resonant subwavelength silicon nanodisk and a non-resonant silicon waveguide, as probed by third harmonic generation microscopy. By placing the nanodisks at different distances from the waveguide,…
In this work, we study second-harmonic generation a monocrystalline nanoparticle with a non-centrosymmetric crystalline lattice. It was shown that breaking the symmetry of the nanoparticle's shape can significantly affect the second harmonic radiation pattern. We propose a method for explaining and predicting the generated field for arbitrary nanoparticles and provide selection rules for nanoparticles with several different symmetries.
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 …
A general concept of perfect nonradiating modes in dielectric nanoparticles of an arbitrary shape is put forward. It is proved that such modes exist in axisymmetric dielectric nanoparticles and have unlimited radiative Q-factors. With smart tuning of the excitation beams, perfect modes appear as deep minima in the scattered radiation spectra (up to complete disappearance), but at the same time, they have a giant amplification of the fields inside the particle. Such modes have no analogs and can be useful for the realization of nanosensors, low threshold nanolasers, and other strong nonlinear e…
In the present paper, we observed both two-photon and three-photon induced distinct photoluminescence from GO nanoparticles under fs laser excitation. Conjugated with PEG molecules, GO nanoparticles exhibited high chemical stability, and could effectively label HeLa cells. Imaged with a two-photon scanning microscope, GO nanoparticles were observed to localize in the mitochondria, endoplasmic reticulum, Golgi and lysosome of HeLa cells. Furthermore, GO nanoparticles were micro-injected into the brain of a black mouse, and in vivo two-photon luminescence imaging illustrated that GO nanoparticle…
Based on full-wave scattering theory with self-consistent mean field approximation, we study the optical multi-stability of graphene-wrapped dielectric nanoparticles. We demonstrate that the optical bistability (OB) of the graphene-wrapped nanoparticle exist in both near-field and far-field spectra, and show the optical multi-stability arising from the contributions of higher-order terms of the incident external field. Moreover, both the optical stable region and the switching threshold values can be tuned by changing either the Fermi level or the size of the nanoparticle. Our results promise …
The study of high-index dielectric nanoparticles currently attracts a lot of attention. They do not suffer from absorption but promise to provide control on the properties of light comparable to plasmonic nanoparticles. To further advance the field, it is important to identify versatile dielectric nanoparticles with unconventional properties. Here, we show that breaking the symmetry of an all-dielectric nanoparticle leads to a geometrically tunable magneto-electric coupling, i.e. an omega-type bianisotropy. The suggested nanoparticle exhibits different backscatterings and, as an interesting co…
We report a method to measure the size of single dielectric nanoparticles with high accuracy and precision using quantitative differential interference contrast (DIC) microscopy. Dielectric nanoparticles are detected optically by the conversion of the optical phase change into an intensity change using DIC. Phase images of individual nanoparticles were retrieved from DIC by Wiener filtering, and a quantitative methodology to extract nanoparticle sizes was developed. Using polystyrene beads of 100 nm radius as size standard, we show that the method determines this radius within a few nm accurac…
Plasmonic nanoparticles provide an ideal environment for the enhancement of fluorescent emission. On the one hand, they locally amplify the electromagnetic fields, increasing the emitter excitation rate, and on the other hand, they provide a high local density of states that accelerates spontaneous emission. However, when the emitter is placed in close proximity to a single metal nanoparticle, the number of nonradiative states increases dramatically, causing the fluorescence to quench. It has been predicted theoretically that, through a judicious placing of the emitter, fluorescence in plasmon…
An efficient method to fabricate transparent glass ceramic fibers containing in-situ grown Er3+-doped oxide nanoparticles is presented. Characterization of the drawn fibers exhibits low loss (0.4 dB/m) and broadened Er3+ emission spectrum. This attractive method offers new scopes for fiber amplifiers.
We study numerically, analytically and experimentally the resonant transmission of light in a waveguide formed by a periodic array of high-index dielectric nanoparticles with a side-coupled resonator. We demonstrate that a resonator with high enough Q-factor provides the conditions for the Fano-type interference allowing to control the resonant transmission of light. We suggest a practical realization of this resonant effect based on the quadrupole resonance of a dielectric particle and demonstrate it experimentally for ceramic spheres at microwaves.
Single gold nanoparticles can act as nanoantennas for enhancing the fluorescence of emitters in their near-fields. Here we present experimental and theoretical studies of scanning antenna-based fluorescence microscopy as a function of the diameter of the gold nanoparticle. We examine the interplay between fluorescence enhancement and spatial resolution and discuss the requirements for deciphering single molecules in a dense sample. Resolutions better than 20 nm and fluorescence enhancement up to 30 times are demonstrated experimentally. By accounting for the tip shaft and the sample interface …
We estimate the electromagnetic fields generated by a cluster of dielectric nanoparticles embedded into a background made of a vacuum. The dielectric nanoparticles are small scaled but enjoy high contrast of their relative permittivity. Such scales/contrasts can be ensured using the Lorentz model with incident frequencies chosen appropriately close to the undamped resonance (appearing in the Lorentz model). Under certain ratio between their size and contrast, these nanoparticles generate resonances, called dielectric resonances. These resonances are characterized and computed via the spectrum …
Nanoparticles levitated in vacuum can be set to spin at ultimate frequencies, limited only by the tensile strength of the material. At such high frequencies, drastic changes to the dynamics of solid-state quantum excitations are to be expected. Here, we theoretically describe the interaction between acoustic phonons and the rotation of a nanoparticle around its own axis, and model how the acoustic and optical properties of the nanoparticle change when it rotates at a fixed frequency. As an example, we analytically predict the scaling of the shape, the acoustic eigenmode spectrum, the permittiv…
We theoretically analyse the hybrid Mie-exciton optical modes arising from the strong coupling of excitons in organic dyes or transition-metal dichalcogenides with the Mie resonances of high-index dielectric nanoparticles. Detailed analytic calculations show that silicon--exciton core--shell nanoparticles are characterised by a richness of optical modes which can be tuned through nanoparticle dimensions to produce large anticrossings in the visible or near infrared, comparable to those obtained in plexcitonics. The complex magnetic-excitonic nature of these modes is understood through spectral…
We propose a novel approach for efficient tuning of optical properties of a high refractive index subwavelength nanoparticle with a magnetic Mie-type resonance by means of femtosecond laser irradiation. This concept is based on ultrafast photo-injection of dense (>10^20 cm^-3) electron-hole plasma within such nanoparticle, drastically changing its transient dielectric permittivity. This allows to manipulate by both electric and magnetic nanoparticle responses, resulting in dramatic changes of its scattering diagram and scattering cross section. We experimentally demonstrate 20 % tuning of refl…
We develop a multipolar theory of second-harmonic generation (SHG) by dielectric nanoparticles made of noncentrosymmetric materials with bulk quadratic nonlinearity. We specifically analyze two regimes of optical excitation: illumination by a plane wave and single-mode excitation, when the laser pump drives the magnetic dipole mode only. Considering two classes of nonlinear crystalline solids (dielectric perovskite material and III-V semiconductor), we apply a symmetry approach to derive selection rules for the multipolar composition of the nonlinear radiation. The developed description can be…
We experimentally observe the dipole scattering of a nanoparticle using a high numerical aperture (NA) imaging system. The optically levitated nanoparticle provides an environment free of particle-substrate interaction. We illuminate the silica nanoparticle in vacuum with a 532 nm laser beam orthogonally to the propagation direction of the 1064 nm trapping laser beam strongly focused by the same high NA objective used to collect the scattering, which results in a dark background and high signal-noise ratio. The dipole orientations of the nanoparticle induced by the linear polarization of the i…
Sometimes it appears, sometimes it does not. We present a theoretical study of circular dichroism in the second-harmonic signal of single dielectric nanostructures with different symmetries and noncentrosymmetric materials. We show that this effect is not fully identified only by macroscopic and lattice symmetries, but their relative orientation as well. Based on the cumbersome symmetry and modal analysis, we provide a general and very simple formula to determine whether the dichroism exists, and a table with the most significant cases.
We propose a method for slowing down light pulses by using composites doped with metal nanoparticles. The underlying mechanism is related to the saturable absorption near the plasmon resonance in a pump-probe regime, leading to strong dispersion of the probe refractive index and significantly reduced group velocities. By using the non-collinear scheme, it is possible to realize the total fractional delay of 43 or larger values. This scheme promises simple and compact slow-light on-chip devices with tunable delay and THz bandwidth.
We demonstrate theoretically that a subwavelength spherical dielectric nanoparticle coated with a gain shell forms a nanolaser. Lasing modes of such a nanolaser are associated with the Mie resonances of the nanoparticle. We establish a general condition for the lasing threshold and show that the use of high refractive index dielectric media allows for lasing with a threshold significantly lower than that for nanolasers incorporating lossy plasmonic metals.
A high index dielectric nano-sphere can be excited and yet remain radiationless. A method to excite the non-radiating anapole mode of a high index isotropic dielectric nanosphere is presented. With tightly focused radially polarized beam illumination, the main-contributing electric dipole mode and magnetic modes can be zero with only a weak electric quadruple contributing to the total scattering. Further, with a standing wave illumination formed by two counter-propagating focused radially polarized beam under $4π$ configuration, the ideal radiationless ananpole can be excited.
Strong enhancement of molecular circular dichroism has the potential to enable efficient asymmetric photolysis, a method of chiral separation that has conventionally been impeded by insufficient yield and low enantiomeric excess. Here, we study experimentally how predicted enhancements in optical chirality density near resonant silicon nanodisks boost circular dichroism. We use fluorescence-detected circular dichroism spectroscopy to measure indirectly the differential absorption of circularly polarized light by a monolayer of optically active molecules functionalized to silicon nanodisk array…
High-index spherical nanoparticles with low material losses support sharp high-Q electric and magnetic resonances and exhibit a number of interesting optical phenomena. Developments in fabrication techniques have enabled the further study of their properties and the investigation of related optical effects. After deposition on a substrate, the optical properties of a particle change dramatically due to mutual interaction. Here, we consider a silicon spherical nanoparticle on a dielectric one-layered substrate. At the normal incidence of light, the layer thickness controls the contribution of t…
The problem of enhanced molecular emission in close proximity to dielectric and metallic interfaces is of great importance for many physical and biological applications. Here we present an exact treatment of the problem from the view point of classical electromagnetism. Self-consistent analytical theory of the surface fluorescence enhancement is developed for configurations consisting of an emitter in proximity to core-shell metal-dielectric nanoparticles. The dependence of the fluorescence enhancement on the excitation laser and fluorescence frequencies and distance of the emitter to the nano…
We show that dielectric spheres can be cloaked by a shell of amorphously arranged metallic nanoparticles. The shell represents an artificial medium with tunable effective properties that can be adjusted such that the scattered signals of shell and sphere almost cancel each other. We provide an analytical model for the cloak design and prove numerically that the cloak operates as desired. We show that more than 70% of the scattered signal of the sphere can be suppressed at the design wavelength. Advantages and disadvantages of such a cloak when compared to other implementations are disclosed.
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 develop multipolar theory of nonlinear generation of entangled photons from subwavelength dielectric particles due to the spontaneous parametric downconversion. We demonstrate that optical excitation in resonance with the high-quality supercavity mode of the aluminum gallium arsenide (AlGaAs) nanodisk leads to a strong enhancement of generation of entangled photon pairs associated with electric and magnetic dipole modes. Our rigorous numerical results are corroborated by an analytical model, universally describing formation of high-$Q$ resonant states and dark states due to the interference…
We introduce a novel hybrid metal-dielectric nanoantenna composed of dielectric (crystalline silicon) and metal (silver) nanoparticles. A high-permittivity dielectric nanoparticle allows to achieve effective light harvesting, and nonlinearity of a metal nanoparticle controls the radiation direction. We show that the radiation pattern of such a nanoantenna can be switched between the forward and backward directions by varying only the light intensity around the level of 11 MW/cm$^2$, with the characteristic switching time of 260 fs.
Controlling the transport, trapping, and filtering of nanoparticles is important for many applications. By virtue of their weak response to gravity and their thermal motion, various physical mechanisms can be exploited for such operations on nanoparticles. However, the manipulation based on optical forces is potentially most appealing since it constitutes a highly deterministic approach. Plasmonic nanostructures have been suggested for this purpose, but they possess the disadvantages of locally generating heat and trapping the nanoparticles directly on surface. Here, we propose the use of diel…
Plasmonic structures interacting with light provide electromagnetic resonances which result in a high degree of local field confinement enabling the enhancement of light-matter interaction. Plasmonic structures typically consist of metals which, however, suffer from very high ohmic losses and heating. High-index dielectrics, on the other hand, can serve as an alternative material due to their low-dissipative nature and strong scattering abilities. We study the optical properties of a system composed of all-dielectric nanoparticle arrays covered with a film of organic dye molecules (IR-792), an…
Simultaneous scattering invisibility and free-space field enhancement have been achieved based on multipolar interferences among all-dielectric nanoparticles. The scattering properties of all-dielectric nanowire quadrumers are investigated and two sorts of scattering invisibilities have been identified: the trivial invisibility where the individual nanowires are not effectively excited; and the nontrivial invisibility with strong multipolar excitations within each nanowire, which results in free-space field enhancement outside the particles. It is revealed that such nontrivial invisibility ori…
We demonstrate the simultaneous generation of second, third, and fourth harmonic from a single dielectric Bismuth Ferrite nanoparticle excited by a telecom fiber laser at 1560 nm. We first characterize the signals associated with different nonlinear orders in terms of spectrum, excitation intensity dependence, and relative signal strengths. Successively, on the basis of the polarization-resolved emission curves of the three harmonics, we discuss the interplay of susceptibility tensor components at the different orders and we show how polarization can be used as an optical handle to control the…
We review a new, rapidly developing field of all-dielectric nanophotonics which allows to control both magnetic and electric response of structured matter by engineering the Mie resonances in high-index dielectric nanoparticles. We discuss optical properties of such dielectric nanoparticles, methods of their fabrication, and also recent advances in all-dielectric metadevices including couple-resonator dielectric waveguides, nanoantennas, and metasurfaces.
We study the interplay between disorder and topology for the localized edge states of light in topological zigzag arrays of resonant dielectric nanoparticles. We characterize topological properties by the winding number that depends on both zigzag angle and spacing between nanoparticles in the array. For equal-spacing arrays, the system may have two values of the winding number $ν=0$ or $1$, and it demonstrates localization at the edges even in the presence of disorder, being consistent with experimental observations for finite-length nanodisk structures. For staggered-spacing arrays, the syst…
Nonradiating current configurations attract attention of physicists for many years as possible models of stable atoms in the field theories. One intriguing example of such a nonradiating source is known as anapole (which means without poles in Greek), and it was originally proposed by Yakov Zeldovich in nuclear physics. Recently, an anapole was suggested as a model of elementary particles describing dark matter in the Universe. Classically, an anapole mode can be viewed as a composition of electric and toroidal dipole moments, resulting in destructive interference of the radiation fields due t…
High-refractive index dielectric nanoparticles may exhibit strong directional forward light scattering at visible and near-infrared wavelengths due to interference of simultaneously excited electric and magnetic dipole resonances. For a spherical high-index dielectric, the so-called first Kerker's condition can be realized, at which the backward scattering practically vanishes for some combination of refractive index and particle size. However, Kerker's condition for spherical particles is only possible at the tail of the scattering resonances, when the particle scatters light weakly. Here we …
By combining analytical and numerical approaches, we study resonantly enhanced second-harmonic generation (SHG) by individual high-index dielectric nanoparticles made of centrosymmetric materials. Considering both bulk and surface nonlinearities, we describe second-harmonic nonlinear scattering from a silicon nanoparticle optically excited in the vicinity of the magnetic and electric dipolar resonances. We discuss the contributions of different nonlinear sources, and the effect of the low-order optical Mie modes on the characteristics of the generated far-field. We demonstrate that the multipo…
We study the interplay between collective and individual optically-induced magnetic responses in quadrumers made of identical dielectric nanoparticles. Unlike their plasmonic counterparts, all-dielectric nanoparticle clusters are shown to exhibit multiple dimensions of resonant magnetic responses that can be employed for the realization of anomalous scattering signatures. We focus our analysis on symmetric quadrumers made from silicon nanoparticles and verify our theoretical results in proof-of-concept radio frequency experiments demonstrating the existence of a novel type of magnetic Fano res…
All-dielectric nanophotonics becomes a versatile tool for various optical applications, including nanothermometry and optical heating. Its general concept includes excitation of Mie resonances in nonplasmonic nanoparticles. However, the potential of resonant dielectric nanoparticles in drug delivery applications still have not been fully realized. Here, optically resonant dielectric iron oxide nanoparticles ($α$-Fe$_2$O$_3$ NPs) are employed for remote rupture of microcontainers used as drug delivery platform. It is theoretically and experimentally demonstrated, that $α$-Fe$_2$O$_3$ NPs has se…
It is well known that Raman scattering and fluorescence can be enhanced by the presence of metallic nanoparticles. Here, we derive simple equations to analyse the influence of metallic nanoparticles on upconversion processes such as non-radiative energy transfer or excited state absorption. We compare the resulting expressions with the more familiar Raman and fluorescence cases, and find significant differences. We use numerical simulations to calculate the upconverted signal enhancement achievable by means of metallic spheres of different radii, and find particles of 100-400nm radius at infra…
We propose a dielectric structure which focuses the laser light well beyond the diffraction limit and thus considerably enhances the exerted optical trapping force upon dielectric nanoparticles. Although the structure supports a Fabry-Perot resonance, it actually acts as a nanoantenna in that the role of the resonance is to funnel the laser light into the structure. In comparison with the lens illuminating the structure, the proposed structure offers roughly a 10000-fold enhancement in the trapping force - part of this enhancement comes from an 80-fold enhancement in the field intensity, and t…
We discuss nanophotonic structures composed of high-index dielectric nanoparticles and present several basic approaches for numerical study of their collective optical response. We also provide comparison on the collective optical properties of dielectric and plasmonic structures, and review experimental demonstrations of Fano resonances in all-dielectric nanoparticle oligomers.
Enhancement of optical response with high-index dielectric nanoparticles is attributed to the excitation of their Mie-type magnetic and electric resonances. Here we study Raman scattering from crystalline silicon nanoparticles and reveal that magnetic dipole modes have much stronger effect on the scattering than electric modes of the same order. We demonstrate experimentally a 140-fold enhancement of Raman signal from individual silicon spherical nanoparticles at the magnetic dipole resonance. Our results confirm the importance of the optically-induced magnetic response of subwavelength dielec…
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…
