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 the nanoparticle's electric and magnetic multipoles to the subsequent optical response. We show that changing the polarization of incident light at a specific excitation angle and layer thickness leads to switching between the multipoles. We further observe a related polarization-driven control over the direction of the scattered radiation.
We study nonlinear response of a dimer composed of two identical Mie-resonant dielectric nanoparticles illuminated normally by a circularly polarized light. We develop a general theory describing hybridization of multipolar modes of the coupled nanoparticles, and reveal nonvanishing nonlinear circular dichroism (CD) in the second-harmonic generation (SHG) signal enhanced by the multipolar resonances in the dimer provided its axis is oriented under an angle to the crystalline lattice of the dielectric material. We present experimental results for this SHG-CD effect obtained for the AlGaAs dimer…
Optical properties of nanoparticles attract continuous attention owing to their high fundamental and applied importance across many disciplines. Recently emerged field of all-dielectric nanophotonics employs optically induced electric and magnetic Mie resonances in dielectric nanoparticles with a high refractive index. This property allows obtaining additional valuable degrees of freedom to control optical responses of nanophotonic structures. Here we propose a conceptually distinct approach towards reaching optical resonances in dielectric nanoparticles. We show that lacking conventional Mie …
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…
A type of 3-dimensional optical negative-refractive-index metamaterials composed of all dielectric nanospheres is proposed and demonstrated theoretically. The metamaterials are constructeded by pairing together two kinds of dielectric nanospheres as concentric shells embedded in a host medium. Mie-based extended effective theory shows that the dielectric core and the dielectric shell provide the negative permeability and the negative permittivity, respectively, both due to the strong Mie resonances. Within the coupled resonant frequency region, the negative index of refraction can be achieved.
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 employ structured light for the second-harmonic generation from subwavelength AlGaAs nanoparticles that support both electric and magnetic multipolar Mie resonances. The vectorial structure of the pump beam allows addressing selectively Mie-resonant modes and control the strength of the generated nonlinear fields. We observe experimentally the enhancement of the second-harmonic generation for the azimuthally polarized vector beams near magnetic dipole resonance, and match our observations with the numerical decomposion of the Mie-type multipoles for the fundamental and generated second-harm…
Hopping of nanoparticles in optical tweezers governed by Mie resonances
Nonlinear Physics Center, Research School of Physics, Australian National University（澳大利亚国立大学物理研究学院非线性物理中心）；School of Optoelectronic Engineering and Instrumentation Science, Dalian University of Technology（大连理工大学光电工程与仪器科学学部）；Department of Electrical and Electronic Engineering, The University of Melbourne（墨尔本大学电气与电子工程系）；Photonics Laboratory, Physics Unit, Tampere University（坦佩雷大学物理学单元光子学实验室）
Resonantly enhanced Raman scattering in dielectric nanostructures has been recently proven to be an effcient tool for developing nanothermometry and experimental determination of their mode- composition. In this paper, we develop a rigorous analytical theory based on the Green's function approach to calculate the Raman emission from crystalline high-index dielectric nanoparticles. As an example, we consider silicon nanoparticles which have a strong Raman response due to active optical phonon modes. We relate enhancement of Raman signal emission to Purcell effect due to the excitation of Mie mo…
Controlling ultraviolet light at the nanoscale using optical Mie resonances holds great promise for a diverse set of applications, such as lithography, sterilization, and biospectroscopy. However, Mie resonances hosted by dielectric nanoantennas are difficult to realize at ultraviolet wavelengths due to the lack of both suitable materials and fabrication methods. Here, we systematically search for improved materials by computing the frequency dependent optical permittivity of 338 binary semiconductors and insulators from first principles, and evaluate their potential performance as high refrac…
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…
Halide perovskites is a family of semiconductor materials demonstrating prospective properties for optical cooling owing to efficient luminescence at room temperature and strong electron-phonon interaction. On the other hand, perovskite based nanophotonic designs would allow for efficient optical cooling at nanoscale. Here we propose a novel strategy for enhancement of optical cooling at nanoscale based on optical resonances engineering in halide perovskite nanoparticles. Namely, photoluminescence up-conversion efficiency in a nanoparticle is optimized via excitation of Mie-resonances both at …
Nanoparticles supporting a distinct series of Mie resonances have enabled a new class of nanoantennas and provide efficient ways to manipulate light at the nanoscale. The ability to flexibly tune the optical resonances and scattering directionality are particularly essential for various applications ranging from biosensing to nanolasers. In this paper, we investigate the core-shell nanoparticles that support both electric and magnetic Mie resonances and for the first time systematically reveal the mode evolution from a pure high-index dielectric nanosphere to a pure plasmonic one, where it has…
Optically induced Mie resonances in dielectric nanoantennas feature low dissipative losses and large resonant enhancement of both electric and magnetic fields. They offer an alternative platform to plasmonic resonances to study light-matter interactions from the weak to the strong coupling regimes. Here, we experimentally demonstrate the strong coupling of bright excitons in monolayer WS$_2$ with Mie surface lattice resonances (Mie-SLRs). We resolve both electric and magnetic Mie-SLRs of a Si nanoparticle array in angular dispersion measurements. At the zero detuning condition, the dispersion …
Laser cooling of solids keeps attracting attention owing to abroad range of its applications that extends from cm-sized all-optical cryocoolers for airborne and space-based applications to cooling on nanoparticles for biological and mesoscopic physics. Laser cooling of nanoparticles is a challenging task. We propose to use Mie resonances to enhance anti-Stokes fluorescence laser cooling in rare-earth (RE) doped nanoparticles made of low-phonon glasses or crystals. As an example, we consider an Yb3+:YAG nanosphere pumped at the long wavelength tail of the Yb3+ absorption spectrum at 1030 nm. We…
A system of periodic poly-disperse coated nano-rods is considered. Both the coated nano-rods and host material are non-magnetic. The exterior nano-coating has a frequency dependent dielectric constant and the rod has a high dielectric constant. A negative effective magnetic permeability is generated near the Mie resonances of the rods while the coating generates a negative permittivity through a field resonance controlled by the plasma frequency of the coating and the geometry of the crystal. The explicit band structure for the system is calculated in the sub-wavelength limit. Tunable pass ban…
It was theoretically proposed and experimentally demonstrated that anti-reflection coating allows one to trap a high dielectric sphere, at the same time enhancing the transverse optical force. Here, by explicitly calculating the gradient force and the scattering force, we rigorously show that these were mainly consequences of the reduction in scattering force due to the suppression of backward scattering, and enhancement in gradient force due to the increased in overall particle size. The reduction of scattering force can be understood within a ray optics theory and also the Mie theory. The co…
Future technologies underpinning high-performance optical communications, ultrafast computations and compact biosensing will rely on densely packed reconfigurable optical circuitry based on nanophotonics. For many years, plasmonics was considered as the only available platform for nanoscale optics, but the recently emerged novel field of Mie resonant metaphotonics provides more practical alternatives for nanoscale optics by employing resonances in high-index dielectric nanoparticles and structures. In this mini-review we highlight some recent trends in the physics of dielectric Mie-resonant na…
Nanoparticle (NP) arrays of noble metals strongly absorb light in the visible to infrared wavelengths through resonant interactions between the incident electromagnetic field and the metal's free electron plasma. Such plasmonic interfaces enhance light absorption and photocurrent in solar cells. We report a cost effective and scalable room temperature/pressure spin-coating route to fabricate broadband plasmonic interfaces consisting of silver NPs. The NP interface yields photocurrent enhancement (PE) in thin film silicon devices by up to 200% which is significantly greater than previously repo…
The complex refractive index m=n+ik of a particle is an intrinsic property which cannot be directly measured, it must be inferred from its extrinsic properties such as the scattering and absorption cross-sections. Bohren and Huffman called this approach describing the dragon from its tracks, since the inversion of Lorenz-Mie theory equations is intractable without the use of computers. This article describes PyMieScatt, an open-source module for Python that contains functionality for solving the inverse problem for complex m using extensive optical and physical properties as input, and calcula…
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…
Based on the Lorenz-Mie theory, we derive analytical expressions of radiative and nonradiative transition rates for different orientations of a point dipole emitter in the vicinity of an infinitely long circular cylinder of arbitrary radius. Special attention is devoted to the spontaneous decay rate of a dipole emitter near a subwavelength-diameter nanowire coated with a graphene monolayer. We show that plasmonic Fano resonances associated with light scattering by graphene-coated nanowires appear in the Purcell factor as a function of transition wavelength. Furthermore, the Fano line shape of …
Metal nanoparticle (NP) surface coatings are known to significantly enhance the ultra-violet luminescence intensity of ZnO. Although there is general agreement that resonantly excited Localized Surface Plasmons (LSPs) in metal NPs can directly couple to excitons in the semiconductor increasing their spontaneous emission rate, the exact mechanisms involved in this phenomenon are currently not fully understood. In this work, LSP-exciton coupling in a ZnO single crystal and ZnO nanorods coated with a 2 nm Al layer has been investigated using correlative photoluminescence and depth-resolved cathod…
The evidence of strong coupling between plasmons and molecular excitons for plasmonic nanoparticle (NP) dimers exhibiting ultra-sensitive surface enhanced resonant Raman scattering is the observation of anti-crossing in the coupled resonance. However, it is not easy to experimentally tune plasmon resonance of such dimers for the observation. In this work, we theoretically investigate the anti-crossing properties of the dimers coated by the thin dye films with thicknesses greater than 0.1 nm and gap distances larger than 1.2 nm according to the principles of classical electromagnetism. The plas…
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.
All-dielectric resonant nanophotonics lies at the heart of modern optics and nanotechnology due to the unique possibilities to control scattering of light from high-index dielectric nanoparticles and metasurfaces. One of the important concepts of dielectric Mie-resonant nanophotonics is associated with the Kerker effect that drives the unidirectional scattering of light from nanoantennas and Huygens' metasurfaces. Here we suggest and demonstrate experimentally a novel effect manifested in the nearly complete simultaneous suppression of both forward and backward scattered fields. This effect is…
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…
Due to their many potential applications, there is an increasing interest in studying hybrid systems composed of optically active media and plasmonic metamaterials. In this work we focus on a particular system which consists of an optically active silica core covered by a gold shell. We find that the spaser (surface plasmon amplification by stimulated emission of radiation) conditions can be found at the poles of the scattering cross section of the system, a result that remains valid beyond the geometry studied. We explored a wide range of parameters that cover most of the usual experimental c…
A potential control over the position of maxima of scattering and absorption cross-sections can be exploited to better tailor nanoparticles for specific light-matter interaction applications. Here we explain in detail the mechanism of an appreciable blue shift of the absorption cross-section peak relative to a metal spherical particle localized surface plasmon resonance (LSPR) and remaining scattering and extinction cross sections. Such a branching of cross sections maxima requires a certain threshold value of size parameter x~0.7 and is a prerequisite for obtaining high fluorescence enhanceme…
Copper phosphate micro-flowers coated with indocyanine green and iron oxide nanoparticles for in vivo localization optoacoustic tomography and magnetic actuation
High-index dielectric metasurfaces featuring Mie-type electric and magnetic resonances have been of a great interest in a variety of applications such as imaging, sensing, photovoltaics and others, which led to the necessity of an efficient large-scale fabrication technique. To address this, here we demonstrate the use of single-pulse laser interference for direct patterning of an amorphous silicon film into an array of Mie resonators. The proposed technique is based on laser-interference-induced dewetting. A precise control of the laser pulse energy enables the fabrication of ordered dielectr…
Hard x-ray emission (20 - 200 keV) from plasmas produced by intense laser pulses on nanoparticle coated targets is compared with that from optically polished targets. The yield enhancement offered by nanoparticles is studied under different prepulse conditions. It is observed that the enhancement reduces when the nanoparticle coated target is irradiated with a prepulse with intensity greater than 10^13 W/cm^2. When the prepulse intensity exceeds 10^14 W/cm^2, the enhancement vanishes completely. This is attributed to preplasma formation on nanoparticles their subsequent structural modifcation …
We demonstrate an enhanced emission of high quantum yield molecules coupled to dielectric metasurfaces formed by periodic arrays of polycrystalline silicon nanoparticles. Radiative coupling of the nanoparticles, mediated by in-plane diffraction, leads to the formation of collective Mie scattering resonances or Mie surface lattice resonances (M-SLRs), with remarkable narrow line widths. These narrow line widths and the intrinsic electric and magnetic dipole moments of the individual Si nanoparticles allow to resolve electric and magnetic M-SLRs. Incidence angle- and polarization-dependent extin…
We investigate electromagnetic scattering of normally irradiated gyrotropic, magneto-optical core-shell cylinders using Lorenz-Mie theory. A general expression for time-averaged electromagnetic energy inside a coated gyroelectric and gyromagnetic scatterer is derived. Using realistic material parameters for a silica core and InSb shell, we calculate the stored electromagnetic energy and the scattering anisotropy. We show that the application of an external magnetic field along the cylinder axis induces a drastic decrease in electromagnetic absorption in a frequency range in the terahertz, wher…
The recently emerged concept of all-dielectric nanophotonics based on optical Mie resonances in high-index dielectric nanoparticles has proven a promising pathway to boost light-matter interactions at the nanoscale. In this work, we discuss the opportunities enabled by the interaction of dielectric nanoresonators with 2D transition metal dichalcogenides (2D TMDCs), leading to weak and strong coupling regimes. We perform a comprehensive analysis of bright exciton photoluminescence (PL) enhancement from various 2D TMDCs, including WS2, MoS2, WSe2, and MoSe2 via their coupling to Mie resonances o…
Two-dimensional semiconducting transition metal dichalcogenides (TMDCs) are extremely attractive materials for optoelectronic applications in the visible and near-IR range. Here, we address for the first time to the best of our knowledge the issue of resonance coupling in hybrid exciton-polariton structures based on single Si nanoparticles coupled to monolayer WS2. We predict a transition from weak to strong coupling regime , with a Rabi splitting energy exceeding 200 meV for a Si nanoparticle covered by monolayer WS 2 at the magnetic optical Mie resonance. This large transition is achieved du…
The Photothermal Heterodyne Imaging method is used to study for the first time the absorption spectra of individual gold nanoparticles with diameters down to 5 nm. Intrinsic size effects wich result in a broadening of the Surface Plasmon resonance are unambiguously observed. Dispersions in the peak energies and homogeneous widths of the single particle resonances are revealed. The experimental results are analysed within the frame of Mie theory.
Research School of Physics, Australian National University（澳大利亚国立大学物理研究学院）；School of Physics and Engineering, ITMO University（ITMO大学物理与工程学院）；Nanophotonic Systems Laboratory, Department of Mechanical and Process Engineering, ETH Zürich（苏黎世联邦理工学院机械与工艺工程系纳米光子系统实验室）
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…
Light-matter interactions at the nanoscale constitute a fundamental ingredient for engineering applications in nanophotonics and quantum optics. To this regard electromagnetic Mie resonances excited in high-refractive index dielectric nanoparticles have recently attracted interest because of their lower losses and better control over the scattering patterns compared to their plasmonic metallic counterparts. The emergence of several resonances in those systems results in an overall high complexity, where the electric and magnetic dipoles have significant overlap in the case of spherical symmetr…
We give a geometrical theory of resonances in Maxwell's equations that generalizes Mie formulae for spheres to any dielectric or metallic particle without sharp edges. We show that the electromagnetic response of a particle is given by a set of modes of internal and scattered fields and reveal a strong analogy between resonances in nanoparticles and excess noise in unstable macroscopic cavities. We give examples of two types of optical resonances: those in which a single pair of internal and scattered modes become strongly aligned in the sense defined in this paper, and those resulting from co…
Manipulating light on the nanoscale has become a central challenge in metadevices, resonant surfaces, nanoscale optical sensors, and many more, and it is largely based on resonant light confinement in dispersive and lossy metals and dielectrics. Here, we experimentally implement a novel strategy for dielectric nanophotonics: Resonant subwavelength confinement of light in air. We demonstrate that voids created in high-index dielectric host materials support localized resonant modes with exceptional optical properties. Due to the confinement in air, the modes do not suffer from the loss and disp…
A nanofiber-based optical tweezer is demonstrated. Trapping is achieved by combining attractive near-field optical gradient forces with repulsive electrostatic forces. Silica-coated Fe$_2$O$_3$ nanospheres of 300 diameter are trapped as close as 50 nm away from the surface with 810 $μ$W of optical power, with a maximum trap stiffness of 2.7 pN $μ$m$^{-1}$. Electrostatic trapping forces up to 0.5 pN are achieved, a factor of 50 larger than those achievable for the same optical power in conventional optical tweezers. Efficient collection of the optical field directly into the nanofiber enables u…
We propose a novel concept for efficient dynamic tuning of optical properties of a high refractive index subwavelength nanoparticle with a magnetic Mie-type resonance by means of femtosecond laser radiation. This concept is based on ultrafast generation of 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 extinction cross section and scattering diagram. Specifically, we demonstrate the effect of ultrafast switching-on a Hu…
Spherical silicon nanoparticles with sizes of a few hundreds of nanometers represent a unique optical system. According to theoretical predictions based on Mie theory they can exhibit strong magnetic resonances in the visible spectral range. The basic mechanism of excitation of such modes inside the nanoparticles is very similar to that of split-ring resonators, but with one important difference that silicon nanoparticles have much smaller losses and are able to shift the magnetic resonance wavelength down to visible frequencies. We experimentally demonstrate for the first time that these nano…
We demonstrated a biosensing approach which, for the first time, combines the high-sensitivity of whispering gallery modes (WGM) with a metallic nanoparticle based assay. We provided a computational model based on generalized Mie theory to explain the higher sensitivity of protein detection through Plasmonic enhancement. We quantitatively analyzed the binding of a model protein (i.e., BSA) to gold nanoparticles from high-Q WGM resonance frequency shifts, and fit the results to an adsorption isotherm, which agrees with the theoretical predictions of a two-component adsorption model.
Plasmonic optical tweezers are a ubiquitous tool for the precise manipulation of nanoparticles and biomolecules at low photon flux, while femtosecond-laser optical tweezers can probe the nonlinear optical properties of the trapped species with applications in biological diagnostics. In order to adopt plasmonic optical tweezers in real-world applications, it is essential to develop large-scale fabrication processes without compromising the trapping efficiency. Here, we develop a novel platform for continuous wave (CW) and femtosecond plasmonic optical tweezers, based on gold-coated black silico…
We have theoretically investigated optical tweezing of gain-functionalized microspheres using a highly focused single beam in the nonparaxial regime. We employ the Mie-Debye theory of optical tweezers to calculate the optical force acting on homogeneous and core-shell Mie microspheres with gain. We demonstrate that the optical gain plays a crucial role in optical manipulation, especially to optimize the restoring force and thus allowing for trapping of large refractive index and plasmonic particles. Indeed we demonstrate that one can trap such particles, which is usually not possible in the ca…
