Directional Fano Resonance in an Individual GaAs Nanospheroid

Fano resonance has been observed in a wide variety of nanophotonic structures such as photonic crystals, plasmonic structures, and metamaterials. It arises from the interference of discrete resonance states with broadband continuum states. As an emerging nanophotonic material, high‐index all‐dielectric nanomaterials provide a new platform to achieve Fano resonance by virtue of the simultaneous excited electric and magnetic resonances. However, to date, Fano resonance in the visible region has not been observed in individual high‐index all‐dielectric nanoparticles. Here, for the first time, the experimental observation of the directional Fano resonance is reported in an individual GaAs nanospheroid. The special geometry enables GaAs nanospheroids to generate spectrally overlapped electric and magnetic dipole resonances, which enhances their spectral coupling, giving rise to asymmetric‐shaped backward scattering spectrum. This directional Fano resonance can be tuned by the aspect ratio of nanospheroids as well as excitation polarization. In addition, efficient directional light scattering is realized at the total scattering peak of the GaAs nanospheroid. The forward‐to‐backward scattering ratio can be largely enhanced due to Fano dip in the backward scattering spectrum. These findings suggest that high‐index all‐dielectric nanospheroid is a promising candidate for directional sources and optical switches.     

Plasmon transmutation: inducing new modes in nanoclusters by adding dielectric nanoparticles

Planar clusters of coupled plasmonic nanoparticles support nanoscale electromagnetic "hot spots" and coherent effects, such as Fano resonances, with unique near and far field signatures, currently of prime interest for sensing applications. Here we show that plasmonic cluster properties can be substantially modified by the addition of individual, discrete dielectric nanoparticles at specific locations on the cluster, introducing new plasmon modes, or transmuting existing plasmon modes to new ones, in the resulting metallodielectric nanocomplex. Depositing a single carbon nanoparticle in the junction between a pair of adjacent nanodisks induces a metal-dielectric-metal quadrupolar plasmon mode. In a ten-membered cluster, placement of several carbon nanoparticles in junctions between multiple adjacent nanoparticles introduces a collective magnetic plasmon mode into the Fano dip, giving rise to an additional subradiant mode in the metallodielectric nanocluster response. These examples illustrate that adding dielectric nanoparticles to metallic nanoclusters expands the number and types of plasmon modes supported by these new mixed-media nanoscale assemblies.     

Double Fano-type resonances in heptamer-hole array transmission spectra with high refractive index sensing

Nanohole arrays or individual nanohole oligomers in metallic films have attracted intense attention due to their unique optical properties such as extraordinary optical transmission or Fano resonance. However, the nanohole oligomer array still remains largely unexplored. In this work, we numerically investigate the heptamer-hole arrays in an optically thin silver film, which can support double Fano-type resonances in the transmission spectra. The two Fano-type transmissions arise from the interference between the non-resonant direct transmission through holes and the resonant indirect scatterings based on the excitations of surface plasmons polaritons (SPPs, set up by the array periodicity) and a sub-radiant localized surface plasmon resonance (LSPR, arising from the anti-bonding hybridization between the central and the surrounding holes). Because of their different physical mechanisms, the two Fano resonances can be tuned independently. In addition, the LSPR-related Fano resonance shows an ultra-high sensitivity to surrounding dielectric medium with a figure of merit of 25 due to its sub-radiant feature, far larger than the SPP-related Fano resonance, offering tremendous potentials for plasmonic biosensors.     

Plasmonic nanoclusters: near field properties of the Fano resonance interrogated with SERS

While the far field properties of Fano resonances are well-known, clusters of plasmonic nanoparticles also possess Fano resonances with unique and spatially complex near field properties. Here we examine the near field properties of individual Fano resonant plasmonic clusters using surface-enhanced Raman scattering (SERS) both from molecules distributed randomly on the structure and from dielectric nanoparticles deposited at specific locations within the cluster. Cluster size, geometry, and interparticle spacing all modify the near field properties of the Fano resonance. For molecules, the spatially dependent SERS response obtained from near field calculations correlates well with the relative SERS intensities observed for individual clusters and for specific Stokes modes of a para-mercaptoaniline adsorbate. In all cases, the largest SERS enhancement is found when both the excitation and the Stokes shifted wavelengths overlap the Fano resonances. In contrast, for SERS from carbon nanoparticles we find that the dielectric screening introduced by the nanoparticle can drastically redistribute the field enhancement associated with the Fano resonance and lead to a significantly modified SERS response compared to what would be anticipated from the bare nanocluster.     

Tunable Fano Resonance and Plasmon–Exciton Coupling in Single Au Nanotriangles on Monolayer WS2 at Room Temperature

Tunable Fano resonances and plasmon–exciton coupling are demonstrated at room temperature in hybrid systems consisting of single plasmonic nanoparticles deposited on top of the transition metal dichalcogenide monolayers. By using single Au nanotriangles (AuNTs) on monolayer WS₂ as model systems, Fano resonances are observed from the interference between a discrete exciton band of monolayer WS₂ and a broadband plasmonic mode of single AuNTs. The Fano lineshape depends on the exciton binding energy and the localized surface plasmon resonance strength, which can be tuned by the dielectric constant of surrounding solvents and AuNT size, respectively. Moreover, a transition from weak to strong plasmon–exciton coupling with Rabi splitting energies of 100–340 meV is observed by rationally changing the surrounding solvents. With their tunable plasmon–exciton interactions, the proposed WS₂–AuNT hybrids can open new pathways to develop active nanophotonic devices.     

Subgroup decomposition of plasmonic resonances in hybrid oligomers: modeling the resonance lineshape

Plasmonic resonances with a Fano lineshape observed in metallic nanoclusters often arise from the destructive interference between a dark, subradiant mode and a bright, super-radiant one. A flexible control over the Fano profile characterized by its linewidth and spectral contrast is crucial for many potential applications such as slowing light and biosensing. In this work, we show how one can easily but significantly tailor the overall spectral profile in plasmonic nanocluster systems, for example, quadrumers and pentamers, by selectively altering the particle shape without a need to change the particle size, interparticle distance, or the number of elements of the oligomers. This is achieved through decomposing the whole spectrum into two separate contributions from subgroups, which are efficiently excited at their spectral peak positions. We further show that different strengths of interference between the two subgroups must be considered for a full understanding of the resulting spectral lineshape. In some cases, each subgroup is separately active in distinct frequency windows with only small overlap, leading to a simple convolution of the subspectra. Variation in particle shape of either subgroup results in the tuning of the overall spectral lineshape, which opens a novel pathway for shaping the plasmonic response in small nanoclusters.     

Directional double Fano resonances in plasmonic hetero-oligomers

We experimentally demonstrate for the first time a very compact plasmonic hetero-oligomer structure where the multiple radiant and subradiant modes can be tailored independently. Unlike previous approaches based on collective excitations in complex plasmonic systems, we show precise engineering of resonances leading to simultaneous spectral overlap of multiple plasmonic modes with opposite radiative character. This asymmetric behavior combined with inherent spatial features of the structure leads to directional double Fano resonances as shown with numerical analysis. A model based on temporal coupled mode theory is also provided to describe the double Fano behavior.     

Dark‐Exciton‐Mediated Fano Resonance from a Single Gold Nanostructure on Monolayer WS2 at Room Temperature

Strong spatial confinement and highly reduced dielectric screening provide monolayer transition metal dichalcogenides with strong many‐body effects, thereby possessing optically forbidden excitonic states (i.e., dark excitons) at room temperature. Herein, the interaction of surface plasmons with dark excitons in hybrid systems consisting of stacked gold nanotriangles and monolayer WS₂ is explored. A narrow Fano resonance is observed when the hybrid system is surrounded by water, and the narrowing of the spectral Fano linewidth is attributed to the plasmon‐enhanced decay of dark K‐K excitons. These results reveal that dark excitons in monolayer WS₂ can strongly modify Fano resonances in hybrid plasmon–exciton systems and can be harnessed for novel optical sensors and active nanophotonic devices.     

Observation of Supercavity Modes in Subwavelength Dielectric Resonators

Electromagnetic response of dielectric resonators with high refractive index is governed by optically induced electric and magnetic Mie resonances facilitating confinement of light with the amplitude enhancement. Traditionally, strong subwavelength trapping of light was associated only with plasmonic or epsilon‐near‐zero structures, which however suffer from material losses. Recently, an alternative localization mechanism was proposed allowing the trapping of light in individual subwavelength optical resonators with a high quality factor in the regime of a supercavity mode. Here, the experimental observation of the supercavity modes in subwavelength ceramic resonators in the radio‐frequency range is presented. It is experimentally demonstrated that the regime of supercavity modes can be achieved via precise tuning of the resonator's dimensions. A huge growth of the unloaded quality factor is achieved with experimental values up to 1.25 × 10⁴, limited only by material losses of ceramics. It is revealed that the supercavity modes can be excited efficiently both in the near‐ and far‐field. In both cases, the supercavity mode manifests itself explicitly as a Fano resonance with characteristic peculiarities of spectral shape and radiation pattern. A comparison of supercavities made of diversified materials for the visible, infrared, THz, and radio‐frequency regimes is provided.     

Controlling the interplay of electric and magnetic modes via Fano-like plasmon resonances

Assemblies of strongly coupled plasmonic nanoparticles can support highly tunable electric and magnetic resonances in the visible spectrum. In this Letter, we theoretically demonstrate Fano-like interference effects between the fields radiated by the electric and magnetic modes of symmetric nanoparticle trimers. Breaking the symmetry of the trimer system leads to a strong interaction between the modes. The near and far-field electromagnetic properties of the broken symmetry trimer are tunable across a large spectral range. We exploit this Fano-like effect to demonstrate spatial and temporal control of the localized electromagnetic hotspots in the plasmonic trimer.     

Magnetic Plasmonic Fano Resonance at Optical Frequency

Plasmonic Fano resonances are typically understood and investigated assuming electrical mode hybridization. Here we demonstrate that a purely magnetic plasmon Fano resonance can be realized at optical frequency with Au split ring hexamer nanostructure excited by an azimuthally polarized incident light. Collective magnetic plasmon modes induced by the circular electric field within the hexamer and each of the split ring can be controlled and effectively hybridized by designing the size and orientation of each ring unit. With simulated results reproducing the experiment, our suggested configuration with narrow line‐shape magnetic Fano resonance has significant potential applications in low‐loss sensing and may serves as suitable elementary building blocks for optical metamaterials.     

Real-space mapping of Fano interference in plasmonic metamolecules

An unprecedented control of the spectral response of plasmonic nanoantennas has recently been achieved by designing structures that exhibit Fano resonances. This new insight is paving the way for a variety of applications, such as biochemical sensing and surface-enhanced Raman spectroscopy. Here we use scattering-type near-field optical microscopy to map the spatial field distribution of Fano modes in infrared plasmonic systems. We observe in real space the interference of narrow (dark) and broad (bright) plasmonic resonances, yielding intensity and phase toggling between different portions of the plasmonic metamolecules when either their geometric sizes or the illumination wavelength is varied.     

Magnetic Plasmon Networks Programmed by Molecular Self‐Assembly

Nanoscale manipulation of magnetic fields has been a long‐term pursuit in plasmonics and metamaterials, as it can enable a range of appealing optical properties, such as high‐sensitivity circular dichroism, directional scattering, and low‐refractive‐index materials. Inspired by the natural magnetism of aromatic molecules, the cyclic ring cluster of plasmonic nanoparticles (NPs) has been suggested as a promising architecture with induced unnatural magnetism, especially at visible frequencies. However, it remains challenging to assemble plasmonic NPs into complex networks exhibiting strong visible magnetism. Here, a DNA‐origami‐based strategy is introduced to realize molecular self‐assembly of NPs forming complex magnetic architectures, exhibiting emergent properties including anti‐ferromagnetism, purely magnetic‐based Fano resonances, and magnetic surface plasmon polaritons. The basic building block, a gold NP (AuNP) ring consisting of six AuNP seeds, is arranged on a DNA origami frame with nanometer precision. The subsequent hierarchical assembly of the AuNP rings leads to the formation of higher‐order networks of clusters and polymeric chains. Strong emergent plasmonic properties are induced by in situ growth of silver upon the AuNP seeds. This work may facilitate the development of a tunable and scalable DNA‐based strategy for the assembly of optical magnetic circuitry, as well as plasmonic metamaterials with high fidelity.     

Actively controllable EIT-like resonance between localized and propagating surface plasmons for optical switching

We theoretically investigate the plasmonic interaction between radiative localized surface plasmon resonances and subradiative propagating surface plasmon modes in a nanostructure consisting of a periodic array of gold nanobars and an optically thick gold film, separated by a silica dielectric spacer layer. A controllable transparency window within the broad dipole resonance profile is observed clearly in the reflectance spectra via tailoring the length of the bar, the periodicity of the nanoparticle array, or the incident angle of applied field, respectively, a classic analog of electromagnetically induced transparency (EIT). We believe that the last excitation configuration is particularly beneficial for the realization of active manipulation of plasmonic optical switching without using coupling/control fields required in the conventional EIT scheme.     

Multiscale patterning of plasmonic metamaterials

The interaction of light with surface plasmons--collective oscillations of free electrons--in metallic nanostructures has resulted in demonstrations of enhanced optical transmission, collimation of light through a subwavelength aperture, negative permeability and refraction at visible wavelengths, and second-harmonic generation from magnetic metamaterials. The structures that display these plasmonic phenomena typically consist of ordered arrays of particles or holes with sizes of the order of 100 nm. However, surface plasmons can interact with each other over much longer distances, so the ability to organize nanoscale particles or holes over multiple length scales could lead to new plasmonic metamaterials with novel optical properties. Here, we present a high-throughput nanofabrication technique-soft interference lithography-that combines the ability of interference lithography to produce wafer-scale nanopatterns with the versatility of soft lithography, and use it to create such plasmonic metamaterials. Metal films perforated with quasi-infinite arrays of 100-nm holes were generated over areas greater than 10 cm(2), exhibiting sharp spectral features that changed in relative amplitude and shifted to longer wavelengths when exposed to increased refractive index environments. Moreover, gold nanohole arrays patterned into microscale patches exhibited strikingly different transmission properties; for instance, patches of nanoholes displayed narrow resonances (<14.5 nm full-width-at-half-maximum) that resulted in high refractive index sensitivities far exceeding those reported previously. Soft interference lithography was also used to produce various infinite and finite-area arrays of nanoparticles, including patterns that contained optically distinct particles side by side and arrays that contained both metallic and dielectric materials.     

Fano-chain: the Fano resonances in a nanoparticles chain

We show that for a linear chain of nanoparticles the Fano resonances can be excited and tuned through particle number manipulation by adding or removing particles from the chain. Fano modes excited in the chain, the spectrally overlapped bright superradiant and dark subradiant modes, are presented with current flow pictures for the first time, which clearly reveal how each individual particle reacts to light and interacts with other particles in the chain. This work may help design new Fano resonances in plasmonic metamaterials and nanostructures.     

Fano resonances in nanoscale plasmonic systems: a parameter-free modeling approach

The interaction between plasmonic resonances, sharp modes, and light in nanoscale plasmonic systems often leads to Fano interference effects. This occurs because the plasmonic excitations are usually spectrally broad and the characteristic narrow asymmetric Fano line-shape results upon interaction with spectrally sharper modes. By considering the plasmonic resonance in the Fano model, as opposed to previous flat continuum approaches, here we show that a simple and exact expression for the line-shape can be found. This allows the role of the width and energy of the plasmonic resonance to be properly understood. As examples, we show how Fano resonances measured on an array of gold nanoantennas covered with PMMA, as well as the hybridization of dark with bright plasmons in nanocavities, are well reproduced with a simple exact formula and without any fitting parameters.     

Controlling steady-state second harmonic signal via linear and nonlinear Fano resonances

ABSTRACT

Nonlinear signal even from a single molecule becomes visible at hot spots of plasmonic nanoparticles. In these structures, Fano resonances can control the nonlinear response in two ways. (i) A linear Fano resonance can enhance the hot spot field, resulting enhanced nonlinear signal. (ii) A nonlinear Fano resonance can enhance the nonlinear signal without enhancing the hot spot. In this study, we compare the enhancement of second harmonic signal at the steady-state obtained via these two methods. Since we are interested in the steady-state signal, we adapt a linear enhancement which works at the steady-state. This is different than the dark-hot resonances that appear in the transparency window due to enhanced plasmon lifetime.     

All‐Dielectric Active Terahertz Photonics Driven by Bound States in the Continuum

The remarkable emergence of all‐dielectric meta‐photonics governed by the physics of high‐index dielectric materials offers a low‐loss platform for efficient manipulation and subwavelength control of electromagnetic waves from microwaves to visible frequencies. Dielectric metasurfaces can focus electromagnetic waves, generate structured beams and vortices, enhance local fields for advanced sensing, and provide novel functionalities for classical and quantum technologies. Recent advances in meta‐photonics are associated with the exploration of exotic electromagnetic modes called the bound states in the continuum (BICs), which offer a simple interference mechanism to achieve large quality factors (Q) through excitation of supercavity modes in dielectric nanostructures and resonant metasurfaces. Here, a BIC‐driven terahertz metasurface with dynamic control of high‐Q silicon supercavities that are reconfigurable at a nanosecond timescale is experimentally demonstrated. It is revealed that such supercavities enable low‐power, optically induced terahertz switching and modulation of sharp resonances for potential applications in lasing, mode multiplexing, and biosensing.     

Janus Magnetic‐Plasmonic Nanoparticles for Magnetically Guided and Thermally Activated Cancer Therapy

Progress of thermal tumor therapies and their translation into clinical practice are limited by insufficient nanoparticle concentration to release therapeutic heating at the tumor site after systemic administration. Herein, the use of Janus magneto‐plasmonic nanoparticles, made of gold nanostars and iron oxide nanospheres, as efficient therapeutic nanoheaters whose on‐site delivery can be improved by magnetic targeting, is proposed. Single and combined magneto‐ and photo‐thermal heating properties of Janus nanoparticles render them as compelling heating elements, depending on the nanoparticle dose, magnetic lobe size, and milieu conditions. In cancer cells, a much more effective effect is observed for photothermia compared to magnetic hyperthermia, while combination of the two modalities into a magneto‐photothermal treatment results in a synergistic cytotoxic effect in vitro. The high potential of the Janus nanoparticles for magnetic guiding confirms them to be excellent nanostructures for in vivo magnetically enhanced photothermal therapy, leading to efficient tumor growth inhibition.