Mode Hybridization in Silicon Core-Gold Shell Nanosphere.

A dielectric core-metal shell nanosphere has attracted scientific and technological interests due to the unique optical resonances arising from the hybridization of surface plasmon modes and cavity modes. The previous studies focus on a low-index dielectric core without its own optical resonances. Here, optical resonances of a core-shell nanosphere with a high refractive index (n ≈ 4) core with the lowest order Mie resonances in the visible range are investigated theoretically and experimentally. Scattering and absorption spectra of a core-shell nanosphere for different values of the core refractive index are first analyzed, and there is a transition of the hybridization scheme around n ≈ 2. Above the value, a characteristic hybridized mode with strong absorption and weak scattering emerges in the near-infrared range. A core-shell nanosphere composed of a silicon core and a gold shell is prepared, and the resonance modes are studied by single particle scattering spectroscopy and electron energy loss spectroscopy (EELS) in a transmission electron microscope. The core-shell nanospheres exhibit the hybridized modes depending on the core diameter. The hybridized mode as well as the higher order one that is not observable in the scattering spectroscopy is observed in the EELS.

Resonance Couplings in Si@MoS2 Core-Shell Architectures.

Heterostructures of transition metal dichalcogenides and optical cavities that can couple to each other are rising candidates for advanced quantum optics and electronics. This is due to their enhanced light-matter interactions in the visible to near-infrared range. Core-shell structures are particularly valuable for their maximized interfacial area. Here, the chemical vapor deposition synthesis of Si@MoS2 core-shells and extensive structural characterization are presented. Compared with traditional plasmonic cores, the silicon dielectric Mie resonator core offers low Ohmic losses and a wider spectrum of optical modes. The magnetic dipole (MD) mode of the silicon core efficiently couples with MoS2 through its large tangential component at the core surface. Using transmission electron microscopy and correlative single-particle scattering spectroscopy, MD mode splitting is experimentally demonstrated in this unique Si@MoS2 core-shell structure. This is evidence for resonance coupling, which is limited to theoretical proposals in this particular system. A coupling constant of 39 meV is achieved, which is ≈1.5-fold higher than previous reports of particle-on-film geometries with a smaller interfacial area. Finally, higher-order systems with the potential to tune properties are demonstrated through a dimer system of Si@MoS2 , forming the basis for emerging architectures for optoelectronic and nanophotonic applications.

Optical spin sorting chain.

Transverse spin angular momentum of light is a key concept in recent nanophotonics to realize unidirectional light transport in waveguides by spin-momentum locking. Herein we theoretically propose subwavelength nanoparticle chain waveguides that efficiently sort optical spins with engineerable spin density distributions. By arranging high-refractive-index nanospheres or nanodisks of different sizes in a zigzag manner, directional optical spin propagation is realized. The origin of efficient spin transport is revealed by analyzing the dispersion relation and spin angular momentum density distributions, being attributed to guided modes that possess transverse spin angular momenta. In contrast to conventional waveguides, the proposed asymmetric waveguide can spatially separate up- and down-spins and locate one parity inside and the other outside the structure. Moreover, robustness against bending the waveguide and its application as an optical spin sorter are presented. Compared to previous reports on spatial engineering of local spins in photonic crystal waveguides, we achieved miniaturization of the entire footprint down to the subwavelength scale.

Colloidal Solutions of Silicon Nanospheres toward All-Dielectric Optical Metafluids.

A colloidal solution of nanophotonic structures exhibiting optical magnetism is dubbed a liquid-phase metamaterial or an optical metafluid. Over the decades, plasmonic nanoclusters have been explored as constituents of a metafluid. However, optical magnetism of plasmonic nanoclusters is usually much weaker than the electric responses; the highest reported intensity ratio of the magnetic-to-electric responses so far is 0.28. Here, we propose an all-dielectric metafluid composed of crystalline silicon nanospheres. First, we address the advantages of silicon as a constituent material of a metafluid among major dielectrics. Next, we experimentally demonstrate for the first time that a silicon nanosphere metafluid exhibits strong electric and magnetic dipolar Mie responses across the visible to near-infrared spectral range. The intensity ratio of the magnetic-to-electric responses reaches unity. Finally, we discuss the perspective to achieve unnaturally high (>3), low, and even near-zero (<1) refractive index in the metafluid.

Visualizing the Nanoscopic Field Distribution of Whispering-Gallery Modes in a Dielectric Sphere by Cathodoluminescence.

A spherical dielectric particle can sustain the so-called whispering-gallery modes (WGMs), which can be regarded as circulating electromagnetic waves, resulting in the spatial confinement of light inside the particle. Despite the wide adoption of optical WGMs as a major light confinement mechanism in salient practical applications, direct imaging of the mode fields is still lacking and only partially addressed by simple photography and simulation work. The present study comprehensively covers this research gap by demonstrating the nanoscale optical-field visualization of self-interference of light extracted from excited modes through experimentally obtained photon maps that directly portray the field distributions of the excited eigenmodes. To selectively choose the specific modes at a given light emission detection angle and resonance wavelength, we use cathodoluminescence-based scanning transmission electron microscopy supplemented with angle-, polarization-, and wavelength-resolved capabilities. Equipped with semi-analytical simulation tools, the internal field distributions of the whispering-gallery modes reveal that radiation emitted by a spherical resonator at a given resonance frequency is composed of the interference between multiple modes, with one or more of them being comparatively dominant, leading to a resulting distribution featuring complex patterns that explicitly depend on the detection angle and polarization. Direct visualization of the internal fields inside resonators enables a comprehensive understanding of WGMs that can shed light on the design of nanophotonic applications.

Color Toning of Mie Resonant Silicon Nanoparticle Color Inks.

An ink of silicon nanoparticles (Si NPs) having the lowest-order Mie resonance in the visible range can generate noniridescent and nonfading structural colors in a wide area through a painting process. However, the strong wavelength dependence of the radiation pattern and the extinction coefficient make the multiple reflection behavior very complicated, and thus, a reliable tool is necessary to predict the hue, saturation, and brightness of the reflection color. In this work, a Monte Carlo simulation to predict the reflection color of Si NP inks is first developed. The simulation takes into account the scattering and absorption cross-sections, a radiation pattern of an individual NP, and multiple scattering in NP dispersion. The simulation shows that the reflection color of a Si NP ink depends strongly on the concentration because of the wavelength dependence of the multiple scattering behavior. To extend the controllable range of the hue, saturation, and brightness of Si NP inks, a mixture ink with light-absorbing carbon black (CB) NPs is developed. It is experimentally demonstrated that the combination of the Kerker-type back scattering of a Si NP and a broad absorption by a CB NP allows us to control the hue, saturation, and brightness in a wide range and to realize vivid reflection colors under room light.