Broadband optical Ta2O5 antennas for directional emission of light.

Highly directive antennas with the ability of shaping radiation patterns in desired directions are essential for efficient on-chip optical communication with reduced cross talk. In this paper, we design and optimize three distinct broadband traveling-wave tantalum pentoxide antennas exhibiting highly directional characteristics. Our antennas contain a director and reflector deposited on a glass substrate, which are excited by a dipole emitter placed in the feed gap between the two elements. Full-wave simulations in conjunction with global optimization provide structures with an enhanced linear directivity as high as 119 radiating in the substrate. The high directivity is a result of the interplay between two dominant TE modes and the leaky modes present in the antenna director. Furthermore, these low-loss dielectric antennas exhibit a near-unity radiation efficiency at the operational wavelength of 780 nm and maintain a broad bandwidth. Our numerical results are in good agreement with experimental measurements from the optimized antennas fabricated using a two-step electron-beam lithography, revealing the highly directive nature of our structures. We envision that our antenna designs can be conveniently adapted to other dielectric materials and prove instrumental for inter-chip optical communications and other on-chip applications.

Unveiling nanometer scale extinction and scattering phenomena through combined electron energy loss spectroscopy and cathodoluminescence measurements.

Plasmon modes of the exact same individual gold nanoprisms are investigated through combined nanometer-resolved electron energy-loss spectroscopy (EELS) and cathodoluminescence (CL) measurements. We show that CL only probes the radiative modes, in contrast to EELS, which additionally reveals dark modes. The combination of both techniques on the same particles thus provides complementary information and also demonstrates that although the radiative modes give rise to very similar spatial distributions when probed by EELS or CL, their resonant energies appear to be different. We trace this phenomenon back to plasmon dissipation, which affects in different ways the plasmon signatures probed by these techniques. Our experiments are in agreement with electromagnetic numerical simulations and can be further interpreted within the framework of a quasistatic analytical model. We therefore demonstrate that CL and EELS are closely related to optical scattering and extinction, respectively, with the addition of nanometer spatial resolution.

Plasmon spectroscopy and imaging of individual gold nanodecahedra: a combined optical microscopy, cathodoluminescence, and electron energy-loss spectroscopy study.

Imaging localized plasmon modes in noble-metal nanoparticles is of fundamental importance for applications such as ultrasensitive molecular detection. Here, we demonstrate the combined use of optical dark-field microscopy (DFM), cathodoluminescence (CL), and electron energy-loss spectroscopy (EELS) to study localized surface plasmons on individual gold nanodecahedra. By exciting surface plasmons with either external light or an electron beam, we experimentally resolve a prominent dipole-active plasmon band in the far-field radiation acquired via DFM and CL, whereas EELS reveals an additional plasmon mode associated with a weak dipole moment. We present measured spectra and intensity maps of plasmon modes in individual nanodecahedra in excellent agreement with boundary-element method simulations, including the effect of the substrate. A simple tight-binding model is formulated to successfully explain the rich plasmon structure in these particles encompasing bright and dark modes, which we predict to be fully observable in less lossy silver decahedra. Our work provides useful insight into the complex nature of plasmon resonances in nanoparticles with pentagonal symmetry.

A multi-mode super-fano mechanism for enhanced third harmonic generation in silicon metasurfaces.

We present strong enhancement of third harmonic generation in an amorphous silicon metasurface consisting of elliptical nano resonators. We show that this enhancement originates from a new type of multi-mode Fano mechanism. These 'Super-Fano' resonances are investigated numerically in great detail using full-wave simulations. The theoretically predicted behavior of the metasurface is experimentally verified by linear and nonlinear transmission spectroscopy. Moreover, quantitative nonlinear measurements are performed, in which an absolute conversion efficiency as high as ηmax ≈ 2.8 × 10-7 a peak power intensity of 1.2 GW cm-2 is found. Compared to an unpatterned silicon film of the same thickness amplification factors of up to ~900 are demonstrated. Our results pave the way to exploiting a strong Fano-type multi-mode coupling in metasurfaces for high THG in potential applications.

Interacting plasmon and phonon polaritons in aligned nano- and microwires.

The availability of macroscopic, nearly periodic structures known as eutectics opens a new path for controlling light at wavelength scales determined by the geometrical parameters of these materials and the intrinsic properties of their component phases. Here, we analyze the optical waveguiding properties of eutectic mixtures of alkali halides, formed by close-packed arrangements of aligned cylindrical inclusions. The wavelengths of phonon polaritons in these constituents are conveniently situated in the infrared and are slightly larger than the diameter and separation of the inclusions, typically consisting on single-crystal wires down to submicrometer diameter. We first discuss the gap mode and the guiding properties of metallic cylindrical waveguides in the visible and near-infrared, and in particular we investigate the transition between cylinder touching and non-touching regimes. Then, we demonstrate that these properties can be extended to the mid infrared by means of phonon polaritons. Finally, we analyze the guiding properties of an actual eutectic. For typical eutectic dimensions, we conclude that crosstalk between neighboring cylindrical wires is small, thus providing a promising platform for signal propagation and image analysis in the mid infrared.

Surface plasmon mapping of dumbbell-shaped gold nanorods: the effect of silver coating.

We report on the identification of surface plasmons in individual gold dumbbell-shaped nanoparticles (AuDBs), as well as AuDBs coated with silver. We use spatially resolved electron energy-loss spectroscopy in a scanning electron microscope, which allows us to map plasmon-energy and intensity spatial distributions. Two dominant plasmon resonances are experimentally resolved in both AuDBs and silver-coated AuDBs. The intensity of these features is peaked either at the tips or at the sides of the nanoparticles. We present boundary element method simulations in good agreement with the experiment, allowing us to elucidate the nature of such modes. While the lower-energy, tip-focused plasmon is of longitudinal character for all dumbbells under consideration, the second side-bound plasmon has a more involved symmetry, starting as a longitudinal quadrupole in homogeneous AuDBs and picking up transversal components when silver coating is added. The longitudinal dipolar mode energy is found to blue-shift upon coating with silver. We find that the substrate produces sizable shifts in the plasmons of silver-coated AuDBs. Our analysis portraits a complex plasmonic scenario in metal nanoparticles coated with silver, including a transition from the original homogeneous gold dumbbell plasmons to the modes of homogeneous silver rods. We believe that these findings can have potential application to plasmon engineering.

Spectral imaging of individual split-ring resonators.

We report on spectral imaging within individual silver split-ring resonators (SRRs) operating in the near infrared-visible range. We classified the optical eigenmodes from the measurement of their energies and nanometer scale spatial distributions. They are plasmonic standing waves that show great similarities with that of nanoantennas. We, however, evidenced marked differences in the near-field electric field lines' spatial distribution and the energies' dispersion. We also showed that the subwavelength defect's influence on the SRRs' eigenmodes spatial distribution is small.

Unveiling and Imaging Degenerate States in Plasmonic Nanoparticles with Nanometer Resolution.

Metal nanoparticles host localized plasmon excitations that allow the manipulation of optical fields at the nanoscale. Despite the availability of several techniques for imaging plasmons, direct access into the symmetries of these excitations remains elusive, thus hindering progress in the development of applications. Here, we present a combination of angle-, polarization-, and space-resolved cathodoluminescence spectroscopy methods to selectively access the symmetry and degeneracy of plasmonic states in lithographically fabricated gold nanoprisms. We experimentally reveal and spatially map degenerate states of multipole plasmon modes with nanometer spatial resolution and further provide recipes for resolving optically dark and out-of-plane modes. Full-wave simulations in conjunction with a simple tight-binding model explain the complex plasmon structure in these particles and reveal intriguing mode-symmetry phenomena. Our approach introduces systematics for a comprehensive symmetry characterization of plasmonic states in high-symmetry nanostructures.

Finite-element method for calculation of the effective permittivity of random inhomogeneous media.

The challenge of designing new solid-state materials from calculations performed with the help of computers applied to models of spatial randomness has attracted an increasing amount of interest in recent years. In particular, dispersions of particles in a host matrix are scientifically and technologically important for a variety of reasons. Herein, we report our development of an efficient computer code to calculate the effective (bulk) permittivity of two-phase disordered composite media consisting of hard circular disks made of a lossless dielectric (permittivity epsilon2) randomly placed in a plane made of a lossless homogeneous dielectric (permittivity epsilon1) at different surface fractions. Specifically, the method is based on (i) a finite-element description of composites in which both the host and the randomly distributed inclusions are isotropic phases, and (ii) an ordinary Monte Carlo sampling. Periodic boundary conditions are employed throughout the simulation and various numbers of disks have been considered in the calculations. From this systematic study, we show how the number of Monte Carlo steps needed to achieve equilibrated distributions of disks increases monotonically with the surface fraction. Furthermore, a detailed study is made of the dependence of the results on a minimum separation distance between disks. Numerical examples are presented to connect the macroscopic property such as the effective permittivity to microstructural characteristics such as the mean coordination number and radial distribution function. In addition, several approximate effective medium theories, exact bounds, exact results for two-dimensional regular arrays, and the exact dilute limit are used to test and validate the finite-element algorithm. Numerical results indicate that the fourth-order bounds provide an excellent estimate of the effective permittivity for a wide range of surface fractions, in accordance with the fact that the bounds become progressively narrower as more microstructural information is incorporated. Future directions of the active field of computational studies of the structure-property relations for composite systems are briefly discussed.

Probing bright and dark surface-plasmon modes in individual and coupled noble metal nanoparticles using an electron beam.

The rich structure of bright and dark surface-plasmon modes localized in individual and coupled gold nanoparticles is unveiled by electron-energy-loss spectroscopy performed in a scanning transmission electron microscope. Spatially resolved maps of surface-plasmon modes in the approximately 1.5-2.5 eV range (wavelengths approximately 500-800 nm), collected for individual nanorods, coupled nanorod dimers, and touching nanosphere dimers, are in excellent agreement with theory. Surface-plasmon maps constructed from the spatially and spectrally resolved energy-loss signals are shown to mimic rather well the near fields calculated for external illumination in the case of bright surface-plasmon modes (i.e., those coupling to external light). Dark surface-plasmon modes that cannot be excited by optical means are also found, and our electron probing technique provides further insight into their corresponding spatial distribution and symmetry, which are not accessible to any other existing techniques. Our results initiate the study of a whole set of new dark surface-plasmon modes that should become a source of new applications in sensing and microscopy but have escaped experimental scrutiny so far.

Modelling the optical response of gold nanoparticles.

This tutorial review presents an overview of theoretical methods for predicting and understanding the optical response of gold nanoparticles. A critical comparison is provided, assisting the reader in making a rational choice for each particular problem, while analytical models provide insights into the effects of retardation in large particles and non-locality in small particles. Far- and near-field spectra are discussed, and the relevance of the latter in surface-enhanced Raman spectroscopy and electron energy-loss spectroscopy is emphasized.