Full-wave electromagnetic modes and hybridization in nanoparticle dimers.

The plasmon hybridization theory is based on a quasi-electrostatic approximation of the Maxwell's equations. It does not take into account magnetic interactions, retardation effects, and radiation losses. Magnetic interactions play a dominant role in the scattering from dielectric nanoparticles. The retardation effects play a fundamental role in the coupling of the modes with the incident radiation and in determining their radiative strength; their exclusion may lead to erroneous predictions of the excited modes and of the scattered power spectra. Radiation losses may lead to a significant broadening of the scattering resonances. We propose a hybridization theory for non-Hermitian composite systems based on the full-Maxwell equations that, overcoming all the limitations of the plasmon hybridization theory, unlocks the description of dielectric dimers. As an example, we decompose the scattered field from silicon and silver dimers, under different excitation conditions and gap-sizes, in terms of dimer modes, pinpointing the hybridizing isolated-sphere modes behind them.

Directional scattering cancellation for an electrically large dielectric sphere.

We demonstrate the directional scattering cancellation for a dielectric sphere of radius up to 10 times the incident wavelength, by coating it with a surface of finite conductivity. Specifically, the problem of determining the values of surface conductivity that guarantee destructive interference among hundreds of multipolar scattering orders at the prescribed angular direction is reduced to the determination of the zeros of a polynomial, whose coefficients are analytically known.

Surface integral formulations for the design of plasmonic nanostructures.

Numerical formulations based on surface integral equations (SIEs) provide an accurate and efficient framework for the solution of the electromagnetic scattering problem by three-dimensional plasmonic nanostructures in the frequency domain. In this paper, we present a unified description of SIE formulations with both singular and nonsingular kernel and we study their accuracy in solving the scattering problem by metallic nanoparticles with spherical and nonspherical shape. In fact, the accuracy of the numerical solution, especially in the near zone, is of great importance in the analysis and design of plasmonic nanostructures, whose operation critically depends on the manipulation of electromagnetic hot spots. Four formulation types are considered: the N-combined region integral equations, the T-combined region integral equations, the combined field integral equations and the null field integral equations. A detailed comparison between their numerical solutions obtained for several nanoparticle shapes is performed by examining convergence rate and accuracy in both the far and near zone of the scatterer as a function of the number of degrees of freedom. A rigorous analysis of SIE formulations and their limitations can have a high impact on the engineering of numerous nano-scale optical devices such as plasmon-enhanced light emitters, biosensors, photodetectors, and nanoantennas.

Multipolar second harmonic generation from planar arrays of Au nanoparticles.

We demonstrate optical Second Harmonic Generation (SHG) in planar arrays of cylindrical Au nanoparticles arranged in periodic and deterministic aperiodic geometries. In order to understand the respective roles of near-field plasmonic coupling and long-range photonic interactions on the SHG signal, we systematically vary the interparticle separation from 60 nm to distances comparable to the incident pump wavelength. Using polarization-resolved measurements under femtosecond pumping, we demonstrate multipolar SHG signal largely tunable by the array geometry. Moreover, we show that the SHG signal intensity is maximized by arranging Au nanoparticles in aperiodic spiral arrays. The possibility to engineer multipolar SHG in planar arrays of metallic nanoparticles paves the way to the development of novel optical elements for nanophotonics, such as nonlinear optical sensors, compact frequency converters, optical mixers, and broadband harmonic generators on a chip.

Genetically engineered plasmonic nanoarrays.

In the present Letter, we demonstrate how the design of metallic nanoparticle arrays with large electric field enhancement can be performed using the basic paradigm of engineering, namely the optimization of a well-defined objective function. Such optimization is carried out by coupling a genetic algorithm with the analytical multiparticle Mie theory. General design criteria for best enhancement of electric fields are obtained, unveiling the fundamental interplay between the near-field plasmonic and radiative photonic coupling. Our optimization approach is experimentally validated by surface-enhanced Raman scattering measurements, which demonstrate how genetically optimized arrays, fabricated using electron beam lithography, lead to order of ten improvement of Raman enhancement over nanoparticle dimer antennas, and order of one hundred improvement over optimal nanoparticle gratings. A rigorous design of nanoparticle arrays with optimal field enhancement is essential to the engineering of numerous nanoscale optical devices such as plasmon-enhanced biosensors, photodetectors, light sources and more efficient nonlinear optical elements for on chip integration.

Particle-swarm optimization of broadband nanoplasmonic arrays.

We used the particle swarm optimization algorithm, an evolutionary computational technique, to design metal nanoparticle arrays that produce broadband plasmonic field enhancement over the entire visible spectral range. The resulting structures turn out to be aperiodic and feature dense Fourier spectra with many closely packed particle clusters. We conclude that broadband field-enhancement effects in nanoplasmonics can be achieved by engineering aperiodic arrays with a large number of spatial frequencies that provide the necessary interplay between long-range diffractive interactions at multiple length scales and near-field quasi-static coupling within small nanoparticle clusters.

The role of nanoparticle shapes and deterministic aperiodicity for the design of nanoplasmonic arrays.

In this paper, we study the role of nanoparticle shape and aperiodic arrangement in the scattering and spatial localization properties of plasmonic modes in deterministic-aperiodic (DA) arrays of metal nanoparticles. By using an efficient coupled-dipole model for the study of the electromagnetic response of large arrays excited by an external field, we demonstrate that DA structures provide enhanced spatial localization of plasmonic modes and a higher density of enhanced field states with respect to their periodic counterparts. Finally, we introduce and discuss specific design rules for the engineering and optimization of field enhancement and localization in DA arrays. Our results, which we fully validated by rigorous Generalized Mie Theory (GMT) and transition matrix (T-matrix) theory, demonstrate that DA arrays provide a robust platform for the design of a variety of novel optical devices with enhanced and controllable plasmonic fields.

Nanoplasmonics of prime number arrays.

In this paper, we investigate the plasmonic near-field localization and the far-field scattering properties of non-periodic arrays of Ag nanoparticles generated by prime number sequences in two spatial dimensions. In particular, we demonstrate that the engineering of plasmonic arrays with large spectral flatness and particle density is necessary to achieve a high density of electromagnetic hot spots over a broader frequency range and a larger area compared to strongly coupled periodic and quasi-periodic structures. Finally, we study the far-field scattering properties of prime number arrays illuminated by plane waves and we discuss their angular scattering properties. The study of prime number arrays of metal nanoparticles provides a novel strategy to achieve broadband enhancement and localization of plasmonic fields for the engineering of nanoscale nano-antenna arrays and active plasmonic structures.