Plasmonic dimer nanoantennas are characterized by a strong enhancement of the optical field, leading to large nonlinear effects. The third harmonic emission spectrum thus depends strongly on the ...antenna shape and size as well as on its gap size. Despite the complex shape of the nanostructure, we find that for a large range of different geometries the nonlinear spectral properties are fully determined by the linear response of the antenna. We find excellent agreement between the measured spectra and predictions from a simple nonlinear oscillator model. We extract the oscillator parameters from the linear spectrum and use the amplitude of the nonlinear perturbation only as scaling parameter of the third harmonic spectra. Deviations from the model only occur for gap sizes below 20 nm, indicating that only for these small distances the antenna hot spot contributes noticeable to the third harmonic generation. Because of its simplicity and intuitiveness, our model allows for the rational design of efficient plasmonic nonlinear light sources and is thus crucial for the design of future plasmonic devices that give substantial enhancement of nonlinear processes such as higher harmonics generation as well as difference frequency mixing for plasmonically enhanced terahertz generation.
We present a comprehensive overview of chirality and its optical manifestation in plasmonic nanosystems and nanostructures. We discuss top-down fabricated structures that range from solid metallic ...nanostructures to groupings of metallic nanoparticles arranged in three dimensions. We also present the large variety of bottom-up synthesized structures. Using DNA, peptides, or other scaffolds, complex nanoparticle arrangements of up to hundreds of individual nanoparticles have been realized. Beyond this static picture, we also give an overview of recent demonstrations of active chiral plasmonic systems, where the chiral optical response can be controlled by an external stimulus. We discuss the prospect of using the unique properties of complex chiral plasmonic systems for enantiomeric sensing schemes.
Electromagnetic fields with strong optical chirality can be formed in the near field of chiral plasmonic nanostructures. We calculate and visualize the degree of chirality to identify regions with ...relatively high values. This analysis leads to design principles for a simple utilization of chiral fields. We investigate planar geometries, which offer a convenient way to access the designated fields, as well as three-dimensional nanostructures, which show a very high local optical chirality.
Electrically switchable metallic polymer nanoantennas Karst, Julian; Floess, Moritz; Ubl, Monika ...
Science (American Association for the Advancement of Science),
2021-Oct-29, 2021-10-29, 20211029, Letnik:
374, Številka:
6567
Journal Article
Recenzirano
Electrical switching of a metal-to-insulator transition would provide a building block for integrated electro-optically active plasmonics. In this work, we realize plasmonic nanoantennas from ...metallic polymers, which show well-pronounced localized plasmon resonances in their metallic state. As a result of the electrochemically driven optical metal-to-insulator transition of the polymer, the plasmonic resonances can be electrically switched fully off and back on at video-rate frequencies of up to 30 hertz by applying alternating voltages of only ±1 volt. With the use of this concept, we demonstrate electrically switchable beam-steering metasurfaces with a 100% contrast ratio in transmission. Our approach will help to realize ultrahigh efficiency plasmonic-based integrated active optical devices, including high-resolution augmented and virtual reality technologies.
We present a comprehensive experimental study of the optical properties of plasmonic oligomers. We show that both the constitution and configuration of plasmonic oligomers have a large influence on ...their resonant behavior, which draws a compelling analogy to molecular theory in chemistry. To elucidate the constitution influence, we vary the size of individual nanoparticles and identify the role of the target nanoparticle from the spectral change. To illustrate the configuration influence, we vary the positions and numbers of nanoparticles in a plasmonic oligomer. Additionally, we demonstrate experimentally a large spectral redshift at the transition from displaced nanoparticles to touching ones. The oligomeric design strategy opens up a rich pathway for the implementation of optimized optical properties into complex plasmonic nanostructures for specific applications.
We study the coupling between the plasmonic resonances of solid and inverse metallic nanostructures. While the coupling between solid-solid and inverse-inverse plasmonic structures is ...well-understood, mixed solid-inverse systems have not yet been studied in detail. In particular, it remains unclear whether or not an efficient coupling is even possible and which prerequisites have to be met. We find that an efficient coupling between inverse and solid resonances is indeed possible, identify the necessary geometrical prerequisites, and demonstrate a novel solid-inverse plasmonic electromagnetically induced transparency (EIT) structure as well as a mixed chiral system. We furthermore show that for the coupling of asymmetric rod-shaped inverse and solid structures symmetry breaking is crucial. In contrast, highly symmetric structures such as nanodisks and nanoholes are straightforward to couple. Our results constitute a significant extension of the plasmonic coupling toolkit, and we thus envision the emergence of a large number of intriguing novel plasmonic coupling phenomena in mixed solid-inverse structures.
Plasmonic oligomer clusters are assemblies of closely packed metallic nanoparticles. They provide a rich set of spectral features such as Fano lineshapes and a simultaneous tunability of the ...supported resonances in the optical wavelength regime. In this study, we investigate numerically and experimentally clusters of plasmonic nanoparticles that exhibit multiple Fano resonances due to the interference of one broad superradiant mode and multiple narrow subradiant modes. In particular we investigate oligomers with multiple ring modes and elongated chains of nanoparticles surrounded by one ring of nanoparticles. We show that the number of nanoparticles and their respective arrangement in the cluster strongly influence the spectral position and modulation depth of the spectral signature of the supported modes. Our study opens up the pathway to “plasmonic super molecules” that show unprecedented tunability, which renders them highly suitable for applications such as multiwavelength surface-enhanced Raman scattering.
We perform second harmonic spectroscopy of aluminum nanoantenna arrays that exhibit plasmonic resonances at the second harmonic wavelength between 450 and 570 nm by focusing sub-30 fs laser pulses ...tunable from 900 to 1140 nm onto the nanoantenna arrays. We find that a plasmonic resonance at the second harmonic wavelength boosts the overall nonlinear process by more than an order of magnitude. In particular, in the measurement the resonant second harmonic polarization component is a factor of about 70 stronger when compared to the perpendicular off-resonant second harmonic polarization. Furthermore, the maximum of the second harmonic conversion efficiency is found to be slightly blue-shifted with respect to the peak of the linear optical far-field spectrum. This fact can be understood from a simple model that accounts for the almost off-resonant absorption at the fundamental wavelength and the resonant emission process at the second harmonic.
The ability to manipulate the phase shift between two resonantly coupled plasmonic oscillators in a controlled fashion has been unavailable up to now. Here we present a strategy to overcome this ...limitation by employing the benefits of near-field coupling on the one hand and retardation effects due to far-field coupling on the other hand. We theoretically and experimentally demonstrate that in the intermediate regime the coupling of a broad dipolar to a narrow dark quadrupolar plasmon resonance is possible while simultaneously allowing for a retardation-induced phase shift. This leads to constructive interference and enhanced absorption. The observed phenomenon can thus be termed a classical analog of electromagnetically induced absorption.
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