The term “metamaterials” refers to engineered structures that interact with electromagnetic fields in an unusual but controllable way that cannot be observed with natural materials. Metamaterial design at optical frequencies oftentimes makes of controllable plasmonic interactions. Light can excite collective oscillations of conduction band electrons on a metallic nanostructure. These oscillations result in localized surface plasmon modes which can provide high confinement of fields at metal-dielectric interfaces at nanoscale. Additionally scattering and absorption characteristics of plasmon modes can be controlled by geometrical features of the metallic nanostructures. This ease of controllability has lead to the development of new concepts in light manipulation and enhancement of light-material interactions. Fano resonance and plasmonic induced transparency (PIT) are among the most promising of those. The interference between different plasmon modes induced on nanostructures generates PIT/Fano resonance at optical frequencies. The unusual dispersion characteristics observed within the PIT window can be used for designing optical metamaterials to be used in various applications including bio-chemical sensing, slow light, modulation, perfect absorption, and all-optical switching. This thesis focuses on design of novel plasmonic devices to be used in these applications. The fundamental idea behind these designs is the generation of higher-order plasmon modes, which leads to PIT/Fano resonance-like output characteristics. These are then exploited together with dynamic tunability supported by graphene and field enhancement provided by nonlinear materials to prototype novel plasmonic devices. More specifically, this thesis proposes the following plasmonic device designs. I. Nano-disk Fano resonator: Open disk-like plasmonic nanostructures are preferred for bio-chemical sensing because of their higher capacity to be in contact with greater volumes of analyte. High effective refractive index required by sensing applications is achieved though the dispersion characteristics within PIT window. Higher order modes required for Fano resonance are generated through geometrical symmetry breaking by embedding a shifted and elongated cavity into a circular disk. The resulting dual band PIT can be geometrically tuned by varying the cavity's width and rotation angle. II. Tunable Terahertz Fano resonator: The possibility to dynamically tune graphene's conductivity has made it an attractive choice over conventional noble metals to generate surface plasmon modes at Terahertz frequencies. Subsequently, a polarization-independent and dynamically tunable hybrid gold-graphene structure is designed to achieve PIT/Fano resonance by allowing graphene and metallic plasmon modes to interfere. The effective group index of the resulting resonator is found to be very high (ng=1400, several times higher than all previously reported PIT devices) within the PIT window. Dynamic tunability achieved through a gate voltage applied to graphene suggests applications in switching. III. Tunable Terahertz Fano absorber: Many photonic and optical devices rely on their ability to efficiently absorb an incoming electromagnetic field. The absorption in atomically thin graphene sheet is already very high i.e., “2.3%” per layer. However, considering its atomic thickness graphene sheet remains practically transparent to Terahertz waves. The proposed absorber design makes of an asymmetrically patterned graphene layer that supports higher order plasmon modes at Terahertz frequencies. Several of these patterned layers backed by dielectric substrates are stacked on top of each other followed by reflector screen. The dynamically controllable resonances from each graphene layer and the spacing between them are fine tuned to achieve a large bandwidth of 6.9 Terahertz (from 4.7 to 11.6 Terahertz) for over 90% absorption, which is significantly higher than that of existing metallic/graphene absorbers. IV. Three state all-optical switch: The plasmonic resonances are extremely sensitive to dielectric properties of the surrounding medium. A slight change in the dielectric constant near the metal surface results in a significant change in the plasmonic resonance. This sensitivity is enhanced in the presence of a nonlinear change in the dielectric constant. To make use of this effect, Fano resonator is used in conjunction with a Kerr nonlinear material. The resulting resonator exploits multiple (higher order) surface plasmons to generate a multi-band tri-stable response in its output. This cannot be obtained using existing nonlinear plasmonic devices that make use of single mode Lorentzian resonances. Multi-band three-state optical switching that can be realized using the proposed resonator has potential applications in optical communications and computing.

Manipulating electromagnetic fields with plasmonic nanostructures has attracted researchers from interdisciplinary areas and opened up a wide variety of applications. Despite the intriguing aspect of inducing unusual optical properties such as negative indices and indefinite permittivity and permeability, engineered plasmonic nanostructures are also capable of concentrating electromagnetic waves into a diffraction-unlimited volume, thus induce incredible light-matter interaction. In this dissertation, I’ll discuss about a class of plasmonic structures that exhibit the Fano resonance. The Fano resonance is in principle the interference between two resonant modes of distinct lifetimes. Through the Fano resonance, the electromagnetic energy can be trapped in the so called “dark” mode and induce strong local field enhancement. A variety of Fano resonant nanostructures ranging from periodic planar arrays to simple clusters composed of only two particles are demonstrated in this dissertation. By artificially designing the dimensions of the structures, these Fano-resonant materials can be operated over a broad frequency range (from visible to mid-IR) to target the specific applications of interest. In this dissertation, I’ll show the following research results obtained during my PhD study: (1) the double-continuum Fano resonant materials that can slow down the speed of light over a broad frequency range with little group velocity dispersion. (2) Ultra-sensitive detection and characterization of proteins using the strong light-matter interaction provided by the Fano-reonant asymmetric metamaterials. (3) Metamaterials absorbers with nearly 100 % absorbance, tunable spectral position, expandable bandwidth, and wide angle absorption. These Fano-resonant materials can have profound influences in the areas of optical signal processing, life science, bio-defense, energy harvesting and so on. / text

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Graphene, a one-atom-thick sheet of hexagonally packed carbon atoms, is a novel material with high electron mobility due to its unique linear and gapless electronic band structure. Its broadband absorption and unusual doping properties, along with superb mechanical flexibility make graphene of promising application in optoeletronic devices such as solar cell, ultrafast photodetectors, and terahertz modulators. How- ever, the current performance of graphene-based devices is quite unacceptable owning to serious limitations by its inherently small absorption cross section and low quan- tum efficiency. Fortunately, nanoscale optical antennas, consisting of closely spaced, coupled metallic nanoparticles, have fascinating optical response since the collective oscillation of electrons in them, namely surface plasmons, can concentrate light into a subwavelength regime close to the antennas and enhance the corresponding field considerably. Given that optical antenna have been applied in various areas such as subwavelength optics, surface enhanced spectroscopies, and sensing, they are also able to assist graphene to harvest visible and near-infrared light with high efficiency. Moreover, the efficient production of hot electrons due to the decay of the surface plasmons can be further implemented to modulate the properties of graphene. Here we choose plasmonic oligomers to serve as optical antenna since they pos- sess tunable Fano resonances, consisting of a transparency window where scattering is strongly suppressed but absorption is greatly enhanced. By placing them in di- rect contact with graphene sheet, we find the internal quantum efficiency of hybrid antenna-graphene devices achieves up to 20%. Meanwhile, doping effect due to hot electron is also observed in this device, which can be used to optically tune the elec- tronic properties of graphene.

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Strongly coupled plasmon-exciton hybrid nanostructures are fabricated and their optical properties are studied. The plasmonic and excitonic systems are gold nanoshells and J-aggregates, respectively. Gold nanoshells are tunable plasmonic core-shell nanoparticles which can sustain distinct dipole and quadrupole plasmons with resonant energies dependent on core-size/shell-thickness ratio. J-aggregates are organic semiconducting material with excitons that possess very high oscillator strength making them suitable for coherent interaction with other kinds of excitations. The J-aggregates are formed on the surface of the nanoshells when a water/ethanol (50:50) solution of the dye molecules (2,2'-dimethyl-8-phenyl-5,6,5',6'-dibenzothiacarbocyanine chloride) is added to an aqueous solution of nanoshells. These nanoshell-J-aggregate complexes exhibit coherent coupling between localized plasmons of the nanoshell and excitons of the molecular J-aggregates. Coherent coupling strengths of 120 meV and 100 meV have been measured for dipole and quadrupole plasmon interactions with excitons, respectively. Femtosecond time-resolved transmission spectroscopy studies are carried out in order to understand the possible sources of optical nonlinearities in the nanoshell-J-aggregate hybrid. Transient absorption of the interacting plasmon-exciton system is observed, in dramatic contrast to the photoinduced transmission of the pristine J-aggregate. An additional, transient Fano-shaped modulation within the Fano dip is also observable. The transient behavior of the J-aggregate-Au nanoshell complex is described by a combined one-exciton and two-exciton state model coupled to the nanoshell plasmon.

Different types of plasmonic nanostructures are proposed and examined experimentally and theoretically, with a view towards sensing applications. First, a self-assembly approach was developed to create arrays of well-ordered glass-supported gold nanoparticles (AuNPs) with controllable particle size and inter-particle spacing. Then, a periodic array of gold nano-disks (AuNDs) supported by a Bragg reflector was proposed and examined in a search for Fano resonances in its optical response. Arrays of heptamer-arranged nanoholes (HNH) in a thin gold film were also proposed and explored theoretically and experimentally, revealing a very rich spectrum of resonances, several exhibiting a Fano lineshape. A commercial implementation of the vectorial finite element method (FEM) was used to model our plasmonic structures. Taking advantage of the periodic nature of the structures, a unit cell containing a single element was modelled. The transmittance, reflectance or absorbance spectra were computed, and the associated electromagnetic fields were obtained by solving the vector wave equations for the electromagnetic field vectors throughout the structures, subject to the applicable boundary conditions, and the applied source fields. The sensing performance of the structures, based on the bulk sensitivity, surface sensitivity and figure of merit (FOM) was calculated. First, a novel bottom-up fabrication approach was applied (by our collaborators) to form a periodic array of AuNPs with controllable size over large areas on SiO2 substrates. In this method, self-assembly of block copolymer micelles loaded with metal precursors was combined with a seeding growth route to create ordered AuNPs of desired size. It was shown that this new fabrication method offers a new approach to tune the AuNP size and edge-to-edge inter-particle spacing while preserving the AuNP ordering. The optical characteristics of the AuNP arrays, such as their size, interparticle spacing, localized surface plasmon resonance (LSPR) wavelength, and bulk sensitivity, were examined, numerically and experimentally. This proposed novel fabrication method is applicable for low-cost mass-production of large-area arrays of high-quality AuNPs on a substrate for sensing applications. Then, we proposed and examined the formation of Fano resonances in a plasmonic-dielectric system consisting of uncoupled gold nano-disk (AuND) arrays on a quarter-wave dielectric stack. The mechanism behind the creation of Fano resonances was explained based on the coherent interference between the reflection of the Bragg stack and the LSPPs of the AuNDs. Fano parameters were obtained by fitting the computational data to the Fano formula. The bulk sensitivities and figure of merit of the Fano resonances were calculated. This plasmonic structure supports Fano resonances with a linewidth around 9 nm which is much narrower than the individual AuND LSPP bandwidth ( 80 nm) and the Bragg stack bandwidth ( 100 nm). Supporting Fano resonances with such a narrow linewidth, the structure has a great potential to be used for sensing applications. Also, this metallic-dielectric nanostructure requires no near-field coupling between AuNDs to generate the Fano resonances. So, the AuNDs can be located far enough from each other to simplify the potential fabrication process. The optical properties of HNH arrays on an SiO2 substrate were investigated, numerically and experimentally. Helium focused ion beam (HeFIB) milling was applied (by Dr. Choloong Hahn) to fabricate well-ordered and well-defined arrays of HNHs. Transmittance spectra of the structures were obtained as the optical response, which exhibits several Fano resonances. Then, the mechanism behind the formation of the Fano resonances was explained, and the sensing performance of the structure was inspected by measuring the bulk sensitivities. This array of nanohole cluster is exciting because it supports propagating SPPs and LSPPs, and also Wood’s anomaly waves, which makes the optical response very rich in excitations and spectral features. Also, as a periodic array of sub-wavelength metallic nanoholes, the system produces extraordinary optical transmission - highly enhanced transmission through (otherwise) opaque metallic films at specific wavelengths, facilitating measurement acquisition in transmission.

Les méta-surfaces permettent de contrôler efficacement es rayonnements électromagnétiques en manipulant la phase, l'amplitude et la polarisation des ondes. Pour de nombreuses applications, telles que des fonctions d’agilité, de commutations et de détection, des surfaces de haute performance sont nécessaires. L’objectif de cette thèse est d'explorer des méthodes innovantes permettant d'améliorer les facteurs de qualité des méta-surfaces dans les domaines micro-ondes et optique. La limitation des méta-surfaces est généralement liée aux pertes par rayonnement et à l'absorption non radiative. L'étude se concentre sur des solutions permettant la suppression des pertes de rayonnement en utilisant des concepts de mode sombre et de résonance de Fano. Un mécanisme d'excitation direct de mode sombre dans un résonateur individuel basé sur l’adaptation de symétrie est proposé. La possibilité d'améliorer l'efficacité de la réponse magnétique en optique est présentée. L'analyse de l'excitation par résonance de Fano dans un système de résonateurs couplés identiques est également réalisée sur la base du formalisme de la théorie des modes couplés. Deux configurations générales correspondant à l'arrangement spatial symétrique et énantiomères des résonateurs sont considérées. Dans le premier cas, le système de cavité formé par les méta-surfaces très proches fournit des caractéristiques spectrales très étroites et une sensibilité efficace élevée par rapport aux cavités Fabry-Perot conventionnelles. Dans le second cas, les caractéristiques de conception permettent de contrôler la suppression des pertes de rayonnement, permettant d'augmenter considérablement le facteur de qualité de la résonance de Fano. / Metasurfaces allows an effective control of electromagnetic radiation by manipulating phase, amplitude and polarization of electromagnetic waves. For numerous applications including tunable, switchable and sensing functionalities, high performance metasurfaces are required. The goal of this thesis is to explore innovative methods enabling to improve the quality factors of metasurfaces in microwave and optical domains. The limitation of metasurfaces is generally related to radiation losses and non-radiative absorption. The study is focused on solutions allowing the suppression of radiative losses by using concepts of dark mode and Fano resonance. A direct dark mode excitation mechanism in individual resonator based on symmetry matching is proposed. The possibility to enhance magnetic response efficiency in optical frequency range is presented. Analysis of Fano resonance excitation in a system of identical coupled resonators is also performed on the basis of coupled mode theory formalism. Two general configurations are considered corresponding to symmetric and enantiomeric space arrangement of resonators. In the first case, cavity system formed by near-field coupled metasurfaces provides sharp spectral characteristics and high efficient sensitivity compared to conventional Fabry-Perot cavities. In the second case the design features enables to control suppression of radiation losses, allowing to considerably increase Fano resonance quality factor.

Dans ce travail, les propriétés des réseaux diffractifs ordonnés de nanoparticules d'or sont étudiées numériquement et expérimentalement. Ces résonances sont beaucoup plus étroites que celles observées dans le cas d'une nanoparticule isolée. D'après les simulations numériques, deux régimes distincts de réponse sont identifiés, l'un correspond à l'anomalie de Rayleigh (RA) l'autre au mode plasmon de réseau 2D (LPM). Dans la partie expérimentale nous avons fabriqué des réseaux de nanoparticules d'or en utilisant la lithographie d'électronique. La transmission spectrale a été mesurée dans le domaine optique pour caractériser ces réseaux. Toutes les caractéristiques essentielles des spectres expérimentaux sont en bon accord avec les simulations numériques. Les distributions du champ électrique pour différents paramètres de réseau sont étudiées pour obtenir le maximum d'augmentation du champ à la surface de la nanoparticule. L'excitation des résonances plasmon dans les réseaux diffractifs de nanoparticules d'or en condition asymétrique de l'indice de réfraction est examinée expérimentalement. L'excitation des modes plasmon à profil spectral étroit dans l'environnement asymétrique a été expérimentalement vérifiée. La possibilité d'accorder la longueur d'onde de ces résonances dans le proche infrarouge en changeant les paramètres structurels des réseaux périodiques en combinant taille et forme des nanoparticules est discutée. Ces résultats sont importants pour les applications telles que les spectroscopies en champ électrique exalté et la détection en biologie ou en chimie. / The properties of ordered diffractive arrays of gold nanoparticles are studied numerically and experimentally. Using numerical simulations I identify, two distinct regimes of lattice response, associated with two-characteristic states of the spectra: Rayleigh anomaly and lattice plasmon mode. In experimental part gold nanoparticle arrays were fabricated using e-beam lithography. Spectroscopic transmission measurements then were carried out to optically characterize these arrays. All the essential features of the experimental spectra were reproduced well by numerical simulations. Electric field distributions for different lattice parameters are studied in order to maximize the enhancement of electric field at the nanoparticle surface. The excitation of plasmon resonances in diffractive arrays of gold nanoparticles placed in asymmetric refractive index environment is examined experimentally. The excitation of the plasmon modes with narrow spectral profile in asymmetric environment was experimentally verified. The ability to tune the wavelength of these resonances in the near infrared range by varying the structural parameters of the periodic arrays in combination with size and geometry of the constituent nanoparticles is discussed. The presented results are of importance for the field enhanced spectroscopy as well as for plasmonic bio and chemical sensing.

Neste trabalho, estudamos a influência de canais de espalhamento inelástico no transporte eletrônico. Primeiramente, expomos o formalismo de Landauer usual para o cálculo da corrente elétrica em sistemas em que o espalhamento é puramente elástico. Como exemplo, calculamos a corrente para um potencial delta de Dirac a partir de suas probabilidades de transmissão. A amostra correspondente é aquela de uma camada muito fina com impurezas (não-magnéticas) contida em uma heterostrutura semicondutora. Mostramos que a distorção do potencial quântico devido à voltagem aplicada pode ser desprezada no cálculo da corrente elétrica, abaixo da energia de Fermi do emissor. Subsequentemente, acoplamos o potencial delta a um oscilador harmônico quântico para modelar a presença de fônons no sistema. Encontramos modos inelásticos de transmissão que se tornam acessíveis para energias cada vez maiores, múltiplas do quantum hω. Devido à conservação de probabilidade, a abertura de cada novo canal corresponde a bicos\" nas probabilidades de transmissão dos modos abaixo deste, em função da energia de incidência do elétron. No caso de uma delta atrativa, ressonâncias assimétricas com perfil de Fano são observadas. Adaptamos o formalismo de Landauer, incluindo canais inelásticos independentes. Seguindo um trabalho anterior de Emberly e Kirczenow (2000), mostramos que existe uma forma de se levar em conta possíveis coincidências nos estados de espalhamento finais aplicando o princípio de exclusão de Pauli. Isto leva as distribuições dos estados de espalhamento a estarem fora de equilíbrio, já que dependem umas das outras. Resolvendo o problema auto-consistentemente, somos capazes de obter a corrente elétrica a partir das probabilidades de transmissão do potencial quântico. Nossos resultados demonstram que as ressonâncias de Fano do potencial atrativo dão origem a uma diminuição da inclinação da corrente elétrica contra a voltagem aplicada, já que elétrons são presos\" ao potencial por um tempo infinito. Mostramos este efeito num regime de voltagens baixas em comparação com a energia de Fermi, para o qual desprezamos a distorção do potencial quântico devido à voltagem aplicada. Além disso, uma comparação com os resultados do formalismo de Landauer mostra que uma discrepância significativa é observada para o caso de o oscilador estar inicialmente excitado e fortemente acoplado ao elétron. / In this work, we study the influence of inelastic scattering channels in electronic transport. We first present the usual Landauer formalism, for calculating the electric current in systems where the scattering is purely elastic. As an example, we calculate the current for a Dirac delta potential from its transmission probabilities. The corresponding sample is that of a very thin layer with (non-magnetic) impurities within a semiconductor heterostructure. We show that the distortion of the quantum potential due to the applied voltage can be ignored in the calculation of an electric current below the Fermi energy of the emitter. Then we couple the delta potential to a quantum harmonic oscillator to model the presence of phonons in the system. We find inelastic transmission modes that become available for increasing energies, multiple of the quantum hω. Due to conservation of probability, the opening of each new channel corresponds to kinks\" in the transmission probabilities of lower modes as a function of the energy of the impinging electrons. In the case of an attractive delta potential, asymmetric resonances with a Fano-like profile are observed. We adapt the Landauer formalism by including the independent inelastic channels. Following a previous work by Emberly and Kirczenow (2000), we show that there is a way to take into account the possible coincidences in the final scattering states using Pauli\'s exclusion principle. This causes the distributions of the scattering states to be out of equilibrium, as they depend on each other. Solving the problem self-consistently, we are able to obtain the electric current from the transmission probabilities of the quantum potential. Our results demonstrate that the Fano resonances of the attractive potential gives rise to a decrease of the slope in the electric current versus the applied voltage, as the electrons are trapped\" in the potential for a finite amount of time. We have shown this effect in a low voltage regime with respect to the Fermi energy, for which we ignore the distortion of the quantum potential due to the applied voltage. Furthermore, a comparison with the results from the Landauer formalism shows that a significant discrepancy is seen for the oscillator initially in its excited mode and strongly coupled to the electron.