Group- III nitride based semiconductors have emerged as the leading material for short wavelength optoelectronic devices. The InGaN alloy system forms a continuous and direct bandgap semiconductor spanning ultraviolet (UV) to blue/green wavelengths. An ideal and highly efficient light-emitting device can be designed by enhancing the spontaneous emission rate. This thesis deals with the design and fabrication of a visible light-emitting device using GaN/InGaN single quantum well (SQW) system with enhanced spontaneous emission. To increase the emission efficiency, layers of different metals, usually noble metals like silver, gold and aluminum are deposited on GaN/InGaN SQWs using metal evaporator. Surface characterization of metal-coated GaN/InGaN SQW samples was carried out using atomic force microscopy (AFM) and scanning electron microscopy (SEM). Photoluminescence is used as a tool for optical characterization to study the enhancement in the light emitting structures. This thesis also compares characteristics of different metals on GaN/InGaN SQW system thus allowing selection of the most appropriate material for a particular application. It was found out that photons from the light emitter couple more to the surface plasmons if the bandgap of former is close to the surface plasmon resonant energy of particular metal. Absorption of light due to gold reduces the effective mean path of light emitted from the light emitter and hence quenches the quantum well emission peak compared to the uncoated sample.

Upconverted light from nanostructured metal surfaces can be produced by harmonic generation and multi-photon luminescence; however, these are weak processes and require extremely high field intensities to produce a measurable signal. Here we report on bright emission, five orders of magnitude greater than harmonic generation, that can be seen from metal tunnel junctions due to light-induced inelastic tunneling. Like inelastic tunneling light emission, which was recently reported to have 2% conversion efficiency per tunneling event, the emission wavelength recorded varies with the local electric field applied; however, here the field is from a 1560 nm femtosecond pulsed laser source. Finite-difference time-domain simulations of the experimental conditions show the local field is sufficient to generate tunneling-based inelastic light emission in the visible regime. This phenomenon is promising for producing ultrafast upconverted light emission with higher efficiency than conventional nonlinear processes. / Graduate

Le but de cette thèse et de la recherche associée est une démonstration des avantages d’une combinaison de propriétés inhabituelles de nanostructures plasmoniques avec des aspects parmi les plus intéressants de l’optique non-linéaire. Pour cet effet, la modélisation analytique et numérique a été combiné avec le travail expérimental, qui comprenait la production de nanostructures et les mesures effectuées au moyen de la microscopie confocale non-linéaire résolue en polarisations et de la technique Z-scan modifiée (nommée “f-scan”).Il a été montré que l’anisotropie efficace de génération de seconde-harmonique dans les cristaux plasmoniques (formés par des réseaux rectangulaires de cavités tétraédriques sur une surface d’argent) peut être contrôlée par un choix approprié des paramètres de maille. Il a aussi été montré que cette anisotropie provient principalement d’une structure de bande photonique elle-même anisotrope, présentant une bande interdite plasmonique avec des états plasmoniques en bord de bande, permettant de renforcer le champ électrique local. Les arrangements chiraux bidimensionnels de nanoparticules triangulaires d’or, forment des “meta-molécules” plasmoniques énantiomériques, ont été analysés par microscopie non-linéaire à la lumière polarisée circulairement et par modélisation numérique, révélant un fort effet chiroptique par génération de seconde harmonique en rétro-réflexion. La petite taille des énantiomères uniques permet de créer “des filigranes” (“watermarks”) codés par la chiralité des meta-molécules, qui peuvent être lu par imagerie de la génération de seconde harmonique excitée par un rayon polarisé circulairement. Les caractéristiques quantitatives de la non-linéarité optique du troisième ordre et de l’efficacité d’absorption saturable des solutions aqueuses de fragments de graphène et de graphène dopé par des nanoparticules d’or a été effectuée par une nouvelle technique “f-scan”, qui a été créée et développée par incorporation d’une lentille à distance focale accordable dans une technique de Z-scan traditionnelle. Ces études ont montrées que le graphène présente une absorption saturable ultra-rapide très efficace, qui est parfois convertie en absorption saturable inverse. Il apparaît alors qu’une décoration du graphène par des nanoparticules d’or peut causer une légère amélioration du paramètre d’efficacité d’absorption saturable dans la plage spectrale de leurs résonances plasmoniques. En résumé, cette thèse présente une variété de propriétés optiques non-linéaires apparaissant dans les nanostructures plasmoniques. Différentes possibilités de contrôle de ces propriétés au moyen d’une démarche de nano-ingénierie, soutenue par des modélisations à la fois analytique et numérique ont été démontrées et analysées. Ces travaux ouvrent la voie à la fabrication et à l‘optimisation sur mesure de nouveaux nano-matériaux et nano-dispositifs photoniques reposant sur des effets de nano-plasmonique non-linéaire. / The aim of this thesis and the underlying research work is to demonstrate the benefits emerging from combination of the peculiar properties of plasmonic nanostructures with the most interesting aspects of nonlinear optics. For this purpose, analytical and numerical modeling was combined with experimental work, which included nanofabrication and measurements performed by means of polarization-resolved nonlinear confocal microscopy and by modified Z-scan technique (called "f-scan").It has been shown that the effective anisotropy of the second-harmonic generation in plasmonic crystals (formed by rectangular arrays of tetrahedral recesses in silver surface) can be controlled by proper choice of lattice constants. It also has been shown that this anisotropy arises mainly from the anisotropic photonic band structure, exhibiting plasmonic band gap with plasmonic band edge states, enabling enhancement of the local electric field.Two-dimensional chiral arrangements of triangular gold nanoparticles, forming plasmonic enantiomeric "meta-molecules", have been studied by nonlinear microscopy operating with circularly polarized light and by numerical modeling, revealing strong chiroptical effect in backscattered second-harmonic radiation. Small size of individual enantiomers allows to create "watermarks", encoded by the chirality of meta-molecules, which can be readout by imaging of second-harmonic generation excited by circularly polarized laser beam.Quantitative characterization of the third-order optical nonlinearity and saturable absorption efficiency of aqueous solutions of graphene and gold-nanoparticle decorated graphene has been performed by novel "f-scan" technique, which has been created and developed by incorporation of a focus-tunable lens into traditional Z-scan. These studies have shown that the graphene exhibits very efficient ultrafast saturable absorption, which is occasionally suppressed by reverse saturable absorption. Moreover, it turns out that decoration of graphene by gold nanoparticles may cause a slight improvement of the saturable absorption efficiency parameter within spectral range of their plasmon resonances.In summary, the following thesis presents various nonlinear optical properties of plasmonic nanostructures. Different possibilities of controlling these properties by means of nano-engineering, supported by analytical and numerical modeling, is also analyzed and demonstrated. This work opens up new perspectives for fabrication and rational design of novel photonic nano-materials and nano-devices based on nonlinear nanoplasmonic phenomena.

Conductors with IR (infrared) plasma frequencies are potentially useful hosts of surface plasmon polaritons (SPPs) with subwavelength mode confinement for sensing applications. The underlying aim of this work is to identify such conductors that also have sharp SPP excitation resonances for biosensor applications at infrared (3-11 m) wavelengths, where biological analytes are strongly differentiated by their IR absorption spectra. In this work, various materials were investigated such as a heavily doped semiconductor, a semimetal, a conducting polymer and its composite. Heavily doped silicon was investigated by tuning its plasma frequency to the infrared region by heavily doping. The measured complex permittivity spectra for p-type silicon with a carrier concentration of 6  1019 and 6  1020 cm -3 show that these materials support SPPs beyond 11 and 6 m wavelengths, respectively. SPP generation was observed in angular reflection spectra of doped-silicon gratings. Photon-to-plasmon coupling resonances, a necessary condition for sensing, were demonstrated near 10 m wavelength for the heaviest doped, and the observed resonances were confirmed theoretically using analytic calculations. The permittivity spectra were also used to calculate SPP mode heights above the silicon surface and SPP propagation lengths. Reasonable merit criteria applied to these quantities suggest that only the heaviest doped material has sensor potential, and then mainly within the wavelength range of 6 to 10 m. iv The semimetal bismuth (Bi) has an infrared plasmon frequency less than the infrared plasma frequency of noble metals such as gold and silver, which is one order of magnitude lower than their plasma frequencies. The excitation of IR surface plasmons on Bi lamellar gratings in the wavelength range of 3.4 µm to 10.6 µm was observed. Distinct SPP resonances were observed although the usual condition for bound SPP is not satisfied in this wavelength range because the real part of the permittivity is positive. The excitation of these resonances agrees theoretically with the electromagnetic surface waves called surface polaritons (SPs). The measured permittivity spectra were used to calculate the SP mode heights above the bismuth surface and SP propagation length, which satisfied our criteria for sensors. A conducting polymer and its composite with graphite were also investigated since their plasma frequency may lie in the infrared region. Polyaniline was chemically synthesized and doped with various acids to prepare its salt form. A composite material of polyaniline with colloidal and nano-graphite was also prepared. Optical constants were measured in the long wave infrared region (LWIR) and were used to calculate SPP propagation length and penetration depth. SPP resonance spectra were calculated and suggested that polyaniline and its composite can be used as a host with sufficient mode confinement for IR sensor application.

Surface plasmon resonances at the nanoscale hold great potential for applications in many areas, and the characterization of plasmonic nanostructures plays a critical role in the realization of these applications. Electron energy loss spectroscopy (EELS) has emerged as a powerful characterization tool to study the response of plasmonic nanostructures due to its high spatial-resolution and the capability to probe bright as well as dark plasmonic modes. The main limiting factor of EELS is the energy resolution. However, in this thesis, we overcome this limitation using a combination of electron monochromation and the use of the Richardson-Lucy algorithm. We show that the algorithm could be used to obtain effective energy resolutions up to 10 meV. Using EELS we analyze the resonances of planar nanostructures, and we found that the supported resonances can be described as edge and cavity or film modes, behaving as 1D and 2D modes respectively. We also demonstrate that edge modes are unaffected by the presence of bends up to the critical angle of 90◦ where the modes start self-interacting producing large energy shifts. The interaction of plasmon resonances is also studied, and we show that the coupling can be reduced to three behaviors: coupling through the edge, coupling through a corner, and non-coupling. We propose a method to control the coupling through the edge in offset nanowires, by tuning the nodal alignment and spectral overlap of the edge modes. Finally, we analyze the plasmon modes supported by Koch snowflake fractal antennas, and we demonstrate that modes present in the fractals are formed by the edge modes supported by their characteristic edges. This thesis provides a complete picture of the surface plasmon resonances supported by planar nanostructures and demonstrates the ability of EELS to probe and image a wide variety of plasmonic resonances. / Thesis / Doctor of Philosophy (PhD)

No description available.

This work presents the first demonstration of a semiconductor based plasmonic near-field superlens, utilizing highly doped GaAs to generate infrared optical images with a spatial resolution beyond the difraction limit. Being easily transferable to other semiconductor materials, the concept described in this thesis can be exploited to realize spectrally adjustable superlenses in a wide spectral range. The idea of superlensing has been introduced theoretically in 2000, followed by numerous publications including experimental studies. The effect initiated great interest in optics, since in contrast to difraction limited conventional optical microscopy it enables subwavelength resolved imaging by reconstructing the evanescent waves emerging from an object. With techniques like scanning near-field optical microscopy (SNOM) and stimulated emission depletion (STED) being already successfully established to overcome the conventional restrictions, the concept of superlensing provides a novel, different route towards high resolution. Superlensing is a resonant phenomenon, relying either on the excitation of surface plasmons in metallic systems or on phonon resonances in dielectric structures. In this respect a superlens based on doped semiconductor benefits from the potential to be controlled in its operational wavelength by shifting the plasma frequency through adjustment of the free carrier concentration. For a proof of principle demonstration, we investigate a superlens consisting of a highly n-doped GaAs layer (n = 4 x 10^18 cm-3) sandwiched between two intrinsic layers. Recording near-field images of subwavelength sized gold stripes through the trilayer structure by means of SNOM in combination with a free-electron laser, we observe both enhanced signal and improved spatial resolution at radiation wavelengths close to l = 22 µm, which is in excellent agreement with simulations based on the Drude-Lorentz model of free electrons. Here, comparative investigations of a purely intrinsic reference sample confirm that the effect is mediated by the charge carriers within the doped layer. Furthermore, slightly differently doped samples provide indications for the expected spectral shift of the resonance. According to our calculations, the wavelength range to be exploited by n-GaAs based superlenses reaches far into the terahertz region, whereas other semiconductor materials are required to explore the near infrared.

This thesis proposes a metallic hole array of a rectangular converging-diverging channel (RCDC) shape with extraordinary transmission. We use a three-dimensional (3D) finite element method to analyze the transmission characteristics of two-dimensional metallic hole arrays (2D-MHA) with RCDC. For a straight channel MHA, when the aperture size is reduced, the transmission peaks have a blue-shift. The same result is observed for a smaller gap throat for the RCDC structure. For the rectangular holes with a high length-width ratio, a similar blue-shift in the transmission peaks as well as a narrower full width at half maximum (FWHM) are observed. The asymmetry from the rectangular shape gives this structure high selectivity for light with different polarizations. Furthermore, the RCDC shape gives extra degrees of geometrical variables to 2D-MHA for tuning the location of the transmission peak and FWHM. The tunable transmission property of this structure shows promise for applications in tunable filters, photonic circuits, and biosensors. / text

All conducting polymers are potentially electrochromic, owing to the injection of charge carriers that changes their electronic structure and results in a shift of their optical absorption towards higher wavelengths. PEDOT-PSS and PEDOT-S are very promising materials in terms of electrochromic properties, due to the good contrast existing between their doped and undoped forms. However this contrast has to be enhanced in order to design more efficient electrochromic devices, and new solutions should thus be found in order to solve this issue. Surface plasmons are described as electromagnetic waves propagating along the surface between a dielectric and a metal. Coupled to an incident radiation, they create an energy loss in the light transmitted and reflected by the interface. When the metallic surface is periodically corrugated, this absorption phenomenon due to plasmonic resonance occurs at a specific wavelength that depends on several parameters, such as the incidence angle, the dielectric constants of the two media and the grating period. By coating metallic gratings with electrochromic polymers, we may thus be able to trigger a plasmonic absorption at a given wavelength and shift it upon reduction or oxidation of the material. Electrochromic devices consisting of PEDOT-PSS or PEDOT-S spin-deposited on gold and silver gratings were investigated by UV-visible reflectance measurements. The periodically corrugated structures were reproduced from commercial gratings by soft nanolithography and were analyzed by AFM. Some electrochromic cells exhibited new colors or a high shift of the plasmonic resonance upon redox switching of the polymer film. Depending on the step and the nature of the grating employed, this shift could reach 20 nm in the case of PEDOT-PSS and more than 100 nm for PEDOT-S. A theoretical model was found to predict the wavelength of plasmonic excitation and the orientation of the shift.

This thesis examines the feasibility of using conventional semiconductors, specifically GaAs, as a plasmonic material at the operating wavelength of 1550nm, due to its many merits such as achievable low losses and mature micro-fabrication technologies. A theoretical study is performed on GaAs that yielded the condition for plasmonic behaviour at a minimum free carrier density of 7.2 x 10^20cm^-3 in bulk materials. The most feasible route to achieving this condition is determined to be intense optical excitation, and the required intensity considering a 150fs pulse at the above bandgap wavelength of 870nm is approximately 2.55TW/cm^2. A Bragg reflection ridge waveguide (BRW) using GaAs-AlGaAs is designed and micro-fabricated, and a counter-propagating pump-probe experiment is devised to test the plasmonic effect using the BRW. Results from two different ultrafast lasers include the observation of pump (870nm and 800nm) coupling to fundamental Bragg modes, and the measurement of the pump transmission spectrum.