Polymer stabilized cholesteric liquid crystals (PSCLCs) provide many advantages over other electro-optical materials. The unique helical structure of the cholesteric liquid crystal (CLC) creates a natural gradient for light interacting across each CLC domain layer. Not only does the CLC helical structure greatly increase the bandwidth tuning and broadening range, it also allows CLCs to act as a polarizer, notch filter, reflector, and optical rotator all in one material. However, while many novel PSCLC materials have been created, little is understood about how complex initial system interactions affect final electro-optical (e-o) properties.1,2 In this work, the principal variables affecting PSCLC blue shift electro-optical behavior have been determined through structural analysis and measurement of electro-optical properties. Typical PSCLC materials must meet both formulation and photopolymerization processing requirements to display blue shift e-o properties. Threshold photoinitiator concentrations (0.5-1.5 wt%) and morpholine containing group concentrations (0.25-1.0 wt%) were both shown to be primary factors, along with sufficient UV exposure time (10-30 min) and light intensity (500 mW/cm2, 365 nm), for PSCLC blue shift bandwidth tuning/broadening to occur. Morpholine was initially identified as a component of photoinitators Irgacure 369 and 907 and was proven to increase PSCLC ion density altering LC-polymer network interactions with several proposed theories included later in this work. The use of an appropriate morpholine containing LC monomer to directly incorporate morpholine into the LC-polymer network was shown to greatly improve PSCLC sample stability. Through the results of this research we successfully induced blue shift e-o behavior in a previous red shift only PSCLC using only 30% of the UV exposure that a model PSCLC blue shift sample required while extending the blue shift broadening range over threefold (from 75 nm to 250 nm). The fundamental understanding and design of PSCLC systems described herein serves as a starting point for engineering PSCLC materials with specific and desirable electro-optical properties.

We correlated experimental results with theoretical estimations of the dielectric function ε(ω) in two contexts: the effect of an electric field in quantum wells and that of the spin polarization of an interacting electron-hole plasma in bulk semiconductors. In the first part, we recorded photoreflectance spectra from Ge/GeSi quantum wells of different widths but having comparable builtin electric fields caused by doping. The reason why the spectra differed in overall shape was difficult to understand by conventional methods, for example, by calculating the allowed transition energies or by fitting the data with lineshape functions at each transition energy. Instead, we computed the photoreflectance spectra from first-principles by using the confined electron and hole wavefunctions. This method showed that the spectra differ in overall shape because of the experimentally hitherto unobserved trend in quantum well electro-optical properties, from the quantum confined Franz-Keldysh effect to the bulk Franz-Keldysh effect, as the well width is increased. The second part develops a threeband microscopic theory for the optical properties due to spin-polarized carriers in quasiequilibrium. We show that calculations based on this theory reproduce all the trends observed in a recent circularly polarized pump-probe experiment reported in the literature. To make the computation less intensive, we proposed a simplified, two-band version of this theory which captured the main experimental features. Besides, we constructed a cw diode laser-based pump-probe setup for our own optical studies of spin-polarized carriers by Kerr rotation. We achieved a sensitivity of detection of Kerr rotation of 3 x 10¯ 8 rad, corresponding to an order of magnitude improvement over the best reports in the literature. The efficacy of our setup allowed for the demonstration of a pumpinduced spin polarization in bulk GaAs, under the unfavorable conditions of steady-state and room temperature.

In recent years, the interest in improving the properties of liquid-crystalline systems by using metallic nanoparticles has grown. This is because these materials have particular optical and electrical characteristics, associated with the plasmon resonance phenomenon. Recently, several studies have shown that the addition of gold nanoparticles affects the electrical response of liquid crystals depending on the nanoparticles geometry and the liquid-crystalline alignment. In this study, we investigated the effects of the addition of gold nanoparticles with different geometries on the relaxation time of the 4-octyl-4-cyanobiphenyl (8CB) liquid crystal, under the helical confinement conditions. We used an experimental setup that explores the Brewster angle to investigate how the application of a external electrical field and temperature of the system affect the reorientation dynamics of the director vector nearby the transition of nematic-smectic-A phase. The results obtained were analyzed within the elastic theory of Franck-Oseen e allowed us to evaluate the effects of nanoparticles on the viscoelastic parameters of the system. Our results show that the addition of nanoparticles significantly affects the electro-optical response of the investigated liquid crystals, especially in conditions of high temperature and low amplitude of the applied electrical field. In addition, we have observed that the geometry of the nanoparticles plays a key role in the modification of the electro-optical properties of the system. / Coordenação de Aperfeiçoamento de Pessoal de Nível Superior / Nos últimos anos, tem crescido o interesse no melhoramento das propriedades de sistemas líquido-cristalinos usando nanopartículas metálicas. Isso porque esses materiais apresentam propriedades ópticas e elétricas particulares, associadas ao fenômeno de ressonância de plásmon. Recentemente, vários trabalhos têm demonstrado que a adição de nanopartículas de ouro afetam a resposta elétrica de cristais líquidos dependendo da geometria das nanopartículas utilizadas e do alinhamento líquido-cristalino. Neste trabalho, nós investigamos os efeitos da adição de nanopartículas de ouro com diferentes geometrias sobre o tempo de relaxação de amostras do cristal liquido 4-octil-4-cianobifenil (8CB) nas condições de confinamento helicoidal. Nós usamos um aparato experimental que explora o ângulo de Brewster para investigar como a aplicação de um campo elétrico externo e a temperatura do sistema afetam a dinâmica de reorientação do vetor diretor nas proximidades da transição de fase nemática-esmética-A. Os resultados obtidos foram analisados dentro da teoria elástica de Franck-Oseen e permitiu-nos avaliar os efeitos das nanopartículas sobre os parâmetros viscoelásticos do sistema. Nossos resultados mostram que a adição de nanopartículas afeta significativamente a resposta elétro-óptica dos cristais líquidos investigados, especialmente nas condições de alta temperatura e baixa amplitude do campo elétrico aplicado. Além disso, nós observamos que a geometria das nanopartículas desempenha um papel fundamental namodificação das propriedades eletro-ópticas do sistema.

This thesis is devoted to the optical properties of low-dimensional structures based on such two-dimensional materials as graphene, silicene and phosphorene. We investigate optical properties of a variety of quasi-one dimensional and quasi-zero-dimensional structures, which are promising for future optoelectronics. Primarily we focus on their low-energy optical properties and how these properties are influenced by the structures’ geometry, external fields, intrinsic strain and edge disorder. As a consequence of this endeavor, we find several interesting effects such as correlation between the optical properties of tubes and ribbons whose periodic and ‘hard wall’ boundary conditions are matched and a universal value of matrix element in narrow-gap tubes and ribbons characterizing probability of transitions across the band gap opened up by intrinsic strain originating from the tube’s surface curvature or ribbon’s edge relaxation. The analytical study of the gapped 2D Dirac materials such as silicene and germanene, which have some similarity to the aforementioned quasi-one-dimensional systems in terms of physical description, reveals a valley- and polarization-dependent selection rules. It was also found that absorption coefficient should change in gapped materials with increasing frequency and become a half of its value for gap edge transitions when the spectrum is linear. Our analysis of the electronic properties of flat clusters of silicene and phosphorene relates the emergence and the number of the peculiar edge states localized at zero energy, so-called zero-energy states, which are know to be of topological origin, to the cluster’s structural characteristics such as shape and size. This allows to predict the presence and the number of such states avoiding complicated topological arguments and provides a recipes for design of metallic and dielectric clusters. We show that zero-energy states are optically active and can be efficiently manipulated by external electric field. However, the edge disorder is important to take into account. We present a new fractal-based methodology to study the effects of the edge disorder which can be applied also to modeling of composite materials. These finding should be useful in design of optoelectronic devices such as tunable emitters and detectors in a wide region of electromagnetic spectrum ranging form the mid-infrared and THz to the optical frequencies.