The molecular compositions of the atmospheres of the giant planets (Jupiter, Saturn, Uranus and Neptune) are fundamental to understanding the processes which formed these planets and the solar system as a whole. Microwave observations of these planets probe regions in their atmospheres from approximately 0.1 to several bars, a process otherwise unachievable by visible and infrared means. Many gases and various cloud layers influence the millimeter wave spectra of the outer planets; however phosphine and ammonia are the main microwave absorbers at Saturn at pressures less than two bars. Understanding the pressure induced absorption of both constituents at observational frequencies is therefore vital to the analysis of any observational data. Laboratory measurements have been conducted to measure the microwave absorptivity and refractivity of phosphine and ammonia at Ka-band (32-40 GHz) and W-band (94 GHz), under conditions characteristic of the atmosphere of Saturn. The results were used to verify the accuracy of the phosphine formalism created by Hoffman et. al (2001) for use at millimeter wavelengths. Based on the laboratory measurements conducted, new formalisms were also created to express the opacity of ammonia at the measured frequencies. An important method for the study of planetary atmospheres is the radio occultation experiment ??method that uses radio links between Earth, and the spacecraft which passes behind the planet. The Cassini mission to Saturn, which will be conducting such experiments at Ka-band as well as S (2.3 GHz) and X (8.4 GHz) bands, has prompted the development of a radio occultation simulator used to calculate excess Doppler shifts and attenuation profiles for Saturn, utilizing the newest formalisms for phosphine and ammonia. The results indicate that there will be unambiguous detection and profiling of phosphine and ammonia, and predictions are made for the pressures at which loss of signal is anticipated.

Transparent polycrystalline aluminum oxide is a promising optical material, particularly in applications that require ballistic protection. However, the rhombohedral crystal structure of alumina limits its transparency due to birefringent scattering. One method of reducing birefringent scattering is to align the particles along the same crystallographic direction, minimizing the refractive index mismatch. This dissertation explores the use of high aspect-ratio platelet-morphology alumina powder in order to process a crystallographically aligned polycrystalline alumina part, with improved optical properties. The optimal hot-pressing parameters of non-pre-aligned platelet alumina were explored, showing that a low pre-load pressure (0MPa), a high maximum temperature (1800°C), a low maximum pressure (10MPa), and a long isothermal hold time (>5hrs) yields dense, transparent parts. These parameters resulted in samples with a high in-line transmission (>65%) despite a large grain size (>60μm). This is due to a high degree of crystallographic orientation, which minimizes the refractive index mismatch between grains, reducing birefringent scattering. Pre-alignment resulted in a further increase in crystallographic orientation, indicating that the pre-alignment procedure effectively aligns the platelets along the same crystallographic orientation. However, pre-alignment resulted in a minimal improvement in optical properties due to the pre-aligned platelets decreasing the densification. Mechanical properties were characterized, resulting in a flexure stress and Vickers hardness of approximately 175MPa and 17GPa, respectively. These low mechanical properties are due to the large grain size. The Vickers hardness was also characterized along different alignment/hot-pressing directions, showing that the hardness matches that of sapphire along corresponding crystallographic directions. Modifications to the Rayleigh-Gans-Debye model were made, accounting for crystallographic orientation. The modified model more closely matches the experimental optical data, illustrating the importance of accounting for crystallographic alignment. This dissertation emphasizes the importance of characterizing optical losses in transparent ceramics and how they relate to the microstructure, as well as the significance of crystallographic alignment in a birefringent transparent ceramic like alumina.

<p> Optical metamaterials have triggered extensive studies driven by their fascinating electromagnetic properties that are not observed in natural materials. Aside from the extraordinary progress, challenges remain in scalable processing and material performance which limit the adoption of metamaterial towards practical applications. The goal of this dissertation is to design and fabricate nanocomposite thin films by combining nitrides with a tunable secondary phase to realize controllable multi-functionalities towards potential device applications. Transition metal nitrides are selected for this study due to the inherit material durability and low-loss plasmonic properties that offer stable two-phase hybridization for potential high temperature optical applications. Using a pulsed laser deposition technique, the nitride-metal nanocomposites are self-assembled into various geometries including pillar-in-matrix, embedded nanoinclusions or complex multilayers, that possess large surface coverage, high epitaxial quality, and sharp phase boundary. The nanostructures can be further engineered upon precise control of growth parameters. </p><p> This dissertation is composed of a general review of related background and experimental approaches, followed by four chapters of detailed research chapters. The first two research chapters involve hybrid metal (Au, Ag) - titanium nitride (TiN) nanocomposite thin films where the metal phase is self-assembled into sub-20 nm nanopillars and further tailored in terms of packing density and tilting angles. The tuning of plasmonic resonance and dielectric constant have been achieved by changing the concentration of Au nanopillars, or the tuning of optical anisotropy and angular selectivity by changing the tilting angle of Ag nanopillars. Towards applications, the protruded Au nanopillars are demonstrated to be highly functional for chemical bonding detection or surface enhanced sensing, whereas the embedded Ag nanopillars exhibit enhanced thermal and mechanical stabilities that are promising for high temperature plasmonic applications. In the last two chapters, dissimilar materials candidates beyond plasmonics have been incorporated to extend the electromagnetic properties, include coupling metal nanoinclusions into a wide bandgap semiconducting aluminum nitride matrix, as well as inserting a dielectric spacer between the hybrid plasmonic claddings for geometrical tuning and electric field enhancement. As a summary, these studies present approaches in addressing material and fabrication challenges in the field of plasmonic metamaterials from fundamental materials perspective. As demonstrated in the following chapters, these hybrid plasmonic nanocomposites provide multiple advantages towards tunable optical or biomedical sensing, high temperature plasmonics, controllable metadevices or nanophotonic chips.</p><div><br></div>

The optical properties of InAs/GaSb heterostructures under applied magnetic fields are studied in experimental and theoretical detail. The InAs/GaSb system is a type-II "crossed-gap" system, where the valence band edge of GaSb lies higher in energy than the conduction band edge of InAs. This leads to a region of energy above the InAs conduction band where conduction and hole states mix. Thin-layer superlattices remain semiconducting due to confinement effects, but thick-layer superlattices experience charge transfer which leads to intrinsic carrier densities approaching 10¹² cm^-2 per layer. Existing multi-band modeling techniques based on the <strong>k·p</strong> formalism are discussed, and a method of solving superlattice band structure (the "momentum-matrix" technique) is presented. The quantizing effects of the superlattice layers and applied magnetic fields are investigated, and the selection rules for optical transitions are derived. Standard cyclotron resonance (CR) is used to study effective masses in InAs/GaSb structures. The heavy hole mass is found to be strongly orientation-dependent, with a mass in the [111] orientation reduced 25% from the [001] mass. The electron mass is found to be roughly isotropic with respect to growth orientation, but shows variation with the InAs width due to quantum confinement effects. CR of InAs/GaSb heterojunctions display hitherto unexplained oscillations in linewidth, intensity, and effective mass. A model is proposed which explains the oscillations, based on the intrinsic nature of the InAs/GaSb system. CR is performed on an InAs/GaSb heterojunction using a free-electron laser, where due to the high intensities (on the order of MW/cm²) the absorption process saturates. This saturation allows for a determination of non-radiative relaxation lifetimes, and through the energy dependence of these lifetimes the magnetophonon effect is observed, allowing a direct measurement of LO-phonon-assisted energy relaxation rates. Coupling is introduced into the standard CR experiment, either by tilting the sample with respect to the magnetic field, or by applying a metal grating to the surface. These coupled CR experiments have striking qualitative results which allow for determination of subband separation energies and coupling matrix elements. Photoconductivity experiments are performed on thin-layer (semiconducting) superlattices, showing optical response at far-infrared wavelengths (5-20 μm). The results are compared with <strong>k·p</strong> calculations. One sample is processed for vertical transport, in which conduction occurs perpendicular to the superlattice layers. Strong optical response from this sample indicates the viability of InAs/GaSb-based far-infrared detectors. The momentum-matrix technique is used to predict optimum parameters for semiconducting superlattices with band gaps in the far-infrared. Semimetallic structures are studied via a multi-band self-consistent model, with results corroborating with and extending previous work. Intrinsic structures under applied magnetic field are modeled theoretically for the first time.

Typescript (photocopy). / Digitized by Kansas Correctional Industries

The chemical and optical properties of particulate organic compounds remain unclear, which leaves large uncertainties in the estimation of global radiative transfer balance. Gas and find particle (PM2.5) phase formic acid concentrations were measured with online instrumentation during separate one-month studies in the summer of 2010 in Los Angeles (LA), CA, and Atlanta, GA, and the gas-particle partitioning behavior was investigated and compared with that of water-soluble organic compounds (WSOC). The diurnal profiles clearly indicated that the photochemistry production serves as a strong source for the formation of organics, while the correlation between the gas and particle phase suggested that another partitioning route, the aqueous reactions, is also very important. Later, the optical properties of light-absorbing organic compounds were examined. Little is known about the optical importance of light absorbing particulate organic compounds (brown carbon), especially its extent and absorption relative to black carbon throughout the tropospheric column. Mie theory was applied to size-resolved spectrophotometric absorption measurements of methanol and water-extracts from cascade impactor substrates collected at three surface sites around Atlanta, GA, including both urban and rural. These results were applied to similar measurements of brown carbon in extracts from aircraft bulk filter samples collected over central USA. At the surface sites predicted light absorption by brown carbon relative to total absorption (brown carbon plus pure black carbon) was about 10% and 30% at 350 nm, versus 1 and 11% at 450 nm, for water and methanol extracts, respectively. The relative contribution of brown carbon was greater in the free troposphere and significantly increased with altitude. Although this approach has limitations, it demonstrates the ubiquity and significant potential contribution of brown carbon.

Dissertation (PhD)--University of Stellenbosch, 2006. / Please refer to full text for abstract.

The two-photon absorption (TPA) coefficient is measured in indium phosphide (InP) using femtosecond pulses to be 45cm/GW at 1.32μm. Nanosecond pulses are subsequently used to find the free-carrier refractive index cross-section, σ_r, and the free-carrier absorption coefficient, σ_fca. The quantity βσ_r is measured to be -113x10⁻²ºcm⁴/GW at 1.064μm and -84x10⁻²ºcm⁴/GW at 1.534μm. At 1.064μm, with β assumed to be 22cm/GW, the value suggested by theory, σ_r is -5.1x10⁻²ºcm³. Similarly, at 1.534μm, assuming β to be 20cm/GW gives a σ_r value of -4.1x10⁻²ºcm³. Due to refraction affecting the measurements of σ_fca, only an upper limit of 1x10⁻¹⁵cm² can be put on its value. The free-carrier experiments are repeated on two samples of cadmium mercury telluride (CMT) having bandgaps of 0.89eV and 0.82eV. For the first sample, β_σr is measured to be -148x10⁻²ºcm⁴/GW. Assuming β to be 89cm/GW gives a σ_r value of -1.7x10⁻²ºcm³ whilst σ_fca is found to be at most 3x10⁻¹⁵cm². Significant linear absorption occurs in the second sample which generates a large free-carrier population. It is shown that this significantly enhances the nonlinearities. Finally, the results of the work are tested by modelling a nonlinear transmission experiment, and the results found in this work give a closer fit to experimental results than the result of theory. Four-wave mixing (FWM) in a photonic crystal fibre is exploited to create a high output power optical parametric amplifier (OPA). To optimise the OPA conversion efficiency, the fibre length has to be increased to 150m, well beyond the walk-off distance between the pump and signal/idler. In this regime, the Raman process can take over from the FWM process and lead to supercontinuum generation. The OPA exhibits up to 40% conversion efficiency, with the idler (0.9μm) and the signal (1.3μm) having a combined output power of over 1.5W.

In order to completely assess the potential of semiconductor nanowires for multifunctional applications such as flexible electronics, nanoelectromechanical systems (NEMS), and composites, a full characterization of their properties must be obtained. While many of their physical properties have been well studied, explorations of mechanical, electromechanical, and optical properties of semiconductor nanowires remain relatively sparse in the literature. Two major hurdles to the elucidation of these properties are: (1) the development of experimental techniques which are capable of mechanical and electromechanical measurements coupled with detailed structural analysis, and (2) the synthesis of high quality nanowires with the high yields necessary to produce the quantities needed for composite fabrication. These issues are addressed in this dissertation by utilizing the supercritical fluid-liquid-solid (SFLS) synthesis method to produce germanium (Ge) nanowire specimens for mechanical and electromechanical measurements coupled with high-resolution transmission electron microscopy (HRTEM). In addition, excellent dispersibility and large quantities allow for optical measurements of dispersions and composites. Ge cantilever nanoelectromechanical resonators were fabricated and induced into resonance. From the frequency response, the Young's modulus of the nanowires was determined to be insensitive to diameter and on par with the literature values for bulk Ge. The mechanical quality factors of the resonators were found to decrease with decreasing diameter. The data indicate that energy dissipation from the oscillating cantilevers occurs predominantly via surface losses. The mechanical strengths of individual Ge nanowires were measured by in situ nanomanipulation in a scanning electron microscope (SEM). The nanowires were found to tolerate diameter-dependent flexural strains more than two orders of magnitude higher than bulk Ge. Corresponding bending strengths were in agreement with the ideal strength of a perfect Ge crystal, indicative of a reduced presence of extended defects. The nanowires also exhibited plastic deformation at room temperature, becoming amorphous at the point of maximum strain. The optical absorbance spectra of Ge nanowires were measured and found to exhibit spectra markedly different from bulk Ge. Simulations using a discrete dipole approximation (DDA) model suggest that the difference in light absorption results from light trapping within the nanowires. / text

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