Microwave dielectrics are widely used to make resonators and filters in telecommunication systems. The production of thin films with high dielectric constant and low loss could potentially enable a marked reduction in the size of devices and systems. However, studies of these materials in thin film form are very sparse. In this research, experiments were carried out on practical high-performance dielectrics including ZrTiO4-ZnNb2O6 (ZTZN) and Ba(Co,Zn)1/3Nb2/3O3 (BCZN) with high dielectric constant and low loss tangent. Thin films were deposited by laser ablation on various substrates, with a systematical study of growth conditions like substrate temperature, oxygen pressure and annealing to optimize the film quality, and the compositional, microstructural, optical and electric properties were characterized. The deposited ZTZN films were randomly oriented polycrystalline on Si substrate and textured on MgO substrate with a tetragonal lattice change at elevated temperature. The BCZN films deposited on MgO substrate showed superior film quality relative to that on other substrates, which grow epitaxially with an orientation of (001) // MgO (001) and (100) // MgO (100) when substrate temperature was above 500 oC. In-situ annealing at growth temperature in 200 mTorr oxygen pressure was found to enhance the quality of the films, reducing the peak width of the X-ray Diffraction (XRD) rocking curve to 0.53o and the χmin of channeling Rutherford Backscattering Spectrometry (RBS) to 8.8% when grown at 800oC. Atomic Force Microscopy (AFM) was used to study the topography and found a monotonic decrease in the surface roughness when the growth temperature increased. Optical absorption and transmission measurements were used to determine the energy bandgap and the refractive index respectively. A low-frequency dielectric constant of 34 was measured using a planar interdigital measurement structure. The resistivity of the film is ~3×1010 ohm·cm at room temperature and has an activation energy of thermal activated current of 0.66 eV.

The mechanism of loss in high performance microwave dielectrics with complex perovskite structure, including Ba(Zn1/3Ta2/3)O3, Ba(Cd1/3Ta2/3)O3, ZrTiO4-ZnNb2O6, Ba(Zn1/3Nb2/3)O3, and BaTi4O9-BaZn2Ti4O11, has been investigated. We studied materials synthesized in our own lab and from commercial vendors. Then the measured loss tangent was correlated to the optical, structural, and electrical properties of the material. To accurately and quantitatively determine the microwave loss and Electron Paramagnetic Resonance (EPR) spectra as a function of temperature and magnetic field, we developed parallel plate resonator (PPR) and dielectric resonator (DR) techniques. Our studies found a marked increase in the loss at low temperatures is found in materials containing transition metal with unpaired d-electrons as a result of resonant spin excitations in isolated atoms (light doping) or exchange coupled clusters (moderate to high doping) ; a mechanism that differs from the usual suspects. The loss tangent can be drastically reduced by applying static magnetic fields. Our measurements also show that this mechanism significantly contributes to room temperature loss, but does not dominate. In order to study the electronic structure of these materials, we grew single crystal thin film dielectrics for spectroscopic studies, including angular resolved photoemission spectroscopy (ARPES) experiment. We have synthesized stoichiometric Ba(Cd1/3Ta2/3)O3 [BCT] (100) dielectric thin films on MgO (100) substrates using Pulsed Laser Deposition. Over 99% of the BCT film was found to be epitaxial when grown with an elevated substrate temperature of 635 C, an enhanced oxygen pressures of 53 Pa and a Cd-enriched BCT target with a 1 mol BCT: 1.5 mol CdO composition. Analysis of ultra violet optical absorption results indicate that BCT has a bandgap of 4.9 eV.

The study of high energy particle irradiation effect on Josephson junction tri-layers is relevant to applications in space and radioactive environments. It also allows us to investigate the influence of defects and interfacial intermixing on the junction electrical characteristics. In this work, we studied the influence of 2MeV Helium ion irradiation with doses up to 5.2×1016 ions/cm2 on the tunneling behavior of Nb/Al/AlOx/Nb Josephson junctions. Structural and analytical TEM characterization, combined with SRIM modeling, indicates that over 4nm of intermixing occurred at the interfaces. EDX analysis after irradiation, suggests that the Al and O compositions from the barrier are collectively distributed together over a few nanometers. Surprisingly, the IV characteristics were largely unchanged. The normal resistance, Rn, increased slightly (<20%) after the initial dose of 3.5×1015 ions/cm2 and remained constant after that. This suggests that tunnel barrier electrical properties were not affected much, despite the significant changes in the chemical distribution of the barrier's Al and O shown in SRIM modeling and TEM pictures. The onset of quasi-particle current, sum of energy gaps (2Δ), dropped systematically from 2.8meV to 2.6meV with increasing dosage. Similarly, the temperature onset of the Josephson current dropped from 9.2K to 9.0K. This suggests that the order parameter at the barrier interface has decreased as a result of a reduced mean free path in the Al proximity layer and a reduction in the transition temperature of the Nb electrode near the barrier. The dependence of Josephson current on the magnetic field and temperature does not change significantly with irradiation, suggesting that intermixing into the Nb electrode is significantly less than the penetration depth.

This work is an investigation into the information provided by the concurrent use of in situ reflection high energy electron diffraction (RHEED) and reflection electron energy loss spectroscopy (REELS). The two analytical methods were employed during growth of metal, semiconductor and superconductor thin films by molecular beam epitaxy (MBE). Surface sensitivity of the REELS spectrometer was found to be less than 1 nm for 20 KeV electrons incident at a 2 degree angle to an atomically flat film surface, agreeing with the standard electron escape depth data when adjusted incident angle. Film surface topography was found to strongly influence the REELS spectra and this was correlated with in situ RHEED patterns and ex situ analysis by comparison with atomic force microscopy (AFM). It was observed in all the experimental results that from very smooth films the plasmon peak maxima did not fall at the predicted surface plasmon values but at slightly higher energies, even for nearly atomically flat films. This suggested the REELS plasmon loss spectra are always a combination of surface and bulk plasmon losses. The resulting summation of these two types of losses shifted the peak to below the bulk plasmon value but held its minimum to a higher energy than the pure surface plasmon value. Curve fitting supported this conclusion.

This thesis focuses on the theoretical work done to determine thermodynamic properties of a chalcopyrite thin-film material for use as a photovoltaic material in a tandem device. The material of main focus here is ZnGeAs2, which was chosen for the relative abundance of constituents, favorable photovoltaic properties, and good lattice matching with ZnSnP2, the other component in this tandem device. This work is divided into two main chapters, which will cover: calculations and method to determine the formation energy and abundance of native point defects, and a model to calculate the vapor pressure over a ternary material from first-principles. The purpose of this work is to guide experimental work being done in tandem to synthesize ZnGeAs2 in thin-film form with high enough quality such that it can be used as a photovoltaic. Since properties of photovoltaic depend greatly on defect concentrations and film quality, a theoretical understanding of how laboratory conditions affect these properties is very valuable. The work done here is from first-principles and utilizes density functional theory using the local density approximation. Results from the native point defect study show that the zinc vacancy (VZn) and the germanium antisite (GeZn) are the more prominent defects; which most likely produce non-stoichiometric films. The vapor pressure model for a ternary system is validated using known vapor pressure for monatomic and binary test systems. With a valid ternary system vapor pressure model, results show there is a kinetic barrier to decomposition for ZnGeAs2.

The challenging search for clean, reliable and environmentally friendly energy sources has fueled increased research in thermoelectric materials, which are capable of recovering waste heat. Among the state-of-the-art thermoelectric materials β-Zn4Sb3 is outstanding because of its ultra-low glass-like thermal conductivity. Attempts to explore ternary phases in the Zn-Sb-In system resulted in the discovery of the new intermetallic compounds, stable Zn5Sb4In2-δ (δ=0.15) and metastable Zn9Sb6In2. Millimeter-sized crystals were grown from molten metal fluxes, where indium metal was employed as a reactive flux medium.Zn5Sb4In2-δ and Zn9Sb6In2 crystallize in new structure types featuring complex framework and the presence of structural disorder (defects and split atomic positions). The structure and phase relations between ternary Zn5Sb4In2-δ, Zn9Sb6In2 and binary Zn4Sb3 are discussed. To establish and understand structure-property relationships, thermoelectric properties measurements were carried out. The measurements suggested that Zn5Sb4In2-δ and Zn9Sb6In2 are narrow band gap semiconductors, similar to β-Zn4Sb3. Also, the peculiar low thermal conductivity of Zn4Sb3 (1 W/mK) is preserved. In the investigated temperature range 10 to 350 K Zn5Sb4In2-δ displays higher thermoelectric figure of merits than Zn4Sb3, indicating a potential significance in thermoelectric applications. Finally, the glass-like thermal conductivities of binary and ternary antimonides with complex structures are compared and the mechanism behind their low thermal conductivities is briefly discussed.

The object of this body of work is to study the properties and suitability of zinc oxide thin films with a view to engineering them for optoelectronics applications, making them a cheap and effective alternative to indium tin oxide (ITO), the most used transparent conducting oxides in the industry. Initially, a study was undertaken to examine the behavior of silver contacts to ZnO and ITO during thermal processing, a step frequently used in materials processing in optoelectronics. The second study involved an attempt to improve the conductivity of ZnO films by inserting a thin copper layer between two ZnO layers. The Hall resistivity of the films was as low as 6.9×10-5 -cm with a carrier concentration of 1.2×1022 cm-3 at the optimum copper layer thickness. The physics of conduction in the films has been examined. In order to improve the average visible transmittance, we replaced the copper layer with gold. The films were then found to undergo a seven orders of magnitude drop in effective resistivity from 200 -cm to 5.2×10-5 -cm The films have an average transmittance between 75% and 85% depending upon the gold thickness, and a peak transmittance of up to 93%. The best Haacke figure of merit was 15.1×10-3 . Finally, to test the multilayer transparent electrodes on a device, ZnO/Au/ZnO (ZAZ) electrodes were evaluated as transparent electrodes for organic light-emitting devices (OLEDs). The electrodes exhibited substantially enhanced conductivity (about 8×10-5 -cm) over conventional indium tin oxide (ITO) electrodes (about 3.2×10-5 -cm). OLEDs fabricated with the ZAZ electrodes showed reduced leakage compared to control OLEDs on ITO and reduced ohmic losses at high current densities. At a luminance of 25000 cd/m2, the lum/W efficiency of the ZAZ electrode based device improved by 5% compared to the device on ITO. A normalized intensity graph of the colour output from the green OLEDs shows that ZAZ electrodes allow for a broader spectral output in the green wavelength region of peak photopic sensitivity compared to ITO. The results have implications for electrode choice in display technology.