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- All Subjects: Materials Science
- Creators: Newman, Nathan
- Resource Type: Text
Description
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.
ContributorsWu, Yang (Author) / Häussermann, Ulrich (Thesis advisor) / Seo, Dong (Committee member) / Petuskey, William T (Committee member) / Newman, Nathan (Committee member) / Arizona State University (Publisher)
Created2011
Description
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.
ContributorsTucker, Jon R (Author) / Van Schilfgaarde, Mark (Thesis advisor) / Newman, Nathan (Committee member) / Adams, James (Committee member) / Arizona State University (Publisher)
Created2011
Description
In this research, our goal was to fabricate Josephson junctions that can be stably processed at 300°C or higher. With the purpose of integrating Josephson junction fabrication with the current semiconductor circuit fabrication process, back-end process temperatures (>350 °C) will be a key for producing large scale junction circuits reliably, which requires the junctions to be more thermally stable than current Nb/Al-AlOx/Nb junctions. Based on thermodynamics, Hf was chosen to produce thermally stable Nb/Hf-HfOx/Nb superconductor tunnel Josephson junctions that can be grown or processed at elevated temperatures. Also elevated synthesis temperatures improve the structural and electrical properties of Nb electrode layers that could potentially improve junction device performance. The refractory nature of Hf, HfO2 and Nb allow for the formation of flat, abrupt and thermally-stable interfaces. But the current Al-based barrier will have problems when using with high-temperature grown and high-quality Nb. So our work is aimed at using Nb grown at elevated temperatures to fabricate thermally stable Josephson tunnel junctions. As a junction barrier metal, Hf was studied and compared with the traditional Al-barrier material. We have proved that Hf-HfOx is a good barrier candidate for high-temperature synthesized Josephson junction. Hf deposited at 500 °C on Nb forms flat and chemically abrupt interfaces. Nb/Hf-HfOx/Nb Josephson junctions were synthesized, fabricated and characterized with different oxidizing conditions. The results of materials characterization and junction electrical measurements are reported and analyzed. We have improved the annealing stability of Nb junctions and also used high-quality Nb grown at 500 °C as the bottom electrode successfully. Adding a buffer layer or multiple oxidation steps improves the annealing stability of Josephson junctions. We also have attempted to use the Atomic Layer Deposition (ALD) method for the growth of Hf oxide as the junction barrier and got tunneling results.
ContributorsHuang, Mengchu, 1987- (Author) / Newman, Nathan (Thesis advisor) / Rowell, John M. (Committee member) / Singh, Rakesh K. (Committee member) / Chamberlin, Ralph (Committee member) / Wang, Robert (Committee member) / Arizona State University (Publisher)
Created2013
Description
Integrated photonics requires high gain optical materials in the telecom wavelength range for optical amplifiers and coherent light sources. Erbium (Er) containing materials are ideal candidates due to the 1.5 μm emission from Er3+ ions. However, the Er density in typical Er-doped materials is less than 1 x 1020 cm-3, thus limiting the maximum optical gain to a few dB/cm, too small to be useful for integrated photonics applications. Er compounds could potentially solve this problem since they contain much higher Er density. So far the existing Er compounds suffer from short lifetime and strong upconversion effects, mainly due to poor quality of crystals produced by various methods of thin film growth and deposition. This dissertation explores a new Er compound: erbium chloride silicate (ECS, Er3(SiO4)2Cl ) in the nanowire form, which facilitates the growth of high quality single crystals. Growth methods for such single crystal ECS nanowires have been established. Various structural and optical characterizations have been carried out. The high crystal quality of ECS material leads to a long lifetime of the first excited state of Er3+ ions up to 1 ms at Er density higher than 1022 cm-3. This Er lifetime-density product was found to be the largest among all Er containing materials. A unique integrating sphere method was developed to measure the absorption cross section of ECS nanowires from 440 to 1580 nm. Pump-probe experiments demonstrated a 644 dB/cm signal enhancement from a single ECS wire. It was estimated that such large signal enhancement can overcome the absorption to result in a net material gain, but not sufficient to compensate waveguide propagation loss. In order to suppress the upconversion process in ECS, Ytterbium (Yb) and Yttrium (Y) ions are introduced as substituent ions of Er in the ECS crystal structure to reduce Er density. While the addition of Yb ions only partially succeeded, erbium yttrium chloride silicate (EYCS) with controllable Er density was synthesized successfully. EYCS with 30 at. % Er was found to be the best. It shows the strongest PL emission at 1.5 μm, and thus can be potentially used as a high gain material.
ContributorsYin, Leijun (Author) / Ning, Cun-Zheng (Thesis advisor) / Chamberlin, Ralph (Committee member) / Yu, Hongbin (Committee member) / Menéndez, Jose (Committee member) / Ponce, Fernando (Committee member) / Arizona State University (Publisher)
Created2013
Description
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.
ContributorsLiu, Lingtao (Author) / Newman, Nathan (Thesis advisor) / Marzke, Robert (Committee member) / Chamberlin, Ralph (Committee member) / Arizona State University (Publisher)
Created2013
Description
I studied the properties of novel Co2FeAl0.5Si0.5 (CFAS), ZnGeAs2, and FeS2 (pyrite) thin films for microelectronic applications ranging from spintronic to photovoltaic. CFAS is a half metal with theoretical spin polarization of 100%. I investigated its potential as a spin injector, for spintronic applications, by studying the critical steps involved in the injection of spin polarized electron populations from tunnel junctions containing CFAS electrodes. Epitaxial CFAS thin films with L21 structure and saturation magnetizations of over 1200 emu/cm3 were produced by optimization of the sputtering growth conditions. Point contact Andreev reflection measurements show that the spin polarization at the CFAS electrode surface exceeds 70%. Analyses of the electrical properties of tunnel junctions with a superconducting Pb counter-electrode indicate that transport through native Al oxide barriers is mostly from direct tunneling, while that through the native CFAS oxide barriers is not. ZnGeAs2 is a semiconductor comprised of only inexpensive and earth-abundant elements. The electronic structure and defect properties are similar in many ways to GaAs. Thus, in theory, efficient solar cells could be made with ZnGeAs2 if similar quality material to that of GaAs could be produced. To understand the thermochemistry and determine the rate limiting steps of ZnGeAs2 thin-film synthesis, the (a) thermal decomposition rate and (b) elemental composition and deposition rate of films were measured. It is concluded that the ZnGeAs2 thin film synthesis is a metastable process with an activation energy of 1.08±0.05 eV for the kinetically-limited decomposition rate and an evaporation coefficient of ~10-3. The thermochemical analysis presented here can be used to predict optimal conditions of ZnGeAs2 physical vapor deposition and thermal processing. Pyrite (FeS2) is another semiconductor that has tremendous potential for use in photovoltaic applications if high quality materials could be made. Here, I present the layer-by-layer growth of single-phase pyrite thin-films on heated substrates using sequential evaporation of Fe under high-vacuum followed by sulfidation at S pressures between 1 mTorr and 1 Torr. High-resolution transmission electron microscopy reveals high-quality, defect-free pyrite grains were produces by this method. It is demonstrated that epitaxial pyrite layer was produced on natural pyrite substrates with this method.
ContributorsVahidi, Mahmoud (Author) / Newman, Nathan (Thesis advisor) / Alford, Terry (Committee member) / Singh, Rakesh (Committee member) / Chen, Tingyong (Committee member) / Arizona State University (Publisher)
Created2013
Description
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.
ContributorsLi, You (Author) / Newman, Nathan (Thesis advisor) / Alford, Terry (Committee member) / Singh, Rakesh (Committee member) / Arizona State University (Publisher)
Created2013
Description
The research described in this dissertation has involved the use of transmission electron microcopy (TEM) to characterize the structural properties of II-VI and III-V compound semiconductor heterostructures and superlattices. The microstructure of thick ZnTe epilayers (~2.4 µm) grown by molecular beam epitaxy (MBE) under virtually identical conditions on GaSb, InAs, InP and GaAs (100) substrates were compared using TEM. High-resolution electron micrographs revealed a highly coherent interface for the ZnTe/GaSb sample, and showed extensive areas with well-separated interfacial misfit dislocations for the ZnTe/InAs sample. Lomer edge dislocations and 60o dislocations were commonly observed at the interfaces of the ZnTe/InP and ZnTe/GaAs samples. The amount of residual strain at the interfaces was estimated to be 0.01% for the ZnTe/InP sample and -0.09% for the ZnTe/GaAs sample. Strong PL spectra for all ZnTe samples were observed from 80 to 300 K. High quality GaSb grown by MBE on ZnTe/GaSb (001) virtual substrates with a temperature ramp at the beginning of the GaSb growth has been demonstrated. High-resolution X-ray diffraction (XRD) showed clear Pendellösung thickness fringes from both GaSb and ZnTe epilayers. Cross-section TEM images showed excellent crystallinity and smooth morphology for both ZnTe/GaSb and GaSb/ZnTe interfaces. Plan-view TEM image revealed the presence of Lomer dislocations at the interfaces and threading dislocations in the top GaSb layer. The defect density was estimated to be ~1 x107/cm2. The PL spectra showed improved optical properties when using the GaSb transition layer grown on ZnTe with a temperature ramp. The structural properties of strain-balanced InAs/InAs1-xSbx SLs grown on GaSb (001) substrates by metalorganic chemical vapor deposition (MOCVD) and MBE, have been studied using XRD and TEM. Excellent structural quality of the InAs/InAs1-xSbx SLs grown by MOCVD has been demonstrated. Well-defined ordered-alloy structures within individual InAs1-xSbx layers were observed for samples grown by modulated MBE. However, the ordering disappeared when defects propagating through the SL layers appeared during growth. For samples grown by conventional MBE, high-resolution images revealed that interfaces for InAs1-xSbx grown on InAs layers were sharper than for InAs grown on InAs1-xSbx layers, most likely due to a Sb surfactant segregation effect.
ContributorsOuyang, Lu (Author) / Smith, David J. (Thesis advisor) / McCartney, Martha (Committee member) / Ponce, Fernando (Committee member) / Chamberlin, Ralph (Committee member) / Menéndez, Jose (Committee member) / Arizona State University (Publisher)
Created2012
Description
Soft magnetic alloys play a significant role for magnetic recording applications and highly sensitivity magnetic field sensors. In order to sustain the magnetic areal density growth, development of new synthesis techniques and materials is necessary. In this work, the effect of oxygen incorporation during electrodeposition of CoFe alloys on magnetic properties, magnetoresistance and structural properties has been studied. Understanding the magnetic properties often required knowledge of oxygen distribution and structural properties of the grown films. Transmission electron microscopy (TEM) was a powerful tool in this study to correlate the oxygen-distribution nanostructure to the magnetic properties of deposited films. Off-axis electron holography in TEM was used to measure magnetic domain wall width in the deposited films. Elemental depth profiles of Fe, Co, O were investigated by secondary ion mass spectroscopy (SIMS). Magnetic properties have been determined by superconducting quantum interference device (SQUID) measurements. Oxygen content in the CoFe deposited films was controlled by electrolyte composition. Films were deposited on Si 100 substrates and on other substrates such as Cu and Al. However, a good film quality was achieved on Si substrate. Electron energy loss and x-ray spectroscopies showed that the low oxygen films contained intragranular Fe2+ oxide (FeO) particles and that the high oxygen films contained intergranular Fe3+ (Fe2O3) along grain boundaries. The films with oxide present at the grain boundary had significantly increased coercivity, magnetoresistance and reduced saturation magnetization relative to the lower oxygen content films with intragranular oxide. The differences in magnetic properties between low oxygen and high oxygen concentration films were attributed to stronger mobile domain wall interactions with the grain boundary oxide layers. The very high magnetoresistance values were achieved for magnetic devices with nanocontact dimension < 100 nm and oxide incorporation in this nanoconfined geometry. The content of oxide phase in nanocontact was controlled by concentration of the Fe3+ ions in the electrodeposition solution. Magnetic device integrity was improved by varying amount of additive into plating solution. These results indicated that electrodeposited CoFe nanocontact is a novel class of materials with large application for magnetic field sensors.
ContributorsElhalawaty, Shereen (Author) / Carpenter, Ray (Thesis advisor) / Chamberlin, Ralph (Committee member) / McCartney, Martha (Committee member) / Alford, Terry (Committee member) / Arizona State University (Publisher)
Created2012
Description
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.
ContributorsStrawbridge, Brett William (Author) / Newman, Nathan (Thesis advisor) / Chamberlin, Ralph (Committee member) / Rizzo, Nicholas (Committee member) / Arizona State University (Publisher)
Created2012