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Next, the growth of selenide heterostructures was explored. Specifically, molecular beam epitaxy was utilized to grow In2Se3 and Bi2Se3 films on h-BN, highly oriented pyrolytic graphite and Si(111) substrates. Growth optimizations of In2Se3 and Bi2Se3 films were carried out by systematically varying the growth parameters. While the growth of these films was demonstrated on h-BN and HOPG surface, the majority of the effort was focused on growth on Si(111). Atomically flat terraces that extended laterally for several hundred nm, which were separated by single quintuple layer high steps characterized surface of the best In2Se3 films grown on Si(111). These In2Se3 films were suitable for subsequent high quality epitaxy of Bi2Se3 .
The last part of this dissertation was focused on a recently initiated and ongoing study of graphene growth on liquid metal surfaces. The initial part of the study comprised a successful modification of an existing growth system to accommodate graphene synthesis and process development for reproducible graphene growth. Graphene was grown on Cu, Au and AuCu alloys at varioua conditions. Preliminary results showed triangular features on the liquid part of the Cu metal surface. For Au, and AuCu alloys, hexagonal features were noticed both on the solid and liquid parts.
First, the surface electronic state configuration was examined with regards to the polarization bound 1013 charges/cm2 that increases with aluminum content. This large bound charge requires compensation either externally by surface states or internally by the space charge regions as relates to band bending. In this work, band bending was measured after different surface treatments of GaN and AlGaN to determine the effects of specific surface states on the electronic state configuration. Results showed oxygen-terminated N-face GaN, Ga-face GaN, and Ga-face Al0.25Ga0.75N surface were characterized by similar band bending regardless of the polarization bound charge, suggesting a Fermi level pinning state ~0.4-0.8 eV below the conduction band minimum. On oxygen-free Ga-face GaN, Al0.15Ga0.85N, Al0.25Ga0.75N, and Al0.35Ga0.65N, band bending increased slightly with aluminum content and thus did not exhibit the same pinning behavior; however, there was still significant compensating charge on these surfaces (~1013 charges/cm2). This charge is likely related to nitrogen vacancies and/or gallium dangling bonds.
In addition, this wozrk investigated the interface electronic state configuration of dielectric/GaN and AlGaN interfaces with regards to deposition conditions and aluminum content. Specifically, oxygen plasma-enhanced atomic layer deposited (PEALD) was used to deposit SiO2. Growth temperature was shown to influence the film quality, where room temperature deposition produced the highest quality films in terms of electrical breakdown. In addition, the valence band offsets (VBOs) appeared to decrease with the deposition temperature, which likely related to an electric field across the Ga2O3 interfacial layer. VBOs were also determined with respect to aluminum content at the PEALD-SiO2/AlxGa1-xN interface, giving 3.0, 2.9, 2.9, and 2.8 eV for 0%, 15%, 25%, and 35% aluminum content, respectively—with corresponding conduction band offsets of 2.5, 2.2, 1.9, and 1.8 eV. This suggests the largest difference manifests in the conduction band, which is in agreement with the charge neutrality level model.
Various deposition methods, both physical and chemical, were used to functionalize the ZnO NWs with metal or alloy nanoparticles (NPs) for catalytic transformations of important molecules which are relevant to energy and environment. Cu and PdZn NPs were epitaxially grown on ZnO NWs to make them resistant to sintering at elevated temperatures and thus improved the stability of such catalytic systems for methanol steam reforming (MSR) to produce hydrogen. A series of Pd/ZnO catalysts with different Pd loadings were synthesized and tested for MSR reaction. The CO selectivity was found to be strongly dependent on the size of the Pd: Both PdZn alloy and single Pd atoms yield low CO selectivity while Pd clusters give the highest CO selectivity.
By dispersing single Pd atoms onto ZnO NWs, Pd1/ZnO single-atom catalysts (SACs) was synthesized and their catalytic performance was evaluated for selected catalytic reactions. The experimental results show that the Pd1/ZnO SAC is active for CO oxidation and MSR but is not desirable other reactions. We further synthesized ZnO NWs supported noble metal (M1/ZnO; M=Rh, Pd, Pt, Ir) SACs and studied their catalytic performances for CO oxidation. The catalytic test data shows that all the fabricated noble metal SACs are active for CO oxidation but their activity are significantly different. Structure-performance relationships were investigated.
The proposed thermal model is then applied to a novel $\Pi$-gate architecture which has been suggested to reduce hot electron generation in the device, compared to the conventional T-gate. Additionally, small signal ac simulations are performed for the determination of cutoff frequencies using the thermal model as well.
Finally, further extensions of the CMC algorithm used in this work are discussed, including 1) higher-order moments of the phonon BTE, 2) coupling to phonon Monte Carlo simulations, and 3) application to other large-bandgap, and therefore high-power, materials such as diamond.
Novel hydride chemistries are employed to deposit light-emitting Ge1-y Snyalloys with y ≤ 0.1 by Ultra-High Vacuum Chemical Vapor Deposition (UHV-CVD) on Ge-buffered Si wafers. The properties of the resultant materials are systematically compared with similar alloys grown directly on Si wafers. The fundamental difference between the two systems is a fivefold (and higher) decrease in lattice mismatch between film and virtual substrate, allowing direct integration of bulk-like crystals with planar surfaces and relatively low dislocation densities. For y ≤ 0.06, the CVD precursors used were digermane Ge2H6 and deuterated stannane SnD4. For y ≥ 0.06, the Ge precursor was changed to trigermane Ge3H8, whose higher reactivity enabled the fabrication of supersaturated samples with the target film parameters. In all cases, the Ge wafers were produced using tetragermane Ge4H10 as the Ge source. The photoluminescence intensity from Ge1-y Sny /Ge films is expected to increase relative to Ge1-y Sny /Si due to the less defected interface with the virtual substrate. However, while Ge1-y Sny /Si films are largely relaxed, a significant amount of compressive strain may be present in the Ge1-y Sny /Ge case. This compressive strain can reduce the emission intensity by increasing the separation between the direct and indirect edges. In this context, it is shown here that the proposed CVD approach to Ge1-y Sny /Ge makes it possible to approach film thicknesses of about 1 μm, for which the strain is mostly relaxed and the photoluminescence intensity increases by one order of magnitude relative to Ge1-y Sny /Si films. The observed strain relaxation is shown to be consistent with predictions from strain-relaxation models first developed for the Si1-x Gex /Si system. The defect structure and atomic distributions in the films are studied in detail using advanced electron-microscopy techniques, including aberration corrected STEM imaging and EELS mapping of the average diamond–cubic lattice.
In this paper, we report on the highly conductive layer formed at the crystalline γ-alumina/SrTiO3 interface, which is attributed to oxygen vacancies. We describe the structure of thin γ-alumina layers deposited by molecular beam epitaxy on SrTiO3 (001) at growth temperatures in the range of 400–800 °C, as determined by reflection-high-energy electron diffraction, x-ray diffraction, and high-resolution electron microscopy. In situ x-ray photoelectron spectroscopy was used to confirm the presence of the oxygen-deficient layer. Electrical characterization indicates sheet carrier densities of ∼1013 cm−2 at room temperature for the sample deposited at 700 °C, with a maximum electron Hall mobility of 3100 cm2V-1s-1 at 3.2 K and room temperature mobility of 22 cm2V-1s-1. Annealing in oxygen is found to reduce the carrier density and turn a conductive sample into an insulator.
The development of non-volatile logic through direct coupling of spontaneous ferroelectric polarization with semiconductor charge carriers is nontrivial, with many issues, including epitaxial ferroelectric growth, demonstration of ferroelectric switching and measurable semiconductor modulation. Here we report a true ferroelectric field effect—carrier density modulation in an underlying Ge(001) substrate by switching of the ferroelectric polarization in epitaxial c-axis-oriented BaTiO3 grown by molecular beam epitaxy. Using the density functional theory, we demonstrate that switching of BaTiO3 polarization results in a large electric potential change in Ge. Aberration-corrected electron microscopy confirms BaTiO3 tetragonality and the absence of any low-permittivity interlayer at the interface with Ge. The non-volatile, switchable nature of the single-domain out-of-plane ferroelectric polarization of BaTiO3 is confirmed using piezoelectric force microscopy. The effect of the polarization switching on the conductivity of the underlying Ge is measured using microwave impedance microscopy, clearly demonstrating a ferroelectric field effect.
We report a study of the magnetic domain structure of nanocrystalline thin films of nickel-zinc ferrite. The ferrite films were synthesized using aqueous spin-spray coating at low temperature (∼90 °C) and showed high complex permeability in the GHz range. Electron microscopy and microanalysis revealed that the films consisted of columnar grains with uniform chemical composition. Off-axis electron holography combined with magnetic force microscopy indicated a multi-grain domain structure with in-plane magnetization. The correlation between the magnetic domain morphology and crystal structure is briefly discussed.
The current work explores the crystalline perovskite oxide, strontium hafnate, as a potential high-k gate dielectric for Ge-based transistors. SrHfO3 (SHO) is grown directly on Ge by atomic layer deposition and becomes crystalline with epitaxial registry after post-deposition vacuum annealing at ∼700 °C for 5 min. The 2 × 1 reconstructed, clean Ge (001) surface is a necessary template to achieve crystalline films upon annealing. The SHO films exhibit excellent crystallinity, as shown by x-ray diffraction and transmission electron microscopy. The SHO films have favorable electronic properties for consideration as a high-k gate dielectric on Ge, with satisfactory band offsets (>2 eV), low leakage current (<10-5 A/cm2 at an applied field of 1 MV/cm) at an equivalent oxide thickness of 1 nm, and a reasonable dielectric constant (k ∼ 18). The interface trap density (Dit) is estimated to be as low as ∼2 × 1012 cm-2 eV-1 under the current growth and anneal conditions. Some interfacial reaction is observed between SHO and Ge at temperatures above ∼650 °C, which may contribute to increased Dit value. This study confirms the potential for crystalline oxides grown directly on Ge by atomic layer deposition for advanced electronic applications.
The unicellular microalga Haematococcus pluvialis has emerged as a promising biomass feedstock for the ketocarotenoid astaxanthin and neutral lipid triacylglycerol. Motile flagellates, resting palmella cells, and cysts are the major life cycle stages of H. pluvialis. Fast-growing motile cells are usually used to induce astaxanthin and triacylglycerol biosynthesis under stress conditions (high light or nutrient starvation); however, productivity of biomass and bioproducts are compromised due to the susceptibility of motile cells to stress. This study revealed that the Photosystem II (PSII) reaction center D1 protein, the manganese-stabilizing protein PsbO, and several major membrane glycerolipids (particularly for chloroplast membrane lipids monogalactosyldiacylglycerol and phosphatidylglycerol), decreased dramatically in motile cells under high light (HL). In contrast, palmella cells, which are transformed from motile cells after an extended period of time under favorable growth conditions, have developed multiple protective mechanisms - including reduction in chloroplast membrane lipids content, downplay of linear photosynthetic electron transport, and activating nonphotochemical quenching mechanisms - while accumulating triacylglycerol. Consequently, the membrane lipids and PSII proteins (D1 and PsbO) remained relatively stable in palmella cells subjected to HL. Introducing palmella instead of motile cells to stress conditions may greatly increase astaxanthin and lipid production in H. pluvialis culture.