An electrical current with high spin polarization is desirable for the performance of novel spintronics devices, such as magnetic tunnel junction and giant magnetoresistance devices. The generation of spin polarized current can be from ferromagnetic materials or triplet superconductors.

Anomalous Hall effect (AHE) is an effective way to study the properties of magnetic structures. The scattering of electrons by the magnetic moments affects the change of resistance, which can be used to detect the magnetization. In this dissertation, AHE is used to study the perpendicular magnetic anisotropy (PMA) structures, including Co/Pt and Ta/CoFeB/MgO.

Domain walls exist in all ferromagnetic materials. This dissertation studies the domain wall movement in the Ta/CoFeB/MgO structure. A single domain is observed by measuring the anomalous Hall effect. On the other hand, a zero Hall step is successfully observed in a single layer of magnetic material for the first time, which can be used to fabricate advanced domain wall spintronics devices.

Besides the normal ferromagnetic material, the generation of spin polarized current in superconductor is also important for Spintronics. The electrons in superconductors form Cooper pairs. In this dissertation, Andreev Reflection Spectroscopy (ARS) is used to study the spin configuration in Cooper pairs.

Generally, ferromagnetism and superconductivity can not co-exist. In this dissertation, the Bi/Ni bilayer structure has been studied with ARS, and the measurement results show a triplet superconductivity below 4K. The appearance of superconductivity is believed to be attributed to the Bi-Ni interface, and the triplet Cooper pair makes it a promising candidate in superconducting spintronics.

Besides, a Bi3Ni single crystal is also studied with ARS. The measurements show a singlet superconductivity in this material, which further proves the importance of the Bi/Ni interface to achieve triplet superconductivity.

Finally, ARS is also used to study NbSe2 monolayer, a 2D superconductor. The monolayer is verified by the measurements of critical temperature and critical field, which are different from the values of multilayer or bulk. Andreev reflection results show that NbSe2 monolayer is a singlet superconductor and there is no node exist in the superconducting gap for a in plane magnetic field up to 58 kOe.

My research has been focusing on the innovations of material and structure designs, and the development of fabrication processes of novel nanoelectronics devices.

My first project addresses the long-existing challenge of implantable neural probes, where high rigidity and high flexibility for the probe need to be satisfied at the same time. Two types of probes that can be used out of the box have been demonstrated, including (1) a compact probe that spontaneously forms three-dimensional bend-up devices only after implantation, and (2) an ultra-flexible probe as thin as 2 µm attached to a small silicon shaft that can be accurately delivered into the tissue and then get fully released in situ without altering its shape and position as the support is fully retracted. This work provides a general strategy to prepare ultra-small and flexible implantable probes that allow high insertion accuracy and minimal surgical damages with best biocompatibility.

My second project focuses on the injection and characterization of carrier spins in single crystal diamond based nanoscale devices. The conventional diamond-based quantum information process that exploits nitrogen vacancy centers faces a major barrier of large scale communication. Electron/hole spin in diamond devices, on the other hand, could also be a good candidate for quantum computing due to the very small spin-orbit coupling and great coherent transport length of spin. To date, there has been no demonstration of carrier spin transport in diamond. In this work, I try to answer this fundamental question of how to inject and characterize electron spins in Boron doped diamond. Nanoscale diamond devices have been fabricated to investigate this question, including Hall bar device for material characterization, and lateral spin valve for injecting spin-polarized current into a mesoscopic diamond bar and detecting induced pure spin current. The preliminary results show signatures of spin transport in heavily doped diamond films.

Looking into the future, the knowledge we obtained in these two projects, including the strategy to integrate thin-film nanoelectronics devices on a flexible bio-probe configuration, and how to build spintronic devices with diamond structures, could be unified in the exploration of spin-based sensors in biological systems.

Photocatalytic water splitting has been proposed as a promising way of generating carbon-neutral fuels from sunlight and water. In one approach, water decomposition is enabled by the use of functionalized nano-particulate photocatalyst composites. The atomic structures of the photocatalysts dictate their electronic and photonic structures, which are controlled by synthesis methods and may alter under reaction conditions. Characterizing these structures, especially the ones associated with photocatalysts’ surfaces, is essential because they determine the efficiencies of various reaction steps involved in photocatalytic water splitting. Due to its superior spatial resolution, (scanning) transmission electron microscopy (STEM/TEM), which includes various imaging and spectroscopic techniques, is a suitable tool for probing materials’ local atomic, electronic and optical structures. In this work, techniques specific for the study of photocatalysts are developed using model systems.

Nano-level structure-reactivity relationships as well as deactivation mechanisms of Ni core-NiO shell co-catalysts loaded on Ta2O5 particles are studied using an aberration-corrected TEM. It is revealed that nanometer changes in the shell thickness lead to significant changes in the H2 production. Also, deactivation of this system is found to be related to a photo-driven process resulting in the loss of the Ni core.

In addition, a special form of monochromated electron energy-loss spectroscopy (EELS), the so-called aloof beam EELS, is used to probe surface electronic states as well as light-particle interactions from model oxide nanoparticles. Surface states associated with hydrate species are analyzed using spectral simulations based on a dielectric theory and a density of states model. Geometry-induced optical-frequency resonant modes are excited using fast electrons in catalytically relevant oxides. Combing the spectral features detected in experiments with classical electrodynamics simulations, the underlying physics involved in this excitation process and the various influencing factors of the modes are investigated.

Finally, an in situ light illumination system is developed for an aberration-corrected environmental TEM to enable direct observation of atomic structural transformations of model photocatalysts while they are exposed to near reaction conditions.

In recent years, there has been increased interest in the Indium Gallium Nitride (InGaN) material system for photovoltaic (PV) applications. The InGaN alloy system has demonstrated high performance for high frequency power devices, as well as for optical light emitters. This material system is also promising for photovoltaic applications due to broad range of bandgaps of InxGa1-xN alloys from 0.65 eV (InN) to 3.42 eV (GaN), which covers most of the electromagnetic spectrum from ultraviolet to infrared wavelengths. InGaN’s high absorption coefficient, radiation resistance and thermal stability (operating with temperature > 450 ℃) makes it a suitable PV candidate for hybrid concentrating solar thermal systems as well as other high temperature applications. This work proposed a high efficiency InGaN-based 2J tandem cell for high temperature (450 ℃) and concentration (200 X) hybrid concentrated solar thermal (CSP) application via numerical simulation. In order to address the polarization and band-offset issues for GaN/InGaN hetero-solar cells, band-engineering techniques are adopted and a simple interlayer is proposed at the hetero-interface rather than an Indium composition grading layer which is not practical in fabrication. The base absorber thickness and doping has been optimized for 1J cell performance and current matching has been achieved for 2J tandem cell design. The simulations also suggest that the issue of crystalline quality (i.e. short SRH lifetime) of the nitride material system to date is a crucial factor limiting the performance of the designed 2J cell at high temperature. Three pathways to achieve ~25% efficiency have been proposed under 450 ℃ and 200 X. An anti-reflection coating (ARC) for the InGaN solar cell optical management has been designed. Finally, effective mobility model for quantum well solar cells has been developed for efficient quasi-bulk simulation.

Thermionic energy conversion, a process that allows direct transformation of thermal to electrical energy, presents a means of efficient electrical power generation as the hot and cold side of the corresponding heat engine are separated by a vacuum gap. Conversion efficiencies approaching those of the Carnot cycle are possible if material parameters of the active elements at the converter, i.e., electron emitter or cathode and collector or anode, are optimized for operation in the desired temperature range.

These parameters can be defined through the law of Richardson–Dushman that quantifies the ability of a material to release an electron current at a certain temperature as a function of the emission barrier or work function and the emission or Richardson constant. Engineering materials to defined parameter values presents the key challenge in constructing practical thermionic converters. The elevated temperature regime of operation presents a constraint that eliminates most semiconductors and identifies diamond, a wide band-gap semiconductor, as a suitable thermionic material through its unique material properties. For its surface, a configuration can be established, the negative electron affinity, that shifts the vacuum level below the conduction band minimum eliminating the surface barrier for electron emission.

In addition, its ability to accept impurities as donor states allows materials engineering to control the work function and the emission constant. Single-crystal diamond electrodes with nitrogen levels at 1.7 eV and phosphorus levels at 0.6 eV were prepared by plasma-enhanced chemical vapor deposition where the work function was controlled from 2.88 to 0.67 eV, one of the lowest thermionic work functions reported. This work function range was achieved through control of the doping concentration where a relation to the amount of band bending emerged. Upward band bending that contributed to the work function was attributed to surface states where lower doped homoepitaxial films exhibited a surface state density of ∼3 × 10[superscript 11] cm[superscript −2]. With these optimized doped diamond electrodes, highly efficient thermionic converters are feasible with a Schottky barrier at the diamond collector contact mitigated through operation at elevated temperatures.

This project details the learning of processes in nanofabrication and sensor detection fields. We sought to apply this knowledge to develop a processing procedure to fabricate sensors used to detect high energy protons.  We seek to create such a sensor to be applied to aid Mayo Clinic’s Proton Beam Therapy center for cancer treatment through providing beam detection measurements. Developed plans would allow for proton beam detectors to be able to measure beam intensity and direction which would allow for more accurate beam treatments. Current detectors require much calibration and solid state detectors can’t withstand the high-energy exposure of the proton beam for long durations. By fabricating pixelated diamond sensors we expect to produce sensitive beam readings, while extending detector length time due to diamonds durable crystalline lattice. We report processing procedures for simple 2-3 contact detectors as well as more complex multi-contact pixelated sensors used for spatial resolution of the beam. Testing of simple sensors is additionally reported with successful radioactive source detection.

Integration of dielectrics with graphene is essential to the fulfillment of graphene based electronic applications. While many dielectric deposition techniques exist, plasma enhanced atomic layer deposition (PEALD) is emerging as a technique to deposit ultrathin dielectric films with superior densities and interfaces. However, the degree to which PEALD on graphene can be achieved without plasma-induced graphene deterioration is not well understood. In this work, we investigate a range of plasma conditions across a single sample, characterizing both oxide growth and graphene deterioration using spectroscopic analysis and atomic force microscopy. Investigation of graphene and film quality produced by these conditions yields insight into plasma effects. Using a specially designed sample configuration, we achieve ultrathin (< 1 nm) aluminum oxide films atop graphene.

Diamond is considered as an ideal material for high field and high power devices due to its high breakdown field, high lightly doped carrier mobility, and high thermal conductivity. The modeling and simulation of diamond devices are therefore important to predict the performances of diamond based devices. In this context, we use Silvaco[superscript ®] Atlas, a drift-diffusion based commercial software, to model diamond based power devices. The models used in Atlas were modified to account for both variable range and nearest neighbor hopping transport in the impurity bands associated with high activation energies for boron doped and phosphorus doped diamond. The models were fit to experimentally reported resistivity data over a wide range of doping concentrations and temperatures. We compare to recent data on depleted diamond Schottky PIN diodes demonstrating low turn-on voltages and high reverse breakdown voltages, which could be useful for high power rectifying applications due to the low turn-on voltage enabling high forward current densities. Three dimensional simulations of the depleted Schottky PIN diamond devices were performed and the results are verified with experimental data at different operating temperatures.

Gallium Nitride (GaN), being a wide-bandgap semiconductor, shows its advantage over the conventional semiconductors like Silicon and Gallium Arsenide for high temperature applications, especially in the temperature range from 300°C to 600°C. Development of stable ohmic contacts to GaN with low contact resistivity has been identified as a prerequisite to the success of GaN high temperature electronics. The focus of this work was primarily derived from the requirement of an appropriate metal contacts to work with GaN-based hybrid solar cell operating at high temperature.

Alloyed Ti/Al/Ni/Au contact and non-alloyed Al/Au contact were developed to form low-resistivity contacts to n-GaN and their stability at high temperature were studied. The alloyed Ti/Al/Ni/Au contact offered a specific contact resistivity (ρc) of 6×10-6 Ω·cm2 at room temperature measured the same as the temperature increased to 400°C. No significant change in ρc was observed after the contacts being subjected to 400°C, 450°C, 500°C, 550°C, and 600°C, respectively, for at least 4 hours in air. Since several device technology prefer non-alloyed contacts Al/Au metal stack was applied to form the contacts to n-type GaN. An initial ρc of 3×10-4 Ω·cm2, measured after deposition, was observed to continuously reduce under thermal stress at 400°C, 450°C, 500°C, 550°C, and 600°C, respectively, finally stabilizing at 5×10-6 Ω·cm2. Both the alloyed and non-alloyed metal contacts showed exceptional capability of stable operation at temperature as high as 600°C in air with low resistivity ~10-6 Ω·cm2, with ρc lowering for the non-alloyed contacts with high temperatures.

The p-GaN contacts showed remarkably superior ohmic behavior at elevated temperatures. Both ρc and sheet resistance (Rsh) of p-GaN decreased by a factor of 10 as the ambient temperature increased from room temperature to 390°C. The annealed Ni/Au contact showed ρc of 2×10-3 Ω·cm2 at room temperature, reduced to 1.6×10-4 Ω·cm2 at 390°C. No degradation was observed after the contacts being subjected to 450°C in air for 48 hours. Indium Tin Oxide (ITO) contacts, which has been widely used as current spreading layer in GaN-base optoelectronic devices, measured an initial ρc [the resistivity of the ITO/p-GaN interface, since the metal/ITO ρc is negligible] of 1×10-2 Ω·cm2 at room temperature. No degradation was observed after the contact being subjected to 450°C in air for 8 hours.

Accelerated life testing (ALT) was performed to further evaluate the contacts stability at high temperatures quantitatively. The ALT results showed that the annealed Ni/Au to p-GaN contacts is more stable in nitrogen ambient, with a lifetime of 2,628 hours at 450°C which is approximately 12 times longer than that at 450°C in air.

LiNbO3 and ZnO have shown great potential for photochemical surface reactions and specific photocatalytic processes. However, the efficiency of LiNbO3 is limited due to recombination or back reactions and ZnO exhibits a chemical instability in a liquid cell. In this dissertation, both materials were coated with precise thickness of metal oxide layers to passivate the surfaces and to enhance their photocatalytic efficiency. LiNbO3 was coated with plasma enhanced atomic layer deposited (PEALD) ZnO and Al2O3, and molecular beam deposited TiO2 and VO2. On the other hand, PEALD ZnO and single crystal ZnO were passivated with PEALD SiO2 and Al2O3.

Metal oxide/LiNbO3 heterostructures were immersed in aqueous AgNO3 solutions and illuminated with ultraviolet (UV) light to form Ag nanoparticle patterns. Alternatively, Al2O3 and SiO2/ZnO heterostructures were immersed in K3PO4 buffer solutions and studied for photoelectrochemical reactions. A fundamental aspect of the heterostructures is the band alignment and band bending, which was deduced from in situ photoemission measurements.

This research has provided insight to three aspects of the heterostructures. First, the band alignment at the interface of metal oxides/LiNbO3, and Al2O3 or SiO2/ZnO were used to explain the possible charge transfer processes and the direction of carrier flow in the heterostructures. Second, the effect of metal oxide coatings on the LiNbO3 with different internal carrier concentrations was related to the surface photochemical reactions. Third is the surface passivation and degradation mechanism of Al2O3 and SiO2 on ZnO was established. The heterostructures were characterized after stability tests using atomic force microscopy (AFM), scanning electron microscopy (SEM), and cross-section transmission electron microscopy (TEM).

The results indicate that limited thicknesses of ZnO or TiO2 on polarity patterned LiNbO3 (PPLN) enhances the Ag+ photoinduced reduction process. ZnO seems more efficient than TiO2 possibly due to a higher carrier mobility. However, an increase of the ZnO thickness (≥ 4 nm) reduced the effect of the PPLN substrate on the Ag nanoparticle pattern. For the case of Al2O3 and SiO2/ZnO heterostructures, SiO2 remains intact through 1 h stability tests. Unlike SiO2, Al2O3 shows surface degradation after a short stability test of a few minutes. Thus, SiO2 provides improved passivation over Al2O3. A detailed microscopy analysis indicates the underneath ZnO photocorrodes in the SiO2/ZnO samples, which is possibly due to transport of ions through the SiO2 protective layer.