Matching Items (8)
Filtering by

Clear all filters

152386-Thumbnail Image.png
Description
In this dissertation, combined photo-induced and thermionic electron emission from low work function diamond films is studied through low energy electron spectroscopy analysis and other associated techniques. Nitrogen-doped, hydrogen-terminated diamond films prepared by the microwave plasma chemical vapor deposition method have been the most focused material. The theme of this

In this dissertation, combined photo-induced and thermionic electron emission from low work function diamond films is studied through low energy electron spectroscopy analysis and other associated techniques. Nitrogen-doped, hydrogen-terminated diamond films prepared by the microwave plasma chemical vapor deposition method have been the most focused material. The theme of this research is represented by four interrelated issues. (1) An in-depth study describes combined photo-induced and thermionic emission from nitrogen-doped diamond films on molybdenum substrates, which were illuminated with visible light photons, and the electron emission spectra were recorded as a function of temperature. The diamond films displayed significant emissivity with a low work function of ~ 1.5 eV. The results indicate that these diamond emitters can be applied in combined solar and thermal energy conversion. (2) The nitrogen-doped diamond was further investigated to understand the physical mechanism and material-related properties that enable the combined electron emission. Through analysis of the spectroscopy, optical absorbance and photoelectron microscopy results from sample sets prepared with different configurations, it was deduced that the photo-induced electron generation involves both the ultra-nanocrystalline diamond and the interface between the diamond film and metal substrate. (3) Based on results from the first two studies, possible photon-enhanced thermionic emission was examined from nitrogen-doped diamond films deposited on silicon substrates, which could provide the basis for a novel approach for concentrated solar energy conversion. A significant increase of emission intensity was observed at elevated temperatures, which was analyzed using computer-based modeling and a combination of different emission mechanisms. (4) In addition, the electronic structure of vanadium-oxide-terminated diamond surfaces was studied through in-situ photoemission spectroscopy. Thin layers of vanadium were deposited on oxygen-terminated diamond surfaces which led to oxide formation. After thermal annealing, a negative electron affinity was found on boron-doped diamond, while a positive electron affinity was found on nitrogen-doped diamond. A model based on the barrier at the diamond-oxide interface was employed to analyze the results. Based on results of this dissertation, applications of diamond-based energy conversion devices for combined solar- and thermal energy conversion are proposed.
ContributorsSun, Tianyin (Author) / Nemanich, Robert (Thesis advisor) / Ponce, Fernando (Committee member) / Peng, Xihong (Committee member) / Spence, John (Committee member) / Treacy, Michael (Committee member) / Arizona State University (Publisher)
Created2013
156109-Thumbnail Image.png
Description
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

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.
ContributorsLiu, Qianlang (Author) / Crozier, Peter A. (Thesis advisor) / Chan, Candace (Committee member) / Buttry, Daniel (Committee member) / Liu, Jingyue (Committee member) / Nemanich, Robert (Committee member) / Arizona State University (Publisher)
Created2018
156122-Thumbnail Image.png
Description
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

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.
ContributorsJiao, Xiangbing (Author) / Qing, Quan (Thesis advisor) / Alford, Terry (Thesis advisor) / Nemanich, Robert (Committee member) / Arizona State University (Publisher)
Created2018
156821-Thumbnail Image.png
Description
In this dissertation I studied the anomalous Hall effect in MgO/Permalloy/Nonmagnetic Metal(NM) based structure, spin polarized current in YIG/Pt based thin films and the origin of the perpendicular magnetic anisotropy(PMA) in the Ru/Co/Ru based structures.

The anomalous Hall effect is the observation of a nonzero voltage difference across a magnetic

In this dissertation I studied the anomalous Hall effect in MgO/Permalloy/Nonmagnetic Metal(NM) based structure, spin polarized current in YIG/Pt based thin films and the origin of the perpendicular magnetic anisotropy(PMA) in the Ru/Co/Ru based structures.

The anomalous Hall effect is the observation of a nonzero voltage difference across a magnetic material transverse to the current that flows through the material and the external magnetic field. Unlike the ordinary Hall effect which is observed in nonmagnetic metals, the anomalous Hall effect is only observed in magnetic materials and is orders of magnitude larger than the ordinary Hall effect. Unlike quantum anomalous Hall effect which only works in low temperature and extremely large magnetic field, anomalous Hall effect can be measured at room temperature under a relatively small magnetic field. This allows the anomalous Hall effect to have great potential applications in spintronics and be a good characterization tool for ferromagnetic materials especially materials that have perpendicular magnetic anisotropy(PMA).

In my research, it is observed that a polarity change of the Hall resistance in the MgO/Permalloy/NM structure can be obtained when certain nonmagnetic metal is used as the capping layer while no polarity change is observed when some other metal is used as the capping layer. This allows us to tune the polarity of the anomalous Hall effect by changing the thickness of a component of the structure. My conclusion is that an intrinsic mechanism from Berry curvature plays an important role in the sign of anomalous Hall resistivity in the MgO/Py/HM structures. Surface and interfacial scattering also make substantial contribution to the measured Hall resistivity.

Spin polarization(P) is one of the key concepts in spintronics and is defined as the difference in the spin up and spin down electron population near the Fermi level of a conductor. It has great applications in the spintronics field such as the creation of spin transfer torques, magnetic tunnel junction(MTJ), spintronic logic devices.

In my research, spin polarization is measured on platinum layers grown on a YIG layer. Platinum is a nonmagnetic metal with strong spin orbit coupling which intrinsically has zero spin polarization. Nontrivial spin polarization measured by ARS is observed in the Pt layer when it is grown on YIG ferromagnetic insulator. This result is contrary to the zero spin polarization in the Pt layer when it is grown directly on SiO2 substrate. Magnetic proximity effect and spin current pumping from YIG into Pt is proposed as the reason of the nontrivial spin polarization induced in Pt. An even higher spin polarization in the Pt layer is observed when an ultrathin NiO layer or Cu layer is inserted between Pt and YIG which blocks the proximity effect. The spin polarization in the NiO inserted sample shows temperature dependence. This demonstrates that the spin current transmission is further enhanced in ultrathin NiO layers through magnon and spin fluctuations.

Perpendicular Magnetic Anisotropy(PMA) has important applications in spintronics and magnetic storage. In the last chapter, I study the origin of PMA in one of the structures that shows PMA: Ru/Co/Ru. By measuring the ARS curve while changing the magnetic field orientation, the origin of the PMA in this structure is determined to be the strain induced by lattice mismatch.
ContributorsLi, Bochao (Author) / Chen, Tingyong (Committee member) / Bennett, Peter (Committee member) / Nemanich, Robert (Committee member) / Qing, Quan (Committee member) / Arizona State University (Publisher)
Created2018
154573-Thumbnail Image.png
Description
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

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.
ContributorsKaur, Manpuneet (Author) / Nemanich, Robert (Thesis advisor) / Dey, Sandwip (Committee member) / Crozier, Peter (Committee member) / Chan, Candace (Committee member) / Arizona State University (Publisher)
Created2016
154972-Thumbnail Image.png
Description
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

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.
ContributorsZhao, Shirong (Author) / Chowdhury, Srabanti (Thesis advisor) / Goodnick, Stephen (Committee member) / Zhao, Yuji (Committee member) / Nemanich, Robert (Committee member) / Arizona State University (Publisher)
Created2016
161443-Thumbnail Image.png
Description
Wide bandgap semiconductors are of much current interest due to their superior electrical properties. This dissertation describes electron microscopy characterization of GaN-on-GaN structures for high-power vertical device applications. Unintentionally-doped (UID) GaN layers grown homoepitaxially via metal-organic chemical vapor deposition on freestanding GaN substrates, were subjected to dry etching, and layers

Wide bandgap semiconductors are of much current interest due to their superior electrical properties. This dissertation describes electron microscopy characterization of GaN-on-GaN structures for high-power vertical device applications. Unintentionally-doped (UID) GaN layers grown homoepitaxially via metal-organic chemical vapor deposition on freestanding GaN substrates, were subjected to dry etching, and layers of UID-GaN/p-GaN were over-grown. The as-grown and regrown heterostructures were examined in cross-section using transmission electron microscopy (TEM). Two different etching treatments, fast-etch-only and multiple etches with decreasing power, were employed. The fast-etch-only devices showed GaN-on-GaN interface at etched location, and low device breakdown voltages were measured (~ 45-95V). In comparison, no interfaces were visible after multiple etching steps, and the corresponding breakdown voltages were much higher (~1200-1270V). These results emphasized importance of optimizing surface etching techniques for avoiding degraded device performance. The morphology of GaN-on-GaN devices after reverse-bias electrical stressing to breakdown was investigated. All failed devices had irreversible structural damage, showing large surface craters (~15-35 microns deep) with lengthy surface cracks. Cross-sectional TEM of failed devices showed high densities of threading dislocations (TDs) around the cracks and near crater surfaces. Progressive ion-milling across damaged devices revealed high densities of TDs and the presence of voids beneath cracks: these features were not observed in unstressed devices. The morphology of GaN substrates grown by hydride vapor-phase epitaxy (HVPE) and by ammonothermal methods were correlated with reverse-bias results. HVPE substrates showed arrays of surface features when observed by X-ray topography (XRT). All fabricated devices that overlapped with these features had typical reverse-bias voltages less than 100V at a leakage current limit of 10-6 A. In contrast, devices not overlapping with such features reached voltages greater than 300V. After etching, HVPE substrate surfaces showed defect clusters and macro-pits, whereas XRT images of ammonothermal substrate revealed no visible features. However, some devices fabricated on ammonothermal substrate failed at low voltages. Devices on HVPE and ammonothermal substrates with low breakdown voltages showed crater-like surface damage and revealed TDs (~25µm deep) and voids; such features were not observed in devices reaching higher voltages. These results should assist in developing protocols to fabricate reliable high-voltage devices.
ContributorsPeri, Prudhvi Ram (Author) / Smith, David J. (Thesis advisor) / Alford, Terry (Committee member) / Mccartney, Martha R (Committee member) / Nemanich, Robert (Committee member) / Zhao, Yuji (Committee member) / Arizona State University (Publisher)
Created2021
161590-Thumbnail Image.png
Description
In this dissertation, far UV spectroscopy is applied to investigate the optical properties of dielectric thin films grown by atomic layer deposition. The far UV (120 – 200 nm) reflectance for several dielectric oxides and fluorides, including AlF3, Al2O3, Ga2O3, HfO2, and SiO2, was measured at variable angles and thicknesses.

In this dissertation, far UV spectroscopy is applied to investigate the optical properties of dielectric thin films grown by atomic layer deposition. The far UV (120 – 200 nm) reflectance for several dielectric oxides and fluorides, including AlF3, Al2O3, Ga2O3, HfO2, and SiO2, was measured at variable angles and thicknesses. Multiple optical calculation methods were developed for the accurate determination of the optical constants from the reflectance. The deduced optical constants were used for optical designs, such as high-reflectivity coatings, and Fabry-Perot bandpass interference filters. Three filters were designed for use at 157 nm, 212 nm, and 248 nm wavelengths, based on multilayer structures consisting of SiO2, Al2O3, HfO2, and AlF3. A thorough error analysis was made to quantify the non-idealities of the optical performance for the designed filters. Far UV spectroscopy was also applied to analyze material mixtures, such as AlF3/Al and h-BN/c-BN mixtures. Using far UV spectroscopy, different phases in the composite can be distinguished, and the volume concentration of each constituent can be determined. A middle UV reflective coating based on A2O3 and AlF3 was fabricated and characterized. The reflective coating has a smooth surface (?? < 1 nm), and a peak reflectance of 25 – 30 % at a wavelength of 196 nm. The peak reflectance deviated from the design, and an analysis of the AlF3 layer prepared by plasma-enhanced atomic layer deposition (PEALD) indicated the presence of Al-rich clusters, which were associated with the UV absorption. Complementary techniques, such as spectroscopic ellipsometry, and X-ray photoelectron spectroscopy, were used to verify the results from far UV spectroscopy. In conclusion, this Dissertation demonstrated the use of in-situ far UV spectroscopy to investigate the optical properties of thin films at short wavelengths. This work extends the application of far UV spectroscopy to ultrawide bandgap semiconductors and insulators. This work supports a path forward for far UV optical filters and devices. Various errors have been discussed with solutions proposed for future research of methods and materials for UV optics.
ContributorsHuang, Zhiyu (Author) / Nemanich, Robert (Thesis advisor) / Ponce, Fernando (Committee member) / Menéndez, Jose (Committee member) / Holman, Zachary (Committee member) / Arizona State University (Publisher)
Created2021