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Description
Photocatalytic activity of titanium dioxide (titania or TiO2) offers enormous potential in solving energy and environmental problems. Immobilization of titania nanoparticles on inert substrates is an effective way of utilizing its photocatalytic activity since nanoparticles enable high mass-transport, and immobilization avoids post-treatment separation. For competitive photocatalytic performance, the morphology of the substrate can be engineered to enhance mass-transport and light accessibility. In this work, two types of fiber architectures (i.e., dispersed polymer/titania phase or D-phase, and multi-phase polymer-core/composite-shell fibers or M-phase) were explored as effective substrate solutions for anchoring titania. These fibers were fabricated using a low-cost and scalable fiber spinning technique. Polymethyl methacrylate (PMMA) was selected as the substrate material due to its ultraviolet (UV) transparency and stability against oxidative radicals. The work systematically investigates the influence of the fiber porosity on mass-transport and UV light scattering. The properties of the fabricated fiber systems were characterized by scanning electron microscopy (SEM), Brunauer–Emmett–Teller (BET), UV-vis spectrophotometry (UV-vis), and mechanical analysis. The photocatalytic performance was characterized by monitoring the decomposition of methylene blue (MB) under UV (i.e., 365 nm) light. Fabrication of photocatalytic support structures was observed to be an optimization problem where porosity improved mass transport but reduced UV accessibility. The D-phase fibers demonstrated the highest MB degradation rate (i.e., 0.116 min-1) due to high porosity (i.e., 33.2 m2/g). The M-phase fibers reported a better degradation rate compared to a D-phase fibers due to higher UV accessibility efficiency.
ContributorsKanth, Namrata (Author) / Song, Kenan (Thesis advisor) / Tongay, Sefaattin (Thesis advisor) / Kannan, Arunachala Mada (Committee member) / Arizona State University (Publisher)
Created2020
Description
The chemical, structural, and electrical properties of niobium-silicon, niobium-germanium, and YBCO-dielectric interfaces are characterized. Reduction in the concentration of interfacial defects in these structures can improve the performance of (i) many devices including low-loss coplanar, microstrip, and stripline microwave resonators used in next-generation cryogenic communication, sensor, and quantum information technologies and (ii) layers used in device isolation, inter-wiring dielectrics, and passivation in microwave and Josephson junction circuit fabrication.
Methods were developed to synthesize amorphous-Ge (a-Ge) and homoepitaxial-Si dielectric thin-films with loss tangents of 1–2×10 -6 and 0.6–2×10 -5 at near single-photon powers and sub-Kelvin temperatures (≈40 mK), making them potentially a better choice over undoped silicon and sapphire substrates used in quantum devices. The Nb/Ge interface has 20 nm of chemical intermixing, which is reduced by a factor of four using 10 nm Ta diffusion layers. Niobium coplanar resonators using this structure exhibit reduced microwave losses.
The nature and concentration of defects near Nb-Si interfaces prepared with commonly-used Si surface treatments were characterized. All samples have H, C, O, F, and Cl in the Si within 50 nm of the interface, and electrically active defects with activation energies of 0.147, 0.194, 0.247, 0.339, and 0.556 eV above the valence band maximum (E vbm ), with concentrations dominated by a hole trap at E vbm +0.556 eV (presumably Nb Si ). The optimum surface treatment is an HF etch followed by an in-situ 100 eV Ar ion mill. RCA etches, and higher energy ion milling processes increase the concentration of electrically active defects.
A thin SrTiO 3 buffer layer used in YBa 2 Cu 3 O 7-δ superconductor/high-performance Ba(Zn 1/3 Ta 2/3 )O 3 and Ba(Cd 1/3 Ta 2/3 )O 3 microwave dielectric trilayers improves the structural quality of the layers and results in 90 K superconductor critical temperatures. This advance enables the production of more compact high-temperature superconductor capacitors, inductors, and microwave microstrip and stripline devices.
Methods were developed to synthesize amorphous-Ge (a-Ge) and homoepitaxial-Si dielectric thin-films with loss tangents of 1–2×10 -6 and 0.6–2×10 -5 at near single-photon powers and sub-Kelvin temperatures (≈40 mK), making them potentially a better choice over undoped silicon and sapphire substrates used in quantum devices. The Nb/Ge interface has 20 nm of chemical intermixing, which is reduced by a factor of four using 10 nm Ta diffusion layers. Niobium coplanar resonators using this structure exhibit reduced microwave losses.
The nature and concentration of defects near Nb-Si interfaces prepared with commonly-used Si surface treatments were characterized. All samples have H, C, O, F, and Cl in the Si within 50 nm of the interface, and electrically active defects with activation energies of 0.147, 0.194, 0.247, 0.339, and 0.556 eV above the valence band maximum (E vbm ), with concentrations dominated by a hole trap at E vbm +0.556 eV (presumably Nb Si ). The optimum surface treatment is an HF etch followed by an in-situ 100 eV Ar ion mill. RCA etches, and higher energy ion milling processes increase the concentration of electrically active defects.
A thin SrTiO 3 buffer layer used in YBa 2 Cu 3 O 7-δ superconductor/high-performance Ba(Zn 1/3 Ta 2/3 )O 3 and Ba(Cd 1/3 Ta 2/3 )O 3 microwave dielectric trilayers improves the structural quality of the layers and results in 90 K superconductor critical temperatures. This advance enables the production of more compact high-temperature superconductor capacitors, inductors, and microwave microstrip and stripline devices.
ContributorsKopas, Cameron Joseph (Author) / Newman, Nathan (Thesis advisor) / Alford, Terry L. (Committee member) / Carpenter, Ray W (Committee member) / Williams, Peter (Committee member) / Arizona State University (Publisher)
Created2020
Description
A new nanoparticle deposition technique, Aerosol Impaction-Driven Assembly (AIDA), was extensively characterized for material structures and properties. Aerogel films can be deposited directly onto a substrate with AIDA without the long aging and drying steps in the sol-gel method. Electron microscopy, pore size analysis, thermal conductivity, and optical measurements show the nanoparticle (NP) films to be similar to typical silica aerogel. Haze of nanoparticle films modeled as scattering sites correlates strongly with pore size distribution. Supporting evidence was obtained from particle sizes and aggregates using electron microscopy and small-angle X-ray scattering. NP films showed interlayers of higher porosity and large aggregates formed by tensile film stress.
To better understand film stress and NP adhesion, chemical bonding analyses were performed for samples annealed up to 900 °C. Analysis revealed that about 50% of the NP surfaces are functionalized by hydroxyl (-OH) groups, providing for hydrogen bonding. Ellipsometric porosimetry was used to further understand the mechanical properties by providing a measure of strain upon capillary pressure from filling pores. Upon annealing to 200 °C, the films lost water resulting in closer bonding of NPs and higher Young’s modulus. Upon further annealing up to 900 °C, the films lost hydroxyl bonds while gaining siloxane bonds, reducing Young’s modulus. The application of ellipsometric porosimetry to hydrophilic coatings brings into question the validity of pore size distribution calculations for materials that hold onto water molecules and result in generally smaller calculated pore sizes.
Doped hydrogenated microcrystalline silicon was grown on crystalline silicon NPs, as a test case of an application for NP films to reduce parasitic absorption in silicon heterojunction solar cells. Parasitic absorption of blue light could be reduced because microcrystalline silicon has a mix of direct and indirect bandgap, giving lower blue absorption than amorphous silicon. Using Ultraviolet Raman spectroscopy, the crystallinity of films as thin as 13 nm was determined rapidly (in 1 minute) and non-destructively. A mono-layer of nanocrystals was applied as seeds for p-doped microcrystalline silicon growth and resulted in higher crystallinity films. Applications of the method could be explored for other nanocrystalline materials.
To better understand film stress and NP adhesion, chemical bonding analyses were performed for samples annealed up to 900 °C. Analysis revealed that about 50% of the NP surfaces are functionalized by hydroxyl (-OH) groups, providing for hydrogen bonding. Ellipsometric porosimetry was used to further understand the mechanical properties by providing a measure of strain upon capillary pressure from filling pores. Upon annealing to 200 °C, the films lost water resulting in closer bonding of NPs and higher Young’s modulus. Upon further annealing up to 900 °C, the films lost hydroxyl bonds while gaining siloxane bonds, reducing Young’s modulus. The application of ellipsometric porosimetry to hydrophilic coatings brings into question the validity of pore size distribution calculations for materials that hold onto water molecules and result in generally smaller calculated pore sizes.
Doped hydrogenated microcrystalline silicon was grown on crystalline silicon NPs, as a test case of an application for NP films to reduce parasitic absorption in silicon heterojunction solar cells. Parasitic absorption of blue light could be reduced because microcrystalline silicon has a mix of direct and indirect bandgap, giving lower blue absorption than amorphous silicon. Using Ultraviolet Raman spectroscopy, the crystallinity of films as thin as 13 nm was determined rapidly (in 1 minute) and non-destructively. A mono-layer of nanocrystals was applied as seeds for p-doped microcrystalline silicon growth and resulted in higher crystallinity films. Applications of the method could be explored for other nanocrystalline materials.
ContributorsCarpenter, Joe Victor (Author) / Holman, Zachary C (Thesis advisor) / Bertoni, Mariana I (Committee member) / Chan, Candace K. (Committee member) / Smith, David J. (Committee member) / Arizona State University (Publisher)
Created2020
Description
AA 7XXX alloys are used extensively in aircraft and naval structures due to their excellent strength to weight ratio. These alloys are often exposed to harsh corrosive environments and mechanical stresses that can compromise their reliability in service. They are also coupled with fasteners that are composed of different materials such as Titanium alloys. Such dissimilar metal contact facilitates galvanic and crevice corrosion, which can further reduce their lifetimes. Despite decades of research in the area, the confluence of mechanical, microstructural, and electrochemical aspects of damage is still unclear. Traditionally, 2D and destructive methods have often been employed to study the corrosion and cracking behavior in these systems which can be severely limiting and lead to inaccurate conclusions. This dissertation is aimed at comprehensively studying the corrosion and cracking behavior of these systems using time-dependent 3D microstructural characterization, as well as correlative microscopy. The microstructural evolution of corrosion in AA 7075 was studied using a combination of potentiodynamic polarization, X-ray Computed Tomography (XCT) and Transmission X-ray Microscopy (TXM). In both experiments, a strong emphasis was placed on studying localized corrosion attack at constituent particles and intergranular corrosion. With an understanding of the alloy’s corrosion behavior, a dissimilar alloy couple comprising AA 7075 / Ti-6Al-4V was then investigated. Ex situ and in situ x-ray microtomography was used extensively to investigate the evolution of pitting corrosion and corrosion fatigue in AA 7075 plates fastened separately with Ti-6Al-4V screws and rivets. The 4D tomography combined with the extensive fractography yielded valuable information pertaining the preferred sites of pit initiation, crack initiation and growth in these complex geometries. The use of correlative microscopy-based methodologies yielded multimodal characterization results that provided a unique and seminal insight on corrosion mechanisms in these materials.
ContributorsNiverty, Sridhar (Author) / Chawla, Nikhilesh (Thesis advisor) / Liu, Yongming (Committee member) / Ankit, Kumar (Committee member) / Xiao, Xianghui (Committee member) / Arizona State University (Publisher)
Created2020
Description
Precursors of carbon fibers include rayon, pitch, and polyacrylonitrile fibers that can be heat-treated for high-strength or high-modulus carbon fibers. Among them, polyacrylonitrile has been used most frequently due to its low viscosity for easy processing and excellent performance for high-end applications. To further explore polyacrylonitrile-based fibers for better precursors, in this study, carbon nanofillers were introduced in the polymer matrix to examine their reinforcement effects and influences on carbon fiber performance. Two-dimensional graphene nanoplatelets were mainly used for the polymer reinforcement and one-dimensional carbon nanotubes were also incorporated in polyacrylonitrile as a comparison. Dry-jet wet spinning was used to fabricate the composite fibers. Hot-stage drawing and heat-treatment were used to evolve the physical microstructures and molecular morphologies of precursor and carbon fibers. As compared to traditionally used random dispersions, selective placement of nanofillers was effective in improving composite fiber properties and enhancing mechanical and functional behaviors of carbon fibers. The particular position of reinforcement fillers with polymer layers was enabled by the in-house developed spinneret used for fiber spinning. The preferential alignment of graphitic planes contributed to the enhanced mechanical and functional behaviors than those of dispersed nanoparticles in polyacrylonitrile composites. The high in-plane modulus of graphene and the induction to polyacrylonitrile molecular carbonization/graphitization were the motivation for selectively placing graphene nanoplatelets between polyacrylonitrile layers. Mechanical tests, scanning electron microscopy, thermal, and electrical properties were characterized. Applications such as volatile organic compound sensing and pressure sensing were demonstrated.
ContributorsFranklin, Rahul Joseph (Author) / Song, Kenan (Thesis advisor) / Jiao, Yang (Thesis advisor) / Liu, Yongming (Committee member) / Arizona State University (Publisher)
Created2020
Description
Single drop impact of liquid on a static powder bed was studied to investigate the granule formation mechanism, droplet penetration time, the characterization of granules (morphology, surface structure and internal structure), as well as the formation regime map. Water was used as the liquid and two pharmaceutical powders, microcrystalline cellulose (MCC) and acetaminophen (APAP), were mixed to make heterogeneous powder beds. The complete drop impact and penetration was recorded by a high-speed camera. Two granule formation mechanisms identified previously occurred: Spreading and Tunneling. Spreading occurred for mixtures of large particle sizes, while Tunneling started to occur when the particle sizes of the mixtures decreased. With an increase of APAP concentration, the overall drop penetration time increased, which was in good agreement with previous literature. The granule morphology, surface structure, and internal structure were characterized by a prism method with image analysis, scanning electron microscope, and X-ray microtomography, respectively. The Spreading mechanism produced flat disks with porous internal structures, while the Tunneling mechanism produced round granules with dense internal structures. Granules that were formed via a hybrid of the mechanisms, Spreading/Tunneling, were hybrid granules, with some dense areas and some porous areas. The results of the granule content uniformity from UV-vis spectrometry revealed that with the increase of APAP proportion, the overall uniformity was compromised for mixtures with fine ingredients, while the content was much more uniform for coarse mixtures. It is believed that the mean particle size of the powder bed is the predominant factor in influencing the formation mechanism, drop penetration time, and granule properties, while the content uniformity is affected by both the particle sizes and the mixture hydrophobicity.
ContributorsGao, Tianxiang (Author) / Emady, Heather N (Thesis advisor) / Chawla, Nikhilesh (Committee member) / Jiao, Yang (Committee member) / Pradhan, Shankali (Committee member) / Oka, Sarang (Committee member) / Arizona State University (Publisher)
Created2020
Description
Miniaturization of microdevices comes at the cost of increased circuit complexity and operating current densities. At high current densities, the resulting electron wind imparts a large momentum to metal ions triggering electromigration which leads to degradation of interconnects and solder, ultimately resulting in circuit failure. Although electromigration-induced defects in electronic materials can manifest in several forms, the formation of voids is a common occurrence. This research aims at understanding the morphological evolution of voids under electromigration by formulating a diffuse interface approach that accounts for anisotropic mobility in the metallic interconnect. Based on an extensive parametric study, this study reports the conditions under which pancaking of voids or the novel void ‘swimming’ regimes are observed. Finally, inferences are drawn to formulate strategies using which the reliability of interconnects can be improved.
ContributorsVemulapalli, Sree Shivani (Author) / Ankit, Kumar (Thesis advisor) / Chawla, Nikhilesh (Committee member) / Singh, Arunima (Committee member) / Arizona State University (Publisher)
Created2020
Description
Mixed-ionic electronic conducting (MIEC) oxides have drawn much attention from researchers because of their potential in high temperature separation processes. Among many materials available, perovskite type and fluorite type oxides are the most studied for their excellent oxygen ion transport property. These oxides not only can be oxygen adsorbent or O2-permeable membranes themselves, but also can be incorporated with molten carbonate to form dual-phase membranes for CO2 separation.
Oxygen sorption/desorption properties of perovskite oxides with and without oxygen vacancy were investigated first by thermogravimetric analysis (TGA) and fixed-bed experiments. The oxide with unique disorder-order phase transition during desorption exhibited an enhanced oxygen desorption rate during the TGA measurement but not in fixed-bed demonstrations. The difference in oxygen desorption rate is due to much higher oxygen partial pressure surrounding the sorbent during the fixed-bed oxygen desorption process, as revealed by X-ray diffraction (XRD) patterns of rapidly quenched samples.
Research on using perovskite oxides as CO2-permeable dual-phase membranes was subsequently conducted. Two CO2-resistant MIEC perovskite ceramics, Pr0.6Sr0.4Co0.2Fe0.8 O3-δ (PSCF) and SrFe0.9Ta0.1O3-δ (SFT) were chosen as support materials for membrane synthesis. PSCF-molten carbonate (MC) and SFT-MC membranes were prepared for CO2-O2 counter-permeation. The geometric factors for the carbonate phase and ceramic phase were used to calculate the effective carbonate and oxygen ionic conductivity in the carbonate and ceramic phase. When tested in CO2-O2 counter-permeation set-up, CO2 flux showed negligible change, but O2 flux decreased by 10-32% compared with single-component permeation. With CO2 counter-permeation, the total oxygen permeation flux is higher than that without counter-permeation.
A new concept of CO2-permselective membrane reactor for hydrogen production via steam reforming of methane (SRM) was demonstrated. The results of SRM in the membrane reactor confirm that in-situ CO2 removal effectively promotes water-gas shift conversion and thus enhances hydrogen yield. A modeling study was also conducted to assess the performance of the membrane reactor in high-pressure feed/vacuum sweep conditions, which were not carried out due to limitations in current membrane testing set-up. When 5 atm feed pressure and 10-3 atm sweep pressure were applied, the membrane reactor can produce over 99% hydrogen stream in simulation.
Oxygen sorption/desorption properties of perovskite oxides with and without oxygen vacancy were investigated first by thermogravimetric analysis (TGA) and fixed-bed experiments. The oxide with unique disorder-order phase transition during desorption exhibited an enhanced oxygen desorption rate during the TGA measurement but not in fixed-bed demonstrations. The difference in oxygen desorption rate is due to much higher oxygen partial pressure surrounding the sorbent during the fixed-bed oxygen desorption process, as revealed by X-ray diffraction (XRD) patterns of rapidly quenched samples.
Research on using perovskite oxides as CO2-permeable dual-phase membranes was subsequently conducted. Two CO2-resistant MIEC perovskite ceramics, Pr0.6Sr0.4Co0.2Fe0.8 O3-δ (PSCF) and SrFe0.9Ta0.1O3-δ (SFT) were chosen as support materials for membrane synthesis. PSCF-molten carbonate (MC) and SFT-MC membranes were prepared for CO2-O2 counter-permeation. The geometric factors for the carbonate phase and ceramic phase were used to calculate the effective carbonate and oxygen ionic conductivity in the carbonate and ceramic phase. When tested in CO2-O2 counter-permeation set-up, CO2 flux showed negligible change, but O2 flux decreased by 10-32% compared with single-component permeation. With CO2 counter-permeation, the total oxygen permeation flux is higher than that without counter-permeation.
A new concept of CO2-permselective membrane reactor for hydrogen production via steam reforming of methane (SRM) was demonstrated. The results of SRM in the membrane reactor confirm that in-situ CO2 removal effectively promotes water-gas shift conversion and thus enhances hydrogen yield. A modeling study was also conducted to assess the performance of the membrane reactor in high-pressure feed/vacuum sweep conditions, which were not carried out due to limitations in current membrane testing set-up. When 5 atm feed pressure and 10-3 atm sweep pressure were applied, the membrane reactor can produce over 99% hydrogen stream in simulation.
ContributorsWu, Han-Chun (Author) / Lin, Jerry Y.S. (Thesis advisor) / Deng, Shuguang (Committee member) / Jiao, Yang (Committee member) / Emady, Heather (Committee member) / Muhich, Christopherq (Committee member) / Arizona State University (Publisher)
Created2020
Description
Photocatalytic water splitting over suspended nanoparticles represents a potential solution for achieving CO2-neutral energy generation and storage. To design efficient photocatalysts, a fundamental understanding of the material’s structure, electronic properties, defects, and how these are controlled via synthesis is essential. Both bulk and nanoscale materials characterization, in addition to various performance metrics, can be combined to elucidate functionality at multiple length scales. In this work, two promising visible light harvesting systems are studied in detail: Pt-functionalized graphitic carbon nitrides (g-CNxHys) and TiO2-supported CeO2-x composites.
Electron energy-loss spectroscopy (EELS) is used to sense variations in the local concentration of amine moieties (defects believed to facilitate interfacial charge transfer) at the surface of a g-CNxHy flake. Using an aloof-beam configuration, spatial resolution is maximized while minimizing damage thus providing nanoscale vibrational fingerprints similar to infrared absorption spectra. Structural disorder in g-CNxHys is further studied using transmission electron microscopy at low electron fluence rates. In-plane structural fluctuations revealed variations in the local azimuthal orientation of the heptazine building blocks, allowing planar domain sizes to be related to the average polymer chain length. Furthermore, competing factors regulating photocatalytic performance in a series of Pt/g-CNxHys is elucidated. Increased polymer condensation in the g-CNxHy support enhances the rate of charge transfer to reactants owing to higher electronic mobility. However, active site densities are over 3x lower on the most condensed g-CNxHy which ultimately limits its H2 evolution rate (HER). Based on these findings, strategies to improve the cocatalyst configuration on intrinsically active supports are given.
In TiO2/CeO2-x photocatalysts, the effect of the support particle size on the bulk
anoscale properties and photocatalytic performance is investigated. Small anatase supports facilitate highly dispersed CeO2-x species, leading to increased visible light absorption and HERs resulting from a higher density of mixed metal oxide (MMO) interfaces with Ce3+ species. Using monochromated EELS, bandgap states associated with MMO interfaces are detected, revealing electronic transitions from 0.5 eV up to the bulk bandgap onset of anatase. Overall, the electron microscopy/spectroscopy techniques developed and applied herein sheds light onto the relevant defects and limiting processes operating within these photocatalyst systems thus suggesting rational design strategies.
Electron energy-loss spectroscopy (EELS) is used to sense variations in the local concentration of amine moieties (defects believed to facilitate interfacial charge transfer) at the surface of a g-CNxHy flake. Using an aloof-beam configuration, spatial resolution is maximized while minimizing damage thus providing nanoscale vibrational fingerprints similar to infrared absorption spectra. Structural disorder in g-CNxHys is further studied using transmission electron microscopy at low electron fluence rates. In-plane structural fluctuations revealed variations in the local azimuthal orientation of the heptazine building blocks, allowing planar domain sizes to be related to the average polymer chain length. Furthermore, competing factors regulating photocatalytic performance in a series of Pt/g-CNxHys is elucidated. Increased polymer condensation in the g-CNxHy support enhances the rate of charge transfer to reactants owing to higher electronic mobility. However, active site densities are over 3x lower on the most condensed g-CNxHy which ultimately limits its H2 evolution rate (HER). Based on these findings, strategies to improve the cocatalyst configuration on intrinsically active supports are given.
In TiO2/CeO2-x photocatalysts, the effect of the support particle size on the bulk
anoscale properties and photocatalytic performance is investigated. Small anatase supports facilitate highly dispersed CeO2-x species, leading to increased visible light absorption and HERs resulting from a higher density of mixed metal oxide (MMO) interfaces with Ce3+ species. Using monochromated EELS, bandgap states associated with MMO interfaces are detected, revealing electronic transitions from 0.5 eV up to the bulk bandgap onset of anatase. Overall, the electron microscopy/spectroscopy techniques developed and applied herein sheds light onto the relevant defects and limiting processes operating within these photocatalyst systems thus suggesting rational design strategies.
ContributorsHaiber, Diane Michelle (Author) / Crozier, Peter (Thesis advisor) / Chan, Candace (Committee member) / Liu, Jingyue (Committee member) / Treacy, Michael (Committee member) / Arizona State University (Publisher)
Created2019
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 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