ASU Electronic Theses and Dissertations
This collection includes most of the ASU Theses and Dissertations from 2011 to present. ASU Theses and Dissertations are available in downloadable PDF format; however, a small percentage of items are under embargo. Information about the dissertations/theses includes degree information, committee members, an abstract, supporting data or media.
In addition to the electronic theses found in the ASU Digital Repository, ASU Theses and Dissertations can be found in the ASU Library Catalog.
Dissertations and Theses granted by Arizona State University are archived and made available through a joint effort of the ASU Graduate College and the ASU Libraries. For more information or questions about this collection contact or visit the Digital Repository ETD Library Guide or contact the ASU Graduate College at gradformat@asu.edu.
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- Creators: Alford, Terry
The SrTiO3/Si system was initially studied to develop a basic understanding of the integration of perovskite oxides with semiconductors, and successful integration with abrupt interfaces was demonstrated. Defect analysis showed no misfit dislocations but only anti-phase boundaries (APBs) in the SrTiO3 (STO) films. Similar defects were later observed in other perovskite oxide heterostructures.
Ferroelectric BaTiO3 (BTO) thin films deposited directly onto STO substrates, or STO buffer layers with Ge substrates, were grown by molecular beam epitaxy (MBE) in order to control the polarization orientation for field-effect transistors (FETs). STEM imaging and elemental mapping by electron energy-loss spectroscopy (EELS) showed structurally and chemically abrupt interfaces, and the BTO films retained the c-axis-oriented tetragonal structure for both BTO/STO and BTO/STO/Ge heterostructures. The polarization displacement in the BTO films of TiN/BTO/STO heterostructures was investigated. The Ti4+ atomic column displacements and lattice parameters were measured directly using HAADF images. A polarization gradient, which switched from upwards to downwards, was observed in the BTO thin film, and evidence was found for positively-charged oxygen vacancies.
Heterostructures grown on Ge substrates by atomic layer deposition (ALD) were characterized and compared with MBE-grown samples. A two-step process was needed to overcome interlayer reaction at the beginning of ALD growth. A-site-rich oxide films with thicknesses of at least 2-nm had to be deposited and then crystallized before initiating deposition of the following perovskite oxide layer in order to suppress the formation of amorphous oxide layers on the Ge surface. BTO/STO/Ge, BTO/Ge, SrHfTiO3/Ge and SrZrO3/Ge thin films with excellent crystallinity were grown using this process.
Metal-insulator-metal (MIM) heterostructures were fabricated as ferroelectric capacitors and then electrically stressed to the point of breakdown to correlate structural changes with electrical and physical properties. BaTiO3 on Nb:STO was patterned with different top metal electrodes by focused-ion-beam milling, Au/Ni liftoff, and an isolation-defined approach.
ranging from survey monitors used to supervise the generated radioactive waste at
nuclear power plants to personal dosimeters which measure the radiation dose
accumulated in individuals. This dissertation work will present two different types of
novel devices developed at Arizona State University for total dose sensing applications.
The first detector technology is a mechanically flexible metal-chalcogenide glass (ChG)
based system which is fabricated on low cost substrates and are intended as disposable
total dose sensors. Compared to existing commercial technologies, these thin film
radiation sensors are simpler in form and function, and cheaper to produce and operate.
The sensors measure dose through resistance change and are suitable for applications
such as reactor dosimetry, radiation chemistry, and clinical dosimetry. They are ideal for
wearable devices due to the lightweight construction, inherent robustness to resist
breaking when mechanically stressed, and ability to attach to non-flat objects. Moreover,
their performance can be easily controlled by tuning design variables and changing
incorporated materials. The second detector technology is a wireless dosimeter intended
for remote total dose sensing. They are based on a capacitively loaded folded patch
antenna resonating in the range of 3 GHz to 8 GHz for which the load capacitance varies
as a function of total dose. The dosimeter does not need power to operate thus enabling
its use and implementation in the field without requiring a battery for its read-out. As a
result, the dosimeter is suitable for applications such as unattended detection systems
destined for covert monitoring of merchandise crossing borders, where nuclear material
tracking is a concern. The sensitive element can be any device exhibiting a known
variation of capacitance with total ionizing dose. The sensitivity of the dosimeter is
related to the capacitance variation of the radiation sensitive device as well as the high
frequency system used for reading. Both technologies come with the advantage that they
are easy to manufacture with reasonably low cost and sensing can be readily read-out.
Autonomous smart windows may be integrated with a stack of active components, such as electrochromic devices, to modulate the opacity/transparency by an applied voltage. Here, we describe the processing and performance of two classes of visibly-transparent photovoltaic materials, namely inorganic (ZnO thin film) and fully organic (PCDTBT:PC70BM), for integration with electrochromic stacks.
Sputtered ZnO (2% Mn) films on ITO, with transparency in the visible range, were used to fabricate metal-semiconductor (MS), metal-insulator-semiconductor (MIS), and p-i-n heterojunction devices, and their photovoltaic conversion under ultraviolet (UV) illumination was evaluated with and without oxygen plasma-treated surface electrodes (Au, Ag, Al, and Ti/Ag). The MS Schottky parameters were fitted against the generalized Bardeen model to obtain the density of interface states (Dit ≈ 8.0×1011 eV−1cm−2) and neutral level (Eo ≈ -5.2 eV). These devices exhibited photoconductive behavior at λ = 365 nm, and low-noise Ag-ZnO detectors exhibited responsivity (R) and photoconductive gain (G) of 1.93×10−4 A/W and 6.57×10−4, respectively. Confirmed via matched-pair analysis, post-metallization, oxygen plasma treatment of Ag and Ti/Ag electrodes resulted in increased Schottky barrier heights, which maximized with a 2 nm SiO2 electron blocking layer (EBL), coupled with the suppression of recombination at the metal/semiconductor interface and blocking of majority carriers. For interdigitated devices under monochromatic UV-C illumination, the open-circuit voltage (Voc) was 1.2 V and short circuit current density (Jsc), due to minority carrier tunneling, was 0.68 mA/cm2.
A fully organic bulk heterojunction photovoltaic device, composed of poly[N-9’-heptadecanyl-2,7-carbazole-alt-5,5-(4’,7’-di-2-thienyli2’,1’,3’-benzothiadiazole)]:phenyl-C71-butyric-acidmethyl (PCDTBT:PC70BM), with corresponding electron and hole transport layers, i.e., LiF with Al contact and conducting
on-conducting (nc) PEDOT:PSS (with ITO/PET or Ag nanowire/PDMS contacts; the illuminating side), respectively, was developed. The PCDTBT/PC70BM/PEDOT:PSS(nc)/ITO/PET stack exhibited the highest performance: power conversion efficiency (PCE) ≈ 3%, Voc = 0.9V, and Jsc ≈ 10-15 mA/cm2. These stacks exhibited high visible range transparency, and provided the requisite power for a switchable electrochromic stack having an inkjet-printed, optically-active layer of tungsten trioxide (WO3), peroxo-tungstic acid dihydrate, and titania (TiO2) nano-particle-based blend. The electrochromic stacks (i.e., PET/ITO/LiClO4/WO3 on ITO/PET and Ag nanowire/PDMS substrates) exhibited optical switching under external bias from the PV stack (or an electrical outlet), with 7 s coloration time, 8 s bleaching time, and 0.36-0.75 optical modulation at λ = 525 nm. The devices were paired using an Internet of Things controller that enabled wireless switching.
sensors. The unique crystalline structure of MOFs in addition to controllability of
their pore size and their intake selectivity makes them a promising method of detection.
Detection of metal ions in water using a binary mixture of luminescent MOFs
has been reported. 3 MOFs(ZrPDA, UiO-66 and UiO-66-NH2) as detectors and 4
metal ions(Pb2+, Ni2+, Ba2+ and Cu2+) as the target species were chosen based on
cost, water stability, application and end goals.
It is possible to detect metal ions such as Pb2+ at concentrations at low as 0.005
molar using MOFs. Also, based on the luminescence responses, a method of distinguishing
between similar metal ions has been proposed. It is shown that using a
mixture of MOFs with dierent reaction to metal ions can lead to unique and specic
3D luminescence maps, which can be used to identify the present metal ions in water
and their amount.
In addition to the response of a single MOF to addition of a single metal ion,
luminescence response of ZrPDA + UiO-66 mixture to increasing concentration of
each of 4 metal ions was studied, and summarized. A new peak is observed in the
mixture, that did not exist before, and it is proposed that this peak requires metal
ions to activate
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.
A multi-chamber UHV system was customized and transformed into a cold wall CVD system to perform experiments. The versatile growth process was completely custom-automated by controlling the process parameters with LabVIEW. Graphene growth was explored on solid electrodeposited, recrystallized and thin sputter deposited Cu films as well as on liquid Cu supported on W/Mo refractory substrates under ambient pressure using Ar, H₂ and CH₄ mixtures.
The results indicate that graphene grown on Cu films using cold wall CVD follows a classical two-dimensional nucleation and growth mechanism. The nucleation density decreases and average size of graphene crystallites increases with increasing dilution of the CH₄/H₂ mixture by Ar, decrease in total flow rate and decrease in CH₄:H₂ ratio at a fixed substrate temperature and chamber pressure. Thus, the resulting morphological changes correspond with those that would be expected if the precursor deposition rate was varied at a fixed substrate temperature for physical deposition using thermal evaporation. The evolution of graphene crystallite boundary morphology with decreasing effective C deposition rate indicates the effect of edge diffusion of C atoms along the crystallite boundaries, in addition to H₂ etching, on graphene crystallite shape.
The roles of temperature gradient, chamber pressure and rapid thermal heating in C precursor-rich environment on graphene growth morphology on thin sputtered Cu films were explained. The growth mechanisms of graphene on substrates annealed under reducing and non-reducing environment were explained from the scaling functions of graphene island size distribution in the pre-coalescence regime. It is anticipated that applying the pre-coalescence size distribution method presented in this work to other 2D material systems may be useful for elucidating atomistic mechanisms of film growth that are otherwise difficult to obtain.
The closely-packed monolayer formation of diatom valves on silicon substrates was accomplished using their hydrodynamic properties and the surface tension of water. Valves dispersed on a hydrophobic surface were able to float-up with a preferential orientation (convex side facing the water surface) when water was added. The floating diatom monolayer was subsequently transferred to a silicon substrate. A closely-packed diatom monolayer on the silicon substrate was obtained after the water evaporated at room temperature.
The diatom monolayer was then directly bonded onto the substrate via a sintering process at high temperature in air. The percentage of bonded valves increased as the temperature increased. The valves started to sinter into the substrate at 1100°C. The sintering process caused shrinkage of the nanopores at temperatures above 1100°C. The more delicate structure was more sensitive to the elevated temperature. The cribellum, the most intricate nanostructure of the diatom (~50 nm), disappeared at 1125°C. The cribrum, consisting of approximated 100-300 nm diameter pores, disappeared at 1150°C. The areola, the micro-chamber-liked structure, can survive up to 1150°C. At 1200°C, the complete nanostructure was destroyed. In addition, cross-section images revealed that the valves fused into the thermally-grown oxide layer that was generated on the substrate at high temperatures.
The silica-sintered diatom close-packed monolayer, processed at 1125°C, was magnesiothermically converted into porous silicon using magnesium silicide. X-ray diffraction, infrared absorption, energy dispersive X-say spectra and secondary electron images confirmed the formation of a Si layer with preserved diatom nano-microstructure. The conversion process and subsequent application of a PEDOT:PSS coating both decreased the light reflection from the sample. The photocurrent and reflectance spectra revealed that the Si-diatom dominantly enhanced light absorption between 414 to 586 nm and 730 to 800 nm. Though some of the structural features disappeared during the sintering process, the diatom is still able to improve light absorption. Therefore, the sintering process can be used for diatom direct bonding in light harvesting applications.
Ultrasonic transducer stacks (modules), which had failed or passed during pulse-echo sensitivity testing, were received from Consortium X. With limited background information on these stacks, the central theme was to determine the origin(s) of failure via the use of thermal and physicochemical characterization techniques.
The optical and scanning electron microscopy revealed that contact electrode layers are discontinuous in all samples, while delaminations between electrodes and pad layer were observed in failed samples. The X-ray diffraction data on the pad PZT revealed an overall c/a ratio of 1.022 ratio and morphotropic boundary composition, with significant variations of the Zr to Ti ratio within a sample and between samples. Electron probe microanalysis confirmed that the overall Zr to Ti ratio of the pad PZT was 52/48, and higher amounts of excess PbO in failed samples, whereas, inductively coupled plasma mass spectrometry revealed the presence of Mn, Al, and Sb (dopants) and presence of Cu (sintering aid) in in this hard (pad) PZT. Additionally, three exothermic peaks during thermal analysis was indicative of incomplete calcination of pad PZT. Moreover, transmission electron microscopy and scanning transmission electron microscopy revealed the presence of parylene at the Ag-pad PZT interface and within the pores of pad PZT (in failed samples subjected to electric fields). This further dilutes the electrical, mechanical, and electromechanical properties of the pad PZT, which in turn detrimentally influences the pulse echo sensitivity.