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Emission of CO2 into the atmosphere has become an increasingly concerning issue as we progress into the 21st century Flue gas from coal-burning power plants accounts for 40% of all carbon dioxide emissions. The key to successful separation and sequestration is to separate CO2 directly from flue gas (10-15% CO2, 70% N2), which can range from a few hundred to as high as 1000°C. Conventional microporous membranes (carbons/silicas/zeolites) are capable of separating CO2 from N2 at low temperatures, but cannot achieve separation above 200°C. To overcome the limitations of microporous membranes, a novel ceramic-carbonate dual-phase membrane for high temperature CO2 separation was proposed. The membrane was synthesized from porous La0.6Sr0.4Co0.8Fe0.2O3-d (LSCF) supports and infiltrated with molten carbonate (Li2CO3/Na2CO3/K2CO3). The CO2 permeation mechanism involves a reaction between CO2 (gas phase) and O= (solid phase) to form CO3=, which is then transported through the molten carbonate (liquid phase) to achieve separation. The effects of membrane thickness, temperature and CO2 partial pressure were studied. Decreasing thickness from 3.0 to 0.375 mm led to higher fluxes at 900°C, ranging from 0.186 to 0.322 mL.min-1.cm-2 respectively. CO2 flux increased with temperature from 700 to 900°C. Activation energy for permeation was similar to that for oxygen ion conduction in LSCF. For partial pressures above 0.05 atm, the membrane exhibited a nearly constant flux. From these observations, it was determined that oxygen ion conductivity limits CO2 permeation and that the equilibrium oxygen vacancy concentration in LSCF is dependent on the partial pressure of CO2 in the gas phase. Finally, the dual-phase membrane was used as a membrane reactor. Separation at high temperatures can produce warm, highly concentrated streams of CO2 that could be used as a chemical feedstock for the synthesis of syngas (H2 + CO). Towards this, three different membrane reactor configurations were examined: 1) blank system, 2) LSCF catalyst and 3) 10% Ni/y-alumina catalyst. Performance increased in the order of blank system < LSCF catalyst < Ni/y-alumina catalyst. Favorable conditions for syngas production were high temperature (850°C), low sweep gas flow rate (10 mL.min-1) and high methane concentration (50%) using the Ni/y-alumina catalyst.
ContributorsAnderson, Matthew Brandon (Author) / Lin, Jerry (Thesis advisor) / Alford, Terry (Committee member) / Rege, Kaushal (Committee member) / Anderson, James (Committee member) / Rivera, Daniel (Committee member) / Arizona State University (Publisher)
Created2011
Description
Thin films of ever reducing thickness are used in a plethora of applications and their performance is highly dependent on their microstructure. Computer simulations could then play a vital role in predicting the microstructure of thin films as a function of processing conditions. FACET is one such software tool designed by our research group to model polycrystalline thin film growth, including texture evolution and grain growth of polycrystalline films in 2D. Several modifications to the original FACET code were done to enhance its usability and accuracy. Simulations of sputtered silver thin films are presented here with FACET 2.0 with qualitative and semi-quantitative comparisons with previously published experimental results. Comparisons of grain size, texture and film thickness between simulations and experiments are presented which describe growth modes due to various deposition factors like flux angle and substrate temperature. These simulations provide reasonable agreement with the experimental data over a diverse range of process parameters. Preliminary experiments in depositions of Silver films are also attempted with varying substrates and thickness in order to generate complementary experimental and simulation studies of microstructure evolution. Overall, based on the comparisons, FACET provides interesting insights into thin film growth processes, and the effects of various deposition conditions on thin film structure and microstructure. Lastly, simple molecular dynamics simulations of deposition on bi-crystals are attempted for gaining insight into texture based grain competition during film growth. These simulations predict texture based grain coarsening mechanisms like twinning and grain boundary migration that have been commonly reported in FCC films.
ContributorsRairkar, Asit (Author) / Adams, James B (Thesis advisor) / Krause, Stephen (Committee member) / Alford, Terry (Committee member) / Arizona State University (Publisher)
Created2011
Description
Programmable metallization cell (PMC) technology is based on an electrochemical phenomenon in which a metallic electrodeposit can be grown or dissolved between two electrodes depending on the voltage applied between them. Devices based on this phenomenon exhibit a unique, self-healing property, as a broken metallic structure can be healed by applying an appropriate voltage between the two broken ends. This work explores methods of fabricating interconnects and switches based on PMC technology on flexible substrates. The objective was the evaluation of the feasibility of using this technology in flexible electronics applications in which reliability is a primary concern. The re-healable property of the interconnect is characterized for the silver doped germanium selenide (Ag-Ge-Se) solid electrolyte system. This property was evaluated by measuring the resistances of the healed interconnect structures and comparing these to the resistances of the unbroken structures. The reliability of the interconnects in both unbroken and healed states is studied by investigating the resistances of the structures to DC voltages, AC voltages and different temperatures as a function of time. This work also explores replacing silver with copper for these interconnects to enhance their reliability. A model for PMC-based switches on flexible substrates is proposed and compared to the observed device behavior with the objective of developing a formal design methodology for these devices. The switches were subjected to voltage sweeps and their resistance was investigated as a function of sweep voltage. The resistance of the switches as a function of voltage pulse magnitude when placed in series with a resistance was also investigated. A model was then developed to explain the behavior of these devices. All observations were based on statistical measurements to account for random errors. The results of this work demonstrate that solid electrolyte based interconnects display self-healing capability, which depends on the applied healing voltage and the current limit. However, they fail at lower current densities than metal interconnects due to an ion-drift induced failure mechanism. The results on the PMC based switches demonstrate that a model comprising a Schottky diode in parallel with a variable resistor predicts the behavior of the device.
ContributorsBaliga, Sunil Ravindranath (Author) / Kozicki, Michael N (Thesis advisor) / Schroder, Dieter K. (Committee member) / Chae, Junseok (Committee member) / Alford, Terry L. (Committee member) / Arizona State University (Publisher)
Created2011
Description
Chalcogenide glass (ChG) materials have gained wide attention because of their applications in conductive bridge random access memory (CBRAM), phase change memories (PC-RAM), optical rewritable disks (CD-RW and DVD-RW), microelectromechanical systems (MEMS), microfluidics, and optical communications. One of the significant properties of ChG materials is the change in the resistivity of the material when a metal such as Ag or Cu is added to it by diffusion. This study demonstrates the potential radiation-sensing capabilities of two metal/chalcogenide glass device configurations. Lateral and vertical device configurations sense the radiation-induced migration of Ag+ ions in germanium selenide glasses via changes in electrical resistance between electrodes on the ChG. Before irradiation, these devices exhibit a high-resistance `OFF-state' (in the order of 10E12) but following irradiation, with either 60-Co gamma-rays or UV light, their resistance drops to a low-resistance `ON-state' (around 10E3). Lateral devices have exhibited cyclical recovery with room temperature annealing of the Ag doped ChG, which suggests potential uses in reusable radiation sensor applications. The feasibility of producing inexpensive flexible radiation sensors has been demonstrated by studying the effects of mechanical strain and temperature stress on sensors formed on flexible polymer substrate. The mechanisms of radiation-induced Ag/Ag+ transport and reactions in ChG have been modeled using a finite element device simulator, ATLAS. The essential reactions captured by the simulator are radiation-induced carrier generation, combined with reduction/oxidation for Ag species in the chalcogenide film. Metal-doped ChGs are solid electrolytes that have both ionic and electronic conductivity. The ChG based Programmable Metallization Cell (PMC) is a technology platform that offers electric field dependent resistance switching mechanisms by formation and dissolution of nano sized conductive filaments in a ChG solid electrolyte between oxidizable and inert electrodes. This study identifies silver anode agglomeration in PMC devices following large radiation dose exposure and considers device failure mechanisms via electrical and material characterization. The results demonstrate that by changing device structural parameters, silver agglomeration in PMC devices can be suppressed and reliable resistance switching may be maintained for extremely high doses ranging from 4 Mrad(GeSe) to more than 10 Mrad (ChG).
ContributorsDandamudi, Pradeep (Author) / Kozicki, Michael N (Thesis advisor) / Barnaby, Hugh J (Committee member) / Holbert, Keith E. (Committee member) / Goryll, Michael (Committee member) / Arizona State University (Publisher)
Created2013
Description
Carrier lifetime is one of the few parameters which can give information about the low defect densities in today's semiconductors. In principle there is no lower limit to the defect density determined by lifetime measurements. No other technique can easily detect defect densities as low as 10-9 - 10-10 cm-3 in a simple, contactless room temperature measurement. However in practice, recombination lifetime τr measurements such as photoconductance decay (PCD) and surface photovoltage (SPV) that are widely used for characterization of bulk wafers face serious limitations when applied to thin epitaxial layers, where the layer thickness is smaller than the minority carrier diffusion length Ln. Other methods such as microwave photoconductance decay (µ-PCD), photoluminescence (PL), and frequency-dependent SPV, where the generated excess carriers are confined to the epitaxial layer width by using short excitation wavelengths, require complicated configuration and extensive surface passivation processes that make them time-consuming and not suitable for process screening purposes. Generation lifetime τg, typically measured with pulsed MOS capacitors (MOS-C) as test structures, has been shown to be an eminently suitable technique for characterization of thin epitaxial layers. It is for these reasons that the IC community, largely concerned with unipolar MOS devices, uses lifetime measurements as a "process cleanliness monitor." However when dealing with ultraclean epitaxial wafers, the classic MOS-C technique measures an effective generation lifetime τg eff which is dominated by the surface generation and hence cannot be used for screening impurity densities. I have developed a modified pulsed MOS technique for measuring generation lifetime in ultraclean thin p/p+ epitaxial layers which can be used to detect metallic impurities with densities as low as 10-10 cm-3. The widely used classic version has been shown to be unable to effectively detect such low impurity densities due to the domination of surface generation; whereas, the modified version can be used suitably as a metallic impurity density monitoring tool for such cases.
ContributorsElhami Khorasani, Arash (Author) / Alford, Terry (Thesis advisor) / Goryll, Michael (Committee member) / Bertoni, Mariana (Committee member) / Arizona State University (Publisher)
Created2013
Description
ABSTRACT Along with the fast development of science and technology, the studied materials are becoming more complicated and smaller. All these achievements have advanced with the fast development of powerful tools currently, such as Scanning electron microscopy (SEM), Focused Ion Beam (FIB), Transmission electron microscopy (TEM), Energy dispersive X-ray spectroscopy (EDX), Electron energy loss spectroscopy (EELS) and so on. SiTiO3 thin film, which is grown on Si (100) single crystals, attracts a lot of interest in its structural and electronic properties close to its interface. Valence EELS is used to investigate the Plasmon excitations of the ultrathin SrTiO3 thin film which is sandwiched between amorphous Si and crystalline Si layers. On the other hand, theoretical simulations based on dielectric functions have been done to interpret the experimental results. Our findings demonstrate the value of valence electron energy-loss spectroscopy in detecting a local change in the effective electron mass. Recently it is reported that ZnO-LiYbO2 hybrid phosphor is an efficient UV-infrared convertor for silicon solar cell but the mechanism is still not very clear. The microstructure of Li and Yb co-doped ZnO has been studied by SEM and EDX, and our results suggest that a reaction (or diffusion) zone is very likely to exist between LiYbO2 and ZnO. Such diffusion regions may be responsible for the enhanced infrared emission in the Yb and Li co-doped ZnO. Furthermore, to help us study the diffusion zone under TEM in future, the radiation damage on synthesized LiYbO2 has been studied at first, and then the electronic structure of the synthesized LiYbO2 is compared with Yb2O3 experimentally and theoretically, by EELS and FEFF8 respectively.
ContributorsYang, Bo (Author) / Alford, Terry (Thesis advisor) / Jiang, Nan (Committee member) / Theodore, N. David (Committee member) / Arizona State University (Publisher)
Created2013
Description
Advances in software and applications continue to demand advances in memory. The ideal memory would be non-volatile and have maximal capacity, speed, retention time, endurance, and radiation hardness while also having minimal physical size, energy usage, and cost. The programmable metallization cell (PMC) is an emerging memory technology that is likely to surpass flash memory in all the listed ideal memory characteristics. A comprehensive physics-based model is needed to fully understand PMC operation and aid in design optimization. With the intent of advancing the PMC modeling effort, this thesis presents two simulation models for the PMC. The first model is a finite element model based on Silvaco Atlas finite element analysis software. Limitations of the software are identified that make this model inconsistent with the operating mechanism of the PMC. The second model is a physics-based numerical model developed for the PMC. This model is successful in matching data measured from a chalcogenide glass PMC designed and manufactured at ASU. Matched operating characteristics observable in the current and resistance vs. voltage data include the OFF/ON resistances and write/erase and electrodeposition voltage thresholds. Multilevel programming is also explained and demonstrated with the numerical model. The numerical model has already proven useful by revealing some information presented about the operation and characteristics of the PMC.
ContributorsOleksy, David Ryan (Author) / Barnaby, Hugh J (Thesis advisor) / Kozicki, Michael N (Committee member) / Edwards, Arthur H (Committee member) / Arizona State University (Publisher)
Created2013
Description
As crystalline silicon solar cells continue to get thinner, the recombination of carriers at the surfaces of the cell plays an ever-important role in controlling the cell efficiency. One tool to minimize surface recombination is field effect passivation from the charges present in the thin films applied on the cell surfaces. The focus of this work is to understand the properties of charges present in the SiNx films and then to develop a mechanism to manipulate the polarity of charges to either negative or positive based on the end-application. Specific silicon-nitrogen dangling bonds (·Si-N), known as K center defects, are the primary charge trapping defects present in the SiNx films. A custom built corona charging tool was used to externally inject positive or negative charges in the SiNx film. Detailed Capacitance-Voltage (C-V) measurements taken on corona charged SiNx samples confirmed the presence of a net positive or negative charge density, as high as +/- 8 x 1012 cm-2, present in the SiNx film. High-energy (~ 4.9 eV) UV radiation was used to control and neutralize the charges in the SiNx films. Electron-Spin-Resonance (ESR) technique was used to detect and quantify the density of neutral K0 defects that are paramagnetically active. The density of the neutral K0 defects increased after UV treatment and decreased after high temperature annealing and charging treatments. Etch-back C-V measurements on SiNx films showed that the K centers are spread throughout the bulk of the SiNx film and not just near the SiNx-Si interface. It was also shown that the negative injected charges in the SiNx film were stable and present even after 1 year under indoor room-temperature conditions. Lastly, a stack of SiO2/SiNx dielectric layers applicable to standard commercial solar cells was developed using a low temperature (< 400 °C) PECVD process. Excellent surface passivation on FZ and CZ Si substrates for both n- and p-type samples was achieved by manipulating and controlling the charge in SiNx films.
ContributorsSharma, Vivek (Author) / Bowden, Stuart (Thesis advisor) / Schroder, Dieter (Committee member) / Honsberg, Christiana (Committee member) / Roedel, Ronald (Committee member) / Alford, Terry (Committee member) / Arizona State University (Publisher)
Created2013
Description
Ball Grid Array (BGA) using lead-free or lead-rich solder materials are widely used as Second Level Interconnects (SLI) in mounting packaged components to the printed circuit board (PCB). The reliability of these solder joints is of significant importance to the performance of microelectronics components and systems. Product design/form-factor, solder material, manufacturing process, use condition, as well as, the inherent variabilities present in the system, greatly influence product reliability. Accurate reliability analysis requires an integrated approach to concurrently account for all these factors and their synergistic effects. Such an integrated and robust methodology can be used in design and development of new and advanced microelectronics systems and can provide significant improvement in cycle-time, cost, and reliability. IMPRPK approach is based on a probabilistic methodology, focusing on three major tasks of (1) Characterization of BGA solder joints to identify failure mechanisms and obtain statistical data, (2) Finite Element analysis (FEM) to predict system response needed for life prediction, and (3) development of a probabilistic methodology to predict the reliability, as well as, the sensitivity of the system to various parameters and the variabilities. These tasks and the predictive capabilities of IMPRPK in microelectronic reliability analysis are discussed.
ContributorsFallah-Adl, Ali (Author) / Tasooji, Amaneh (Thesis advisor) / Krause, Stephen (Committee member) / Alford, Terry (Committee member) / Jiang, Hanqing (Committee member) / Mahajan, Ravi (Committee member) / Arizona State University (Publisher)
Created2013
Description
The dissolution of metal layers such as silver into chalcogenide glass layers such as germanium selenide changes the resistivity of the metal and chalcogenide films by a great extent. It is known that the incorporation of the metal can be achieved by ultra violet light exposure or thermal processes. In this work, the use of metal dissolution by exposure to gamma radiation has been explored for radiation sensor applications. Test structures were designed and a process flow was developed for prototype sensor fabrication. The test structures were designed such that sensitivity to radiation could be studied. The focus is on the effect of gamma rays as well as ultra violet light on silver dissolution in germanium selenide (Ge30Se70) chalcogenide glass. Ultra violet radiation testing was used prior to gamma exposure to assess the basic mechanism. The test structures were electrically characterized prior to and post irradiation to assess resistance change due to metal dissolution. A change in resistance was observed post irradiation and was found to be dependent on the radiation dose. The structures were also characterized using atomic force microscopy and roughness measurements were made prior to and post irradiation. A change in roughness of the silver films on Ge30Se70 was observed following exposure. This indicated the loss of continuity of the film which causes the increase in silver film resistance following irradiation. Recovery of initial resistance in the structures was also observed after the radiation stress was removed. This recovery was explained with photo-stimulated deposition of silver from the chalcogenide at room temperature confirmed with the re-appearance of silver dendrites on the chalcogenide surface. The results demonstrate that it is possible to use the metal dissolution effect in radiation sensing applications.
ContributorsChandran, Ankitha (Author) / Kozicki, Michael N (Thesis advisor) / Holbert, Keith E. (Committee member) / Barnaby, Hugh (Committee member) / Arizona State University (Publisher)
Created2012