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Description
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
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
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
Programmable Metallization Cell (PMC) is a resistance-switching device based on migration of nanoscale quantities of cations in a solid electrolyte and formation of a conducting electrodeposit by the reductions of these cations. This dissertation presents electrical characterization results on Cu-SiO2 based PMC devices, which due to the na- ture of materials can be easily integrated into the current Complimentary metal oxide semiconductor (CMOS) process line. Device structures representing individual mem- ory cells based on W bottom electrode and n-type Si bottom electrode were fabricated for characterization. For the W bottom electrode based devices, switching was ob- served for voltages in the range of 500mV and current value as low as 100 nA showing the electrochemical nature and low power potential. The ON state showed a direct de- pendence on the programming current, showing the possibility of multi-bit storage in a single cell. Room temperature retention was demonstrated in excess of 105 seconds and endurance to approximately 107 cycles. Switching was observed for microsecond duration 3 V amplitude pulses. Material characterization results from Raman, X-ray diffraction, Rutherford backscattering and Secondary-ion mass spectroscopy analysis shows the influence of processing conditions on the Cu concentration within the film and also the presence of Cu as free atoms. The results seemed to indicate stress-induced void formation in the SiO2 matrix as the driving mechanism for Cu diffusion into the SiO2 film. Cu/SiO2
Si based PMC devices were characterized and were shown to have inherent isolation characteristics, proving the feasibility of such a structure for a passive array. The inherent isolation property simplifies fabrication by avoiding the need for a separate diode element in an array. The isolation characteristics were studied mainly in terms of the leakage current. The nature of the diode interface was further studied by extracting a barrier potential which shows it can be approximated to a Cu-nSi metal semiconductor Schottky diode.
Si based PMC devices were characterized and were shown to have inherent isolation characteristics, proving the feasibility of such a structure for a passive array. The inherent isolation property simplifies fabrication by avoiding the need for a separate diode element in an array. The isolation characteristics were studied mainly in terms of the leakage current. The nature of the diode interface was further studied by extracting a barrier potential which shows it can be approximated to a Cu-nSi metal semiconductor Schottky diode.
ContributorsPuthenthermadam, Sarath (Author) / Kozicki, Michael N (Thesis advisor) / Diaz, Rodolfo (Committee member) / Schroder, Dieter K. (Committee member) / Alford, Terry (Committee member) / Arizona State University (Publisher)
Created2011
Description
Transparent conductive oxides (TCOs) are used as electrodes for a number of optoelectronic devices including solar cells. Because of its superior transparent and conductive properties, indium (In) tin (Sn) oxide (ITO) has long been at the forefront for TCO research activities and high-volume product applications. However, given the limited supply of In and potential toxicity of Sn-based compounds, attention has shifted to alternative TCOs like ZnO doped with group-III elements such as Ga and Al. Employing a variety of deposition techniques, many research groups are striving to achieve resistivities below 1E-4 ohm-cm with transmittance approaching the theoretical limit over a wide spectral range. In this work, Ga-doped ZnO is deposited using pulsed laser deposition (PLD). Material properties of the films are characterized using a number of techniques. For deposition in oxygen at pressures >1 mTorr, post-deposition annealing in forming gas (FG) is required to improve conductivity. At these higher oxygen pressures, thermodynamic analysis coupled with a study using the Hall effect measurements and photoluminescence spectroscopy suggest that conductivity is limited by oxygen-related acceptor-like defects in the grains that compensate donors, effectively reducing the net carrier concentration and creating scattering centers that reduce electron mobility. Oxygen is also responsible for further suppression of conductivity by forming insulative metal oxide regions at the grain edges and oxygen-related electron traps at the grain boundaries. The hydrogen component in the FG is thought to passivate the intra-grain acceptor-like defects and improve carrier transport across these grain boundaries. Given this deleterious effect of oxygen on conductivity, depositions are performed in pure argon (Ar), i.e., the only oxygen species in the growth ambient are those ejected directly from the PLD solid source target. Ga-doped ZnO deposited in Ar at 200 °C and 10 mTorr have resistivities of 1.8E-4 ohm-cm without the need for post deposition annealing. Average transmittance of the Ga-doped films is 93% over the visible and near infrared (IR) spectral regions, but free carrier absorption is a limiting factor further into the IR. After annealing in FG at 500 °C, a 300 nm Ar film has a Haacke figure of merit of 6.61E-2 sq. ohm.
ContributorsScott, Robin Charis (Author) / Zhang, Yong Hang (Thesis advisor) / Alford, Terry (Committee member) / Krause, Stephen (Committee member) / Leedy, Kevin (Committee member) / Arizona State University (Publisher)
Created2011
Description
Silicon carbide (SiC), long touted as a material that can satisfy the specific property requirements for high temperature and high power applications, was studied quantitatively using various techniques. The electronic band structure of 4H SiC is examined in the first half of this dissertation. A brief introduction to band structure calculations, with particular emphasis on the empirical pseudopotential method, is given as a foundation for the subsequent work. Next, the crystal pseudopotential for 4H SiC is derived in detail, and a novel approach using a genetic algorithm search routine is employed to find the fitting parameters needed to generate the band structure. Using this technique, the band structure is fitted to experimentally measured energy band gaps giving an indirect band gap energy of 3.28 eV, and direct f¡, M, K and L energy transitions of 6.30, 4.42, 7.90 and 6.03 eV, respectively. The generated result is also shown to give effective mass values of mMf¡*=0.66m0, mMK*=0.31m0, mML*=0.34m0, in close agreement with experimental results. The second half of this dissertation discusses computational work in finding the electron Hall mobility and Hall scattering factor for 6H SiC. This disscussion begins with an introductory chapter that gives background on how scattering rates are dervied and the specific expressions for important mechanisms. The next chapter discusses mobility calculations for 6H SiC in particular, beginnning with Rode's method to solve the Boltzmann transport equation. Using this method and the transition rates of the previous chapter, an acoustic deformation potential DA value of 5.5 eV, an inter-valley phonon deformation potential Dif value of 1.25~1011 eV/m and inter-valley phonon energy ℏfÖif of 65 meV that simultaneously fit experimental data on electron Hall mobility and Hall scattering factor was found.
ContributorsNg, Garrick (Author) / Schroder, Dieter K. (Thesis advisor) / Vasileska, Dragica (Committee member) / Skromme, Brian (Committee member) / Alford, Terry (Committee member) / Marinella, Matthew (Committee member) / Arizona State University (Publisher)
Created2010
Description
Metal-organic frameworks (MOFs) are a new set of porous materials comprised of metals or metal clusters bonded together in a coordination system by organic linkers. They are becoming popular for gas separations due to their abilities to be tailored toward specific applications. Zirconium MOFs in particular are known for their high stability under standard temperature and pressure due to the strength of the Zirconium-Oxygen coordination bond. However, the acid modulator needed to ensure long range order of the product also prevents complete linker deprotonation. This leads to a powder product that cannot easily be incorporated into continuous MOF membranes. This study therefore implemented a new bi-phase synthesis technique with a deprotonating agent to achieve intergrowth in UiO-66 membranes. Crystal intergrowth will allow for effective gas separations and future permeation testing. During experimentation, successful intergrown UiO-66 membranes were synthesized and characterized. The degree of intergrowth and crystal orientations varied with changing deprotonating agent concentration, modulator concentration, and ligand:modulator ratios. Further studies will focus on achieving the same results on porous substrates.
ContributorsClose, Emily Charlotte (Author) / Mu, Bin (Thesis director) / Shan, Bohan (Committee member) / Chemical Engineering Program (Contributor) / Barrett, The Honors College (Contributor)
Created2016-12
Description
Wide Bandgap (WBG) semiconductor materials are shaping day-to-day technologyby introducing powerful and more energy responsible devices. These materials have
opened the door for building basic semiconductor devices which are superior in terms of
handling high voltages, high currents, power, and temperature which is not possible using
conventional silicon technology. As the research continues in the field of WBG based
devices, there is a potential chance that the power electronics industry can save billions of
dollars deploying energy-efficient circuits in high power conversion electronics. Diamond,
silicon carbide and gallium nitride are the top three contenders among which diamond can
significantly outmatch others in a variety of properties. However, diamond technology is
still in its early phase of development and there are challenges involved in many aspects of
processing a successful integrated circuit. The work done in this research addresses three
major aspects of problems related to diamond technology. In the first part, the applicability
of compact modeling and Technology Computer-Aided Design (TCAD) modeling
technique for diamond Schottky p-i-n diodes has been demonstrated. The compact model
accurately predicts AC, DC and nonlinear behavior of the diode required for fast circuit
simulation. Secondly, achieving low resistance ohmic contact onto n-type diamond is one
of the major issues that is still an open research problem as it determines the performance
of high-power RF circuits and switching losses in power converters circuits. So, another
portion of this thesis demonstrates the achievement of very low resistance ohmic contact
(~ 10-4 Ω⋅cm2) onto n-type diamond using nano crystalline carbon interface layer. Using
the developed TCAD and compact models for low resistance contacts, circuit level
predictions show improvements in RF performance. Lastly, an initial study of breakdown
characteristics of diamond and cubic boron nitride heterostructure is presented. This study
serves as a first step for making future transistors using diamond and cubic boron nitride –
a very less explored material system in literature yet promising for extreme circuit
applications involving high power and temperature.
ContributorsJHA, VISHAL (Author) / Thornton, Trevor (Thesis advisor) / Goodnick, Stephen (Committee member) / Nemanich, Robert (Committee member) / Alford, Terry (Committee member) / Hoque, Mazhar (Committee member) / Arizona State University (Publisher)
Created2023
Description
Global photovoltaic (PV) module installation in 2018 is estimated to exceed 100 GW, and crystalline Si (c-Si) solar cell-based modules have a share more than 90% of the global PV market. To reduce the social cost of PV electricity, further developments in reliability of solar panels are expected. These will lead to realize longer module lifetime and reduced levelized cost of energy. As many as 86 failure modes are observed in PV modules [1] and series resistance increase is one of the major durability issues of all. Series resistance constitutes emitter sheet resistance, metal-semiconductor contact resistance, and resistance across the metal-solder ribbon. Solder bond degradation at the cell interconnect is one of the primary causes for increase in series resistance, which is also considered to be an invisible defect [1]. Combination of intermetallic compounds (IMC) formation during soldering and their growth due to solid state diffusion over its lifetime result in formation of weak interfaces between the solar cell and the interconnect. Thermal cycling under regular operating conditions induce thermo-mechanical fatigue over these weak interfaces resulting in contact reduction or loss. Contact reduction or loss leads to increase in series resistance which further manifests into power and fill factor loss. The degree of intermixing of metallic interfaces and contact loss depends on climatic conditions as temperature and humidity (moisture ingression into the PV module laminate) play a vital role in reaction kinetics of these layers. Modules from Arizona and Florida served as a good sample set to analyze the effects of hot and humid climatic conditions respectively. The results obtained in the current thesis quantifies the thickness of IMC formation from SEM-EDS profiles, where similar modules obtained from different climatic conditions were compared. The results indicate the thickness of the IMC and detachment degree to be growing with age and operating temperatures of the module. This can be seen in CuxSny IMC which is thicker in the case of Arizona module. The results obtained from FL
ii
aged modules also show that humidity accelerates the formation of IMC as they showed thicker AgxSny layer and weak interconnect-contact interfaces as compared to Arizona modules. It is also shown that climatic conditions have different effects on rate at which CuxSny and AgxSny intermetallic compounds are formed.
ii
aged modules also show that humidity accelerates the formation of IMC as they showed thicker AgxSny layer and weak interconnect-contact interfaces as compared to Arizona modules. It is also shown that climatic conditions have different effects on rate at which CuxSny and AgxSny intermetallic compounds are formed.
ContributorsBuddha, Viswa Sai Pavan (Author) / Tamizhmani, Govindasamy (Thesis advisor) / Alford, Terry (Thesis advisor) / Srinivasan, Devarajan (Committee member) / Arizona State University (Publisher)
Created2018
Description
Recent technology advancements in photovoltaics have enabled crystalline silicon (c-Si) solar cells to establish outstanding photoconversion efficiency records. Remarkable progresses in research and development have been made both on the silicon feedstock quality as well as the technology required for surface passivation, the two dominant sources of performance loss via recombination of photo-generated charge carriers within advanced solar cell architectures.
As these two aspects of the solar cell framework improve, the need for a thorough analysis of their respective contribution under varying operation conditions has emerged along with challenges related to the lack of sensitivity of available characterization techniques. The main objective of my thesis work has been to establish a deep understanding of both “intrinsic” and “extrinsic” recombination processes that govern performance in high-quality silicon absorbers. By studying each recombination mechanism as a function of illumination and temperature, I strive to identify the lifetime limiting defects and propose a path to engineer the ultimate silicon solar cell.
This dissertation presents a detailed description of the experimental procedure required to deconvolute surface recombination contributions from bulk recombination contributions when performing lifetime spectroscopy analysis. This work proves that temperature- and injection-dependent lifetime spectroscopy (TIDLS) sensitivity can be extended to impurities concentrations down to 109 cm-3, orders of magnitude below any other characterization technique available today. A new method for the analysis of TIDLS data denominated Defect Parameters Contour Mapping (DPCM) is presented with the aim of providing a visual and intuitive tool to identify the lifetime limiting impurities in silicon material. Surface recombination velocity results are modelled by applying appropriate approaches from literature to our experimentally evaluated data, demonstrating for the first time their capability to interpret temperature-dependent data. In this way, several new results are obtained which solve long disputed aspects of surface passivation mechanisms. Finally, we experimentally evaluate the temperature-dependence of Auger lifetime and its impact on a theoretical intrinsically limited solar cell. These results decisively point to the need for a new Auger lifetime parameterization accounting for its temperature-dependence, which would in turn help understand the ultimate theoretical efficiency limit for a solar cell under real operation conditions.
As these two aspects of the solar cell framework improve, the need for a thorough analysis of their respective contribution under varying operation conditions has emerged along with challenges related to the lack of sensitivity of available characterization techniques. The main objective of my thesis work has been to establish a deep understanding of both “intrinsic” and “extrinsic” recombination processes that govern performance in high-quality silicon absorbers. By studying each recombination mechanism as a function of illumination and temperature, I strive to identify the lifetime limiting defects and propose a path to engineer the ultimate silicon solar cell.
This dissertation presents a detailed description of the experimental procedure required to deconvolute surface recombination contributions from bulk recombination contributions when performing lifetime spectroscopy analysis. This work proves that temperature- and injection-dependent lifetime spectroscopy (TIDLS) sensitivity can be extended to impurities concentrations down to 109 cm-3, orders of magnitude below any other characterization technique available today. A new method for the analysis of TIDLS data denominated Defect Parameters Contour Mapping (DPCM) is presented with the aim of providing a visual and intuitive tool to identify the lifetime limiting impurities in silicon material. Surface recombination velocity results are modelled by applying appropriate approaches from literature to our experimentally evaluated data, demonstrating for the first time their capability to interpret temperature-dependent data. In this way, several new results are obtained which solve long disputed aspects of surface passivation mechanisms. Finally, we experimentally evaluate the temperature-dependence of Auger lifetime and its impact on a theoretical intrinsically limited solar cell. These results decisively point to the need for a new Auger lifetime parameterization accounting for its temperature-dependence, which would in turn help understand the ultimate theoretical efficiency limit for a solar cell under real operation conditions.
ContributorsBernardini, Simone (Author) / Bertoni, Mariana I (Thesis advisor) / Coletti, Gianluca (Committee member) / Bowden, Stuart (Committee member) / Alford, Terry (Committee member) / Arizona State University (Publisher)
Created2018