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This dissertation provides a fundamental understanding of the impact of bulk polymer properties on the nanometer length scale modulus. The elastic modulus of amorphous organic thin films is examined using a surface wrinkling technique. Potential correlations between thin film behavior and intrinsic properties such as flexibility and chain length are explored. Thermal properties, glass transition temperature (Tg) and the coefficient of thermal expansion, are examined along with the moduli of these thin films. It is found that the nanometer length scale behavior of flexible polymers correlates to its bulk Tg and not the polymers intrinsic size. It is also found that decreases in the modulus of ultrathin flexible films is not correlated with the observed Tg decrease in films of the same thickness. Techniques to circumvent reductions from bulk modulus were also demonstrated. However, as chain flexibility is reduced the modulus becomes thickness independent down to 10 nm. Similarly for this series minor reductions in Tg were obtained. To further understand the impact of the intrinsic size and processing conditions; this wrinkling instability was also utilized to determine the modulus of small organic electronic materials at various deposition conditions. Lastly, this wrinkling instability is exploited for development of poly furfuryl alcohol wrinkles. A two-step wrinkling process is developed via an acid catalyzed polymerization of a drop cast solution of furfuryl alcohol and photo acid generator. The ability to control the surface topology and tune the wrinkle wavelength with processing parameters such as substrate temperature and photo acid generator concentration is also demonstrated. Well-ordered linear, circular, and curvilinear patterns are also obtained by selective ultraviolet exposure and polymerization of the furfuryl alcohol film. As a carbon precursor a thorough understanding of this wrinkling instability can have applications in a wide variety of technologies.
ContributorsTorres, Jessica (Author) / Vogt, Bryan D (Thesis advisor) / Stafford, Christopher M (Committee member) / Richert, Ranko (Committee member) / Rege, Kaushal (Committee member) / Dai, Lenore (Committee member) / Arizona State University (Publisher)
Created2011
Description
Current economic conditions necessitate the extension of service lives for a variety of aerospace systems. As a result, there is an increased need for structural health management (SHM) systems to increase safety, extend life, reduce maintenance costs, and minimize downtime, lowering life cycle costs for these aging systems. The implementation of such a system requires a collaborative research effort in a variety of areas such as novel sensing techniques, robust algorithms for damage interrogation, high fidelity probabilistic progressive damage models, and hybrid residual life estimation models. This dissertation focuses on the sensing and damage estimation aspects of this multidisciplinary topic for application in metallic and composite material systems. The primary means of interrogating a structure in this work is through the use of Lamb wave propagation which works well for the thin structures used in aerospace applications. Piezoelectric transducers (PZTs) were selected for this application since they can be used as both sensors and actuators of guided waves. Placement of these transducers is an important issue in wave based approaches as Lamb waves are sensitive to changes in material properties, geometry, and boundary conditions which may obscure the presence of damage if they are not taken into account during sensor placement. The placement scheme proposed in this dissertation arranges piezoelectric transducers in a pitch-catch mode so the entire structure can be covered using a minimum number of sensors. The stress distribution of the structure is also considered so PZTs are placed in regions where they do not fail before the host structure. In order to process the data from these transducers, advanced signal processing techniques are employed to detect the presence of damage in complex structures. To provide a better estimate of the damage for accurate life estimation, machine learning techniques are used to classify the type of damage in the structure. A data structure analysis approach is used to reduce the amount of data collected and increase computational efficiency. In the case of low velocity impact damage, fiber Bragg grating (FBG) sensors were used with a nonlinear regression tool to reconstruct the loading at the impact site.
ContributorsCoelho, Clyde (Author) / Chattopadhyay, Aditi (Thesis advisor) / Dai, Lenore (Committee member) / Wu, Tong (Committee member) / Das, Santanu (Committee member) / Rajadas, John (Committee member) / Papandreou-Suppappola, Antonia (Committee member) / Arizona State University (Publisher)
Created2011
Description
Ordered mesoporous materials have tunable pore sizes between 2 and 50 nm and are characterized by ordered pore structures and high surface areas (~1000 m2/g). This makes them particularly favorable for a number of membrane applications such as protein separation, polymer extrusion, nanowire fabrication and membrane reactors. These membranes can be fabricated as top-layers on macroporous supports or as embedded membranes in a dense matrix. The first part of the work deals with the hydrothermal synthesis and water-vapor/oxygen separation properties of supported MCM-48 and a new Al-MCM-48 type membrane for potential use in air conditioning systems. Knudsen-type permeation is observed in these membranes. The combined effect of capillary condensation and the aluminosilicate matrix resulted in the highest separation factor (142) in Al-MCM-48 membranes, with a water vapor permeance of 6×10-8mol/m2Pas. The second part focuses on synthesis of embedded mesoporous silica membranes with helically ordered pores by a novel Counter Diffusion Self-Assembly (CDSA) method. This method is an extension of the interfacial synthesis method for fiber synthesis using tetrabutylorthosilicate (TBOS) and cetyltrimethylammonium bromide (CTAB) as the silica source and surfactant respectively. The initial part of this study determined the effect of TBOS height and humidity on fiber formation. From this study, the range of TBOS heights for best microscopic and macroscopic ordering were established. Next, the CDSA method was used to successfully synthesize membranes, which were characterized to have good support plugging and an ordered pore structure. Factors that influence membrane synthesis and plug microstructure were determined. SEM studies revealed the presence of gaps between the plugs and support pores, which occur due to shrinking of the plug on drying. Development of a novel liquid deposition method to seal these defects constituted the last part of this work. Post sealing, excess silica was removed by etching with hydrofluoric acid. Membrane quality was evaluated at each step using SEM and gas permeation measurements. After surfactant removal by liquid extraction, the membranes exhibited an O2 permeance of 1.65x10-6mol/m2.Pa.s and He/O2 selectivity of 3.30. The successful synthesis of this membrane is an exciting new development in the area of ordered mesoporous membrane technology.
ContributorsSeshadri, Shriya (Author) / Lin, Jerry Y. S. (Thesis advisor) / Dai, Lenore (Committee member) / Rege, Kaushal (Committee member) / Smith, David J. (Committee member) / Vogt, Bryan (Committee member) / Arizona State University (Publisher)
Created2011
Description
Temporary bonding-debonding of flexible plastic substrates to rigid carriers may facilitate effective substrate handling by automated tools for manufacture of flexible microelectronics. The primary challenges in implementing practical temporary bond-debond technology originate from the stress that is developed during high temperature processing predominately through thermal-mechanical property mismatches between carrier, adhesive and substrate. These stresses are relaxed through bowing of the bonded system (substrate-adhesive-carrier), which causes wafer handling problems, or through delamination of substrate from rigid carrier. Another challenge inherent to flexible plastic substrates and linked to stress is their dimensional instability, which may manifest itself in irreversible deformation upon heating and cooling cycles. Dimensional stability is critical to ensure precise registration of different layers during photolithography. The global objective of this work is to determine comprehensive experimental characterization and develop underlying fundamental engineering concept that could enable widespread adoption and scale-up of temporary bonding processing protocols for flexible microelectronics manufacturing. A series of carriers with different coefficient of thermal expansion (CTE), modulus and thickness were investigated to correlate the thermo-mechanical properties of carrier with deformation behavior of bonded systems. The observed magnitude of system bow scaled with properties of carriers according to well-established Stoney's equation. In addition, rheology of adhesive impacted the deformation of bonded system. In particular, distortion-bowing behavior correlated directly with the relative loss factor of adhesive and flexible plastic substrate. Higher loss factor of adhesive compared to that of substrate allowed the stress to be relaxed with less bow, but led to significantly greater dimensional distortion. Conversely, lower loss factor of adhesive allowed less distortion but led to larger wafer bow. A finite element model using ANSYS was developed to predict the trend in bow-distortion of bonded systems as a function of the viscoelastic properties of adhesive. Inclusion of the viscoelasticity of flexible plastic substrate itself was critical to achieving good agreement between simulation and experiment. Simulation results showed that there is a limited range within which tuning the rheology of adhesive can control the stress-distortion. Therefore, this model can aid in design of new adhesive formulations compatible with different processing requirements of various flexible microelectronics applications.
ContributorsHaq, Jesmin (Author) / Raupp, Gregory B (Thesis advisor) / Vogt, Bryan D (Thesis advisor) / Dai, Lenore (Committee member) / Loy, Douglas (Committee member) / Li, Jian (Committee member) / Arizona State University (Publisher)
Created2011
Description
Mesoporous materials that possess large surface area, tunable pore size, and ordered structures are attractive features for many applications such as adsorption, protein separation, enzyme encapsulation and drug delivery as these materials can be tailored to host different guest molecules. Films provide a model system to understand how the pore orientation impacts the potential for loading and release of selectively sized molecules. This research work aims to develop structure-property relationships to understand how pore size, geometry, and surface hydrophobicity influence the loading and release of drug molecules. In this study, the pore size is systematically varied by incorporating pore-swelling agent of polystyrene oligomers (hPS) to soft templated mesoporous carbon films fabricated by cooperative assembly of poly(styrene-block-ethylene oxide) (SEO) with phenolic resin. To examine the impact of morphology, different compositions of amphiphilic triblock copolymer templates, poly(ethylene oxide)-block-poly(propylene oxide)-block-poly(ethylene oxide) (PEO-PPO-PEO), are used to form two-dimensional hexagonal and cubic mesostructures. Lastly, the carbonization temperature provides a handle to tune the hydrophobicity of the film. These mesoporous films are then utilized to understand the uptake and release of a model drug Mitoxantrone dihydrochloride from nanostructured materials. The largest pore size (6nm) mesoporous carbon based on SEO exhibits the largest uptake (3.5μg/cm2); this is attributed to presence of larger internal volume compared to the other two films. In terms of release, a controlled response is observed for all films with the highest release for the 2nm cubic film (1.45 μg/cm2) after 15 days, but this is only 56 % of the drug loaded. Additionally, the surface hydrophobicity impacts the fraction of drug release with a decrease from 78% to 43%, as the films become more hydrophobic when carbonized at higher temperatures. This work provides a model system to understand how pore morphology, size and chemistry influence the drug loading and release for potential implant applications.
ContributorsLabiano, Alpha (Author) / Vogt, Bryan (Thesis advisor) / Rege, Kaushal (Committee member) / Dai, Lenore (Committee member) / Potta, Thrimoorthy (Committee member) / Arizona State University (Publisher)
Created2011
Description
Biological membranes are critical to cell sustainability by selectively permeating polar molecules into the intracellular space and providing protection to the interior organelles. Biomimetic membranes (model cell membranes) are often used to fundamentally study the lipid bilayer backbone structure of the biological membrane. Lipid bilayer membranes are often supported using inorganic materials in an effort to improve membrane stability and for application to novel biosensing platforms. Published literature has shown that a variety of dense inorganic materials with various surface properties have been investigated for the study of biomimetic membranes. However, literature does not adequately address the effect of porous materials or supports with varying macroscopic geometries on lipid bilayer membrane behavior. The objective of this dissertation is to present a fundamental study on the synthesis of lipid bilayer membranes supported by novel inorganic supports in an effort to expand the number of available supports for biosensing technology. There are two fundamental areas covered including: (1) synthesis of lipid bilayer membranes on porous inorganic materials and (2) synthesis and characterization of cylindrically supported lipid bilayer membranes. The lipid bilayer membrane formation behavior on various porous supports was studied via direct mass adsorption using a quartz crystal microbalance. Experimental results demonstrate significantly different membrane formation behaviors on the porous inorganic supports. A lipid bilayer membrane structure was formed only on SiO2 based surfaces (dense SiO2 and silicalite, basic conditions) and gamma-alumina (acidic conditions). Vesicle monolayer adsorption was observed on gamma-alumina (basic conditions), and yttria stabilized zirconia (YSZ) of varying roughness. Parameters such as buffer pH, surface chemistry and surface roughness were found to have a significant impact on the vesicle adsorption kinetics. Experimental and modeling work was conducted to study formation and characterization of cylindrically supported lipid bilayer membranes. A novel sensing technique (long-period fiber grating refractometry) was utilized to measure the formation mechanism of lipid bilayer membranes on an optical fiber. It was found that the membrane formation kinetics on the fiber was similar to its planar SiO2 counterpart. Fluorescence measurements verified membrane transport behavior and found that characterization artifacts affected the measured transport behavior.
ContributorsEggen, Carrie (Author) / Lin, Jerry Y.S. (Thesis advisor) / Dai, Lenore (Committee member) / Rege, Kaushal (Committee member) / Thornton, Trevor (Committee member) / Vogt, Bryan (Committee member) / Arizona State University (Publisher)
Created2011
Description
The theme for this work is the development of fast numerical algorithms for sparse optimization as well as their applications in medical imaging and source localization using sensor array processing. Due to the recently proposed theory of Compressive Sensing (CS), the $\ell_1$ minimization problem attracts more attention for its ability to exploit sparsity. Traditional interior point methods encounter difficulties in computation for solving the CS applications. In the first part of this work, a fast algorithm based on the augmented Lagrangian method for solving the large-scale TV-$\ell_1$ regularized inverse problem is proposed. Specifically, by taking advantage of the separable structure, the original problem can be approximated via the sum of a series of simple functions with closed form solutions. A preconditioner for solving the block Toeplitz with Toeplitz block (BTTB) linear system is proposed to accelerate the computation. An in-depth discussion on the rate of convergence and the optimal parameter selection criteria is given. Numerical experiments are used to test the performance and the robustness of the proposed algorithm to a wide range of parameter values. Applications of the algorithm in magnetic resonance (MR) imaging and a comparison with other existing methods are included. The second part of this work is the application of the TV-$\ell_1$ model in source localization using sensor arrays. The array output is reformulated into a sparse waveform via an over-complete basis and study the $\ell_p$-norm properties in detecting the sparsity. An algorithm is proposed for minimizing a non-convex problem. According to the results of numerical experiments, the proposed algorithm with the aid of the $\ell_p$-norm can resolve closely distributed sources with higher accuracy than other existing methods.
ContributorsShen, Wei (Author) / Mittlemann, Hans D (Thesis advisor) / Renaut, Rosemary A. (Committee member) / Jackiewicz, Zdzislaw (Committee member) / Gelb, Anne (Committee member) / Ringhofer, Christian (Committee member) / Arizona State University (Publisher)
Created2011
Description
Cancer diseases are among the leading cause of death in the United States. Advanced cancer diseases are characterized by genetic defects resulting in uncontrollable cell growth. Currently, chemotherapeutics are one of the mainstream treatments administered to cancer patients but are less effective if administered in the later stages of metastasis, and can result in unwanted side effects and broad toxicities. Therefore, current efforts have explored gene therapy as an alternative strategy to correct the genetic defects associated with cancer diseases, by administering genes which encode for proteins that result in cell death. While the use of viral vectors shows high level expression of the delivered transgene, the potential for insertion mutagenesis and activation of immune responses raise concern in clinical applications. Non-viral vectors, including cationic lipids and polymers, have been explored as potentially safer alternatives to viral delivery systems. These systems are advantageous for transgene delivery due to ease of synthesis, scale up, versatility, and in some cases due to their biodegradability and biocompatibility. However, low efficacies for transgene expression and high cytotoxicities limit the practical use of these polymers. In this work, a small library of twenty-one cationic polymers was synthesized following a ring opening polymerization of diglycidyl ethers (epoxides) by polyamines. The polymers were screened in parallel and transfection efficacies of individual polymers were compared to those of polyethylenimine (PEI), a current standard for polymer-mediated transgene delivery. Seven lead polymers that demonstrated higher transgene expression efficacies than PEI in pancreatic and prostate cancer cells lines were identified from the screening. A second related effort involved the generation of polymer-antibody conjugates in order to facilitate targeting of delivered plasmid DNA selectively to cancer cells. Future work with the novel lead polymers and polymer-antibody conjugates developed in this research will involve an investigation into the delivery of transgenes encoding for apoptosis-inducing proteins both in vitro and in vivo.
ContributorsVu, Lucas (Author) / Rege, Kaushal (Thesis advisor) / Nielsen, David (Committee member) / Sierks, Michael (Committee member) / Arizona State University (Publisher)
Created2011
Description
This dissertation presents a systematic study of the sorption mechanisms of hydrophobic silica aerogel (Cabot Nanogel®) granules for oil and volatile organic compounds (VOCs) in different phases. The performance of Nanogel for removing oil from laboratory synthetic oil-in-water emulsions and real oily wastewater, and VOCs from their aqueous solution, in both packed bed (PB) and inverse fluidized bed (IFB) modes was also investigated. The sorption mechanisms of VOCs in the vapor, pure liquid, and aqueous solution phases, free oil, emulsified oil, and oil from real wastewater on Nanogel were systematically studied via batch kinetics and equilibrium experiments. The VOC results show that the adsorption of vapor is very slow due to the extremely low thermal conductivity of Nanogel. The faster adsorption rates in the liquid and solution phases are controlled by the mass transport, either by capillary flow or by vapor diffusion/adsorption. The oil results show that Nanogel has a very high capacity for adsorption of pure oils. However, the rate for adsorption of oil from an oil-water emulsion on the Nanogel is 5-10 times slower than that for adsorption of pure oils or organics from their aqueous solutions. For an oil-water emulsion, the oil adsorption capacity decreases with an increasing proportion of the surfactant added. An even lower sorption capacity and a slower sorption rate were observed for a real oily wastewater sample due to the high stability and very small droplet size of the wastewater. The performance of Nanogel granules for removing emulsified oil, oil from real oily wastewater, and toluene at low concentrations in both PB and IFB modes was systematically investigated. The hydrodynamics characteristics of the Nanogel granules in an IFB were studied by measuring the pressure drop and bed expansion with superficial water velocity. The density of the Nanogel granules was calculated from the plateau pressure drop of the IFB. The oil/toluene removal efficiency and the capacity of the Nanogel granules in the PB or IFB were also measured experimentally and predicted by two models based on equilibrium and kinetic batch measurements of the Nanogel granules.
ContributorsWang, Ding (Author) / Lin, Jerry Y.S. (Thesis advisor) / Pfeffer, Robert (Thesis advisor) / Westerhoff, Paul (Committee member) / Nielsen, David (Committee member) / Lind, Mary Laura (Committee member) / Arizona State University (Publisher)
Created2011
Description
Damage assessment and residual useful life estimation (RULE) are essential for aerospace, civil and naval structures. Structural Health Monitoring (SHM) attempts to automate the process of damage detection and identification. Multiscale modeling is a key element in SHM. It not only provides important information on the physics of failure, such as damage initiation and growth, the output can be used as "virtual sensing" data for detection and prognosis. The current research is part of an ongoing multidisciplinary effort to develop an integrated SHM framework for metallic aerospace components. In this thesis a multiscale model has been developed by bridging the relevant length scales, micro, meso and macro (or structural scale). Micro structural representations obtained from material characterization studies are used to define the length scales and to capture the size and orientation of the grains at the micro level. Parametric studies are conducted to estimate material parameters used in this constitutive model. Numerical and experimental simulations are performed to investigate the effects of Representative Volume Element (RVE) size, defect area fraction and distribution. A multiscale damage criterion accounting for crystal orientation effect is developed. This criterion is applied for fatigue crack initial stage prediction. A damage evolution rule based on strain energy density is modified to incorporate crystal plasticity at the microscale (local). Optimization approaches are used to calculate global damage index which is used for the RVE failure prediciton. Potential cracking directions are provided from the damage criterion simultaneously. A wave propagation model is incorporated with the damage model to detect changes in sensing signals due to plastic deformation and damage growth.
ContributorsLuo, Chuntao (Author) / Chattopadhyay, Aditi (Thesis advisor) / Papandreou-Suppappola, Antonia (Committee member) / Jiang, Hanqing (Committee member) / Dai, Lenore (Committee member) / Li, Jian (Committee member) / Arizona State University (Publisher)
Created2011