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Articles 1 - 18 of 18
Full-Text Articles in Physical Sciences and Mathematics
Vapor Deposition Strategies For Tuning Surface And Interface Chemistry For Optoelectronics And Biosensors, Kwang-Won Park
Vapor Deposition Strategies For Tuning Surface And Interface Chemistry For Optoelectronics And Biosensors, Kwang-Won Park
Doctoral Dissertations
Ordered assemblies of molecular semiconductors have been of particular interest for their integral role in organic optoelectronics, originating from interesting optical and charge transport properties. Compared with disordered films, organized nanostructured organic semiconductors display enhanced optoelectronic characteristics. However, past studies using template layer and self-assembly strategies are not applicable to molecular heterointerfaces and cannot be practically integrated into existing device fabrication routines to achieve large-area optoelectronic devices. This dissertation demonstrates unprecedented strategies to create one-dimensional (1D) nanostructures of molecular semiconductors using vapor deposition techniques. We begin this work by investigating how the interplay between dipole-dipole and van der Waals interactions …
Frontiers In The Self-Assembly Of Charged Macromolecules, Khatcher O. Margossian
Frontiers In The Self-Assembly Of Charged Macromolecules, Khatcher O. Margossian
Doctoral Dissertations
The self-assembly of charged macromolecules forms the basis of all life on earth. From the synthesis and replication of nucleic acids, to the association of DNA to chromatin, to the targeting of RNA to various cellular compartments, to the astonishingly consistent folding of proteins, all life depends on the physics of the organization and dynamics of charged polymers. In this dissertation, I address several of the newest challenges in the assembly of these types of materials. First, I describe the exciting new physics of the complexation between polyzwitterions and polyelectrolytes. These materials open new questions and possibilities within the context …
Intracellular Delivery Of Therapeutic Biomolecules Through Versatile Polymer Nanotechnology, David C. Luther
Intracellular Delivery Of Therapeutic Biomolecules Through Versatile Polymer Nanotechnology, David C. Luther
Doctoral Dissertations
Advancing pharmaceutical technology has made it possible to treat diseases once considered ‘undruggable.’ Access to these new pharmaceutical targets is possible thanks to the advent of protein and nucleic acid therapeutics. Responses to the COVID-19 pandemic, as well as cutting-edge treatments for cancer and multiple sclerosis have centered on these biologic therapies, promising even greater value in the future. However, their utility is limited at a cellular level by inability to cross the plasma membrane. Nanocarrier technologies encapsulate therapeutics and facilitate uptake into the cell but are often trapped and degraded in endosomes. Arginine-functionalized gold nanoparticles (Arg-NPs) provide efficient, direct …
Elucidating The Function Of Ions In Hybrid Perovskite Photovoltaics, Emily C. Smith
Elucidating The Function Of Ions In Hybrid Perovskite Photovoltaics, Emily C. Smith
Doctoral Dissertations
Perovskite solar cells (PSCs) have risen to the forefront of versatile thin-film technologies with power conversion efficiencies rivaling traditional silicon and the potential to be fabricated at a fraction of the cost. However, one crucial drawback to PSCs is their instability to illumination, which is likely due in part to mobile ions during operation. It is difficult to predict the influences of ion dynamics in devices, and the exact nature and impact of these ions remain elusive. In this dissertation work, I have set out to unravel the complex interplay between ions and device operation in PSCs. Through the development …
Formation Of Doped Semiconductor Nanocrystals From Doped Molecular Clusters, Jillian E. Denhardt
Formation Of Doped Semiconductor Nanocrystals From Doped Molecular Clusters, Jillian E. Denhardt
Doctoral Dissertations
Transition metal doping of semiconductor nanomaterials, particularly magnetic dopant ions, is of great interest for the synthesis of diluted magnetic semiconductors (DMS) with spintronic-based applications. The incorporation of magnetic ions into quantum dots (QDs) would be particularly useful since the quantum confinement of these materials is theorized to enhance magneto-optical related properties. One major challenge in this field is the segregation of dopant ions towards the outer regions of the QD due to the exclusion of dopants during the nucleation process, thereby inhibiting the magneto-optical properties. In this dissertation, we address the dopant segregation challenge by exploring the underlying mechanisms …
Expanding The Polymer Zwitterion Library – Novel Phosphonium-Based Polymer Zwitterions And Analogous Structures, Marcel U. Brown
Expanding The Polymer Zwitterion Library – Novel Phosphonium-Based Polymer Zwitterions And Analogous Structures, Marcel U. Brown
Doctoral Dissertations
This dissertation encompasses the synthesis, characterization and application of novel polymer zwitterions that significantly expand the library of available zwitterionic polymers. Their facile synthesis is facilitated by the preparation of a novel functional sultone precursor molecule, which can be ring-opened by commercially available phosphine, amine and sulfide nucleophiles, affording phosphonium, ammonium or sulfonium sulfonate monomers, respectively. Most notably, this work describes the invention of phosphonium-based polymer zwitterions, establishing a new class of zwitterionic polymer structures with unique solution and interfacial properties. Furthermore, the incorporation of these phosphonium sulfonates into block copolymer architectures with conventional polymer zwitterions, and the resulting switchable …
Enabling Nanoimprint Lithography Techniques Across Multiple Manufacturing Processes, Vincent Einck
Enabling Nanoimprint Lithography Techniques Across Multiple Manufacturing Processes, Vincent Einck
Doctoral Dissertations
Advanced nanooptics in the areas of flat lenses, diffractive elements, and tunable emissivity require a route to high throughput manufacturing. Nanooptics are often demanding of high refractive index materials, nanometer precision and ease of fabrication. Nanoimprint lithography (NIL) is a low-cost, high throughput manufacturing technique beginning to be realized in commercial industry.1,2 The NIL process is an ideal manufacturing candidate due to its ability to have a fast process time, efficient use of materials, repeatability and high precision while also having wide diversity of potential structures and material choices. Appling NIL techniques to other facets of manufacturing enable the …
Chromatographic Dynamic Chemisorption, Shreya Thakkar
Chromatographic Dynamic Chemisorption, Shreya Thakkar
Masters Theses
Reaction rates of catalytic cycles over supported metal catalysts are normalized by the exposed metal atoms on the catalyst surface, reported as site time yields which provide a rigorous standard to compare distinct metal surfaces. Defined as the fraction of exposed metal surface atoms to the total number of metal atoms, it is important to measure the dispersion of supported metal catalysts to report standardized rates for kinetic investigations. Multiple characterization techniques such as electron microscopy, spectroscopy and chemisorption are exploited for catalyst dispersion measurements. While effective, electron microscopy and spectroscopy are not readily accessible due to cost and maintenance …
Molecular Vibrations And Shape-Selectivity: A Computational Model Of Biofuel Precursors In Zeolites, Babgen Manookian
Molecular Vibrations And Shape-Selectivity: A Computational Model Of Biofuel Precursors In Zeolites, Babgen Manookian
Doctoral Dissertations
We have used Density Functional Theory (DFT) to model acyclic and cyclic olefins in acidic zeolites. We have studied the impact of host-guest interactions between adsorbed molecules and zeolite frameworks through the lens of molecular vibrations and shape-selectivity. This work considered three zeolite frameworks with varying pore structures and environments: large pore zeolite HMOR and medium pore zeolites HZSM-5 and HZSM-22. A key finding is that for acyclic olefins in acidic zeolites there exists two regimes of host-guest interaction: a strong interaction leading to protonation and a weak interaction between charged guest and zeolite framework. We found that these interactions …
Designing Polymer-Protein Complexes For Intracellular Delivery, Hazel Davis
Designing Polymer-Protein Complexes For Intracellular Delivery, Hazel Davis
Doctoral Dissertations
Previous work in the Tew group has demonstrated polymer cell-penetrating peptide mimics (CPPMs) as effective transporters of biological agents, including proteins and antibodies. These synthetic polymers non-covalently bind to cargo, offering a mechanism to deliver proteins in a way that does not alter protein secondary structure. However, correlations of the protein binding-delivery relationship or the role of polymer-protein complexation on intracellular activity of protein cargo are understudied. The work presented herein connects a fundamental understanding of polymer-protein complexation with intracellular internalization and cargo activity. Characterization and quantification of polymer-protein binding relationships were established using fluorescence quenching assays. In particular, the …
Developing Injectable And Implantable Polymer Zwitterion Platforms For Glioblastoma Treatment, Sarah Ward
Developing Injectable And Implantable Polymer Zwitterion Platforms For Glioblastoma Treatment, Sarah Ward
Doctoral Dissertations
This dissertation describes the synthesis, characterization, and application of novel polymer zwitterion-drug conjugates intended for treating glioblastoma, with a particular focus on phosphorylcholine (PC) and temozolomide (TMZ). Using versatile TMZ-containing monomers, injectable polymer prodrugs and implantable polymeric hydrogels were prepared over a broad range of drug incorporations with tunable properties, making them ideally suited for further in vivo and clinical evaluations. The work presented here greatly expands the knowledge base of TMZ formulations and gives rise to several routes which circumvent the challenges associated with its use. Chapter 2 describes the incorporation of a novel TMZ-methacrylate monomer into random and …
Deciphering Protein Higher-Order Structure And Interactions Via Diethylpyrocarbonate Labeling-Mass Spectrometry, Xiao Pan
Doctoral Dissertations
The study of protein higher-order structures is vital because it is closely related to the investigation of protein folding, aggregation, interaction and protein therapeutics. Consequently, numerous biochemical and biophysical tools have been developed to study protein higher-order structures in many different situations. The combination of covalent labeling (CL) and mass spectrometry (MS) has emerged as a powerful tool for studying protein structures and offers many advantages over other traditional techniques, such as better structural coverage, high throughput, high sensitivity, and the ability to study proteins in mixtures. This dissertation focuses on diethylpyrocarbonate (DEPC) as an effective CL reagent that can …
Synthesis, Fabrication, And Assembly Of Mesoscale Polymer Filaments, Dylan M. Barber
Synthesis, Fabrication, And Assembly Of Mesoscale Polymer Filaments, Dylan M. Barber
Doctoral Dissertations
Mesoscale materials, with feature sizes in the range of one hundred nanometers to tens of micrometers, are ubiquitous in Nature. In organisms, mesoscale building blocks connect the properties of underlying molecular and nanoscructures to those of macroscale, organism-scale materials through hierarchical assemblies of recurring structural motifs. The collective action of large numbers of mesoscale features can afford stunning features like the structural color of the morpho butterfly wing, calcium ion-mediated movement in muscle, and wood structures like xylem that can support enormous external compressive loads and negative internal pressure to transport nutrients throughout an organism. In synthetic systems, the design, …
The Thermoelectric, Thermoresistive, And Hygroresistive Properties And Applications Of Vapor Printed Pedot-Cl, Linden K. Allison
The Thermoelectric, Thermoresistive, And Hygroresistive Properties And Applications Of Vapor Printed Pedot-Cl, Linden K. Allison
Doctoral Dissertations
Wearable electronics are a valuable tool to increase consumer access to real-time and long-term health care monitoring. The development of these technologies can also lead to major advancements in the field, such as self-charging systems that are completely removed from the electrical grid. However, much of the wearable technology available commercially contain rigid components, use unsustainable synthetic methods, or undesirable materials. The field has thus been moving towards wearables that mimic textiles or use textiles as a substrate. Herein, we discuss the use of oxidative chemical vapor deposition (oCVD) to produce textiles coated with poly(3,4-ethylenedioxythiophene) known as PEDOT-Cl. We evaluate …
Designing Nonflammable Polymers And Blends Containing Deoxybenzoin Derivatives, Elizabeth Stubbs
Designing Nonflammable Polymers And Blends Containing Deoxybenzoin Derivatives, Elizabeth Stubbs
Doctoral Dissertations
The importance of synthetic polymers in everyday life continues to grow, owing to their societal importance for improving our standard-of-living and enabling advances spanning medicine, electronics, construction materials, transportation. While niche applications occupy a small fraction of the overall volume of polymers produced, large scale applications tend to employ lower cost materials, such as polyethylene, polypropylene, and polystyrene. In addition to environmental considerations connected to these polymerized hydrocarbons, produced in excess of 380 million tons per year worldwide, their inherent flammability creates additional requirements associated with their manufacturing and use. Societal benefits of such polymers are extensive, and thus, there …
Quantitative Imaging Of Tensile Forces At Cell-Cell Junction With Dna-Based Probes, Puspam Keshri
Quantitative Imaging Of Tensile Forces At Cell-Cell Junction With Dna-Based Probes, Puspam Keshri
Doctoral Dissertations
Mechanical forces are an integral part in biology, they regulate several cellular properties, such as morphology, proliferation, migration. These forces are also involved in receptor signaling and the differentiation of different cell types. Different proteins and biomolecules such as cadherin, integrin, notch proteins are essential elements of these processes. Measuring these intercellular forces are challenging considering the minimal intensity (piconewton-level) of these molecular forces. In our lab, we have developed a membrane DNA tension probe (MDTP) that uses a DNA hairpin module to sense tensile forces and has a lipid anchor to modify onto live-cell membranes. The programmability of DNA …
Tailoring Interfaces And Composition For Stable And Efficient Perovskite Solar Cells, Hamza Javaid
Tailoring Interfaces And Composition For Stable And Efficient Perovskite Solar Cells, Hamza Javaid
Doctoral Dissertations
Metal halide perovskite solar cells (PSCs) have revolutionized the field of thin film photovoltaics. Within a decade, the power conversion efficiencies (PCEs) have increased at a phenomenal rate, rising from 3.8% to more than 25% in single-junction devices, moving them ahead of the current silicon-based technology. The high efficiencies of perovskite solar cells (PSCs) and their other unique properties arise from a combination of organic and inorganic components and electronic-ionic conduction, making them excellent candidates for a plethora of applications. However, PSCs face a significant—and ironic—roadblock to commercialization: these light-harvesting materials degrade under sunlight—the very condition they would need …
Manipulating The Properties Of Light-Responsive Active Lipid Bilayer Membranes: Measuring Mechanics And Probing Mechanisms, Arash Manafirad
Manipulating The Properties Of Light-Responsive Active Lipid Bilayer Membranes: Measuring Mechanics And Probing Mechanisms, Arash Manafirad
Doctoral Dissertations
This thesis explores an experimental system probing the effect of energy input (in light-responsive bilayers) on membrane physicomechanical properties and dynamics of response to a trigger. We were inspired by the ability of cell membranes to alter their elastic and permeability properties and shape in response to energy input, change in lipid chemistry, or bilayer composition. Our work demonstrates and sheds new light on the roles of lipid chemical character, light-responsive moieties' incorporation in the membrane, and the lipid bilayer's mechanical properties on membrane response to chemical tuning or energy input. To observe how lipid chemistry affects membrane physical properties …