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Polymers have been used in thin film coatings as a way to produce tailor made surfaces. These thin films have been explored for use in a variety of applications to produce antifouling coatings, corrosion resistant coatings, biocompatible surfaces, and biomedical devices. Polymer brushes, polymer chains tethered to a substrate or surface, synthesized by surface-initiated polymerization have gained significant attention in recent years. As brushes offer a new pathway towards the preparation of functional surfaces and offer long term stability, even in adverse environments, they are attractive for use as high-tech coatings. Patterned polymer thin films have also seen growing interest for various applications. This dissertation will focus on the top-down direct patterning of polymer brushes and the bottom-up self-assembly of block copolymer thin films. A new approach to creating patterned polymer brushes is highlighted, which is a simpler approach than what is conventionally done. Various polymer brushes were patterned directly using electron beam lithography to create high resolution patterned polymer brushes in a single step. This method was then used to demonstrate the unique ability to create sub-surface patterns within the brush. Additionally, direct patterning was used to create high resolution patterned binary polymer brushes of PMMA and PEGMA. With this binary patterned surface, a surface that responds to its local environment was created. This thesis also details characterization techniques used in probing polymer thin films to better understand how to improve block copolymer self-assembly. By using a powerful technique called grazing incidence small angle X-ray scattering (GISAXS) on solvent vapor annealed block copolymer thin films while monitoring the solvent vapor swollen film thickness and controlling the film swelling with a nitrogen counterflow, the work presented demonstrates how to accurately determine the processing conditions necessary for the annealing process to take place. This process also provides information as to what changes are occurring during the annealing process. Another characterization technique known as near edge X-ray absorption fine structure (NEXAFS) is also highlighted. A more exact calculation of the electron escape depth (EED) for NEXAFS is done using polymer brushes as the calibration sample. With this information, we can do composition depth profiling on our polymer thin films to identify what is at the surface.
Very thin film materials have emerged as a highly interesting and useful quasi 2D-state functionality. They have given rise to numerous applications ranging from protective and smart coatings to electronics, sensors and display technology as well as serving biological, analytical and medical purposes. The tailoring of polymer film properties and functions has become a major research field. As opposed to the traditional treatise on polymer and resin-based coatings, this one-stop reference is the first to give readers a comprehensive view of the latest macromolecular and supramolecular film-based nanotechnology. Bringing together all the important facets and state-of-the-art research, the two well-structured volumes cover film assembly and depostion, functionality and patterning, and analysis and characterization. The result is an in-depth understanding of the phenomena, ordering, scale effects, fabrication, and analysis of polymer ultrathin films. This book will be a valuable addition for Materials Scientists, Polymer Chemists, Surface Scientists, Bioengineers, Coatings Specialists, Chemical Engineers, and Scientists working in this important research field and industry.
The ability to pattern functional polymers at different length scales is important for the advancement of modern science and technology. This dissertation mainly describes the work done on the high resolution patterning of polymer thin films that have a variety of potential uses. The nanoscale patterning of spun-coated polar polymers was demonstrated using environmentally benign supercritical carbon dioxide (scCO2) as a processing solvent. The use of scCO2 as a processing solvent has several technical advantages that help resolve some of the key problems faced in lithography. In addition, it helps reduce the energy and resource usage that can negatively affect the environment. scCO2 is generally a poor solvent for high molecular weight polymers that are used as standard photoresists. Chapter 2 describes a series of fluorinated quaternary ammonium salts that were synthesized and used as CO2 compatible additives to aid the dissolution of polar polymer photoresists in scCO2. Using these dissolution aids, patterns as small as 100 nm lines were obtained with scCO2 development. Chapters 3 and 4 focus on the patterning of high-tech thin polymer films referred to as polymer brushes. In these films the polymer chains are covalently attached to a surface. A direct method of patterning polymer brushes in a single step using electron beam lithography has been described. Polymer brushes of different structures such as poly(methyl methacrylate) (PMMA) brushes , poly(2-hydroxyethyl methacrylate) (PHEMA) brushes, poly(isobutyl methacrylate) (PIBMA) brushes, poly(neopentyl methacrylate) (PNPMA) brushes and poly(2,2,2-trifluoroethyl methacrylate) (PTFEMA) brushes were grown via atom transfer radical polymerization. These brushes were directly patterned using e-beam and their sensitivity to e-beam patterning has been compared and explained. This direct patterning approach produced polymer brush patterns down to 50 nm lines. Due to the number of advantages of using scCO2 as a processing solvent, the dry development of a directly patterned low surface energy coating composed of PTFEMA brushes in scCO2 has been demonstrated in Chapter 4. Using scCO2 as a developer, patterned PTFEMA brushes with 150 nm lines were obtained. Polymer brushes have been used to prepare biocompatible surfaces with reduced non-specific adsorption. Chapter 5 describes the synthesis of a new oligo(ethylene glycol) containing ATRP intiator to prevent non-specific adsorption of biomolecules on polymer brush coated gold electrodes. The adsorption of non-specific antibodies on modified gold electrodes was studied using cyclic voltammetry. Poly(acrylic acid) brushes grown using this new ATRP initiator showed reduced nonspecific binding of the gold electrodes. There has been a continuing need for developing new medical countermeasures for emerging infectious diseases. Chapter 6 describes the role of functionalized poly(acrylic acid) brushes in the development of a biosensor based on sensitive electrochemical detection of the intrinsic catalytic activity of antibodies. Poly(acrylic acid) brushes have been functionalized with 2,4-dinitrophenyl groups (model antigen) and Ni-NTA to immobilize specific antibodies on the sensor surface. The modification of gold surfaces with polymer brushes provides a bio- and electronically compatible substrate with high density of specific haptens with reduced non-specific adsorption.
This volume includes contributions to the 10th Dresden Polymer Discussion which was held in Meißen near Dresden from April 10 to 13, 2005 organized by the Leibniz Institute of Polymer Research Dresden and the Institute of Macromolecular and Textile Chemistry of the Technische Universität Dresden. The meeting was focussed on Characterization of Polymer Surfaces and Thin Films. Comprehensive characterization of surfaces and interfaces is essential to relate surface and thin film properties to micro structure and molecular origin, which is, on the other hand, the key to technological control and improvement of materials. The contributions in this volume cover a representative spectrum of surface sensitive techniques and their application to polymer surface and thin film characterization as well as recent examples of technologically relevant materials and process development.
Materials scientists, polymer chemists, surface physicists and materials engineers will find this book a complete and detailed treatise on the field of polymer brushes, their synthesis, characterization and manifold applications. In a first section, the various synthetic pathways and different surface materials are introduced and explained, followed by a second section covering important aspects of characterization and analysis in both flat surfaces and particles. These specific surface initiated polymerization (SIP) systems such as linear polymers, homopolymers, block copolymers, and hyperbranched polymers are unique compared to previously reported systems by chemisorption or physisorption. They have found their way in both large-scale and miniature applications of polymer brushes, which is covered in the last section. Such 'hairy' surfaces offer fascinating opportunities for addressing numerous problems of both academic and, in particular, industrial interest: high-quality, functional or protective coatings, composite materials, surface engineered particles, metal-organic interfaces, biological applications, micro-patterning, colloids, nanoparticles, functional devices, and many more. It is the desire of the authors that this book will be of benefit to readers who want to "brush-up on polymers".
Very thin film materials have emerged as a highly interesting and useful quasi 2D-state functionality. They have given rise to numerous applications ranging from protective and smart coatings to electronics, sensors and display technology as well as serving biological, analytical and medical purposes. The tailoring of polymer film properties and functions has become a major research field. As opposed to the traditional treatise on polymer and resin-based coatings, this one-stop reference is the first to give readers a comprehensive view of the latest macromolecular and supramolecular film-based nanotechnology. Bringing together all the important facets and state-of-the-art research, the two well-structured volumes cover film assembly and depostion, functionality and patterning, and analysis and characterization. The result is an in-depth understanding of the phenomena, ordering, scale effects, fabrication, and analysis of polymer ultrathin films. This book will be a valuable addition for Materials Scientists, Polymer Chemists, Surface Scientists, Bioengineers, Coatings Specialists, Chemical Engineers, and Scientists working in this important research field and industry.
This book is about thin films; what they are, how they are prepared, how they are characterized, and what they are used for. The contents of this book not only showcase the diversity of thin films, but also reveals the commonality among the work performed in a variety of areas. The chapters in this volume are based on invited papers presented by prominent researchers in the field at a Symposium on "Thin Films: Preparation, Characterization, Applications" at the 221st National Meeting of the American Chemical Society held in San Diego, California. The coverage of the symposium was extensive; topics ranged from highly-ordered metal adlayers on well-defined electrode surfaces to bio-organic films on non-metallic nanoparticles. An objective of this book is for the readers to be able to draw from the experience and results of others in order to improve and expand the understanding of the science and technology of their own thin films systems.
Ch. 1. Block copolymer thin films / J.-Y. Wang, S. Park and T. P. Russell -- ch. 2. Equilibration of block copolymer films on chemically patterned surfaces / G. S. W. Craig, H. Kang and P. F. Nealey -- ch. 3. Structure formation and evolution in confined cylinder-forming block copolymers / G. J. A. Sevink and J. G. E. M. Fraaije -- ch. 4. Block copolymer lithography for magnetic device fabrication / J. Y. Cheng and C. A. Ross -- ch. 5. Hierarchical structuring of polymer nanoparticles by self-organization / M. Shimomura ... [et al.] -- ch. 6. Wrinkling polymers for surface structure control and functionality / E. P. Chan and A. J. Crosby -- ch. 7. Crystallization in polymer thin films: morphology and growth / R. M. Van Horn and S. Z. D. Cheng -- ch. 8. Friction at soft polymer surface / M. K. Chaudhury, K. Vorvolakos and D. Malotky -- ch. 9. Relationship between molecular architecture, large-strain mechanical response and adhesive performance of model, block copolymer-based pressure sensitive adhesives / C. Creton and K. R. Shull -- ch. 10. Stability and dewetting of thin liquid films / K. Jacobs, R. Seemann and S. Herminghaus -- ch. 11. Anomalous dynamics of polymer Films / O. K. C. Tsui.
Given such problems as rejection, the interface between an implant and its human host is a critical area in biomaterials. Surfaces and Interfaces for Biomaterials summarizes the wealth of research on understanding the surface properties of biomaterials and the way they interact with human tissue. The first part of the book reviews the way biomaterial surfaces form. Part Two then discusses ways of monitoring and characterizing surface structure and behavior. The final two parts of the book look at a range of in vitro and in vivo studies of the complex interactions between biomaterials and the body. Chapters cover such topics as bone and tissue regeneration, the role of interface interactions in biodegradable biomaterials, microbial biofilm formation, vascular tissue engineering and ways of modifying biomaterial surfaces to improve biocompatibility. Surfaces and Interfaces for Biomaterials will be a standard work on how to understand and control surface processes in ensuring biomaterials are used successfully in medicine.
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