The presented doctoral research was aimed at preparation and characterization of ultra thin polymer films on solid substrates using different physical techniques. Each of these physical techniques probes selectively different characteristics of the films. While some of the techniques are strong in the predetermination of some unique properties of the layers, they might be limited and give no specific/conclusive information about some other important characteristics. Therefore, only the combination of the techniques provides a profound picture of the thickness, architecture, composition and functionality of the films/layers. This combined characterization approach elucidates in details the physical characteristics and the mechanisms responsible for the unique behavior of different polymer films/layers in the application that they are intended for. In the thesis, of particular interest were films of high biomedical, biotechnological and tissue engineering importance, such as: 1. poly(lactide) films formed by grafting "from-" a silanized alacrite thin films (L605 Co-based super alloy), 2. polydopamine (PDA) films that could serve as substrate independent mod- ification platform for further surface modification steps, 3. poly(ethylene oxide)films formed by "grafting to-" PDA modified surfaces, 4....

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科学研究費補助金 研究種目:基盤研究(A)(2) 課題番号:08405005 研究代表者:後藤 俊夫 研究期間:1996-1998年度

Self-assembled monolayers (SAMs) provide well-defined and ordered films of molecules spontaneously chemisorbed on a surface. By designing molecules with desired functionalities, such molecular film can be interesting for a range of applications from molecular electronics to catalysis. Important parameters for SAM applications are the film structure and quality, which are dependent on the structure of molecular constituents, the substrate, and the self-assembly process. In this work, SAMs on Au(111) of a variety of functionalized molecules, with thiol and silane headgroups, have been studied using high-resolution X-ray photoemission spectroscopy (HRXPS), near-edge X-ray absorption fine structure (NEXAFS) spectroscopy, Infrared reflection absorption spectroscopy (IRRAS), contact angle measurements and Kelvin probe measurements. In particular, the effects of varying the size of the backbone, varying the headgroup, inclusion of a porphyrin tailgroup, different ways of deprotection of the headgroups, and mixed molecular layers have been investigated. The first part of thesis work is focused on SAMs of oligo(phenyleneethynylene) (OPE) derivatives. First the effect of the extent of the conjugated system on the structure of SAM was investigated. As the lateral π-system in the OPE backbone increases, molecular surface densities become lower and molecular inclinations larger. Subsequently, a bulky porphyrin tailgroup was added onto the OPE molecule. Porphyrin-functionalized OPE with several headgroups were compared and the thioacetyl anchor group was found to form a high quality SAM. In the second part of the work, the molecular orientation of thiol-derivatized tetraphenylporphyrin layers was studied. The geometry of the molecular layer and the number of linkers that bind to the gold surface depend strongly on preparation schemes, i.e. whether or not the acetyl protection groups on the thiol were removed before adsorption. Finally, mixed SAMs of a ferrocene-terminated alkanethiol and alkanethiols were studied. By diluting the ferrocene-functionalized molecules in unfunctionalized alkanethiols, the orientational order and the packing density improved. The geometrical structure and the fraction of the ferrocene-terminated molecules can be tuned by controlling the parameters in the preparation scheme.