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Sum frequency generation (SFG) vibrational spectroscopy was used to investigate the interfacial properties of several amino acids, peptides, and proteins adsorbed at the hydrophilic polystyrene solid-liquid and the hydrophobic silica solid-liquid interfaces. The influence of experimental geometry on the sensitivity and resolution of the SFG vibrational spectroscopy technique was investigated both theoretically and experimentally. SFG was implemented to investigate the adsorption and organization of eight individual amino acids at model hydrophilic and hydrophobic surfaces under physiological conditions. Biointerface studies were conducted using a combination of SFG and quartz crystal microbalance (QCM) comparing the interfacial structure and concentration of two amino acids and their corresponding homopeptides at two model liquid-solid interfaces as a function of their concentration in aqueous solutions. The influence of temperature, concentration, equilibration time, and electrical bias on the extent of adsorption and interfacial structure of biomolecules were explored at the liquid-solid interface via QCM and SFG. QCM was utilized to quantify the biological activity of heparin functionalized surfaces. A novel optical parametric amplifier was developed and utilized in SFG experiments to investigate the secondary structure of an adsorbed model peptide at the solid-liquid interface.
Sum frequency generation (SFG) vibrational spectroscopy was used to investigate the interfacial properties of several amino acids, peptides, and proteins adsorbed at the hydrophilic polystyrene solid-liquid and the hydrophobic silica solid-liquid interfaces. The influence of experimental geometry on the sensitivity and resolution of the SFG vibrational spectroscopy technique was investigated both theoretically and experimentally. SFG was implemented to investigate the adsorption and organization of eight individual amino acids at model hydrophilic and hydrophobic surfaces under physiological conditions. Biointerface studies were conducted using a combination of SFG and quartz crystal microbalance (QCM) comparing the interfacial structure and concentration of two amino acids and their corresponding homopeptides at two model liquid-solid interfaces as a function of their concentration in aqueous solutions. The influence of temperature, concentration, equilibration time, and electrical bias on the extent of adsorption and interfacial structure of biomolecules were explored at the liquid-solid interface via QCM and SFG. QCM was utilized to quantify the biological activity of heparin functionalized surfaces. A novel optical parametric amplifier was developed and utilized in SFG experiments to investigate the secondary structure of an adsorbed model peptide at the solid-liquid interface.
Sum frequency generation (SFG) vibrational spectroscopy has been established as one of the most essential tools to investigate chemistry of the surfaces and interfaces for several decades. Orientation, structure, and chemical reaction of molecules at the interfaces have been examined by using temporally and spatially resolved SFG. As a unique method to observe the chemistry at the interfaces, SFG has a great potential for further developments. In this dissertation, the possibility of extending the SFG field is gauged, including the introduction of detailed theory and formulation of SFG. Firstly, the principle of sum frequency vibrational depletion spectroscopy (SVDS) technique is presented. Newly developed SVDS has been established for observing vibrational behaviors of molecules on the surface with high spatial resolution below the diffraction limit. This technique is accomplished by depletion of the ground state molecules around the center of probing focal spot on the surface. High energy density IR generated is employed to deplete the ground state molecules to its first vibrational excited state. Then, SFG technique has been conducted to measure the vibrational dipoles of the surface molecules from the confined probing area. The instrumentation, theoretical simulation, depletion efficiency and the preliminary experimental results of this technique is reported. In the following chapter, SFG from acetonitrile on rutile TiO2 (110) surface has been measured using distinct polarization combinations and compared to the spectra obtained by polarization mapping and null angle methods. By varying the polarization combinations of SFG, the magnitude and shape of the spectra undergo substantial change, originating from the interference between the non-resonant signal inherent from the rutile substrate and the resonant signal from the adsorbed molecules. Theory, simulation, and analytical methods for obtaining quantitative orientation information in the presence of non-resonant signal of the adsorbed molecules on a semiconductor are presented. In the last chapter, a refined analytical procedure for SFG imaging microscope (SFGIM) is discussed. In order to determine the surface properties, the images need to be fitted using an SFG model equation which contains the physical properties relevant to interpret the surface. Experimental results obtained from SFGIM analysis of binary system of self-assembled monolayers on gold surface have been reported.
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The principal motivation behind surface engineering and modification for improved biocompatibility of a biomaterial is to control interactions of the biomaterial with components of living systems or subsets thereof in a manner that mimics the normal physiological state or produces a desired change in biological state. This pursuit of biomimicry is discussed in this chapter within the context of the core mechanisms of the biological response to materials. A tutorial on surfaces, interfaces, and interphases leads to the identification of specific targets for surface engineering and modification. These targets include water wettability (surface energy), surface chemistry, surface chemical patterns and surface textures, and surface presentation of biomimetic motifs. The chapter concludes with a discussion of the essential conceptual tools required for building a biomaterials surface science laboratory, illustrated with an example of modifying surfaces for improved cardiovascular biomaterials.
The first book on the topic, and written by the founder of the technique, this comprehensive resource provides a detailed overview of sum-frequency spectroscopy, its fundamental principles, and the wide range of applications for surfaces, interfaces, and bulk. Beginning with an overview of the historical context, and introductions to the basic theory of nonlinear optics and surface sum-frequency generation, topics covered include discussion of different experimental arrangements adopted by researchers, notes on proper data analysis, an up-to-date survey commenting on the wide range of successful applications of the tool, and a valuable insight into current unsolved problems and potential areas to be explored in the future. With the addition of chapter appendices that offer the opportunity for more in-depth theoretical discussion, this is an essential resource that integrates all aspects of the subject and is ideal for anyone using, or interested in using, sum-frequency spectroscopy.
ABSTRACT: Our work investigates theoretical approximations to the interface specific sum frequency generation (SFG) spectra at aqueous interfaces constructed using time correlation function (TCF) and instantaneous normal mode (INM) methods. Both approaches lead to signals in excellent agreement with experimental measurements. This work demonstrates how TCF and INM methods can be used in a complementary fashion to describe interfacial vibrational spectroscopy. Our approach is to compare TCF spectra with experiment to establish that our molecular dynamics (MD) methods can reliably describe the system of interest. We then employ INM methods to analyze the molecular and dynamical basis for the observed spectroscopy. We have been able to elucidate, on a molecularly detailed basis, a number of interfacial line shapes, most notably the origin of the complex O-H stretching SFG signal, and the identity of several intermolecular modes in the SFG spectra for the water/vapor interface.
"There is an increasing interest in research and applications of biosensors and bio-compatability in relation to environmental protection, food and medical safety, implants, early detection of diseases and pollutant detection. This book describes how to characterise amino acids, protein or bacterial strain adsorption on metal and oxide surfaces by using infrared spectroscopy, in a vacuum, in the air or in an aqueous medium. Features description of the principles, experimental setups and parameter interpretation, and the theory for several advanced IR-based techniques for interface characterisation Contains examples which demonstrate the capacity, potential and limits of the IR techniques Helps finding the most adequate mode of analysis."--Publisher.