Dielectric spectroscopy and SAXS investigations on self-organization mechanism of biologically-originated systems

本研究的主要目标是阐明生物来源的两亲聚合物在水中的自组织机制，其中静态结构（如颗粒结构和颗粒间相互作用势）与动态方面（如溶剂的高频动力学和水合行为）之间的相互作用已经通过精心组合的光谱和散射技术进行了仔细研究，例如，介电谱和小角X射线散射（SAXS），首次阐明了氢键液体介电谱和拉曼谱之间关系的一般规律，即氢键液体的集体弛豫过程，对涉及长程偶极-偶极相互作用的氢键液体特有的介电光谱的主要贡献实际上不是拉曼活性的。这些结果将为全面理解氢键液体动力学的微观-宏观关联奠定基础。 关于我们 纳米组装体（特别是胶束）的结构和分子动力学，所述纳米组装体由生物来源的以及合成的两亲物在水中形成。我们已经发现，一个准确的静态结构因子分析GIFT（广义间接傅立叶变换）技术结合动态水化数分析介电谱可以定量解释的影响，水化水的胶束排除体积和它的贡献的等温压缩系统。我们的SAXS和流变学数据清楚地表明，糖基表面活性剂微乳液的相行为与自由能优化导致的胶束伸长为棒状或蠕虫状胶束密切相关。此外，我们尝试构建一种新的方法来计算径向分布函数（RDF）和/或由实验静态结构因子计算的成对相关函数，介绍了SQ-IFT（结构因子间接傅立叶变换）方法，并证实了其广泛的适用性。为了从液体衍射数据计算分子液体的RDFs，不再需要传统使用的散射矢量加权结构函数。同时，SQ-IFT可以提供潜在的无模型的真实的空间信息的蛋白质-蛋白质的空间相关性在解决方案。少

The main goal of this study is to clarify self-organization mechanisms of biologically-originated amphiphilic polymers in water, where an interplay between static structures, such as particle structure and interparticle interaction potential, and dynamical aspects like high-frequency dynamics of solvents and hydration behavior has been scrutinized by elaborately combined spectroscopic and scattering techniques, e.g., dielectric spectroscopy and small-angle X-ray scattering (SAXS).A general rule that can consistently explain relation between dielectric and Raman spectra of hydrogen-bond liquids has been for the first time elucidated ; the collective relaxation process, i.e., the main contribution to the dielectric spectrum specific to hydrogen-bond liquids involving a long range dipole-dipole interaction, is virtually not Raman active. The results will lay the foundation for complete understanding microscopic-macroscopic correlation in hydrogen-bond liquid dynamics.We have examined stat … More ic structures and molecular dynamics of a nano-assembly (in particular, a micelle) that is formed by biologically-originated as well as synthetic amphihilie in water. We have found that an accurate static structure factor analysis by GIFT (generalized indirect Fourier transformation) technique combined with dynamic hydration number analysis by dielectric spectroscopy can quantitatively explain the effects of hydrated water on excluded volume of micelles and its contribution to isothermal compressibility of the system. Our SAXS and rheology data clearly demonstrate that phase behavior of sugar-based surfactant microemulsions are closely linked with elongation of a micelle into rodlike or wormlike ones due to free-energy optimization.Furthermore, we have attempted to construct a new approach to the calculation of the radial distribution functions (RDFs) and/or pair correlation functions from experimental static structure factor, introducing the so-called SQ-IFT (structure factor indirect Fourier transformation) method, and confirmed its versatile applicability. To calculate the RDFs of molecular liquids from liquid diffraction data, a conventionally utilized scattering vector-weighted structure function is no longer required. Simultaneously, SQ-IFT can provide potential model-free real space information on protein-protein spatial correlations in solution. Less