THEORETICAL STUDIES ON THE DYNAMIC ASPECTS OF MACROMOLECULAR FUNCTION

系统上的吸光度测量理论（例如， 蛋白质），其经历由线性 产生了任意强度的偏振激光脉冲。 为了 提供了一个完整的框架，可用于分析实验， 多种并发症（例如，同时进行重新定向运动 规模作为强烈的激励脉冲，内部运动的影响， 化学动力学）进行了明确的处理。 为了描述 大分子在时间尺度上的动力学， （障碍跨越）发生，我们表明，记忆功能的纠正必须 被添加到优化的Rouse-Zimm理论，并开发了一个新的， 高效的计算方式。 一个简单的分析理论 需要分析细胞-细胞融合的荧光研究， 开发 这一理论是基于这样的认识，即扩散 探针在通过小孔连接的两个细胞表面之间的转移可以 可以用双态化学动力学来精确描述。 的速率常数 通过利用严格的 将原胞问题映射到一个涉及扩散的问题上 具有熵势垒的三维位势。 的解析 偶极晶格对新产生的变化的响应理论， 基于动态平均球近似公式化。 的 该理论对溶剂化动力学的预测已经过测试， 计算机模拟 静电相互作用的影响， 扩散对蛋白质-蛋白质缔合动力学速率的影响， 考察 本文提出了一种新的边界元法， 两个大分子之间的静电相互作用能， 开发 这个程序可以处理不规则形状的分子 表面，内部的小介电常数和存在 盐离子在溶液中。

The theory of absorbance measurements on a system (e.g. a chromophore in a protein) that undergoes a sequence of reactions initiated by a linearly polarized laser pulse of arbitrary intensity is developed. In order to provide a complete framework that could be used to analyze experiments, a wide variety of complications (e.g. reorientational motion on the same time scale as the intense excitation pulse,the influence of internal motions and chemical kinetics) were explicitly treated. In order to describe the dynamics of macromolecules on time scales where comformational transitions (barrier crossings) occur, we showed that memory function corrections must be added to the optimized Rouse-Zimm theory and developed a new, computationally efficient way of doing so. A simple analytic theory required to analyze fluorescence studies of cell-cell fusion has been developed. This theory is based on the realization that the diffusive transfer of probes between two cell surfaces connected by a small pore can be accurately described by two state chemical kinetics. The rate constants were expressed in terms of microscopic parameters by exploiting a rigorous mapping of the cell problem onto one involving diffusion on a one dimensional bistable potential with an entropic barrier. An analytic theory for the response of a dipolar lattice to a newly created change has been formulated based on a dynamic mean spherical approximation. The predictions of this theory for solvation dynamics has been tested against computer simulations. The influence of electrostatic interactions and diffusion on the rate of protein-protein association kinetics have been examined. A new method (boundary elements) for calculating the electrostastic interaction energy between two macromolecules has been developed. This procedure can handle the irregular shape of the molecular surfaces, the small dielectric constant in the interior and the presence of salt ions in solution.