Statistical Mechanics of Dynamics and Structure in Liquids

液体动力学和结构的统计力学

• 批准号: 0078458
• 负责人: David Chandler
• 金额: $ 62.9万
• 依托单位: University of California-Berkeley
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2000
• 资助国家: 美国
• 起止时间: 2000-08-15 至 2006-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0078458&HistoricalAwards=false
• 关键词: Statistical; Mechanics; Dynamics; Structure; Liquids

David Chandler of the University of California, Berkeley, is supported by the Theoretical and Computational Chemistry Program to continue his research in statistical mechanics directed at understanding structure and dynamics of liquids and related systems. In the first project, charge frustrated models of oil-water-surfactant systems will be used to develop and exploit isomorphisms between very different phenomena, including metal-insulator transitions in liquid solutions and vitrification of supercooled liquids. In another project, hydrophobicity at small and large length scales will be exploited to develop a generally applicable statistical field theory. This formulation will be applied as a bridge between large length scale phenomenology and small scale atomistic theories of complex fluids, and used to analyze systems such as polymer melts and blends, and liquid crystals. These techniques are also expected to enable development of an equilibrium theory for water and other associated fluids. In the area of dynamics, transition path sampling will be used to devise phenomenological theories for weak acid dissociation and proton transfer in aqueous systems. Methods for treating quantum effects within the context of transition path sampling will be explored, with the goal of enabling quantitative treatments of kinetics involving light atoms such as protons in water. In a final project, concepts governing ensembles of trajectories will be developed further, especially for systems far from equilibrium. Outcomes are expected to enable the analysis of broken symmetry, corresponding to broken ergodicity and to phase transitions of driven systems. Improved understanding of liquid systems structure and dynamics has far-reaching implications for fundamental science and technology applications. Outcomes from this project will impact materials science, including polymers and liquid crystal systems. As well, new results on proton transfer and the hydrophobic effect will have strong connections to biologically relevant systems, including protein folding.

加州大学伯克利分校的大卫·钱德勒在理论和计算化学计划的支持下，继续他在统计力学方面的研究，目的是了解液体和相关系统的结构和动力学。在第一个项目中，将使用油-水-表面活性剂体系的电荷受阻模型来开发和利用非常不同的现象之间的同构，包括液体溶液中的金属-绝缘体转变和过冷液体的玻璃化。在另一个项目中，将利用小尺度和大尺度上的疏水性来发展普遍适用的统计场理论。该公式将作为大尺度现象学和复杂流体的小尺度原子学理论之间的桥梁，并用于分析聚合物熔体和混合物以及液晶等体系。这些技术还有望使水和其他相关流体的平衡理论得以发展。在动力学领域，将利用跃迁路径采样来建立水体系中弱酸解离和质子转移的唯象理论。将探索在过渡路径采样的背景下处理量子效应的方法，目的是能够对涉及水中质子等轻原子的动力学进行定量处理。在最后一个项目中，管理轨迹集合的概念将进一步发展，特别是对于远离平衡的系统。预计结果将能够分析对称性的破缺，对应于破缺的遍历性和受驱动系统的相变。提高对液体体系结构和动力学的理解对基础科学和技术应用具有深远的影响。该项目的成果将影响材料科学，包括聚合物和液晶系统。此外，关于质子转移和疏水效应的新结果将与包括蛋白质折叠在内的生物相关系统有很强的联系。