Statistical Mechanics of Dynamics and Structure in Liquids

David Chandler得到了理论和计算化学计划的资助，继续他对液体动力学和结构的统计力学的研究。将针对四个具体的研究领域：1)将研究溶剂化动力学，以试图了解溶质和溶剂的松弛时间和长度尺度之间的相互作用；2)将研究受限流体及其表面诱导相变的动力学，以努力了解限制在时间尺度上对相的松弛和成核的影响；3)将研究膜的自组装和稳定性，以表征复杂流体结构的稳定性和组装条件；以及4)将研究流体中的金属化，以了解和对比金属和绝缘液体相的结构，如在金属/氨溶液中观察到的结构。在所有这些领域，钱德勒将通过模型的发展来解决自然现象，并用统计场理论和模拟来处理这些模型。气相系统的理论模型在很大程度上依赖于基于弱相互作用粒子经历弹性碰撞的简化。固态模型依赖于由固态的对称性和有序性引起的简化。在这两个领域，理论模型都得到了很好的发展，并与实验数据吻合较好。另一方面，液体的理论处理一直很困难，因为系统并不有序，但相互作用很强。在过去的20年里，一些好的理论模型开始出现，例如钱德勒和其他合作者开发的所谓的参考交互站点模型。钱德勒正在继续改进液体的理论模型，并将其应用于具有重要化学意义的新体系，如分子组装和经历构象变化和化学反应的分子。

David Chandler is supported by a grant from the Theoretical and Computational Chemistry Program to continue his research on the statistical mechanics of dynamics and structure of liquids. Four specific research areas are targeted: 1) dynamics of solvation will be studied in an attempt to understand the interplay between solute and solvent relaxation times and length scales; 2) confined fluids and the dynamics of their surface induced phase transitions will be studied in an effort to understand the effects of confinement on time scales for relaxation and nucleation of phases; 3) self assembly and the stability of membranes will be studied to characterize conditions for stability and assembly of complex fluid structures; and 4) metallization in fluids will be studied to understand and contrast the structures of metallic and insulating liquid phases such as are observed in metal/ammonia solutions. In all of these areas Chandler will address natural phenomena with the development of models, and treat those models with statistical field theory and simulations. Theoretical models for gas phase systems have relied heavily on simplifications based on weakly interacting particles undergoing elastic collisions. Models for the solid state rely on simplifications arising from the symmetry and order of the solid state. In both of these areas, theoretical models are quite well developed, and agree well with experimental data. Theoretical treatment of the liquid phase, on the other hand has been difficult because the systems are not orderly, and yet the interactions are strong. Over the past 20 years, several good theoretical models have started to emerge, for example, the so-called `reference interaction site model` developed in part by Chandler and other collaborators. Chandler is continuing to improve upon the theoretical models for liquids, and to apply them to new systems which have important chemical significance such as molecular assemblies and molecules undergoing conformational changes and chemical reactions.