CRC: Ordering Processes in Water, Aqueous Solutions, and Water-Biomolecule Systems

该奖项支持了C。奥斯汀安吉尔（亚利桑那州立大学），巴勃罗G. Debenedetti（普林斯顿大学），Peter Rossky（德克萨斯大学奥斯汀分校），H.尤金斯坦利（波士顿大学）和Srikanth Sastry（印度班加罗尔尼赫鲁高级科学研究中心）在理解水和水溶液的合作转变。本项目将研究溶剂组织和结构如何影响合作转型，并探讨这些合作转型是否存在共同的特征或原则。这种跨学科的合作将包括一种新的实验方法来研究蛋白质折叠的能量学和动力学（和其他有序现象）使用非结晶但非扰动溶剂;涉及自由能扰动和“转向”动力学的自组装的分子模拟;研究过冷水中相变和动力学的新计算方法，包括动态不均匀性的量化及其与构型熵的关系，以及用于计算液体和无定形水的自由能表面的基于能量交换的方法;一种新的形式主义，用于在纯水和溶质和表面附近的水的模拟中量化结构顺序;对水和共溶质在分子有序中的作用的更好理解对于先进材料的定向自组装和生命过程的分子基础具有深远的影响，包括基因表达的代谢控制，蛋白质折叠（和疾病状态下的错误折叠）以及天然组织和材料的长期保存和储存。拟议的工作还将为本科生，研究生和博士后研究人员提供出色的机会，将实验和理论相结合，并在化学和生物学的接口团队工作。该项目由NSF化学部的化学合作研究计划（CRC）和国际科学与工程办公室的非洲，近东和南亚（ANESA）计划资助。

This award supports the collaborative efforts of C. Austen Angell (Arizona State University), Pablo G. Debenedetti (Princeton University),Peter Rossky (University of Texas at Austin), H. Eugene Stanley (Boston University) and Srikanth Sastry (Jawajaral Nehru Centre for Advanced Scientific Research in Bangalore, India) in understanding cooperative transitions in water and aqueous solutions. This project will investigate how solvent organization and structure affects cooperative transitions and explore whether there exist common features or principles across a broad range of these cooperative transitions. This interdisciplinary collaboration will include a novel experimental approach to study the energetics and kinetics of protein folding (and other ordering phenomena) using non-crystallizing but non-perturbing solvents; molecular simulations of self-assembly involving free energy perturbation and "steered" dynamics; new computational approaches to the study of phase transitions and dynamics in supercooled water, including quantification of dynamic heterogeneity and its relationship to configurational entropy, and energy landscape-based approaches for calculating liquid and amorphous water's free energy surface; a new formalism for the quantification of structural order in simulations of neat water and of water near solutes and surfaces; and novel computational approaches for the study of polypeptide aggregation.An improved understanding of the role of water and co-solutes on molecular order has far-reaching consequences for directed self-assembly of advanced materials and the molecular basis of life processes, including metabolic control of gene expression, protein folding (and misfolding in disease states) and the long-term preservation and storage of natural tissues and materials. The proposed work will also provide outstanding opportunities for undergraduates, graduate students, and postdoctoral researchers to integrate experiment and theory and work in a team at the interface of chemistry and biology. This project is funded through the Collaborative Research in Chemistry Program (CRC) in the NSF Division of Chemistry and the Africa, Near East and South Asia (ANESA) Program in the Office of International Science and Engineering.