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

该奖项支持C. Austen Angell（亚利桑那州立大学）、Pablo G. Debenedetti（普林斯顿大学）、Peter Rossky（德克萨斯大学奥斯汀分校）、H. Eugene Stanley（波士顿大学）和Srikanth Sastry（印度班加罗尔贾瓦贾拉尔·尼赫鲁高级科学研究中心）在理解水和水溶液中的协同转变方面的合作努力。该项目将研究溶剂组织和结构如何影响合作过渡，并探索在这些广泛的合作过渡中是否存在共同的特征或原则。这项跨学科合作将包括一种新的实验方法来研究蛋白质折叠（和其他有序现象）的能量学和动力学，使用非结晶但非扰动的溶剂；涉及自由能扰动和“导向”动力学的自组装分子模拟研究过冷水相变和动力学的新计算方法，包括动态非均质性的量化及其与构型熵的关系，以及基于能量景观的液体和非晶态水自由能面计算方法；纯水和靠近溶质和表面的水模拟中结构顺序量化的一种新形式以及研究多肽聚集的新计算方法。更好地理解水和共溶质在分子秩序中的作用，对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（以及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。这项工作还将为本科生、研究生和博士后研究人员提供出色的机会，使他们能够将实验和理论结合起来，并在化学和生物学的界面上进行团队工作。该项目由美国国家科学基金会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.