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

这个由实验物理化学项目颁发的奖项支持Pablo G. Debenedetti（普林斯顿大学），C。奥斯汀·安吉尔（亚利桑那州立大学）、彼得·罗斯基（德克萨斯大学奥斯汀分校）和h·尤金·斯坦利（波士顿大学）对水和水溶液中的协同现象的理解。该项目将研究溶剂的组织和结构如何影响微观（如蛋白质折叠）、介观（如纤维化）或宏观（如相变）长度尺度上发生的协同过程，并探索在这些广泛的协同转变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；具有类水动力学和溶剂化热力学的双尺度球对称模型系统相变的计算机模拟蛋白质相图和定向进化的理论和计算研究使用水显式晶格模型；以及蛋白粉水化过程中分子迁移率的计算研究。对水和共溶质在协同过程和分子秩序中的作用的进一步了解，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。

This award by the Experimental Physical Chemistry Program supports the collaborative efforts of Pablo G. Debenedetti (Princeton University),C. Austen Angell (Arizona State University), Peter Rossky (University of Texas at Austin), and H. Eugene Stanley (Boston University) in understanding cooperative phenomena in water and aqueous solutions. This project will investigate how solvent organization and structure affects cooperative processes occurring over microscopic (e.g., protein folding), mesoscopic (e.g., fibrilization), or macroscopic (e.g., phase transitions) length scales, 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; computer simulations of phase transitions in two-scale spherically-symmetric model systems that exhibit water-like dynamics and solvation thermodynamics; theoretical and computational investigations of protein phase diagrams and directed evolution using water-explicit lattice models; and computational studies of the emergence of molecular mobility upon hydration of protein powders. An improved understanding of the role of water and co-solutes on cooperative processes and 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.