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

这项由实验物理化学计划颁发的奖项支持Pablo G.Debenderti(普林斯顿大学)、C.Austen Angell(亚利桑那州立大学)、Peter Rossky(德克萨斯大学奥斯汀分校)和H.Eugene Stanley(波士顿大学)在理解水和水溶液中的合作现象方面的合作努力。该项目将研究溶剂的组织和结构如何影响微观(例如蛋白质折叠)、介观(例如纤化)或宏观(例如相变)长度尺度上发生的合作过程，并探索在广泛的这些合作转变中是否存在共同的特征或原则。这种跨学科的合作将包括：使用非结晶但非扰动溶剂研究蛋白质折叠(和其他有序化现象)的能量学和动力学的新的实验方法；计算机模拟呈现类水动力学和溶剂化热力学的双尺度球对称模型系统中的相变；使用水显式晶格模型对蛋白质相图和定向进化的理论和计算研究；以及对蛋白质粉末水化时出现的分子迁移率的计算研究。更好地理解水和共溶质在合作过程和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，包括对基因表达、蛋白质折叠(和疾病状态下的错误折叠)的代谢控制，以及自然组织和材料的长期保存和储存。这项拟议的工作还将为本科生、研究生和博士后研究人员提供绝佳的机会，使他们能够将实验和理论结合起来，并在化学和生物的界面上进行团队合作。

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.