CDS&E: Development and application of cluster-integral methods for dispersions and complex solutions

有了这个奖项，化学部的化学理论，模型和计算方法项目正在支持布法罗/纽约州立大学的大卫科夫克和安德鲁舒尔茨开发一个分层的理论和计算方法来研究化学溶液。 化学溶液在自然和人造系统中无处不在，它们的行为对许多技术应用至关重要，包括医疗保健，能源储存，环境保护以及食品和消费品。描述化学溶液的一种方法是通过溶质相互作用的层次结构，首先考虑单个溶质分子，然后考虑成对的溶质分子，然后考虑三个、四个等一组溶质分子，在这个层次结构中的每一个层次都引入了关于混合物的新信息，这样人们就可以通过对这些相互作用的适当分析来推断整个行为。该配方所需的量原则上可以从详细的分子考虑来计算，这是期望的，因为它导致更大的预测和描述能力。然而，为实际目的进行这些计算的手段尚未开发，因此整个方法的全部潜力相对未经测试。 开发和基准测试这种方法是本研究项目的重点。 该项目将研究生的培训与推广活动以及学习材料和计算机工具的开发相结合，使其他人能够从该项目的发展中受益。渗透维里方程形成了工作的理论框架。的研究目标是：（1）开发强大的和准确的方法来计算渗透维里系数至少达到5阶，从分子模型，同时制定近似扩展其范围;（2）检查硬凸颗粒的混合物的行为，特别是集中在熵驱动的聚集和流体-流体相不稳定性。高通量筛选，使用这些集群积分方法预计将产生至少5000个物种对的数据;（3）调查协会的蛋白质在溶液中，特别是考虑到拥挤的分子对这种行为的影响。

With this award, the the Chemical Theory, Models and Computational Methods Program in the Chemistry Division is supporting David Kofke and Andrew Schultz of the University at Buffalo/SUNY to develop a hierarchal theoretical and computational approach to studying chemical solutions. Chemical solutions are ubiquitous in natural and man-made systems, and their behavior is critical to many applications in technology, including healthcare, energy storage, environmental preservation, and food and consumer products. One approach to the description of chemical solutions is via a hierarchy of solute interactions, considering first the solute molecules individually, then taken in pairs, then groups of three, four, and so on. Each level in this hierarchy introduces new information about the mixture, such that one can infer the full behavior by proper analysis of these interactions. The quantities needed for this formulation can in principle be computed from detailed molecular considerations, which is desirable because it leads to greater predictive and descriptive capability. However, the means to perform these calculations for practical purposes have not been developed, so the full potential of the overall approach is relatively untested. Developing and benchmarking this approach is the focus of this research projects. The project integrates training of graduate students with outreach activities and development of learning materials and computer-based tools that permit others to benefit from the developments in this project.The osmotic virial equation forms the theoretical framework the work. The research objectives of are: (1) to develop robust and accurate methods for calculating osmotic virial coefficients up to at least 5th order, from a molecular model, while formulating approximants that extend their reach; (2) to examine behavior of mixtures of hard convex particles, focusing in particular on entropy-driven aggregation and fluid-fluid phase instability. High-throughput screening using these cluster-integral methods is anticipated to yield data for at least 5000 species pairs; (3) to investigate association of proteins in solution, considering in particular the effect of crowder molecules on this behavior.