GOALI: Development of Transferable Force Fields for Phase Equilibria and Simulation Studies of Aggregation and Solvation in Microheterogeneous Fluids

目标：相平衡可转移力场的开发以及微异质流体中聚集和溶剂化的模拟研究

• 批准号: 0553911
• 负责人: Joern Ilja Siepmann
• 金额: $ 10万
• 依托单位: University of Minnesota-Twin Cities
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2006
• 资助国家: 美国
• 起止时间: 2006-04-01 至 2009-03-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0553911&HistoricalAwards=false
• 关键词: GOALI; Development; Transferable; Force; Fields

ABSTRACTGOALI: Development of Transferable Force Fields for Phase Equilibriaand Simulation Studies of Aggregation and Solvationin Microheterogeneous FluidsAccurate knowledge of the phase equilibria and other thermophysical properties of complex fluidmixtures is of enormous fundamental and practical importance. The success of molecular simulation in predicting thermophysical properties and in advancing our understanding of the relationship between molecular architecture and macroscopic observable depends on the availability of efficient simulation algorithms and accurate force fields. The goals of the proposed research are to develop three levels of transferable force fields and of biased Monte Carlo methods. The first-level force field, called TraPPE-UA (transferable potentials for phase equilibria united atom), employs the united-atom representation for alkyl segments and simple Lennard-Jones and Coulombic terms. In the second level, called TraPPE{EH (explicit hydrogen), all atoms including alkyl group hydrogens and somelone-pair electron and bond-center sites are treated explicitly. In the third-level, called TraPPE-pol (polarizable), both the van der Waals and electrostatic interactions can respond to changes in the environment. Whereas the first level is designed for simplicity and computational efficiency with good accuracy, the second level is aimed at improved accuracy for mixtures of non-polar or a polar non-hydrogen-bonding compounds. The third level is directed solely at the highest possible level of accuracy and transferability. The project will extend the TraPPE-UA force field to alkynes; alkene oxides; 5-membered homo- and hetero-aromatic rings; halogenated hydrocarbons; primary, secondary, and tertiary hydrofluoro alcohols, ethers, and oxides; and silicon and phosphorous containing functionalities. The TraPPE-EH force field will be extended to cyclic alkanes, alkenes, and arenes. An the development of the TraPPE-pol force field will be continued with common parameters for water, alkanes, alcohols, and ethers.In addition to force field development, this project also addresses novel simulation strategiesfor first principles simulations of phase equilibria. Molecular simulations using the transferableforce fields will be employed as engineering tool to predict thermophysical properties of a variety of systems, thereby adding to the available experimental database. The simulations provide microscopic-level information for complex chemical systems, thereby giving new physical insight into how molecular architecture and composition determine macroscopic phenomena. In particular, simulations will be carried out to investigate (i) homogeneous nucleation phenomena, (ii) interfacial properties, aggregation, and solubilities in mixtures containing non-ionic surfactants, and (iii) miscibility in monomer/oligomer/polymer systems. The broader impacts of the proposed work include the development of transferable force fields, advanced algorithms, and software packages that are made freely available through print publications, a web interface, and GNU General Public Licenses. These tools are eagerly awaited by a large research community. Furthermore, the proposed project will have a major impact on various educational, training, and mentoring activities and will allow continued outreach. This project will project from extensive collaboration of a tight university-industry team consisting of the PI, two graduate students, and Drs. Ross and Caldwell of 3M Central Research, St. Paul, MN.

AbstractGoali：开发用于相聚和溶剂化的相位平衡和溶剂化研究中的可转移力场的开发，对相位平衡和复杂流体流体的其他热物理特性的知识具有巨大的基本和实际重要性。分子模拟在预测热物理特性以及促进我们对分子结构与宏观可观察到的关系的理解方面的成功取决于有效的仿真算法和准确的力场的可用性。 拟议的研究的目标是发展三个级别的可转移力场和有偏见的蒙特卡洛方法。一级力场称为trappe-ua（相位平衡原子的可转移电位），采用了烷基段的联合原子代表，简单的Lennard-Jones和Colombic术语。在第二层中，称为trappe {eh（显式氢），所有原子在内的所有原子（包括烷基氢）和somelone pair电子和邦德中心位点均已明确处理。在称为trappe-pol（可极化）的第三级中，范德华和静电相互作用都可以响应环境的变化。尽管第一级是为了简单性和计算效率而设计的，但第二级旨在提高非极性或极性非氢键化合物混合物的精度。第三级仅针对最高的准确性和可传递性水平。 该项目将将Trappe-UA力场扩展到炔烃；烯烃氧化物； 5元的同型和异芳族环；卤代烃；原发性，二级和第三级氢醇，醚和氧化物；以及含有硅和磷的功能。 Trappe-eh力场将扩展到环烷烃，烷烃和竞技场。 Trappe-Pol力场的发展将继续使用水，烷烃，醇和醚的常见参数。除了力场发展外，该项目还解决了新型的模拟策略，用于相位平衡的第一原理模拟。使用转移Force场的分子模拟将被用作工程工具来预测各种系统的热物理特性，从而增加了可用的实验数据库。这些模拟为复杂的化学系统提供了微观级别的信息，从而为分子结构和组成如何确定宏观现象提供了新的物理见解。特别是，将进行模拟以研究（i）（ii）含有非离子表面活性剂混合物的界面特性，聚集和溶解度（III）（iii）单体/寡聚/聚合物系统中的混杂性。 拟议工作的更广泛的影响包括通过印刷出版物，Web界面和GNU通用公共许可证免费提供的可转移力领域，高级算法和软件包的开发。大型研究社区热切期待这些工具。此外，拟议的项目将对各种教育，培训和指导活动产生重大影响，并允许继续宣传。 该项目将来自一个由PI，两名研究生和DRS组成的紧密大学行业团队的广泛合作。 3M中央研究的Ross and Caldwell，明尼苏达州圣保罗。