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.

摘要目标：开发用于相平衡的可传递力场以及微异质流体中聚集和溶剂化的模拟研究准确了解复杂流体混合物的相平衡和其他热物理性质具有巨大的基础和实际意义。分子模拟在预测热物理性质以及增进我们对分子结构与宏观可观测之间关系的理解方面的成功取决于有效的模拟算法和精确的力场的可用性。 拟议研究的目标是开发三个级别的可转移力场和有偏差的蒙特卡罗方法。第一级力场称为 TraPPE-UA（相平衡联合原子的可转移势），采用烷基链段的联合原子表示以及简单的 Lennard-Jones 和库仑项。在第二层中，称为 TraPPE{EH（显式氢），所有原子（包括烷基氢和无人对电子和键中心位点）都经过显式处理。在第三层，称为 TraPPE-pol（可极化），范德华力和静电相互作用都可以响应环境的变化。第一级的设计是为了简单性和计算效率以及良好的准确性，第二级旨在提高非极性或极性非氢键化合物的混合物的准确性。第三级仅针对尽可能高的准确性和可转移性。 该项目将把 TraPPE-UA 力场扩展到炔烃；烯烃氧化物； 5元同芳香环和杂芳香环；卤代烃；伯、仲、叔氢氟醇、醚和氧化物；以及含硅和磷的官能团。 TraPPE-EH力场将扩展到环烷烃、烯烃和芳烃。 TraPPE-pol 力场的开发将继续使用水、烷烃、醇和醚的通用参数。除了力场开发之外，该项目还解决了相平衡第一原理模拟的新颖模拟策略。使用可转移力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性质，从而添加到可用的实验数据库中。这些模拟为复杂的化学系统提供了微观层面的信息，从而为分子结构和组成如何决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）均匀成核现象，（ii）含有非离子表面活性剂的混合物中的界面性质、聚集和溶解度，以及（iii）单体/低聚物/聚合物体系中的混溶性。 拟议工作的更广泛影响包括开发可转移力场、先进算法和软件包，这些软件包可通过印刷出版物、网络界面和 GNU 通用公共许可证免费提供。这些工具受到大型研究界的热切期待。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，并将继续进行推广。 该项目将由一个紧密的大学工业团队进行广泛合作，该团队由 PI、两名研究生和博士组成。明尼苏达州圣保罗 3M 中央研究中心的 Ross 和 Caldwell。