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Development of Molecular Simulation Methods to Compute Phase and Interfacial Properties of Complex Fluids

计算复杂流体的相和界面性质的分子模拟方法的发展

基本信息

批准号：
1900344
负责人：
Jeffrey Errington
金额：
$ 39.44万
依托单位：
SUNY at Buffalo
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2019
资助国家：
美国
起止时间：
2019-06-01 至 2025-05-31
项目状态：
未结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1900344&HistoricalAwards=false
关键词：
Development Molecular Simulation Methods Compute

项目摘要

Jeffrey Errington and Andrew Schultz of SUNY at Buffalo are supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to develop computational methods and tools to predict properties of complex molecular systems. This project is co-funded by the Computational and Data-Enabled Science and Engineering in Chemical, Bioengineering, Environmental and Transport Systems Program in the Division of Engineering. The project focuses on phase (gas, liquid, solid) and interfacial (e.g. where air and water meet) properties. The properties play a key role in many natural phenomena and in numerous industrial processes. Of particular value to scientists and engineers is an understanding of the relationship between the microscopic interactions, for example at the atomic level, and the macroscopic behavior it exhibits. Such information can be used to tune the molecular-level details of a system to obtain a desired behavior. In principle, molecular simulation provides an ideal tool for studying the phase and interfacial behaviors of complex fluids. Although tremendous advancements have been made in this area, there is still a huge need for efficient and effective computational methods. Professors Errington and Schultz and their groups are developing robust new strategies for interrogating the phase and interfacial properties of complex fluids via molecular simulation. Examples that illustrate the need for such methods include the design of separation technologies, energy storage devices, carbon capture strategies, and surface coatings. The results of this research will be implemented in software that is freely available to the broader research community. The focus of this research is to develop molecular simulation methods that enable one to deduce the bulk and interfacial properties of complex fluids. Two methodological advances are being pursued: (1) a new rigorous strategy for computing the bulk liquid-vapor saturation properties of fluids and (2) a force-based strategy to determine the spreading interface potential within an isothermal-isobaric ensemble. For the first, virial pressure measurements are collected at multiple densities that span the liquid-vapor coexistence region, and subsequently used to construct a volume probability distribution within the isothermal-isobaric ensemble. The method provides the same level of information as commonly-used flat histogram approaches, does not require molecule insertions/deletions, and can be implemented within a molecular dynamics framework. The second methodological advance is aimed at increasing the accessibility of the spreading interface potential method. The interface potential provides important insight regarding qualitative and quantitative aspects of a system's wetting behavior. The general approach provides a means to determine the contact angle of a liquid droplet on a solid substrate in a mother vapor. The project addresses challenges associated with implementing the method within the commonly-used isothermal-isobaric ensemble. The standard approach results in highly elongated simulation boxes that are difficult to work with in practice. The research team has identified a means to significantly reduce the size of the simulation box required via use of a virtual box. The approach leverages force-based strategies to compute the interface potential. When combined with previous developments, this advance provides a rigorous, efficient, and accessible approach for determining the wetting properties of model systems. In a third effort, tools are developed to facilitate coupling of Monte Carlo and molecular dynamics algorithms within a single molecular simulation framework. Such a coupling enhances the efficiency of the methods noted above. Specifically, the group is contributing additional Monte Carlo move types to the publically- and freely-available LAMMPS Molecular Dynamics Simulator. These contributions are expected to be beneficial to the broad LAMMPS user community.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

纽约州立大学布法罗分校的杰弗里·埃林顿 (Jeffrey Errington) 和安德鲁·舒尔茨 (Andrew Schultz) 获得化学系化学理论、模型和计算方法项目的资助，开发计算方法和工具来预测复杂分子系统的特性。该项目由工程系化学、生物工程、环境和运输系统计算和数据科学与工程项目共同资助。该项目侧重于相（气体、液体、固体）和界面（例如空气和水相遇的地方）特性。这些特性在许多自然现象和众多工业过程中发挥着关键作用。对于科学家和工程师来说，特别有价值的是了解微观相互作用（例如原子水平）与其表现出的宏观行为之间的关系。此类信息可用于调整系统的分子水平细节以获得所需的行为。原则上，分子模拟为研究复杂流体的相和界面行为提供了理想的工具。尽管该领域已经取得了巨大进步，但仍然非常需要高效且有效的计算方法。 Errington 和 Schultz 教授及其团队正在开发强大的新策略，通过分子模拟来探究复杂流体的相和界面特性。说明需要此类方法的例子包括分离技术、能量存储装置、碳捕获策略和表面涂层的设计。这项研究的结果将在软件中实现，该软件可供更广泛的研究界免费使用。这项研究的重点是开发分子模拟方法，使人们能够推断出复杂流体的体积和界面特性。正在追求两项方法论进展：（1）计算流体的体液-气饱和特性的新的严格策略；（2）基于力的策略来确定等温-等压系综内的扩展界面势。首先，以跨越液-气共存区域的多个密度收集维里压力测量值，随后用于构建等温-等压系综内的体积概率分布。该方法提供与常用的平面直方图方法相同水平的信息，不需要分子插入/删除，并且可以在分子动力学框架内实施。第二个方法论进展旨在提高扩展界面电位方法的可访问性。界面势提供了有关系统润湿行为的定性和定量方面的重要见解。一般方法提供了一种确定母蒸气中固体基质上液滴的接触角的方法。该项目解决了与在常用的等温等压系综中实施该方法相关的挑战。标准方法会导致模拟盒高度拉长，在实践中很难使用。研究团队已经找到了一种通过使用虚拟盒子来显着减小所需模拟盒尺寸的方法。该方法利用基于力的策略来计算界面势。与之前的发展相结合，这一进步提供了一种严格、高效且易于使用的方法来确定模型系统的润湿特性。第三项工作是开发工具来促进蒙特卡罗和分子动力学算法在单个分子模拟框架内的耦合。这种耦合提高了上述方法的效率。具体来说，该小组正在向公开且免费提供的 LAMMPS 分子动力学模拟器贡献更多蒙特卡罗移动类型。这些贡献预计将有益于广大的 LAMMPS 用户社区。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力价值和更广泛的影响审查标准进行评估，被认为值得支持。