Theoretical Studies of Intermolecular Forces

分子间力的理论研究

• 批准号: 1152899
• 负责人: Krzysztof Szalewicz
• 金额: $ 44.4万
• 依托单位: University of Delaware
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2012
• 资助国家: 美国
• 起止时间: 2012-05-01 至 2016-04-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1152899&HistoricalAwards=false
• 关键词: Theoretical; Studies; Intermolecular; Forces

Krzysztof Szalewicz of the University of Delaware is supported by an award from the Chemical Theory, Models and Computational Methods program to perform theoretical investigations of molecular clusters, condensed phases, and biochemical aggregates. The goal of this work is to increase understanding of physical, chemical, and biochemical phenomena that depend on inter-molecular forces. These properties can be predicted theoretically if high-accuracy potential energy surfaces, or force fields, are known. Such surfaces are computed ab initio using symmetry-adapted perturbation theory (SAPT) co-developed by the PI. SAPT provides a unique ability to interpret properties dependent on intermolecular forces in terms of the four fundamental physical mechanisms that lead to the electrostatic, exchange, induction, and dispersion contributions to the interaction energies. Such interpretation also provides a connection between the cluster properties and the properties of the constituent monomers. A version of SAPT based on monomers described by density-functional theory is currently the only method which can be applied to compute interactions between molecules containing about 100 atoms with uncertainties of only a few percent. SAPT is undergoing further developments, in particular applying localization techniques that should further increase the range of tractable systems. Several applications intended to assist interpretation of experimental data for systems ranging from diatoms to molecular crystals are underway. Such applications include developments of system-specific force fields which are then used in nuclear dynamics calculations and molecular simulations. Also, system-universal force fields are developed. The proposed activity will result in a better understanding of intermolecular interactions which govern properties of condensed phases and biological aggregates. Novel ideas aimed at improvement of theoretical tools for investigations of these interactions are investigated. The development of first-principle-based universal force fields has the promise of transforming the field of biomolecular simulation. This activity will also result in new pressure and temperature standards, help in developments of "green chemistry", aid explorations of energy resources, provide data for constructing models of the atmosphere, help to understand processes in interstellar molecular clouds, guide development of nanomaterials, make simulations of biological phenomena more reliable, and assist pharmaceutical industry in predictions of polymorphic forms of medical drugs. The SAPT software available free to all interested researchers and used by about 500 groups worldwide is continuously improved in efficiency and user friendliness.

特拉华大学的 Krzysztof Szalewicz 获得了化学理论、模型和计算方法项目的奖项，以进行分子簇、凝聚相和生化聚集体的理论研究。这项工作的目标是增进对依赖分子间力的物理、化学和生化现象的理解。如果高精度势能面或力场已知，则可以从理论上预测这些特性。这些表面是使用 PI 共同开发的对称适应扰动理论 (SAPT) 从头开始​​计算的。 SAPT 提供了一种独特的能力，可以根据导致静电、交换、感应和色散对相互作用能贡献的四种基本物理机制来解释依赖于分子间力的属性。这种解释还提供了簇性质和组成单体的性质之间的联系。基于密度泛函理论描述的单体的 SAPT 版本是目前唯一可用于计算包含约 100 个原子的分子之间相互作用的方法，且不确定性仅为百分之几。 SAPT 正在进一步发展，特别是应用本地化技术，这将进一步扩大可处理系统的范围。一些旨在帮助解释从硅藻到分子晶体等系统的实验数据的应用正在进行中。此类应用包括开发系统特定的力场，然后将其用于核动力学计算和分子模拟。此外，还开发了系统通用力场。拟议的活动将有助于更好地理解控制凝聚相和生物聚集体特性的分子间相互作用。研究了旨在改进研究这些相互作用的理论工具的新想法。基于第一原理的通用力场的发展有望改变生物分子模拟领域。这项活动还将产生新的压力和温度标准，有助于“绿色化学”的发展，帮助勘探能源，为构建大气模型提供数据，帮助了解星际分子云的过程，指导纳米材料的发展，使生物现象的模拟更加可靠，并协助制药行业预测医疗药物的多晶型。 SAPT 软件免费提供给所有感兴趣的研究人员，并被全球约 500 个团体使用，其效率和用户友好性不断提高。