Intermolecular Chemistry from Density-Functional Theory

密度泛函理论的分子间化学

• 批准号: RGPIN-2021-02394
• 负责人: Johnson, Erin
• 金额: $ 4.66万
• 依托单位: Dalhousie University
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2022
• 资助国家: 加拿大
• 起止时间: 2022-01-01 至 2023-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=747930
• 关键词: Intermolecular; Chemistry; Density; Functional; Theory

Theoretical chemistry complements experiment by allowing researchers to model chemical processes computationally. Theory can interpret and explain experimental findings, and is poised to guide experimental design of new drugs, catalysts, and materials, reducing required laboratory time and resources. Density-functional theory (DFT) is the workhorse of computational chemistry, being the most widely used modeling technique for applications ranging from biochemistry to materials physics. However, while accurate application of DFT to covalent bonding and intramolecular chemistry was primarily a challenge for the 20th century, its application to non-covalent interactions and intermolecular chemistry remains a challenge for the 21st. London dispersion, while being the weakest intermolecular interaction, is ubiquitous in chemistry. Accurate modeling of dispersion is essential in controlling the 3D structure of biomolecules, solute-solvent interactions, friction and adhesion, molecular self assembly, surface adsorption, molecular crystal packings, and phase transitions. Within the realm of materials chemistry, accurate theoretical description of intermolecular interactions is particularly relevant for computational design and screening of functional materials and interfaces with targeted properties. The long-term objectives of my research program are to develop a comprehensive set of tools to allow routine theoretical treatment of intermolecular chemistry, with simultaneous high accuracy and computational efficiency, and to use these tools to tackle outstanding challenges in the field of materials chemistry. To address these objectives, the present proposal focuses on three central research themes: (i) fundamental research on London dispersion, improving the accuracy and efficiency of DFT-based dispersion methods (ii) development of hierarchical techniques for molecular crystal-structure prediction; and (iii) large-scale computational modeling of 2D materials and interfaces. Impacts of the work within the field will be the advancement of our fundamental understanding of London dispersion, electronic interactions, and density-functional theory. The new methods and implementations to be developed should become widely used within the computational chemistry community, both within Canada and worldwide, for applications including modeling of biomolecular systems, organic chemistry, catalysis, materials chemistry, and solid-state physics. This will serve to further strengthen Canada's long-held position as an international leader in the field of density-functional theory. These methods can also be used to facilitate rapid, high-throughput screening of candidate materials, streamlining the design of functional materials for clean-energy and technology applications, and leading to devices that will eventually improve the standard of living for Canadians.

理论化学通过允许研究人员对化学过程进行计算建模来补充实验。理论可以解释和解释实验结果，并准备指导新药物、催化剂和材料的实验设计，减少所需的实验室时间和资源。密度泛函理论 (DFT) 是计算化学的主力，是从生物化学到材料物理等应用领域中使用最广泛的建模技术。然而，虽然 DFT 准确应用于共价键合和分子内化学主要是 20 世纪的挑战，但其在非共价相互作用和分子间化学中的应用仍然是 21 世纪的挑战。伦敦色散虽然是最弱的分子间相互作用，但在化学中普遍存在。准确的分散建模对于控制生物分子的 3D 结构、溶质-溶剂相互作用、摩擦和粘附、分子自组装、表面吸附、分子晶体堆积和相变至关重要。在材料化学领域，分子间相互作用的准确理论描述对于具有目标特性的功能材料和界面的计算设计和筛选特别重要。我的研究计划的长期目标是开发一套全面的工具，以便对分子间化学进行常规理论处理，同时具有高精度和计算效率，并使用这些工具来应对材料化学领域的突出挑战。 为了实现这些目标，本提案重点关注三个中心研究主题：（i）伦敦色散的基础研究，提高基于DFT的色散方法的准确性和效率（ii）开发分子晶体结构预测的分层技术； (iii) 二维材料和界面的大规模计算建模。该领域工作的影响将是加深我们对伦敦色散、电子相互作用和密度泛函理论的基本理解。待开发的新方法和实施应在加拿大和全世界的计算化学界广泛使用，其应用包括生物分子系统建模、有机化学、催化、材料化学和固态物理学。这将有助于进一步加强加拿大长期以来作为密度泛函理论领域国际领导者的地位。这些方法还可用于促进候选材料的快速、高通量筛选，简化清洁能源和技术应用功能材料的设计，并开发出最终将提高加拿大人生活水平的设备。