Intermolecular Chemistry from Density-Functional Theory

理论化学通过允许研究人员计算化学过程来补充实验。理论可以解释和解释实验结果，并准备指导新药，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应用中最广泛使用的建模技术。然而，虽然精确应用密度泛函理论的共价键和分子内化学主要是一个挑战的世纪，其应用到非共价相互作用和分子间化学仍然是一个挑战的21世纪。伦敦色散是分子间相互作用最弱的一种，但在化学中却普遍存在。分散体的精确建模在控制生物分子的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、分子晶体填充和相变中是必不可少的。在材料化学领域内，分子间相互作用的精确理论描述对于具有目标性质的功能材料和界面的计算设计和筛选特别相关。我研究计划的长期目标是开发一套全面的工具，以实现分子间化学的常规理论处理，同时具有高准确性和计算效率，并使用这些工具来解决材料化学领域的突出挑战。为了实现这些目标，本提案侧重于三个中心研究主题：（i）伦敦分散的基础研究，提高基于DFT的分散方法的准确性和效率;（ii）分子晶体结构预测的分层技术的发展;和（iii）大规模的二维材料和界面的计算建模。该领域内的工作的影响将是我们的伦敦分散，电子相互作用和密度泛函理论的基本理解的进步。新的方法和实施将被开发，应成为广泛使用的计算化学界，无论是在加拿大和世界范围内，包括生物分子系统的建模，有机化学，催化，材料化学和固态物理的应用。这将有助于进一步加强加拿大长期以来在密度泛函理论领域的国际领导地位。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的功能材料的设计，并导致最终提高加拿大人生活水平的设备。

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.