Density-Functional Theory for Intermolecular Chemistry

分子间化学的密度泛函理论

• 批准号: RGPIN-2016-05795
• 负责人: Johnson, Erin
• 金额: $ 2.62万
• 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: 2017
• 资助国家: 加拿大
• 起止时间: 2017-01-01 至 2018-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=632417
• 关键词: Density; Functional; Theory; Intermolecular; Chemistry

My research program focuses on development and application of density-functional theory (DFT), with the goal of expanding the range of chemical systems to which DFT can be reliably applied. Density-functional theory has become the de facto standard electronic-structure method in computational chemistry. It is used in academic and industrial settings across virtually all areas of chemistry, including design of new drugs, catalysts, and materials. DFT methods have advanced to the point where they are highly accurate for small molecules or network solids. However, the next frontier is development of methods for accurate and efficient computation of the energetics of intermolecular interactions, as are prevalent in liquids, molecular solids, and super-molecular assemblies. Thus, a particular emphasis of my research program is placed on development of methods for computational study of intermolecular interactions. My group is engaged in the iterative process of expanding our understanding of where density functionals break down for intermolecular chemistry, developing and testing improved methods, and then applying them to gain new physical and chemical insights. The proposed research involves application of density-functional dispersion methods developed in my group to address major challenges in materials chemistry, including crystal polymorph ranking, as well as separation of scalemic mixtures of chiral molecules. This work involves computational investigation of the relative energetics of various crystal polymorphs, and of phase equilibria and lamellar twinning of chiral crystals, all of which require highly-accurate prediction of the energetics of intermolecular interactions. Complementary projects focus on development of new approaches for computation of electron delocalization indices and development of improved density functionals with reduced charge-transfer errors, both for molecular solids. These projects all fit into the overarching theme of development and application of DFT for intermolecular chemistry. Over the next five years, my research program will provide HQP training for undergraduate students, graduate students, and post-doctoral researchers. Our findings will impact the diverse fields of crystal-structure prediction, crystal engineering, organic synthesis, drug discovery, and materials chemistry.

我的研究计划着重于密度功能理论（DFT）的开发和应用，目的是扩大可靠应用DFT的化学系统范围。密度功能理论已成为计算化学中事实上的标准电子结构方法。它用于几乎所有化学领域的学术和工业环境中，包括新药，催化剂和材料的设计。 DFT方法已经发展到了它们对于小分子或网络固体高度准确的程度。但是，下一个前沿是开发用于准确有效地计算分子间相互作用的方法的发展，以及在液体，分子固体和超分子组件中普遍存在的方法。因此，我的研究计划的特别重点是开发用于分子间相互作用的计算研究方法。我的小组正在进行迭代过程，以扩展我们对密度功能分解的密度函数的理解，用于分子间化学，开发和测试改进的方法，然后应用它们以获得新的物理和化学见解。拟议的研究涉及在我的小组中开发的密度功能分散方法的应用，以应对材料化学的主要挑战，包括晶体多晶型级排名，以及手性分子的鳞状混合物的分离。这项工作涉及对手性晶体的各种晶体多晶型物的相对能量以及相位平衡和层状孪生的计算研究，所有这些都需要高度准确地预测分子间相互作用的能量。互补项目着重于开发电子定位指数计算的新方法，以及用于分子固体的电荷转移误差的改进密度函数的发展。这些项目都符合DFT开发和应用分子间化学的总体主题。在接下来的五年中，我的研究计划将为本科生，研究生和博士后研究人员提供HQP培训。我们的发现将影响晶体结构预测，晶体工程，有机合成，药物发现和材料化学的各种领域。