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: 2020
• 资助国家: 加拿大
• 起止时间: 2020-01-01 至 2021-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=709875
• 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.

我的研究项目侧重于密度泛函理论 (DFT) 的开发和应用，目标是扩大 DFT 可以可靠应用的化学系统的范围。密度泛函理论已成为计算化学中事实上的标准电子结构方法。它几乎用于所有化学领域的学术和工业环境，包括新药、催化剂和材料的设计。 DFT 方法已经发展到对于小分子或网络固体高度准确的程度。然而，下一个前沿领域是开发精确有效计算分子间相互作用能量的方法，这种相互作用在液体、分子固体和超分子组装体中很常见。因此，我的研究计划的特别重点是开发分子间相互作用的计算研究方法。我的团队致力于扩大我们对密度泛函在分子间化学中分解的理解，开发和测试改进的方法，然后应用它们来获得新的物理和化学见解。拟议的研究涉及应用我的小组开发的密度泛函分散方法来解决材料化学中的主要挑战，包括晶体多晶型排序以及手性分子的尺度混合物的分离。这项工作涉及各种晶体多晶型的相对能量学以及手性晶体的相平衡和层状孪生的计算研究，所有这些都需要对分子间相互作用的能量学进行高精度预测。补充项目侧重于开发计算电子离域指数的新方法，以及开发改进的密度泛函，以减少电荷转移误差，两者均适用于分子固体。这些项目都符合分子间化学 DFT 开发和应用的总体主题。未来五年，我的研究项目将为本科生、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等各个领域。