Density-Functional Theory for Intermolecular Chemistry

我的研究重点是密度泛函理论(DFT)的发展和应用，目的是扩大DFT可以可靠应用到的化学体系的范围。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。它被用于几乎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方法已经发展到了对小分子或网络固体高度精确的程度。然而，下一个前沿是发展准确和有效地计算分子间相互作用的能量学的方法，因为分子间相互作用在液体、分子固体和超分子组件中很普遍。因此，我的研究计划的一个特别重点是发展分子间相互作用的计算研究方法。我的团队致力于迭代过程，扩大我们对分子间化学的密度泛函在哪里分解的理解，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。这项拟议的研究涉及应用我的团队开发的密度泛函分散方法来解决材料化学中的主要挑战，包括晶体多晶型排名以及手性分子比例混合物的分离。这项工作涉及各种晶型的相对能量学的计算研究，以及手性晶体的相平衡和片层孪生，所有这些都需要对分子间相互作用的能量学进行高精度的预测。补充项目侧重于开发计算电子离域指数的新方法，以及开发具有减少电荷转移误差的改进的密度泛函，两者都适用于分子固体。这些项目都符合分子间化学密度泛函的开发和应用这一主旋律。在接下来的五年里，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个领域。

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.**