Density-Functional Theory for 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.