CAREER: Development of Constrained Multicomponent Density Functional Theory and Accurate and Efficient Incorporation of Nuclear Quantum Effects in ab initio Molecular Dynamics

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With support from the Chemical Theory, Models and Computational Methods (CTMC) program in the Division of Chemistry, Dr. Yang Yang of the University of Wisconsin–Madison is developing methods that can accurately and efficiently describe and simulate systems with significant nuclear quantum effects. Nuclear quantum effects are ubiquitous in chemical and biological systems and can strongly influence many of their static and dynamical properties. However, the accurate and efficient incorporation of nuclear quantum effects remains a challenge. Dr. Yang and his research group will tackle this challenge by developing a new framework for molecular dynamics simulations with nuclear quantum effects incorporated. They will develop the theory under periodic boundary conditions, utilize the new theory to study a series of water related systems, and elucidate the impacts of nuclear quantum effects on the structural and vibrational properties of water. All methods developed will be freely available to the public in open-source software packages. Additionally, as a synergetic educational effort, to help undergraduate students better understand nuclear quantum effects in chemistry, the Yang research group will transform their research materials into educational materials by developing a computational physical chemistry lab module for undergraduate students. In the computational lab module, students will experiment with both classical molecular dynamics and cNEO-MD in both model and real molecular systems, leading to a deep understanding of the importance of nuclear quantum effects in chemistry.In this project, the Yang research group will continue their development of constrained nuclear-electronic orbital density functional theory (cNEO-DFT) as well as its integration with molecular dynamics (cNEO-MD). They will develop cNEO-DFT under periodic boundary conditions so that cNEO-MD can be efficiently applied to condensed phase systems. For practical applications, Dr. Yang and his research group will utilize cNEO-MD to study a series of water related systems ranging from (protonated) water clusters to water in the condensed phase in order to elucidate the impact of nuclear quantum effects on their structural and vibrational properties as well as demonstrate the efficacy of cNEO-MD. To broaden the scientific impact of these studies, the codes for molecules and periodic systems will be made freely available to the community through the open-source software packages PySCF and CP2K, respectively.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.