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

在化学系化学理论、模型和计算方法（CTMC）项目的支持下，威斯康星大学麦迪逊分校的杨洋博士正在开发能够准确有效地描述和模拟具有重要核量子效应的系统的方法。核量子效应在化学和生物系统中无处不在，并能强烈地影响它们的许多静态和动态特性。然而，核量子效应的精确和有效结合仍然是一个挑战。杨博士和他的研究小组将通过开发一个包含核量子效应的分子动力学模拟的新框架来应对这一挑战。他们将在周期边界条件下发展理论，利用新理论研究一系列与水有关的系统，并阐明核量子效应对水的结构和振动性质的影响。所有开发的方法都将以开源软件包的形式免费提供给公众。此外，作为一项协同教育努力，为了帮助本科生更好地理解化学中的核量子效应，杨研究小组将通过为本科生开发计算物理化学实验室模块，将他们的研究材料转化为教育材料。在计算实验模块中，学生将在模型和真实分子系统中进行经典分子动力学和cNEO-MD实验，从而深入了解核量子效应在化学中的重要性。在这个项目中，杨研究小组将继续发展约束核电子轨道密度泛函理论（cNEO-DFT）及其与分子动力学（cNEO-MD）的整合。他们将在周期边界条件下发展cNEO-DFT，使cNEO-MD能够有效地应用于凝聚相体系。在实际应用方面，杨博士和他的研究小组将利用cNEO-MD研究一系列与水相关的系统，从（质子化）水团簇到凝聚态水，以阐明核量子效应对其结构和振动特性的影响，并证明cNEO-MD的有效性。为了扩大这些研究的科学影响，分子和周期系统的代码将分别通过开源软件包PySCF和CP2K免费提供给社区。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

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.