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

职业：约束多组分密度泛函理论的发展以及从头算分子动力学中准确有效地结合核量子效应

• 批准号: 2238473
• 负责人: Yang Yang
• 金额: $ 65万
• 依托单位: University of Wisconsin-Madison
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-12-01 至 2027-11-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2238473&HistoricalAwards=false
• 关键词: CAREER; Development; Constrained; Multicomponent; Density

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.

在化学理论，模型和计算方法（CTMC）方案的支持下，威斯康星大学 - 麦迪逊分校的阳阳博士正在开发可以准确有效地描述和模拟具有重大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，可以强烈影响其许多静态和动态特性。但是，核量子效应的准确性和有效掺入仍然是一个挑战。杨博士和他的研究小组将通过为核量子效应制定新的分子动力学模拟框架来应对这一挑战。他们将在周期性边界条件下发展理论，利用新理论研究一系列与水相关的系统，并阐明核量子对水的结构和振动特性的影响。开发的所有方法将以开源软件包为公众免费。此外，作为一种协同的教育工作，为了帮助本科生更好地了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其研究材料转变为教育材料。在计算实验室模块中，学生将在模型和真实分子系统中尝试经典的分子动力学和CNEO-MD，从而深刻了解核量子效应在化学中的重要性。在该项目中，YANG研究小组将继续他们开发约束的核核 - 轨道密度函数理论（CNEO-DFT）以及与Molecular Morecular Morecular Morecration（Cneo-Morecular-Melecular-Melecular）（CNEO-MERECURAL-MERECTARIDIAD（CNEO-MORECURAL）（CNE-MERECURAL）（CNE-MERECURAL）（CNE-MORECURAL MORECURAL）（CNE）。他们将在周期性的边界条件下开发CNEO-DFT，以便可以有效地应用于冷凝相系统。对于实际应用，杨博士和他的研究小组将利用欧洲血体 - 研究一系列相关的系统，从（质子化的）水簇到水中的水，以阐明核量子对其结构和振动性能的影响，以及证明CNEO-MD的有效性。为了扩大这些研究的科学影响，分别将通过开源软件软件包PYSCF和CP2K为社区免费提供分子和周期系统的代码。该奖项反映了NSF的法定任务，并通过使用该基金会的智力功能和广泛的影响来评估Criteria criteria criteria。

项目成果

Calculating Vibrational Excited State Absorptions with Excited State Constrained Minimized Energy Surfaces

使用激发态约束最小化能量面计算振动激发态吸收

• DOI: 10.1021/acs.jpca.3c01420
• 发表时间: 2023
• 期刊: The Journal of Physical Chemistry A
• 作者: Wang, Yiwen;Chen, Zehua;Yang, Yang
• 通讯作者: Yang, Yang