New Extensions to Symmetry-adapted Perturbation Theory: Spin Splittings, Explicitly Correlated Dispersion, and Intramolecular Interactions

对称适应微扰理论的新扩展：自旋分裂、显式相关色散和分子内相互作用

• 批准号: 1955328
• 负责人: Konrad Patkowski
• 金额: $ 43.36万
• 依托单位: Auburn University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-07-01 至 2024-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1955328&HistoricalAwards=false
• 关键词: New; Extensions; Symmetry; adapted; Perturbation

Professor Konrad Patkowski of Auburn University is supported by an award from the Chemical Theory, Models, and Computational Methods program in the Division of Chemistry to develop new computational methods that extend the capabilities of calculating weak interaction energies between molecules. These methods combine high accuracy with interpretive power, providing insight into the physical origins of interactions between molecules. This kind of insight is aids in the understanding, simulation, and rational design of interactions that play key roles in chemistry, physics, biochemistry, and materials science. The new methods developed by Patkowski and his group, which are being implemented in an open-source computer program, are useful for describing interactions relevant to atmospheric chemistry, molecular magnetism, and transition metal catalysis. They also provide a new route to quantifying and interpreting interactions between different fragments of the same molecule, such as those that control the three-dimensional structure of proteins and nucleic acids. In addition, Patkowski continues to develop hands-on computational chemistry modules within the framework of the Auburn University Summer Science Institute, providing realistic research experiences to high-school students and enhancing their awareness of careers in science. He is also facilitating course redesign workshops for Auburn University faculty to facilitate active learning techniques into their classes.The approaches developed by Professor Patkowski and his group extend the symmetry-adapted perturbation theory (SAPT) method for calculating interaction energies between molecules in terms of electrostatic, induction, dispersion, and exchange interactions. In its most common closed-shell formulation, SAPT is widely used to construct intermolecular potential energy surfaces, interpret, and compare the origins of bonding for different complexes and structures, and aid in the construction of force fields. Patkowski is developing three new approaches that enhance the basis set convergence of existing SAPT treatments through an explicitly correlated framework. This will extend the method to complexes in low-spin states by building explicit spin-flip excitations into the exchange energy expressions, and open up a new avenue of application to intramolecular noncovalent interactions, based on range separation of the Coulomb potential rather than fragmentation of the system. Applications of the newly constructed SAPT variants include the elucidation of spin splittings in organic ferromagnets, radical cation-radical anion interactions, and pancake-bonded dimers, the refinement of benchmark energy component databases for force field fitting and classification of complexes according to interaction types. This enables the quantitative description of intramolecular interactions responsible for the stability of sterically crowded molecules and the conformational profiles of molecular balances.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.

奥本大学的Konrad Patkowski教授得到了化学系化学理论、模型和计算方法计划的支持，以开发新的计算方法，扩展计算分子之间弱相互作用能的能力。这些方法结合了高精度和解释力，提供了对分子之间相互作用的物理起源的洞察。这种洞察力有助于理解、模拟和合理设计在化学、物理、生物化学和材料科学中发挥关键作用的相互作用。帕特科夫斯基和他的团队开发的新方法正在一个开源计算机程序中实施，对于描述与大气化学、分子磁性和过渡金属催化有关的相互作用是有用的。它们还提供了一条量化和解释同一分子不同片段之间相互作用的新途径，例如那些控制蛋白质和核酸三维结构的片段。此外，帕特科夫斯基继续在奥本大学暑期科学学院的框架内开发动手计算化学模块，为高中生提供现实的研究体验，并增强他们对科学职业的意识。帕特科夫斯基教授和他的团队开发的方法扩展了对称适应微扰理论(SAPT)方法，从静电、感应、色散和交换相互作用的角度计算分子之间的相互作用能。在其最常见的闭壳公式中，SAPT被广泛用于构建分子间势能面，解释和比较不同络合物和结构的成键来源，并帮助构建力场。Patkowski正在开发三种新的方法，通过一个明确相关的框架来增强现有SAPT治疗的基础集收敛。这将通过在交换能表达式中建立显式的自旋翻转激发，将该方法扩展到低自旋态的络合物，并基于库仑势的范围分离而不是系统的碎裂，开辟了一条应用于分子内非共价相互作用的新途径。新构建的SAPT变体的应用包括阐明有机铁磁体中的自旋分裂、自由基阳离子-自由基阴离子相互作用和煎饼键二聚体，完善用于力场拟合的基准能量分量数据库，以及根据相互作用类型对络合物进行分类。这使得能够定量描述分子内相互作用对空间拥挤分子的稳定性和分子平衡的构象分布的影响。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Nonapproximated third-order exchange induction energy in symmetry-adapted perturbation theory

对称适应微扰理论中的非近似三阶交换感应能

• DOI: 10.1063/5.0035050
• 发表时间: 2021
• 期刊: The Journal of Chemical Physics
• 作者: Waldrop, Jonathan M.;Patkowski, Konrad
• 通讯作者: Patkowski, Konrad

Collisional line-shape effects in accurate He-perturbed H 2 spectra

精确 He 扰动 H 2 光谱中的碰撞线形效应

• DOI: 10.1016/j.jqsrt.2021.107951
• 发表时间: 2022
• 期刊: Journal of Quantitative Spectroscopy and Radiative Transfer
• 影响因子: 2.3
• 作者: Słowiński, Michał;Jóźwiak, Hubert;Gancewski, Maciej;Stankiewicz, Kamil;Stolarczyk, Nikodem;Tan, Yan;Wang, Jin;Liu, An-Wen;Hu, Shui-Ming;Kassi, Samir
• 通讯作者: Kassi, Samir

Efficient Density-Fitted Explicitly Correlated Dispersion and Exchange Dispersion Energies

• DOI: 10.1021/acs.jctc.0c01158
• 发表时间: 2021-02-19
• 期刊: JOURNAL OF CHEMICAL THEORY AND COMPUTATION
• 影响因子: 5.5
• 作者: Kodrycka, Monika;Patkowski, Konrad
• 通讯作者: Patkowski, Konrad

Overcoming Artificial Multipoles in Intramolecular Symmetry-Adapted Perturbation Theory

克服分子内对称性微扰理论中的人工多极子

• DOI: 10.1021/acs.jpca.2c06465
• 发表时间: 2023
• 期刊: The Journal of Physical Chemistry A
• 作者: Luu, Du;Patkowski, Konrad
• 通讯作者: Patkowski, Konrad

Ab Initio Study of Chiral Discrimination in the Glycidol Dimer

缩水甘油二聚体手性辨别的从头算研究

• DOI: 10.1021/acs.jpca.0c07764
• 发表时间: 2020
• 期刊: The Journal of Physical Chemistry A
• 作者: Hemmati, Reza;Patkowski, Konrad
• 通讯作者: Patkowski, Konrad