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

奥本大学的Konrad Patkowski教授获得了化学系化学理论、模型和计算方法项目的奖励，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。这些方法结合了联合收割机的高精度与解释能力，提供了深入了解分子之间相互作用的物理起源。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。Patkowski和他的团队开发的新方法正在开源计算机程序中实现，可用于描述与大气化学，分子磁性和过渡金属催化相关的相互作用。它们还提供了一种新的途径来量化和解释同一分子的不同片段之间的相互作用，例如那些控制蛋白质和核酸三维结构的片段。此外，Patkowski继续在奥本大学暑期科学研究所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经验，提高他们对科学职业的认识。他还为奥本大学教师举办课程重新设计研讨会，以促进课堂上的主动学习技术。Patkowski教授和他的团队开发的方法扩展了自适应微扰理论（SAPT）方法，用于计算分子之间的静电、感应、色散和交换相互作用的相互作用能。在其最常见的闭壳层公式中，SAPT被广泛用于构建分子间势能面，解释和比较不同复合物和结构的键合起源，并帮助构建力场。Patkowski正在开发三种新方法，通过显式相关框架增强现有SAPT治疗的基集收敛。 这将扩展的方法，以配合物在低自旋状态下，通过建立明确的自旋翻转激发到交换能的表达式，并开辟了一个新的途径的应用分子内的非共价相互作用的基础上，范围分离的库仑势，而不是破碎的系统。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，以及煎饼键合的二聚体，用于力场拟合的基准能量分量数据库的改进和根据相互作用类型对复合物进行分类。 该奖项反映了NSF的法定使命，并通过使用基金会的智力价值和更广泛的影响审查标准进行评估，被认为值得支持。

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.