Czakó Gábor, Győri Tibor, Papp Dóra, Tajti Viktor, Tasi Domonkos A
MTA-SZTE Lendület Computational Reaction Dynamics Research Group, Interdisciplinary Excellence Centre and Department of Physical Chemistry and Materials Science, Institute of Chemistry, University of Szeged, Rerrich Béla tér 1, Szeged H-6720, Hungary.
J Phys Chem A. 2021 Apr 1;125(12):2385-2393. doi: 10.1021/acs.jpca.0c11531. Epub 2021 Feb 25.
Moving beyond the six-atomic benchmark systems, we discuss the new age and future of first-principles reaction dynamics, which investigates complex, multichannel chemical reactions. We describe the methodology starting from the benchmark ab initio characterization of the stationary points, followed by full-dimensional potential energy surface (PES) developments and reaction dynamics computations. We highlight our composite ab initio approach providing benchmark stationary-point properties with subchemical accuracy, the Robosurfer program system enabling automatic PES development, and applications for the Cl + CH, F + CH, and OH + CHI post-six-atom reactions focusing on ab initio issues and their solutions as well as showing the excellent agreement between theory and experiment.
超越六原子基准系统，我们讨论第一性原理反应动力学的新时代和未来，该动力学研究复杂的多通道化学反应。我们描述了从驻点的基准从头算表征开始的方法，随后是全维势能面（PES）的开发和反应动力学计算。我们强调了我们的复合从头算方法，它能提供具有亚化学精度的基准驻点性质；Robosurfer程序系统能够实现PES的自动开发；以及针对Cl + CH、F + CH和OH + CHI后六原子反应的应用，重点关注从头算问题及其解决方案，并展示理论与实验之间的出色一致性。
