First-Principles Reaction Dynamics beyond Six-Atom Systems

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 stationarypoint properties with subchemical accuracy, the ROBOSURFER program system enabling automatic PES development, and applications for the Cl + C2H6, F + C2H6, and OH- + CH3I post-six-atom reactions focusing on ab initio issues and their solutions as well as showing the excellent agreement between theory and experiment.

Automated summary

This study discusses the new era and future of first-principles reaction dynamics beyond the six-atomic benchmark systems, focusing on complex, multichannel chemical reactions. Methodology involves benchmark ab initio characterization of stationary points, full-dimensional PES developments, and reaction dynamics computations. The composite ab initio approach, ROBOSURFER program system, and applications for post-six-atom reactions highlight issues, solutions, and excellent agreement between theory and experiment.