Prediction of transition state structures of gas-phase chemical reactions via machine learning

Abstract

The elucidation of transition state (TS) structures is essential for understanding the mechanisms of chemical reactions and exploring reaction networks. Despite significant advances in computational approaches, TS searching remains a challenging problem owing to the difficulty of constructing an initial structure and heavy computational costs. In this paper, a machine learning (ML) model for predicting the TS structures of general organic reactions is proposed. The proposed model derives the interatomic distances of a TS structure from atomic pair features reflecting reactant, product, and linearly interpolated structures. The model exhibits excellent accuracy, particularly for atomic pairs in which bond formation or breakage occurs. The predicted TS structures yield a high success ratio (93.8%) for quantum chemical saddle point optimizations, and 88.8% of the optimization results have energy errors of less than 0.1 kcal mol−1. Additionally, as a proof of concept, the exploration of multiple reaction paths of an organic reaction is demonstrated based on ML inferences. I envision that the proposed approach will aid in the construction of initial geometries for TS optimization and reaction path exploration.