Evaluation of Rate Coefficients in the Gas Phase Using Machine-Learned Potentials.

Abstract

We assess the capability of machine-learned potentials to compute rate coefficients by training a neural network (NN) model and applying it to describe the chemical landscape on the C5H5 potential energy surface, which is relevant to molecular weight growth in combustion and interstellar media. We coupled the resulting NN with an automated kinetics workflow code, KinBot, to perform all necessary calculations to compute the rate coefficients. The NN is benchmarked exhaustively by evaluating its performance at the various stages of the kinetics calculations: from the electronic energy through the computation of zero point energy, barrier heights, entropic contributions, the portion of the PES explored, and finally the overall rate coefficients as formulated by transition state theory.