Uncertainty Qualification for Deep Learning-Based Elementary Reaction Property Prediction

Abstract

The prediction of the thermodynamic and kinetic properties of elementary reactions has shown rapid improvement due to the implementation of deep learning (DL) methods. While various studies have reported the success in predicting reaction properties, the quantification of prediction uncertainty has seldom been investigated, thus compromising the confidence in using these predicted properties in practical applications. Here, we integrated graph convolutional neural networks (GCNN) with three uncertainty prediction techniques, including deep ensemble, Monte Carlo (MC)-dropout, and evidential learning, to provide insights into the uncertainty quantification and utility. The deep ensemble model outperforms others in accuracy and shows the highest reliability in estimating prediction uncertainty across all elementary reaction property data sets. We also verified that the deep ensemble model showed a satisfactory capability in recognizing epistemic and aleatoric uncertainties. Additionally, we adopted a Monte Carlo Tree Search method for extracting the explainable reaction substructures, providing a chemical explanation for DL predicted properties and corresponding uncertainties. Finally, to demonstrate the utility of uncertainty qualification in practical applications, we performed an uncertainty-guided calibration of the DL-constructed kinetic model, which achieved a 25% higher hit ratio in identifying dominant reaction pathways compared to that of the calibration without uncertainty guidance.