Outlier-detection for reactive machine learned potential energy surfaces

Uncertainty quantification (UQ) to detect samples with large expected errors (outliers) is applied to reactive molecular potential energy surfaces (PESs). Three methods-Ensembles, deep evidential regression (DER), and Gaussian Mixture Models (GMM)-were applied to the H-transfer reaction between syn-Criegee and vinyl hydroxyperoxide. The results indicate that ensemble models provide the best results for detecting outliers, followed by GMM. For example, from a pool of 1000 structures with the largest uncertainty, the detection quality for outliers is ~90% and ~50%, respectively, if 25 or 1000 structures with large errors are sought. On the contrary, the limitations of the statistical assumptions of DER greatly impact its prediction capabilities. Finally, a structure-based indicator was found to be correlated with large average error, which may help to rapidly classify new structures into those that provide an advantage for refining the neural network.