Using principal component analysis for neural network high-dimensional potential energy surface

Abstract

Potential energy surfaces (PESs) play a central role in our understanding of chemical reactions. Despite the impressive development of efficient electronic structure methods and codes, such computations still remain a difficult task for the majority of relevant systems. In this context, artificial neural networks (NNs) are promising candidates to construct the PES for a wide range of systems. However, the choice of suitable molecular descriptors remains a bottleneck for these algorithms. In this work, we show that a principal component analysis (PCA) is a powerful tool to prepare an optimal set of descriptors and to build an efficient NN: this protocol leads to a substantial improvement of the NNs in learning and predicting a PES. Furthermore, the PCA provides a means to reduce the size of the input space (i.e., number of descriptors) without losing accuracy. As an example, we applied this novel approach to the computation of the high-dimensional PES describing the keto-enol tautomerism reaction occurring in the acetone molecule.