PiNN: Equivariant Neural Network Suite for Modeling Electrochemical Systems.

Abstract

Electrochemical energy storage and conversion play increasingly important roles in electrification and sustainable development across the globe. A key challenge therein is to understand, control, and design electrochemical energy materials with atomistic precision. This requires inputs from molecular modeling powered by machine learning (ML) techniques. In this work, we have upgraded our pairwise interaction neural network Python package PiNN via introducing equivariant features to the PiNet2 architecture for fitting potential energy surfaces along with PiNet2-dipole for dipole and charge predictions as well as PiNet2-χ for generating atom-condensed charge response kernels. By benchmarking publicly accessible data sets of small molecules, crystalline materials, and liquid electrolytes, we found that the equivariant PiNet2 shows significant improvements over the original PiNet architecture and provides a state-of-the-art overall performance. Furthermore, leveraging on plug-ins such as PiNNAcLe for an adaptive learn-on-the-fly workflow in generating ML potentials and PiNNwall for modeling heterogeneous electrodes under external bias, we expect PiNN to serve as a versatile and high-performing ML-accelerated platform for molecular modeling of electrochemical systems.