Efficient determination of Born-effective charges, LO-TO splitting, and Raman tensors of solids with a real-space atom-centered deep learning approach.

We introduce a deep neural network (DNN) framework called the Real-space Atomic Decomposition NETwork (RADNET), which is capable of making accurate predictions of polarization and of electronic dielectric permittivity tensors in solids. This framework builds on previous, atom-centered approaches while utilizing deep convolutional neural networks. We report excellent accuracies on direct predictions for two prototypical examples: GaAs and BN. We then use automatic differentiation to calculate the Born-effective charges, longitudinal optical-transverse optical (LO-TO) splitting frequencies, and Raman tensors of these materials. We compute the Raman spectra, and find agreement with ab initio results. Lastly, we explore ways to generalize polarization predictions while taking into account periodic boundary conditions and symmetries.