Predicting Lattice Vibrational Frequencies Using Deep Graph Neural Networks.

Abstract

Lattice vibrational frequencies are related to many important materials properties such as thermal and electrical conductivity as well as superconductivity. However, computational calculation of vibrational frequencies using density functional theory methods is computationally too demanding for large number of samples in materials screening. Here we propose a deep graph neural network based algorithm for predicting crystal vibrational frequencies from crystal structures. Our algorithm addresses the variable dimension of vibrational frequency spectrum using the zero padding scheme. Benchmark studies on two data sets with 15,000 mixed-structure and 35,552 rhombohedra samples show that the aggregated R2 scores of the prediction reach 0.554 and 0.724. We also evaluate the structural transferability by predicting the vibration frequencies for 239 individual cubic target structures. The R2 scores for more than 40% of the targets are greater than 0.8 and can reach as high as 0.98 for the model trained with mixed samples, while the average mean absolute error is 43.69 Thz showing low transferability across structure types. Our work demonstrates the capability of deep graph neural networks to learn to predict lattice vibration frequency when sufficient number of training samples are available.