Principal component analysis enables the design of deep learning potential precisely capturing LLZO phase transitions

Abstract The development of accurate and efficient interatomic potentials using machine learning has emerged as an important approach in materials simulations and discovery. However, the systematic construction of diverse, converged training sets remains challenging. We develop a deep learning-based interatomic potential for the Li7La3Zr2O12 (LLZO) system. Our interatomic potential is trained using a diverse dataset obtained from databases and first-principles simulations. We propose using the coverage of the training and test sets as the convergence criteria for the training iterations, where the coverage is calculated by principal component analysis. This results in an accurate LLZO interatomic potential that can describe the structure and dynamical properties of LLZO systems meanwhile greatly reducing computational costs compared to density functional theory calculations. The interatomic potential accurately describes radial distribution functions and thermal expansion coefficient consistent with experiments. It also predicts the tetragonal-to-cubic phase transition behaviors of LLZO systems. Our work provides an efficient training strategy to develop accurate deep-learning interatomic potential for complex solid-state electrolyte materials, providing a promising simulation tool to accelerate solid-state battery design and applications.