ECD: A Machine Learning Benchmark for Predicting Enhanced-Precision Electronic Charge Density in Crystalline Inorganic Materials

摘要

Supervised machine learning techniques are increasingly being adopted to speed up electronic structure predictions, serving as alternatives to first-principles methods like Density Functional Theory (DFT). Although current DFT datasets mainly emphasize chemical properties and atomic forces, the precise prediction of electronic charge density is essential for accurately determining a system's total energy and ground state properties. In this study, we introduce a novel electronic charge density dataset named ECD, which encompasses 140,646 stable crystal geometries with medium-precision Perdew–Burke–Ernzerhof (PBE) functional data. Within this dataset, a subset of 7,147 geometries includes high-precision electronic charge density data calculated using the Heyd–Scuseria–Ernzerhof (HSE) functional in DFT. By designing various benchmark tasks for crystalline materials and emphasizing training with large-scale PBE data while fine-tuning with a smaller subset of high-precision HSE data, we demonstrate the efficacy of current machine learning models in predicting electronic charge densities.The ECD dataset and baseline models are open-sourced to support community efforts in developing new methodologies and accelerating materials design and applications.