Novel inorganic crystal structures predicted using autonomous simulation agents

We report a dataset of 96,962 new crystal structures discovered and computed using our previously published autonomous, density functional theory (DFT) based, active-learning workflow named CAMD (Computational Autonomy for Materials Discovery). Of these, 931 are within 1 meV/atom of the convex hull and 27,075 are within 200 meV/atom of the convex hull. The dataset contains DFT-optimized pymatgen crystal structure objects, DFT-computed formation energies and phase stability calculations from the convex hull. It contains a variety of spacegroups and symmetries derived from crystal prototypes derived from known experimental compounds, and was generated from active learning campaigns of various chemical systems. This dataset can be used to benchmark future active-learning or generative efforts for structure prediction, to seed new efforts of experimental crystal structure discovery, or to construct new models of structure-property relationships.