Solving Inorganic Crystal Structures from X-ray Powder Diffraction Using a Generative First-Principles Framework

X-ray powder diffraction (XRD) is a powerful structure characterization technique, but solving unknown inorganic crystal structures from powder diffraction patterns can often be labor-intensive or speculative. We introduce an Automated XRD to Structure (AXS) solution method based on the crystal symmetry obtained from XRD patterns, an efficient search of candidate structures spanning the available degrees of freedom, and density functional theory (DFT). This methodology is completely agnostic to structural prototypes and robust in solving inorganic structures of various chemistries, crystal systems, and unit cell sizes; 92% of all crystal structures were accurately determined from the simulated XRD patterns in our benchmark set. In addition, we demonstrate the efficacy of this methodology on experimental XRD patterns by solving the crystal structures of Li8HfO6, Li3CrO4, and LiFeO2.