Solving Unknown Crystal Structures in a High-Throughput Manner

Databases of density functional theory (DFT) calculations, such as the Open Quantum Materials Database (OQMD), have paved the way for accelerated materials discovery. DFT requires a crystal structure as input; however, due to inherent challenges in solving a compound’s structure from powder diffraction data alone, there are thousands of known compounds whose structures remain unsolved. Although structure solution methods involving DFT-based algorithmic optimization have been demonstrated, their computational cost limits their applicability. We present a more rapid DFT-based structure solution method in which we search the OQMD for structure types that match the cell geometry and stoichiometry of the compound, and evaluate them as possible solutions using DFT and match to diffraction pattern. As this approach is straightforward and inexpensive, we employed it in a high-throughput manner to solve hundreds of previously-undetermined structures from the Powder Diffraction File, including many new elpasolites, transition metal oxides, and mixed anion structures, as well as wide range of scarcely explored structure types.