Identifying Crystal Structures Beyond Known Prototypes from X-ray Powder Diffraction Spectra

Abstract: The large amount of powder diffraction data for which the corresponding crystal structures have not yet been identified suggests the existence of numerous undiscovered, physically relevant crystal structure prototypes. In this paper, we present a scheme to resolve powder diffraction data into crystal structures with precise atomic coordinates by screening the space of all possible atomic arrangements, i.e., structural prototypes, including those not previously observed, using a pre-trained ML model. This involves (i) enumerating all possible symmetry-confined ways in which a given composition can be accommodated in a given spacegroup, (ii) ranking the element-assigned prototype representations using energies predicted using the Wren ML model [Sci.Adv.8, eabn4117 (2022)], (iii) assigning and perturbing atoms along the degree of freedom allowed by the Wyckoff positions to match the experimental diffraction data (iv) validating the thermodynamic stability of the material using density-functional theory (DFT). An advantage of the presented method is that it does not rely on a database of previously observed prototypes and is, therefore capable of finding crystal structures with entirely new symmetric arrangements of atoms. We demonstrate the workflow on unidentified XRD spectra from the ICDD database and identify a number of stable structures, where a majority turns out to be derivable from known prototypes. However, at least two are found not to be part of our prior structural data sets.