Are diffusion models ready for materials discovery in unexplored chemical space?

Abstract

While diffusion models are attracting increasing attention for materials discovery, their ability to generate low-energy structures in unexplored chemical spaces has not been systematically assessed. Here, we evaluate the performance of the diffusion models MatterGen and DiffCSP against three databases: a ternary oxide set (constructed by a genetic algorithm), a ternary nitride set (constructed by template informatics), and the GNoME database (constructed by a combination of both). We find that diffusion models generally perform stably in well-sampled chemical spaces (oxides and nitrides) but are less effective in uncommon ones (GNoME), which contains many compositions involving rare-earth elements and unconventional stoichiometry. Finally, we assess their size-extrapolation capability and observe a significant drop in performance when the number of atoms exceeds the trained range. This is attributed to the limitations imposed by periodic boundary conditions, which we refer to as the curse of periodicity.