Crystal structure generation with autoregressive large language modeling

Abstract

Abstract The generation of plausible crystal structures is often the first step in predicting the structure and properties of a material from its chemical composition. However, most current methods for crystal structure prediction are computationally expensive, slowing the pace of innovation. Seeding structure prediction algorithms with quality generated candidates can overcome a major bottleneck. Here, we introduce CrystaLLM, a methodology for the versatile generation of crystal structures, based on the autoregressive large language modeling (LLM) of the Crystallographic Information File (CIF) format. Trained on millions of CIF files, CrystaLLM focuses on modeling crystal structures through text. CrystaLLM can produce plausible crystal structures for a wide range of inorganic compounds unseen in training, as demonstrated by ab initio simulations. Our approach challenges conventional representations of crystals, and demonstrates the potential of LLMs for learning effective models of crystal chemistry, which will lead to accelerated discovery and innovation in materials science.