General-purpose LLMs as constrained crystal composition generators

Abstract

Abstract The targeted discovery of inorganic materials remains challenging due to the vastness of compositional design spaces and the high cost of exhaustive screening. Task-specific generative artificial intelligence represents a particularly efficient alternative to screening, yet demands tedious collection of training data before providing real benefit. General-purpose large language models (LLMs) have recently shown tremendous potential for the targeted generation of single, optimal materials compositions without the need for task-specific fine-tuning. However, it is unclear whether LLMs generally pose an advantage compared to specialized generative models, in particular in large design spaces. Here, we demonstrate that such models are capable of covering entire regions of the targeted property space effectively and systematically. Using Elpasolite materials as an established benchmark for generative tasks in large chemical spaces, we find that an iterative prompt-and-response framework is able to recover on average 96% of all low-energy Elpasolites in the target region. This performance, driven mainly by iterative in-context learning, surpasses the generative abilities of previous, task-specific models. Our results establish general-purpose LLMs as flexible and accessible components for inverse materials design workflows.