LLMs as Acquisition Policies for Finite-Pool Materials Optimization: A Controlled Study

Abstract

Discovering materials with desirable properties often requires searching large candidate spaces while experimental or computational evaluations remain costly. Active learning addresses this challenge by using previous observations to select which candidate to evaluate next, typically through probabilistic surrogate models. We investigate whether open-weight large language models (LLMs) can serve as standalone acquisition policies in this setting. We evaluate five LLMs across four retrospective finite-pool materials optimization tasks under different candidate-presentation strategies and compare them with random selection and conventional Gaussian-process methods. LLM policies generally reach the global optimum in fewer iterations than random selection, indicating that they provide a useful acquisition signal without task-specific training. Their performance relative to Gaussian-process methods is mixed: conventional acquisition performs better on most tasks, while LLMs match or outperform it in some settings. Performance varies substantially across tasks, models, initializations, and candidate presentations, with no LLM approach performing best across all tasks. Overall, open-weight LLMs show potential as acquisition policies for finite-pool materials search, although their reliability remains sensitive to the task and to how candidates and scientific context are presented.