Closed‐Loop Solid‐State Synthesis Planning for Materials Discovery With Large Language Models

Developing reliable synthesis routes for complex materials remains a major bottleneck in accelerating materials discovery. This study establishes a large language model-based framework for predicting and optimizing synthesis conditions directly from the literature data. Key synthesis information, including target compounds, precursors, and processing parameters, was systematically extracted from 4407 open-access solid-state synthesis papers and organized into a structured recipe dataset. Using a retrieval-augmented generation (RAG) approach, the system first retrieves similar recipes from the corpus and then generates a new candidate recipe conditioned on those exemplars. The generated recipes were benchmarked against literature data using quantitative scoring metrics, achieving strong agreement with experimentally reported conditions. To validate the predictive capability, the framework was applied to unreported solid-state electrolyte candidates identified through first-principles screening, and multiple oxy-selenide compounds were successfully synthesized through iterative feedback between the model and experiment. The recipe generator accurately refined synthesis parameters over successive trials, demonstrating its ability to reproduce phase-pure products while minimizing trial-and-error. This approach establishes a data-driven, feedback-optimized route to accelerate synthesis design, offering a generalizable paradigm for integrating language models into experimental materials research.