Coupling Language Models with Physics-based Simulation for Synthesis of Inorganic Materials

Edward W Staley, Tom Arbaugh, Michael Pekala, Alexander New, Christopher D Stiles, Nam Q Le, Gregory Bassen, Wyatt Bunstine, Tyrel McQueen

Keywords: LLM simulation, materials synthesis, LLM for materials, LLM-guided synthesis, inorganic materials

TL;DR: We demonstrate that a reasoning LLM can leverage a materials synthesis simulator to suggest plausible recipes for synthesizing materials in the niobium-oxygen system.

Abstract: Modern generative Machine Learning (ML) models can propose novel inorganic crystalline materials with targeted properties; however, synthesis planning of these materials remains difficult due to the complexity of the associated physical processes and limited availability of computational tools. We introduce a novel hybrid framework to evaluate Large Language Models (LLMs) in inorganic synthesis planning by combining thermodynamic databases with simplified kinetics models to approximate realistic synthesis conditions. As a case study, we focus on the niobium–oxygen system, which features multiple industrially relevant oxide phases with well-characterized data. In computational simulations, we compare LLM-generated synthesis routes with classical path-planning algorithms, showing that the implicit priors in LLMs can yield more viable strategies. In our evaluation setting, classical search methods serve primarily as a foil rather than a direct competitor. This illustrates the relative complexity of the problem and highlights where the LLM’s implicit priors add value.

Submission Track: Paper Track (Short Paper)

Submission Category: AI-Guided Design

Institution Location: Baltimore, United States

Submission Number: 102