SimMOF: AI agent for Automated MOF Simulations

Inverse design of metal-organic frameworks (MOFs) requires searching a combinatorially vast space where property labels are expensive and most machine-learning models reveal little about why a structure succeeds. We introduce LLM4MOF, a closed-loop framework in which language-model agents reason about chemistry, build candidate MOFs, and test them in simulation, refining hypotheses over ten autonomous iterations. One agent proposes interpretable design hypotheses over metal nodes, linkers, pore geometry, and functional chemistry, and a second translates them into constraints that select candidate MOFs, each made of a metal node, organic linker, and matching topology. Each hypothesis is tested through four diagnostic beams that apply different subsets of its constraints, so comparing them shows whether geometry, chemistry, or metal choice drives performance. Even when blind to the global property landscape of databases, LLM4MOF concentrates its search on top-performing structures across six adsorption, separation, and electronic-structure tasks within 400 property evaluations. The same loop also generates new MOFs de novo and validates them in live simulation, where it adapts the geometry to each requested condition, outperforming random search and a genetic algorithm at roughly $1 per campaign. LLM4MOF shows that language-model agents can run interpretable, simulation-grounded inverse design without training a model per objective.

The coordination of multi-scale tasks is an effective strategy for computational materials discovery, yet the repeated application of diverse algorithms and tools renders it challenging. We report MAESTRO, a large language model (LLM) agent system capable of executing the entire screening pipeline for metal-organic frameworks (MOFs). It processes a large body of MOF literature, links relevant publications to their crystal structures, and curates the results into a computation-ready database, which is then screened through a strategy of progressively increasing computational cost. The promising candidates identified for separation under wet flue gas conditions all originate from unrelated studies. By connecting the heterogeneous stages of computational materials discovery, the LLM-based agents of MAESTRO can operate across application domains and uncover high-performance materials that conventional screening approaches would be unlikely to consider.

Large language models are increasingly used as reasoning components in AI-driven materials Co-Scientists, yet the reliability of the resulting verification pipeline remains unclear. Metal-organic frameworks (MOFs) provide a particularly challenging setting because structures may appear under different identifiers, synthesis outcomes depend strongly on experimental conditions, evidence is distributed across heterogeneous sources, and some hypotheses require computation rather than literature alone. We introduce a diagnostic benchmark with four task families covering structural grounding, synthesis-condition verification, evidence-sufficiency verification, and MLIP-based computational verification. T-MOF-1-3 are evaluated under closed-book, retrieval-enabled, and oracle-evidence settings to localize failures in knowledge access, evidence acquisition, and reasoning, while T-MOF-4 separately evaluates computational verification. Guided by these diagnosed failure modes, we develop MOF-Verify, a failure-aware agentic harness that targets structural, literature, evidence-sufficiency, and computational bottlenecks before producing a final verdict. Across multiple backbone LLMs, MOF-Verify substantially improves hypothesis-verification performance over direct inference and retrieval-based baselines. Benchmark datasets are released at https://github.com/IMMS-Ewha/MOF-Verify-Benchmark.