MatterMind: A User‐Friendly Material Design Platform Assisted by Large Language Model

ABSTRACT Machine learning and AI assistants are reshaping materials research; however, their day‐to‐day application in experimental and computational workflows is still inconsistent, limited by insufficient software documentation and software engineering practices, fragmented software engineering ecosystem and brittle integration between computational tools. Especially in the field of materials informatics, the lack of user‐friendly tool interfaces has restricted the popularization of data‐driven methods in daily scientific research. In this study, we present MatterMind, a user‐friendly agentic interface that closes the loop between first‐principles computation, generative structure design, and large language model (LLM) analysis. The platform unifies (i) plane‐wave first‐principles workflows through Vienna Ab initio Simulation Package (VASP), (ii) crystal generation via diffusion models, and (iii) LLM assistance for error diagnosis, result interpretation, and report drafting. With simple “button‐click” operations or natural‐language prompts, users can: (1) build, launch, and monitor VASP jobs with automated parsing and recovery; (2) sample candidate crystals using modern generative models (MatterGen); and (3) obtain LLM‐guided summaries, comparisons, and next‐step suggestions for screening decisions. We illustrate end‐to‐end case studies that couple crystal generation to DFT relaxation and LLM‐assisted assessment, reducing scripting overhead and improving transparency and reuse from a software engineering perspective. It provides an intelligent scientific tool with comprehensive software documentation, enhancing the efficiency and reliability of scientific exploration in chemical and materials science research.