Finetuning-Free Diffusion Model with Adaptive Constraint Guidance for Inorganic Crystal Structure Generation

Abstract

The discovery of inorganic crystal structures with targeted properties is a significant challenge in materials science. Generative models, especially state-of-the-art diffusion models, offer the promise of modeling complex data distributions and proposing novel, realistic samples. However, current generative AI models still struggle to produce diverse, original, and reliable structures of experimentally achievable materials suitable for high-stakes applications. In this work, we propose a generative machine learning framework based on diffusion models with adaptive constraint guidance, which enables the incorporation of user-defined physical and chemical constraints during the generation process. This approach is designed to be practical and interpretable for human experts, allowing transparent decision-making and expert-driven exploration. To ensure the robustness and validity of the generated candidates, we introduce a multi-step validation pipeline that combines graph neural network estimators trained to achieve DFT-level accuracy and convex hull analysis for assessing thermodynamic stability. Our approach has been tested and validated on several classical examples of inorganic families of compounds, as case studies. As a consequence, these preliminary results demonstrate our framework's ability to generate thermodynamically plausible crystal structures that satisfy targeted geometric constraints across diverse inorganic chemical systems.