用流匹配生成无序材料,突破传统模型只限于有序晶体的局限。
DMFlow: Disordered Materials Generation by Flow Matching
- 统一表示有序、替代无序和位置无序晶体,用流匹配联合生成结构
- 提出黎曼流匹配与球面重参数化,确保无序权重在概率单纯形上物理有效
- 适用于材料设计、催化、电池等需要无序结构的领域
材料性能定制对技术进步至关重要,但现有深度生成模型主要聚焦于完美有序晶体,忽略了重要的一类无序材料。为此,本文提出DMFlow,一种专为无序晶体设计的生成框架。该方法统一表示有序、替代无序(SD)和位置无序(PD)晶体,并采用流匹配模型联合生成所有结构组分。关键创新在于引入黎曼流匹配框架与球面重参数化,确保无序权重在概率单纯形上物理合理。向量场由融合物理对称性与专用消息传递机制的新型图神经网络学习。最后通过两阶段离散化过程将连续权重转为多热原子分配。为支持该领域研究,我们发布了基于开源晶格数据库(Crystallography Open Database)构建的基准数据集,包含SD、PD及混合结构。在晶体结构预测(CSP)与从头生成(DNG)任务中,DMFlow显著优于现有基于有序晶体生成的先进基线方法。希望本工作为人工智能驱动的无序材料发现奠定基础。
原文摘要 · Abstract (English)
The design of materials with tailored properties is crucial for technological progress. However, most deep generative models focus exclusively on perfectly ordered crystals, neglecting the important class of disordered materials. To address this gap, we introduce DMFlow, a generative framework specifically designed for disordered crystals. Our approach introduces a unified representation for ordered, Substitutionally Disordered (SD), and Positionally Disordered (PD) crystals, and employs a flow matching model to jointly generate all structural components. A key innovation is a Riemannian flow matching framework with spherical reparameterization, which ensures physically valid disorder weights on the probability simplex. The vector field is learned by a novel Graph Neural Network (GNN) that incorporates physical symmetries and a specialized message-passing scheme. Finally, a two-stage discretization procedure converts the continuous weights into multi-hot atomic assignments. To support research in this area, we release a benchmark containing SD, PD, and mixed structures curated from the Crystallography Open Database. Experiments on Crystal Structure Prediction (CSP) and De Novo Generation (DNG) tasks demonstrate that DMFlow significantly outperforms state-of-the-art baselines adapted from ordered crystal generation. We hope our work provides a foundation for the AI-driven discovery of disordered materials.
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