arXiv:2608.06448cs.LGcs.AI2026-08

用电子衍射数据直接生成晶体结构,突破传统检索限制。

ED-CSP: Crystal Structure Prediction from Electron Diffraction

论文配图:ED-CSP: Crystal Structure Prediction from Electron Diffraction
图 1 · 摘自论文原文
  • 结合关系编码与多视角聚合,从衍射点预测晶格参数和原子坐标。
  • 在2075个材料上达到57.49%的结构匹配率,优于同类模型。
  • 可生成训练库外的新结构,适合材料发现与实验数据迁移研究。

从稀疏、未索引的电子衍射(ED)观测中恢复周期性三维晶体结构,是一项具有挑战性的生成式逆问题。现有基于ED的学习方法主要预测晶格标签、从索引反射重构结构或从有限结构库中检索候选。本文提出ED-CSP,一种基于化学组成、原子数及多个探测器平面衍射点集的机器学习框架,联合预测晶格参数与分数原子坐标。模型融合关系集编码器、排列不变的多视图聚合与周期性流生成器。为训练模型,构建了包含485万组模拟多视角ED晶体结构的ED-CS数据集,去重自七个材料库,并过滤掉与CHILI-100K的重叠。在2,075个预留的CHILI-100K材料上,仅用CHILI训练的ED-CSP达到57.49%的MR@5,优于当前最优的粉末X射线衍射模型PXRDGen(52.92%)。扩大训练数据后,初始化于一百万结构预训练模型使MR@5提升至66.27%。对训练库中无对应组成的1,024种组合,仍实现53.52%的MR@5,证明其真正生成能力。将目标衍射替换为同组成但非同构结构的衍射时,MR@5下降22.09个百分点,证实预测依赖输入衍射模式而非仅组成。ED-CSP与ED-CS为稀疏ED观测下的生成式晶体结构预测建立基准,并为未来向实验数据迁移奠定基础。

原文摘要 · Abstract (English)

Recovering a periodic 3D crystal structure from sparse, unindexed electron diffraction (ED) observations is a challenging generative inverse problem. Existing ED-based learning methods mainly predict crystallographic labels, reconstruct structures from indexed reflections, or retrieve candidates from finite structure libraries. Here, we introduce ED-CSP, a machine learning framework that predicts crystal structures from chemical composition, atom count, and multiple detector-plane ED spot sets. ED-CSP combines a relational set encoder, permutation-invariant multi-view aggregation, and a periodic flow generator to jointly predict lattice parameters and fractional atomic coordinates. To train the model, we construct ED-CS, a dataset of 4.85 million simulated multi-view ED crystal structures, deduplicated across seven materials repositories and filtered to exclude CHILI-100K overlaps. On 2,075 held-out CHILI-100K materials, ED-CSP trained only on CHILI achieves a structural match rate of 57.49% MR@5, outperforming PXRDGen (52.92%), a state-of-the-art crystal structure prediction model conditioned on powder X-ray diffraction. Scaling training data further improves performance: initializing from a one-million-structure precursor raises MR@5 to 66.27%. On 1,024 compositions absent from the training retrieval library, the model still achieves 53.52% MR@5, demonstrating true generative capability beyond exact-formula retrieval. Replacing target ED observations with diffraction from non-isomorphic structures of identical composition decreases MR@5 by 22.09 percentage points, confirming that predictions depend on the input diffraction patterns rather than composition alone. ED-CSP and ED-CS establish a benchmark for generative crystal structure prediction from sparse ED observations and provide a foundation for future transfer to experimental data.

晶体结构预测电子衍射生成模型材料发现

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