SimXRD-4M: Big Simulated X-ray Diffraction Data and Crystal Symmetry Classification Benchmark

Powder X-ray diffraction (XRD) patterns are highly effective for crystal identification and play a pivotal role in materials discovery. Although machine learning (ML) has advanced the analysis of powder XRD patterns, progress has been constrained by the limited availability of training data and established benchmarks. To address this, we introduce SimXRD-4M, the largest open-source simulated XRD pattern dataset to date, aimed at accelerating the development of crystallographic informatics. We developed a novel XRD simulation method that incorporates comprehensive physical interactions, resulting in a high-fidelity database. SimXRD comprises 4,065,346 simulated powder XRD patterns, representing 119,569 unique crystal structures under 33 simulated conditions that reflect real-world variations. We benchmark 21 sequence models in both in-library and out-of-library scenarios and analyze the impact of class imbalance in longtailed crystal label distributions. Remarkably, we find that: (1) current neural networks struggle with classifying low-frequency crystals, particularly in out-oflibrary situations; (2) models trained on SimXRD can generalize to real experimental data.