Scalable machine learning framework for multiphase identification from powder X-ray diffraction

Abstract

X-ray diffraction (XRD) is the primary tool for identifying crystalline phases following synthesis, but automated phase identification remains challenging, particularly for multiphase samples with overlapping peaks and experimental artifacts. While deep-learning methods have been proposed to improve upon classical search-match algorithms, most formulate phase identification as a single closed-set classification problem, requiring one shared model to discriminate among all candidate phases. Here we introduce GALAXI, which instead decouples the identification task into independent one-versus-all binary classifiers that each specialize in recognizing a single phase. These pre-trained classifiers first narrow the search space to a small set of plausible phases, which are then evaluated through Rietveld refinement to identify the combination of phases that best explains the full diffraction pattern. On a curated set of experimental patterns, GALAXI identifies the correct phases with a micro-F1 score of 0.935, outperforming classical search-match and prior deep-learning models. The method remains robust to common experimental artifacts, including low impurity phase fractions, small crystallite size, peak shifts, sample displacement, and texture, and performs well when applied to time-resolved in-situ XRD data from solid-state reactions. Moreover, because the phase-specific models are independent, GALAXI can expand to large reference libraries without retraining existing models. This modular architecture enables us to train classifiers for 64,594 structures from the Crystallography Open Database and deploy them through a public web interface at https://galaxi-xrd.com.