TCSP3.0: Template-Based Crystal Structure Prediction with Coefficient-Preserving Element Substitution and Structural Diversity

Ying Feng, Jeffrey Hu, Lai Wei, Liang Tao, Madeline Miklos +3

Template-based crystal structure prediction (CSP) transfers a known crystal structure to a new composition by element substitution, so its accuracy depends on retrieving suitable templates, mapping elements and ranking the resulting candidates correctly. Auditing the original TCSP2.0 implementation on the T180 benchmark, we found that 469 of its 2,347 selected structures (20%) have the wrong composition, caused by element mappings that ignore stoichiometric coefficients and by sequential text substitution that cascades or corrupts element symbols. We propose TCSP3.0, which enforces coefficient-preserving mappings, substitutes species simultaneously on parsed structures and validates every candidate's composition and cell. It further adds periodic-number retrieval, soft oxidation-state evidence, radius-compatibility scoring, structural deduplication, and ORB-v3 machine-learning-potential relaxation and energy ranking of its candidates, as used by deep generative CSP baselines. TCSP3.0 achieves Top-1 and Top-20 match rates of 72.2% and 90.6% on T180, compared with 28.3% and 45.6% for TCSP2.0, and a Top-20 match rate of 74.0% on a new 800-target benchmark (T800). On T180 it also…