Polymorphism Crystal Structure Prediction with Adaptive Space Group Diversity Control
This work addresses a critical bottleneck in materials science by enabling more efficient discovery of polymorphs with desired properties, though it is incremental as it builds on existing genetic algorithm methods.
The paper tackles the problem of predicting polymorph crystal structures for inorganic materials, proposing ParetoCSP2, a multi-objective genetic algorithm with adaptive space group diversity control, which achieves up to 8.62 times higher accuracy in space group and structural similarity compared to baselines and improves key performance metrics by 44.8% to 87.04%.
Crystalline materials can form different structural arrangements (i.e. polymorphs) with the same chemical composition, exhibiting distinct physical properties depending on how they were synthesized or the conditions under which they operate. For example, carbon can exist as graphite (soft, conductive) or diamond (hard, insulating). Computational methods that can predict these polymorphs are vital in materials science, which help understand stability relationships, guide synthesis efforts, and discover new materials with desired properties without extensive trial-and-error experimentation. However, effective crystal structure prediction (CSP) algorithms for inorganic polymorph structures remain limited. We propose ParetoCSP2, a multi-objective genetic algorithm for polymorphism CSP that incorporates an adaptive space group diversity control technique, preventing over-representation of any single space group in the population guided by a neural network interatomic potential. Using an improved population initialization method and performing iterative structure relaxation, ParetoCSP2 not only alleviates premature convergence but also achieves improved convergence speed. Our results show that ParetoCSP2 achieves excellent performance in polymorphism prediction, including a nearly perfect space group and structural similarity accuracy for formulas with two polymorphs but with the same number of unit cell atoms. Evaluated on a benchmark dataset, it outperforms baseline algorithms by factors of 2.46-8.62 for these accuracies and improves by 44.8\%-87.04\% across key performance metrics for regular CSP. Our source code is freely available at https://github.com/usccolumbia/ParetoCSP2.