A Symmetry-Oriented Crystal Structure Prediction Method for Crystals with Rigid Bodies

Abstract

We have developed an efficient crystal structure prediction (CSP) method for desired chemical compositions, specifically suited for compounds featuring recurring molecules or rigid bodies. We applied this method to two metal chalcogenides: Li3PS4and Na6Ge2Se6, treating PS4as a tetrahedral rigid body and Ge2Se6as an ethane-like dimer rigid body. Initial trials not only identified the experimentally observed structures of these compounds but also uncovered several novel phases, including a new stannite-type Li3PS4structure and a potential stable structure for Na6Ge2Se6that exhibits significantly lower energy than the observed phase, as evaluated by density functional theory calculations. We compared our results with those obtained using USPEX, a popular CSP package leveraging genetic algorithms. Both methods predicted the same lowest energy structures in both compounds. However, our method demonstrated better performance in predicting metastable structures. the method is implemented with Python code which is available athttps://github.com/ColdSnaap/sgrcsp.git.

Department(s)

Chemistry

Second Department

Physics

Keywords and Phrases

crystal structure prediction; first-principles calculations; metal chalcogenides; simulated annealing

International Standard Serial Number (ISSN)

1361-648X

Document Type

Article - Journal

Document Version

Citation

File Type

text

Language(s)

English

Rights

© 2025 IOP Publishing, All rights reserved.

Publication Date

23 Dec 2024

PubMed ID

39671790

Link to Full Text

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