Accurate Crystal Structure Prediction of New 2D Hybrid Organic Inorganic Perovskites (2403.06955v1)

Abstract: Low dimensional hybrid organic-inorganic perovskites (HOIPs) represent a promising class of electronically active materials for both light absorption and emission. The design space of HOIPs is extremely large, since a diverse space of organic cations can be combined with different inorganic frameworks. This immense design space allows for tunable electronic and mechanical properties, but also necessitates the development of new tools for in silico high throughput analysis of candidate structures. In this work, we present an accurate, efficient, transferable and widely applicable machine learning interatomic potential (MLIP) for predicting the structure of new 2D HOIPs. Using the MACE architecture, an MLIP is trained on 86 diverse experimentally reported HOIP structures. The model is tested on 73 unseen perovskite compositions, and achieves chemical accuracy with respect to the reference electronic structure method. Our model is then combined with a simple random structure search algorithm to predict the structure of hypothetical HOIPs given only the proposed composition. Success is demonstrated by correctly and reliably recovering the crystal structure of a set of experimentally known 2D perovskites. Such a random structure search is impossible with ab initio methods due to the associated computational cost, but is relatively inexpensive with the MACE potential. Finally, the procedure is used to predict the structure formed by a new organic cation with no previously known corresponding perovskite. Laboratory synthesis of the new hybrid perovskite confirms the accuracy of our prediction. This capability, applied at scale, enables efficient screening of thousands of combinations of organic cations and inorganic layers.