A Machine Learned Potential for Investigating Single Crystal to Single Crystal Transformations in Complex Organic Molecular Systems

The packing of organic molecular crystals is often dominated by weak non-covalent interactions, making their in-situ rearrangement under external stimuli challenging to understand. We investigate a pressure-induced single-crystal-to-single- crystal (SCSC) transformation between two polymorphs of 2,4,5-triiodo-1H-imidazole using machine learning potentials. This process involves the rearrangement of halogen and hydrogen bonds combined with proton transfer within a complex solid- state system. We developed a strategy to progressively approach the transition state along the phase transition path from both ends by using both the α and β crystal phases as initial structures for active learning. This method allowed us to develop a DFT-based machine learning potential that faithfully describes both of the stable phases and the transition processes. Our results demonstrate that these anisotropic interactions are represented accurately during molecular dynamic simulations. Bond breaking and reforming during proton transfer is observed and analysed in detail. This approach holds promise for simulating SCSC transitions in organic molecular crystals that involving anisotropic interactions and chemical bond changes.