2D hybrid perovskite materials are attractive from the perspective of providing a much larger design space of organic ligand chemistries in comparison with bulk 3D materials. Likewise, many recent reports have highlighted how tuning the ligand chemistry can impact the electronic properties and stability profiles of the resulting 2D materials. In this talk, we’ll describe how we have implemented a high-throughput molecular simulation framework to screen prospective ligand chemistries for synthesizability and stabilization of the perovskite lattice. ML models have been also incorporated to accelerate the prediction. Using this framework, we have been able to characterize thousands of perovskite materials and establish some novel design rules for ligand chemistries. Several novel aspects of the methodology will also be highlighted, including extending our screening approach to elucidate differences in design rules with transitioning from 2D to Quasi-2D perovskite.
Our framework is versatile, extending beyond ligand design to various related applications. As a case study, we examine a novel class of bidentate (BD) phase ligands for n=1 perovskites—ligands that are structurally distinct from conventional 2D Ruddlesden–Popper (RP) phase ligands. Using molecular dynamics simulations with enhanced sampling techniques, we evaluated ligand dissociation free energies to assess the thermal stability of BD-phase ligands compared to existing options. Furthermore, our simulations predicted the crystal structures of three new bidentate ligands and confirmed the stability of the corresponding BD-phase n=1 perovskites. Experimental tests on polycrystalline thin films further demonstrated that BD-phase perovskites exhibit superior thermal resistance, outperforming both RP and Dion–Jacobson (DJ) phase devices.
