Insight into the pressure-engineered structure-property relationship of organic-inorganic hybrid perovskites through high-throughput first-principles calculations

Searching for novel organic-inorganic hybrid perovskite materials with long-term stability and excellent optoelectronic properties is the focus of optoelectronic field. High-pressure as a special thermodynamic parameter, offers a promising avenue for discovering and designing materials with optimized performance. However, the data-driven pressure-engineered structure-property relationships remains scarce, leading to an insufficiently understanding of the physical rules by which pressure regulation influences the microstructure and electronic properties of materials. In this study, we conduct high-throughput first-principles calculation to construct a database of hundreds of cubic ABX3 candidates and evaluate their property evolutions under pressures ranging from 0 to 10 GPa. Through systematic assessments of the crystallographic stability, thermodynamic stability, and electronic properties, we obtain the following findings: the B-site metal predominantly determines crystal structure stability; the X-site halogen governs thermodynamic stability; and the ionic radius of A-site organic cation plays a pivotal role in modulating the electronic properties. Based on extensive theoretical calculations, this study confirms the influence of “single-component” effect, further enriching the existing knowledge that the synergistic changes in bond length or bond angle between B-site and X-site under pressure are the main factors affecting material properties. The insights derived from current analysis provide a valuable foundation for rational design of the optimized OIHP materials under pressure.