Proceedings of Asia-Pacific International Conference on Perovskite, Organic Photovoltaics and Optoelectronics (IPEROP27)
Publication date: 22nd October 2026
Hybrid organic–inorganic perovskites (HOIPs) exhibit remarkable optoelectronic properties but understanding is limited by complex structure–property coupling between the inorganic BX6 framework and dynamic organic A-site cations. While most studies emphasize the inorganic lattice, A-site cations indirectly tune octahedral tilting, local strain, and defect behavior through hydrogen bonding and steric effects. Quasi-2D HOIPs provide a versatile platform to probe these effects beyond the compositional limits of 3D systems. Here we systematically investigate a series of phase-pure (PA)2APb2I7 thin films with various A-site cations (where PA is n-pentylammonium, and A represents methylammonium (MA), formamidinium (FA), dimethylammonium (DMA), guanidinium (GA), or acetamidinium (AA)) to elucidate A-site control of structure and charge transport. Our findings reveal that incorporating larger A-site cations, which deviate from the ideal tolerance factor, distort the inorganic octahedral network and tune the bandgap. Optical-pump terahertz-probe (OPTP) spectroscopy identifies (PA)2FAPb2I7 as exhibiting the highest charge-carrier mobility among all compositions. These results reveal direct structure-property coupling via A-site cation chemistry and highlight FA-based quasi-2D perovskites as exceptionally promising candidates for high-performance perovskite devices.
