Impact of Structural Dimensionality on the Optoelectronic Behavior of Lead–Halide Perovskites

This study investigates how structural dimensionality affects the optoelectronic behavior of organic lead–halide hybrid perovskites. Using the chiral cation R-1-phenylethylammonium (PEA), which is known to be able to form both one-dimensional (1D) and two-dimensional (2D) lead–iodide frameworks, we synthesize 1D (PEA)PbI3 and 2D (PEA)2PbI4 compounds through tailored crystallization and deposition routes. X ray diffraction confirms structural purity, while ultraviolet photoelectron spectroscopy (UPS) provides insight into the electronic structure and photoresponse. Both materials exhibit a surface photo-voltage (SPV) under visible illumination, reaching a maximum work function shift of 1.5 eV for the 2D phase and 0.4 eV for the 1D phase in the thin-film samples. These results suggest that the 1D phase exhibits a reduced tendency for iodide-vacancy formation, which may result in a more stable response under visible illumination, accompanied by faster relaxation dynamics and more anisotropic charge transport. Overall, our findings highlight the central role of electronic confinement in shaping photoinduced processes in hybrid perovskites and support the consideration of structural dimensionality as a key design parameter for the design of next-generation optoelectronic materials.