Numerical Simulation of Lead-Free Absorbers in 2D Dion-Jacobson Phase Perovskite Solar Cells Using SCAPS-1D: Towards 41% Efficiency

Abstract: With the rapid advancement of photovoltaic science, there has been an increasing focus on the development of environment-friendly and structurally advanced perovskite solar cells (PSCs). In this context, this study investigates an architectural configuration employing 2D Dion-Jacobson phase perovskites as both electron and hole transport layers within a 2D/absorber/2D structure. The primary objective is to identify optimal absorber materials and enhance the overall efficiency of the device. While the reduction of lead content remains a significant challenge in PSC development, the present work focuses on the evaluation of seven lead-free absorber materials: MASnBr3, Sr3PI3/Sr3SbI3, p-CuBi2O4, p-Si, CH3NH3SnI3, Sb2Se3, and CZTSSe. These materials were assessed in the context of an FTO/PeDAMA8Pb6I19/IDL1/absorber/IDL2/PeDAMA2Pb3I10/C architecture utilizing SCAPS-1D simulation software. The study includes a comprehensive analysis of band alignment, pre-optimization screening, and performance optimization through the adjustment of absorber thickness, doping levels, and defect densities. Additionally, the temperature sensitivity and the substitution of the FTO layer with ITO, IZO, and MZO were also investigated. The simulation results indicated that Sb2Se3 and CZTSSe achieved the highest efficiencies of 41.00% and 41.19%, respectively. Furthermore, MZO was identified as a strong candidate for replacing FTO, maintaining consistent performance across all absorber types analyzed. Overall, this study provides a comparative framework for the material selection within layered PSC architectures and significantly contributes to the advancement of stable, efficient, and lead-free photovoltaic technologies.