Abstract Low-dimensional bismuth-based perovskite solar cells (PSCs) have demonstrated some benefits over lead-based PSCs for nontoxicity and remarkable stability. These two factors are now the primary concerns in the photovoltaic community. The power conversion efficiency (PCE) of PSCs using the lead Pb-free chemical methylammonium bismuth iodide (CH3NH3)3Bi2I9 is severely limited due to the poor quality of the photoactive material. Herein, the photovoltaic performance of the (CH3NH3)3Bi2I9 PSCs was investigated. The objective of this study was to investigate the intrinsic impacts of (CH3NH3)3Bi2I9 perovskite by using SCAPS-1D (Solar Cell Capacitance Simulator) to simulate the PSCs and the adjustment of relevant physical parameters to closely match experimental results. Moreover, the cells were optimized based on (CH3NH3)3Bi2I9 film thickness, total defect density of (CH3NH3)3Bi2I9, optical bandgap, and interfacial defects. By conducting a comprehensive analysis of the current-voltage (J-V) plots and quantum efficiency feature, the best values of perovskite thickness, bandgap, and defect density were determined to be 100 nm, 1.6 eV, and 1014 cm-3, respectively. Furthermore, defects in the interfaces between the electron-transporting layer (ETL)/(CH3NH3)3Bi2I9 and hole transport layer (HTL)/(CH3NH3)3Bi2I9 were considered, and their influence on performance was also investigated. Accordingly, the optimized cell has realized a record PCE of 9.043% and a high quantum efficiency exceeding 60%, which is comparable to those of some Pb-free perovskite analogues. The operational temperature calucations showed that all parameters remain relatively constant with increasing temperature. Therefore, the results imply that the simulated Pb-free PSCs can be stable in a thermal environment. The proposed structural layout and optimization approach can encourage more study and actual applications for Pb-free organometallic perovskite solar cells.
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