Full Optoelectronic Simulation of Lead-Free Perovskite/Organic Tandem Solar Cells

Organic and perovskite semiconductor materials are considered an interesting combination thanks to their similar processing technologies and band gap tunability. Here, we present the design and analysis of perovskite/organic tandem solar cells (TSCs) by using a full optoelectronic simulator (SETFOS). A wide band gap lead-free ASnI₂Br perovskite top subcell is utilized in conjunction with a narrow band gap DPPEZnP-TBO:PC61BM heterojunction organic bottom subcell to form the tandem configuration. The top and bottom cells were designed according to previous experimental work keeping the same materials and physical parameters. The calibration of the two cells regarding simulation and experimental data shows very good agreement, implying the validation of the simulation process. Accordingly, the two cells are combined to develop a 2T tandem cell. Further, upon optimizing the thickness of the front and rear subcells, a current matching condition is satisfied for which the proposed perovskite/organic TSC achieves an efficiency of 13.32%, J of 13.74 mA/cm², and V of 1.486 V. On the other hand, when optimizing the tandem by utilizing full optoelectronic simulation, the tandem shows a higher efficiency of about 14%, although it achieves a decreased J of 12.27 mA/cm². The study shows that the efficiency can be further improved when concurrently optimizing the various tandem layers by global optimization routines. Furthermore, the impact of defects is demonstrated to highlight other possible routes to improve efficiency. The current simulation study can provide a physical understanding and potential directions for further efficiency improvement for lead-free perovskite/organic TSC.