The interface and its role in carrier transfer/recombination dynamics for the planar perovskite solar cells prepared under fully open air conditions

Abstract

The planar heterojunction perovskite solar cells, where the perovskite film is deposited directly onto a flat hole blocking layer, have recently attracted a great deal of attention owing to their high performance and ease of processing. However, the interface and its underlying role in carrier transport/recombination kinetics for such perovskite devices prepared under ambient air is still obscure. Herein, we addressed this issue by a dynamic intensity modulated photovoltage spectroscopy (IMVS) model using a continuity equation. The interface and its role in charge-carrier transport/recombination kinetics have been explored and discussed as an approach to understand the origin of the photovoltaic properties for the devices prepared under ambient air. The experimental IMVS responses were measured and satisfactorily fitted to the analytical results. Compared to the typical IMVS model based on dye-sensitized solar cells (DSSCs), the better IMVS fitting results presented in this study indicated that there was a discrepancy between the planar perovskite devices and those of DSSCs in electron transport/recombination properties, because carrier transfer across the TiO2/liquid electrolyte interface in DSSCs has been modified. That is, the Schottky interface in DSSCs needs to be replaced by the semiconductor heterojunction interface in perovskite solar cells (PSCs). Besides, the interface exhibits a more significant role in determining the carrier transport/recombination process by influencing the boundary conditions in a continuity equation. Furthermore, the intensity modulated photocurrent/photovoltage spectroscopy responses demonstrated that the carrier recombination characteristic is ultimately related with the surface and defect density in the interface. Interfacial modification, such as air-annealing, resulting in crystallographic changes, oxygen passivation, and variation in grain domain size, could suppress carrier recombination and prolong charge lifetime, which can yield more photo-generated electrons to be collected by anode, subsequently resulting in strikingly improving photovoltaic performance of the devices. In short, the dynamic IMVS model would help in elucidating the role of interface and the importance of interfacial modification or even interface design in order to obtain a highly efficient solar cell. The study can not only pave the way to construct the current−voltage curve using a continuity equation model, but also provide new insights into the performance-improving steps for the PSCs prepared under fully open air conditions, which is of great importance for their future commercialization.