Correlation between Interfacial Structures and Device Performance: The Double-Edged Sword Effect of Lead Iodide in Perovskite Solar Cells

The interfacial electronic structure of perovskite layers and transport layers is critical for the performance and stability of perovskite solar cells (PSCs). The device performance of PSCs can generally be improved by adding a slight excess of lead iodide (PbI2) to the precursor solution. However, its underlying working mechanism is controversial. Here, we performed a comprehensive study of the electronic structures at the interface between CH3NH3PbI3 and C-60 with and without the modification of PbI2 using in situ photoemission spectroscopy measurements. The correlation between the interfacial structures and the device performance was explored based on performance and stability tests. We found that there is an interfacial dipole reversal, and the downward band bending is larger at the CH3NH3PbI3/C-60 interface with the modification of PbI2 as compared to that without PbI2. Therefore, PSCs with PbI2 modification exhibit faster charge carrier transport and slower carrier recombination. Nevertheless, the modification of PbI2 undermines the device stability due to aggravated iodide migration. Our findings provide a fundamental understanding of the CH3NH3PbI3/C-60 interfacial structure from the perspective of the atomic layer and insight into the double-edged sword effect of PbI2 as an additive.

Automated summary

In this study, the electronic structures at the interface between CH3NH3PbI3 and C-60 with and without the modification of PbI2 were comprehensively studied using in situ photoemission spectroscopy measurements. The results showed that the addition of PbI2 improves charge carrier transport and slows down carrier recombination in perovskite solar cells (PSCs). However, PbI2 modification undermines device stability due to aggravated iodide migration.