Persistent Ion Accumulation at Interfaces Improves the Performance of Perovskite Solar Cells

The mixed ionic-electronic nature of lead halide perovskites makes their performance in solar cells complex in nature. Ion migration is often associated with negative impacts-such as hysteresis or device degradation-leading to significant efforts to suppress ionic movement in perovskite solar cells. In this work, we demonstrate that ion trapping at the perovskite/electron transport layer interface induces band bending, thus increasing the built-in potential and open-circuit voltage of the device. Quantum chemical calculations reveal that iodine interstitials are stabilized at that interface, effectively trapping them at a remarkably high density of ∼10²¹ cm^-3 which causes the band bending. Despite the presence of this high density of ionic defects, the electronic structure calculations show no sub-band-gap states (electronic traps) are formed due to a pronounced perovskite lattice reorganization. Our work demonstrates that ionic traps can have a positive impact on device performance of perovskite solar cells.