Reducing Anomalous Hysteresis in Perovskite Solar Cells by Suppressing the Interfacial Ferroelectric Order.

Despite the booming research in organometal halide perovskite solar cells (PSCs) of recent years, considerable roadblocks remain for their large-scale deployment, ranging from undesirable current-voltage hysteresis to inferior device stability. Among various plausible origins of hysteresis, interfacial ferroelectricity is particularly intriguing and warrants a close scrutiny. Here, we examine interfacial ferroelectricity in MAPbI3 (FAPbI3)/TiO2 and MAPbI3/phenyl-C61-butyric-acid-methyl-ester (PCBM) heterostructures and explore the correlations between the interfacial ferroelectricity and the hysteresis from the perspective of nonadiabatic electronic dynamics. It is found that the ferroelectric order develops at the MAPbI3/TiO2 interface owing to the interaction between the polar MA ions and TiO2. The polarization switching of the MA ions under an applied gate field would drastically result in different rates in interfacial photoelectron injection and electron-hole recombination, contributing to the undesirable hysteresis. In sharp contrast, ferroelectricity is suppressed at the FAPbI3/TiO2 and MAPbI3/PCBM interfaces, thanks to elimination of the interfacial electric field between perovskite and TiO2 via substitution of strong polar MA (dipole moment: 2.29 debye) by weak polar FA ions (dipole moment: 0.29 debye) and interface passivation, leading to consistent interfacial electronic dynamics and the absence of hysteresis. The present work sheds light on the physical cause for hysteresis and points to the direction to which the hysteresis could be mitigated in PSCs.