Insight into Diphenyl Phosphine Oxygen-Based Molecular Additives as Defect Passivators toward Efficient Quasi-2D Perovskite Light-Emitting Diodes.

The introduction of additives has become an important method for enhancing the device performance of quasi-two-dimensional perovskite light-emitting diodes. In this work, we systematically studied the electronic and spatial effects of molecular additives on defect passivation abilities using the methyl, hydrogen, and hydroxyl groups substituted three diphenyl phosphine oxygen additives. The electron-donating conjugation effect of the hydroxyl group on diphenylphosphinic acid (OH-DPPO) leads to a more electron-rich region in OH-DPPO, and the hydroxyl group has a moderate steric hindrance. All these factors endow it with best passivation ability than the other two additives. Furthermore, ion migration was suppressed due to hydrogen bonding between the hydroxyl group and Br. Ultimately, the OH-DPPO passivated devices achieved an external quantum efficiency of 22.44% and a 6-fold improvement in lifetime. These findings provide guidance for developing multifunctional additives in the field of perovskite optoelectronics.