Fine-Modulation of Perovskite Ion-Additive Binding Interaction Using Multidentate Ligation for High Performance Perovskite Light-Emitting Diodes

Research on perovskite light-emitting diodes (PeLEDs) has primarily focused on modulating crystal growth to achieve smaller grain sizes and defect passivation using organic additives. However, challenges remain in controlling the intermolecular interactions between these organic additives and perovskite precursor ions for precise modulation of crystal growth. In this study, we synthesize two triphenylphosphine oxide (TPPO)-based multidentate additives: bidentate hexane-1,6-diyl-bis(oxy-4-triphenylphosphine oxide) (2-TPPO) and tetradentate pentaerythrityl-tetrakis(oxy-4-triphenylphosphine oxide) (4-TPPO). We investigate the crystallization of perovskites through real-time crystal growth analyses and theoretical calculations. As the extent of multidentate binding increases, perovskite crystallization slows down gradually. The multidentate TPPO additives exhibit strong binding to Pb