Chemical Reaction Modulated Low-Dimensional Phase Toward Highly Efficient Sky-Blue Perovskite Light-Emitting Diodes.

Blue perovskite light-emitting diodes (PeLEDs) are crucial avenues for achieving full-color displays and lighting based on perovskite materials. However, the relatively low external quantum efficiency (EQE) has hindered their progression towards commercial applications. Quasi-two-dimensional (quasi-2D) perovskites stand out as promising candidates for blue PeLEDs, with optimized control over low-dimensional phases contributing to enhanced radiative properties of excitons. Herein, the impact of organic molecular dopants on the crystallization of various n-phase structures in quasi-2D perovskite films. The results reveal that the highly reactive bis(4-(trifluoromethyl)phenyl)phosphine oxide (BTF-PPO) molecule could effectively restrain the formation of organic spacer cation-ordered layered perovskite phases through chemical reactions, simultaneously passivate those uncoordinated Pb2+ defects. Consequently, the prepared PeLEDs exhibited a maximum EQE of 16.6% (@ 490 nm). The finding provides a new route to design dopant molecules for phase modulation in quasi-2D PeLEDs.

In Situ Hydrolysis of Phosphate Enabling Sky-Blue Perovskite Light-Emitting Diode with EQE Approaching 16.32.

The performance of blue perovskite light-emitting diodes (PeLEDs) lags behind the green and red counterparts owing to high trap density and undesirable red shift of the electroluminescence spectrum under operation conditions. Organic molecular additives were employed as passivators in previous reports. However, most commonly have limited functions, making it challenging to effectively address both efficiency and stability issues simultaneously. Herein, we reported an innovatively dynamic in situ hydrolysis strategy to modulate quasi-2D sky-blue perovskites by the multifunctional passivator phenyl dichlorophosphate that not only passivated the defects but also underwent in situ hydrolysis reaction to stabilize the emission. Moreover, hydrolysis products were beneficial for low-dimensional phase manipulation. Eventually, we obtained high-performance sky-blue PeLEDs with a maximum external quantum efficiency (EQE) of 16.32% and an exceptional luminance of 5740 cd m-2. More importantly, the emission peak of devices located at 485 nm remained stable under different biases. Our work signified the significant advancement toward realizing future applications of PeLEDs.

Bio-Inspired Pangolin Design for Self-Healable Flexible Perovskite Light-Emitting Diodes.

Despite tremendous developments in the luminescene performance of perovskite light-emitting diodes (PeLEDs), the brittle nature of perovskite crystals and their poor crystallinity on flexible substrates inevitably lead to inferior performance. Inspired by pangolins' combination of rigid scales and soft flesh, we propose a bionic structure design for self-healing flexible PeLEDs by employing a polymer-assisted crystal regulation method with a soft elastomer of diphenylmethane diisocyanate polyurethane (MDI-PU). The crystallinity and flexural strain resistance of such perovskite films on plastics with silver-nanowire-based flexible transparent electrodes are highly enhanced. The detrimental cracks induced during repeated deformation can be effectively self-healed under heat treatment via intramolecular/intermolecular hydrogen bonds with MDI-PU. Upon collective optimization of the perovskite films and device architecture, the blue-emitting flexible PeLEDs can achieve a record external quantum efficiency of 13.5% and high resistance to flexural strain, which retain 87.8 and 80.7% of their initial efficiency after repeated bending and twisting operations of 2000 cycles, respectively.