Liu Yuqiang, Ono Luis K, Tong Guoqing, Bu Tongle, Zhang Hui, Ding Chenfeng, Zhang Wei, Qi Yabing
Energy Materials and Surface Sciences Unit (EMSSU), Okinawa Institute of Science and Technology Graduate University (OIST), 1919-1 Tancha, Onna-son, Kunigami-gun, Okinawa 904-0495, Japan.
College of Textiles & Clothing, Qingdao University, Qingdao 266071, China.
J Am Chem Soc. 2021 Dec 1;143(47):19711-19718. doi: 10.1021/jacs.1c07757. Epub 2021 Nov 18.
The spectral instability issue is a challenge in blue perovskite light-emitting diodes (PeLEDs). Dion-Jacobson (DJ) phase perovskites are promising alternatives to achieve high-quality blue PeLEDs. However, the current exploration of DJ phase perovskites is focused on symmetric divalent cations, and the corresponding efficiency of blue PeLEDs is still inferior to that of green and red ones. In this work, we report a new type of DJ phase CsPb(Br/Cl) perovskite via introduction of an asymmetric molecular configuration as the organic spacer cation in perovskites. The primary and tertiary ammonium groups on the asymmetric cations bridge with the lead halide octahedra forming the DJ phase structures. Stable photoluminescence spectra were demonstrated in perovskite films owing to the suppressed halide segregation. Meanwhile, the radiative recombination efficiency of charges is improved significantly as a result of the confinement effects and passivation of charge traps. Finally, we achieved an external quantum efficiency of 2.65% in blue PeLEDs with stable spectra emission under applied bias voltages. To our best knowledge, this is the first report of asymmetric cations used in PeLEDs, which provides a facile solution to the halide segregation issue in PeLEDs.
光谱不稳定性问题是蓝色钙钛矿发光二极管(PeLEDs)面临的一项挑战。狄翁-雅各布森(DJ)相钙钛矿是实现高质量蓝色PeLEDs的有前景的替代材料。然而,目前对DJ相钙钛矿的探索集中在对称二价阳离子上,且相应蓝色PeLEDs的效率仍低于绿色和红色PeLEDs。在这项工作中,我们通过引入一种不对称分子构型作为钙钛矿中的有机间隔阳离子,报道了一种新型的DJ相CsPb(Br/Cl)钙钛矿。不对称阳离子上的伯铵基和叔铵基与卤化铅八面体桥连,形成DJ相结构。由于卤化物偏析受到抑制,在钙钛矿薄膜中展示出了稳定的光致发光光谱。同时,由于限域效应和电荷陷阱的钝化,电荷的辐射复合效率显著提高。最后,我们在施加偏置电压下实现了具有稳定光谱发射的蓝色PeLEDs的2.65%的外量子效率。据我们所知,这是首次在PeLEDs中使用不对称阳离子的报道,它为解决PeLEDs中的卤化物偏析问题提供了一种简便的解决方案。