Zhang Jibin, Zhang Tiankai, Ma Zhuangzhuang, Yuan Fanglong, Zhou Xin, Wang Heyong, Liu Zhe, Qing Jian, Chen Hongting, Li Xinjian, Su Shijian, Xie Jianing, Shi Zhifeng, Hou Lintao, Shan Chongxin
Key Laboratory of Materials Physics of Ministry of Education, School of Physics and Microelectronics, Zhengzhou University, Daxue Road 75, Zhengzhou, 450052, China.
Guangdong Provincial Key Laboratory of Optical Fiber Sensing and Communications, Siyuan laboratory, Guangzhou Key Laboratory of Vacuum Coating Technologies and New Energy Materials, Department of Physics, Jinan University, Guangzhou, 510632, P. R. China.
Adv Mater. 2023 Feb;35(8):e2209002. doi: 10.1002/adma.202209002. Epub 2022 Dec 22.
Pure-red perovskite LEDs (PeLEDs) based on CsPb(Br/I) nanocrystals (NCs) usually suffer from a compromise in emission efficiency and spectral stability on account of the surface halide vacancies-induced nonradiative recombination loss, halide phase segregation, and self-doping effect. Herein, a "halide-equivalent" anion of benzenesulfonate (BS ) is introduced into CsPb(Br/I) NCs as multifunctional additive to simultaneously address the above challenging issues. Joint experiment-theory characterizations reveal that the BS can not only passivate the uncoordinated Pb -related defects at the surface of NCs, but also increase the formation energy of halide vacancies. Moreover, because of the strong electron-withdrawing property of sulfonate group, electrons are expected to transfer from the CsPb(Br/I) NC to BS for reducing the self-doping effect and altering the n-type behavior of CsPb(Br/I) NCs to near ambipolarity. Eventually, synergistic boost in device performance is achieved for pure-red PeLEDs with CIE coordinates of (0.70, 0.30) and a champion external quantum efficiency of 23.5%, which is one of the best value among the ever-reported red PeLEDs approaching to the Rec. 2020 red primary color. Moreover, the BS -modified PeLED exhibits negligible wavelength shift under different operating voltages. This strategy paves an efficient way for improving the efficiency and stability of pure-red PeLEDs.
基于CsPb(Br/I)纳米晶体(NCs)的纯红色钙钛矿发光二极管(PeLEDs)通常由于表面卤化物空位诱导的非辐射复合损失、卤化物相分离和自掺杂效应而在发光效率和光谱稳定性方面有所折衷。在此,将苯磺酸盐(BS)的“卤化物等效”阴离子作为多功能添加剂引入CsPb(Br/I) NCs中,以同时解决上述具有挑战性的问题。联合实验-理论表征表明,BS不仅可以钝化NCs表面未配位的Pb相关缺陷,还可以提高卤化物空位的形成能。此外,由于磺酸根基团的强吸电子性质,预计电子会从CsPb(Br/I) NC转移到BS,以减少自掺杂效应,并将CsPb(Br/I) NCs的n型行为改变为近双极性。最终,对于CIE坐标为(0.70, 0.30)且最佳外量子效率为23.5%的纯红色PeLEDs,实现了器件性能的协同提升,这是有史以来报道的接近Rec. 2020红色原色的红色PeLEDs中的最佳值之一。此外,BS修饰的PeLED在不同工作电压下表现出可忽略不计的波长偏移。该策略为提高纯红色PeLEDs的效率和稳定性铺平了一条有效途径。