Department of Materials Science and Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan, 44919, Republic of Korea.
Department of Chemistry, Korea University, Seoul, 02841, Republic of Korea.
Adv Mater. 2023 Jun;35(24):e2210511. doi: 10.1002/adma.202210511. Epub 2023 Apr 29.
Further optimization of perovskite light-emitting diodes (PeLEDs) is impeded by crystal deformation caused by residual stress and defect formation with subsequent non-radiative recombination. Molecular additives for defect passivation are widely studied; however, the majority have insulating properties that hinder charge injection and transport. Herein, highly efficient green-emitting PeLEDs are reported by introducing semiconducting molecular additives (Fl-OEGA and Fl-C8A). Transmission electron microscopy shows that conjugated additives exist primarily at the grain boundaries of perovskite, and Kelvin probe force microscopy confirms that the variation in contact potential difference between grain boundaries and perovskite crystal domains is significantly reduced. The residual tensile stress is reduced by 13% and the activation energy for ion migration increases in the Fl-OEGA-treated perovskite film, compared to those of the film without additives. Compared to insulating 2,2'-(ethylenedioxy)diethylamine (EDEA), the introduction of semiconducting additives prevents a significant reduction in the charge-transport capability. Furthermore, the PeLEDs with Fl-OEGA show a negligible shift in the turn-on voltage and a significantly smaller decrease in the current density with increasing Fl-OEGA compared to the devices with EDEA. Finally, the 3D CsPbBr -PeLEDs show the highest external quantum efficiency of 21.3% by the incorporation of semiconducting Fl-OEGA as a new multifunctional additive.
进一步优化钙钛矿发光二极管 (PeLEDs) 受到由残余应力引起的晶体变形和随后的非辐射复合造成的缺陷形成的阻碍。用于缺陷钝化的分子添加剂得到了广泛的研究;然而,大多数添加剂具有绝缘性质,阻碍了电荷注入和传输。在此,通过引入半导体分子添加剂(Fl-OEGA 和 Fl-C8A),报道了高效绿色发光 PeLEDs。透射电子显微镜显示,共轭添加剂主要存在于钙钛矿的晶界处,而 Kelvin 探针力显微镜证实晶界和钙钛矿晶体畴之间的接触电位差的变化显著降低。与不含添加剂的薄膜相比,Fl-OEGA 处理的钙钛矿薄膜中的残余拉伸应力降低了 13%,离子迁移的激活能增加。与绝缘的 2,2'-(乙二氧基)二乙胺 (EDEA) 相比,引入半导体添加剂可防止载流子输运能力的显著降低。此外,与使用 EDEA 的器件相比,在 Fl-OEGA 存在的情况下,PeLED 的开启电压几乎没有变化,并且电流密度随 Fl-OEGA 增加的下降幅度明显较小。最后,通过将半导体 Fl-OEGA 作为新的多功能添加剂掺入,3D CsPbBr 钙钛矿 PeLED 的外量子效率达到了 21.3%的最高值。