Rational Design of Efficient Organometallic Ir(III) Complexes for High-Performance, Flexible, Monochromatic, and White Light-Emitting Electrochemical Cells

Highly efficient light-emitting electrochemical cells (LECs) have attracted tremendous interest because of their simple structures and low-cost fabrication processing, showing great potential for full-color displays and solid-state lighting. In this work, we rationally designed and synthesized two red-emitting cationic Ir(III) complexes, [Ir(tBuPBI)2(biq)]PF6 (R1) and [Ir(tBuPBI)2(qibi)]PF6 (R2), in which a tert-butyl-functionalized 1,2-diphenyl-1H-benzo[d]imidazole (PBI) unit and conjugated 2,2′-biquinoline (biq) and 2-(1-phenyl-1H-benzo[d]imidazol-2-yl)quinolone (qibi) were employed as cyclometalated and ancillary ligands, respectively. The introduced tert-butyl group led to homogeneous and highly emissive thin films by increasing the solubility and suppressing the strong intermolecular interactions due to steric hindrance. Based on the abovementioned high-quality emissive layer, high-efficiency LECs were achieved. An efficient red-emitting LEC fabricated on a glass substrate achieved a current efficiency (ηC) of 7.18 cd/A and an external quantum efficiency (ηext) of 9.32%. By doping both complexes into a blue-green-emitting cationic Ir(III) complex, high-performance white LECs were also successfully fabricated with Commission International de L’Eclairage (CIE) coordinates of (0.39,0.39), a ηC of 17.43 cd/A, and a ηext of 8.92%. In addition, we also fabricated flexible red and white LECs with outstanding efficiencies and mechanical flexibilities. The ηC and ηext values of a flexible white LEC could be as high as 13.50 cd/A and 6.86%, respectively. The efficiency of the flexible device remained at approximately 95% of the initial value after 500 bends with a radius of curvature of 5 mm, demonstrating the great potential of these complexes for full-color displays and flexible optoelectronics.