Enhancing Horizontal Ratio of Transition Dipole Moment in Homoleptic Ir Complexes for High Outcoupling Efficiency of Organic Light‐Emitting Diodes

Abstract The light‐emitting dipole orientation (EDO) of a phosphorescent emitter is a key to improving the external quantum efficiency (EQE) of organic light‐emitting diodes (OLEDs) without structural modification of the device. Here, four homoleptic Ir complexes as a phosphorescent emitter are systematically designed based on the molecular structure of tris(2‐phenylpyridine)iridium(III) (Ir(ppy) 3 ) to control the EDO. Trimethylsilane, methyl, 2‐methylpropyl, and cyclopentylmethyl group substituted to pyridine ring of the ligand contribute to the improvement of the EDO from 76.5% for Ir(ppy) 3 to 87.5%. A linear relationship between the EDO and the aspect ratio (geometric anisotropy factor) is founded, implying the importance of the effective area for the nonbonding force between host and dopant molecules. Also, it is investigated that the EDO enhancement mainly originates from the vertical alignment of the C3 axis of molecule in the substrate axis rather than the change in the direction of the transition dipole alignment in the molecular axis. The optical simulation reveals that the outcoupling efficiency of phosphorescent OLEDs adopting new dopants reaches 38.4%. The green OLEDs exhibiting 28.3% of EQE, 103.2 cd A –1 of current efficiency, and 98.2 lm W –1 of power efficiency are demonstrated, which is understood to have little electrical loss.