Color Tunable Phosphorescent Neutral Manganese(II) Complexes Through Steric Hindrance Driven Bond Angle Distortion

Phosphorescent manganese(II) complexes with high photoluminescence quantum yields (PLQYs) and low cost exhibit great potential in organic light‐emitting diodes (OLEDs), information security, and X‐ray imaging. However, it is still a challenge to tune their emission colors. Herein, an effective strategy for engineering the phosphorescence colors of tetrahedral Mn(II) complexes through steric hindrance‐driven bond angle distortion is proposed. Modulating the steric hindrance between phosphine and benzofuran and varying the O─Mn─O bond angles allows these Mn(II) complexes to emit from 498 to 548 nm. Interestingly, these achiral single crystals of Mn(II) complexes exhibit significant circularly polarized luminescence signals due to symmetry breaking. Furthermore, high‐performance green OLEDs are achieved by using these Mn(II) complexes as dopants, providing a record‐high external quantum efficiency of 15.7%. These super‐duper results greatly inspire the development of multi‐color Mn(II) complexes and low‐cost Mn‐based devices.