Abstract
Transition metal complexes exhibiting thermally activated delayed fluorescence (TADF) remain underdeveloped for organic light-emitting diodes (OLEDs). Here, we describe a design of TADF Pd(II) complexes featuring metal-perturbed intraligand charge-transfer excited states. Two orange- and red-emitting complexes with efficiencies of 82 and 89% and lifetimes of 2.19 and 0.97 μs have been developed. Combined transient spectroscopic and theoretical studies on one complex reveal a metal-perturbed fast intersystem crossing process. OLEDs using the Pd(II) complexes show maximum external quantum efficiencies of 27.5 to 31.4% and small roll-offs down to 1% at 1000 cd m(-2). Moreover, the Pd(II) complexes show exceptional operational stability with LT(95) values over 220 hours at 1000 cd m(-2), benefiting from the use of strong σ-donating ligands and the presence of multiple intramolecular noncovalent interactions beside their short emission lifetimes. This study demonstrates a promising approach for developing efficient and robust luminescent complexes without using the third-row transition metals.