Short-lived TADF-Cu(I) complex for red OLEDs with EQE max of 25.9% and <2% roll-off at 10,000 cd m−2
Cu(I) complexes exhibiting thermally activated delayed fluorescence (TADF) have emerged as promising alternatives to noble-metal-based emitters for organic light-emitting diodes (OLEDs). However, the development of red-emitting Cu(I) complexes has been hindered by slow radiative decay and fast nonradiative decay. In this study, a linear two-coordinate Cu(I) complex, ICuTMC, was designed and synthesized. By pairing a pyrazine-fused N-heterocyclic carbene and a tetra-methylcarbazolyl ligand, a strong ligand-to-ligand charge transfer excited state is generated. Single-crystal structure authenticates close intramolecular C–H···Cu contacts, providing good steric shielding to the metal center. C–H···π interactions between ligands are also revealed. The complex exhibits highly efficient red TADF with emission maximum at 622 nm, photoluminescence quantum yield of 76%, and short delayed fluorescence lifetime of 0.24 μs. This is enabled by a large oscillator strength from the coplanar donor-Cu-acceptor conformation, a small singlet-triplet energy gap from spatial separation of frontier molecular orbitals, and strong spin-orbit coupling from the metal center. Vacuum-deposited OLEDs based on ICuTMC achieve a peak external quantum efficiency of 25.9% and a significantly small roll-off of 1.9% at 10,000 cd m−2. These performances demonstrate a way to overcome the energy gap law for linear coinage metal complexes toward red OLEDs.