Stable Tetradentate Gold(III)-TADF Emitters with Close to Unity Quantum Yield and Radiative Decay Rate Constant of up...

High maximum external quantum efficiency (EQE_max ), small efficiency roll-offs, and long operational lifetime at practical luminances are three crucial parameters for commercialization of organic light-emitting diodes (OLEDs). To simultaneously achieve these goals, it is desirable to have the radiative decay rate constant (k_r ) as large as possible, which, for a thermally activated delayed fluorescent (TADF) emitter, requires both a large S₁ →S₀ radiative decay rate constant (k_r ^S ) and a small singlet-triplet energy gap (ΔE_ST ). Here, the design of a class of tetradentate gold(III) TADF complexes for narrowing the ΔE_ST while keeping the k_r ^S large is reported. The as-synthesized complexes display green emission with close to unity emission quantum yields, and k_r approaching 2 × 10⁶ s^-1 in thin films. The vacuum-deposited green OLEDs based on 1 and 4 demonstrate maximum EQEs of up to 24 and 27% with efficiency roll-offs of 5.5 and 2.2% at 1000 cd m^-2 , respectively; the EQEs maintain high at 10 000 cd m^-2 (19% (1) and 24% (4)). A long LT₉₀ device lifetime of 1820 h at 1000 cd m^-2 for complex 1 is achieved, which is one of the longest device lifetimes of TADF-OLEDs reported in the literature.