Sterically Hindered Tetradentate [Pt(O

Described here are sterically hindered tetradentate [Pt(O^N^C^N)] emitters (Pt-1, Pt-2, and Pt-3) developed for stable and high-performance green phosphorescent organic light-emitting diodes (OLEDs). These Pt(II) emitters exhibit strong saturated green phosphorescence (λmax = 517-531 nm) in toluene and mCP thin films with emission quantum yields as high as 0.97, radiative rate constants (kr) as high as 4.4-5.3 × 105 s-1 and reduced excimer emission, and with a preferential horizontally oriented transition dipole ratio of up to 84%. Theoretical calculations show that p-(hetero)arene substituents at the periphery of the ligand scaffolds in Pt-1, Pt-2, and Pt-3 can i) enhance the spin-orbit coupling (SOC) between the lower singlet excited states and the T1 state, and S0→Sn (n = 1 or 2) transition dipole moment, and ii) introducing additional SOC activity and the bright 1ILCT[π(carbazole)→π*(N^C^N)] excited state (Pt-2 and Pt-3), which are the main contributors to the increased kr values. Utilizing these tetradentate Pt(II) emitters, green phosphorescent OLEDs are fabricated with narrow-band electroluminescence (FWHM down to 36 nm), high external quantum efficiency, current efficiency up to 27.6% and 98.7 cd A-1, and an unprecedented device lifetime (LT95) of up to 9270 h at 1000 cd m-2 under laboratory conditions.

Stable Tetradentate Gold(III)-TADF Emitters with Close to Unity Quantum Yield and Radiative Decay Rate Constant of up to 2 × 106 s-1 : High-Efficiency Green OLEDs with Operational Lifetime (LT90 ) Longer than 1800 h at 1000 cd m-2.

High maximum external quantum efficiency (EQEmax ), 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 (kr ) as large as possible, which, for a thermally activated delayed fluorescent (TADF) emitter, requires both a large S1 →S0 radiative decay rate constant (kr S ) and a small singlet-triplet energy gap (ΔEST ). Here, the design of a class of tetradentate gold(III) TADF complexes for narrowing the ΔEST while keeping the kr S large is reported. The as-synthesized complexes display green emission with close to unity emission quantum yields, and kr 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.