Sterically Hindered Tetradentate \[PtO^NCN\] Emitters with Radiative Decay Rates up to 5.3 × 10(5) s(-1) for Phosphorescent Organic Light-Emitting Diodes with LT(95) Lifetime over 9200 h at 1000 cd m(-2).

Described here are sterically hindered tetradentate \[PtO^NCN\] 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 λ = 517-531 nm in toluene and mCP thin films with emission quantum yields as high as 0.97, radiative rate constants (k) as high as 4.4-5.3 × 10 s 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 T state, and S→S n = 1 or 2 transition dipole moment, and ii) introducing additional SOC activity and the bright ILCT\[π(carbazole)→π*N^CN\] excited state (Pt-2 and Pt-3), which are the main contributors to the increased k 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, and an unprecedented device lifetime (LT) of up to 9270 h at 1000 cd m under laboratory conditions.