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Ir(III) carbene complexes have been explored as one of the best blue phosphors for their high performance. Herein, the authors designed and synthesized a series of blue‐emitting Ir(III) phosphors (f‐ct9a–c), featuring fac‐coordinated cyano‐imidazo[4,5‐b]pyridin‐2‐ylidene cyclometalates. These Ir(III) complexes exhibit true‐blue emission with a peak maximum spanning 448–467 nm, with high photoluminescence quantum yields of 81–88% recorded in degassed toluene. Moreover, OLED devices bearing phosphors f‐ct9a and f‐ct9b deliver maximum external quantum efficiencies (EQEmax) of 25.9% and 30.3%, together with Commission Internationale de L'Eclairage (CIEx,y) coordinates of (0.157, 0.225) and (0.142, 0.169), respectively. Remarkably, the f‐ct9b‐based device displays an incredible EQE of 29.0% at 5000 cd·m−2. The hyper‐OLED device based on f‐ct9b and ν‐DABNA exhibits an EQEmax of 34.7% and CIEx,y coordinates of (0.122, 0.131), affirming high potentials in achieving efficient blue electroluminescence. [ABSTRACT FROM AUTHOR]

Bis-tridentate Ir(III) metal complexes are expected to show great potential in organic light-emitting diode (OLED) applications due to the anticipated, superb chemical and photochemical stability. Unfortunately, their exploitation has long been hampered by lack of adequate methodology and with inferior synthetic yields. This hurdle can be overcome by design of the first homoleptic, bis-tridentate Ir(III) complex [Ir(pzpyph)(pzHpyph)] ( 1), for which the abbreviation (pzpyph)H (or pzHpyph) stands for the parent 2-pyrazolyl-6-phenyl pyridine chelate. After that, methylation and double methylation of 1 afford the charge-neutral Ir(III) complex [Ir(pzpyph)(pzMepyph)] ( 2) and cationic complex [Ir(pzMepyph)2][PF6] ( 3), while deprotonation of 1 gives formation of anionic [Ir(pzpyph)2][NBu4] ( 4), all in high yields. These bis-tridentate Ir(III) complexes 2- 4 are highly emitted in solution and solid states, while the charge-neutral 2 and corresponding t-butyl substituted derivative [Ir(pzpyBuph)(pzMepyBuph)] ( 5) exhibit superior photostability versus the tris-bidentate references [Ir(ppy)2(acac)] and [Ir(ppy)3] in toluene under argon, making them ideal OLED emitters. For the track record, phosphor 5 gives very small efficiency roll-off and excellent overall efficiencies of 20.7%, 66.8 cd A−1, and 52.8 lm W−1 at high brightness of 1000 cd m−2. These results are expected to inspire further studies on the bis-tridentate Ir(III) complexes, which are judged to be more stable than their tris-bidentate counterparts from the entropic point of view. [ABSTRACT FROM AUTHOR]