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Two novel N‐embedded polycyclic units functionalized phosphorescent iridium(III) complexes ( Ir‐1  and  Ir‐2 ) with substituents in different positions have been prepared. Complex  Ir‐1  bearing the substituent at the 3‐position shows a distinct blue shift single‐peak emission (524 nm) with a higher luminescence efficiency (Φ PL =42 %) and shorter emission lifetime (τ=282 ns) by comparison with 4‐position substitution based complex  Ir‐2  (Φ PL =23 %, τ=562 ns), which exhibits a dual‐peak emission (564 nm and 602 nm), and phosphorescence color can be tuned from green to yellow. In addition, DFT calculations demonstrate that unusual ligand‐to‐metal charge transfer ( 3 LMCT) excited state property can be found in  Ir‐2 , which is in contrast to metal‐to‐ligand charge transfer ( 3 MLCT) excited state character in  Ir‐1 . This result can be attribute to strong electron‐donating character and 4‐position substitution effect of the unit.

Tuning the Photophysical and Excited State Properties of Phosphorescent Iridium(III) Complexes by Polycyclic Unit Substitution