High-Performance Multicolor Organic Light-Emitting Diodes Based on a Pt(II) Carbene Complex Featuring Hemiligand Interaction

Utilizing a single organic light-emitting diode (OLED) architecture for multicolor emissions can significantly simplify manufacturing progress and broaden applications. Here, we report on a carbene-based Pt(II) complex, designated as Pt(pyiOppy), which exhibits an unusual dimeric packing mode solely by hemiligand π···π stacking. This feature is distinct from the well-known Pt···Pt or Pt···ligand interactions. The dimer persists in new types of orbital combinations, along with its triplet transition state, which are evidenced for the first time. Pt(pyiOppy), under various doping concentrations in a solid matrix, demonstrates multicolor emissions ranging from green to red, all exhibiting high photoluminescent quantum efficiencies (48-97%). The devices incorporating Pt(pyiOppy) can emit green, yellow, orange, and red lights, covering a CIE coordinate range of (0.28-0.65, 0.61-0.34). All the devices also achieve appreciable maximum external quantum efficiencies (9.4-17.2%) and impressive lifetimes of hundreds of hours (LT₇₀ at 1000 cd/m²). These findings showcase a new type of Pt(II) aggregate enabling well-controlled, multicolor high-performance phosphorescent OLEDs.