Bipolar Solid-Solution Hosts for Efficient Crystalline Organic Light-Emitting Diodes

Crystalline organic semiconductors, recognized for their highly ordered structures and high carrier mobility, have emerged as a focal point in the field of high-performance optoelectronic devices. Nevertheless, the intrinsic unipolar properties, characterized by imbalanced hole and electron transport capabilities, have continuously represented a significant challenge in the advancement of high-performance crystalline thin-film organic light-emitting diodes (C-OLEDs). Here, a bipolar solid-solution thin film with a maintained crystal structure has been fabricated using 2-(4-(9H-carbazol-9-yl)phenyl)-1(3,5-difluorophenyl)-1H-phenanthro [9,10-d]imidazole (2FPPICz) and 4-(1-(3,5-difluorophenyl)-1H-imidazo[4,5-<i>f</i>][1,10]phenanthrolin-2-yl)-N,N-diphenylaniline (2Fn) via a weak epitaxial growth (WEG) process, exhibiting nearly equivalent hole and electron mobilities (10^-2-10^-1 cm² V^-1 s^-1). We have demonstrated a blue C-OLED that achieves high efficiency while maintaining low-efficiency roll-off, employing the bipolar solid-solution thin film as the crystalline host matrix and 4,4'-bis[2-(4-(<i>N</i>,<i>N</i>-diphenylamino)phenyl)vinyl]biphenyl (DPAVBi) as the doped emitter. This device achieves a maximum external quantum efficiency (EQE) of 4.6% with Commission Internationale de L'Eclairage (CIE) coordinates lying around (0.15, 0.22). Among crystalline light-emitting devices utilizing carrier-balanced transport, this EQE stands as one of the highest recorded values. Notable advancements include enhanced photon emission capabilities, optimized driving voltage (4.0 V @ 1000 cd m^-2), and a lower series resistance Joule heat loss ratio (11.8% @ 1000 cd m^-2). This research marks a significant stride in modulating the inherent electrical properties of crystalline host materials, offering a novel and efficacious strategy for the advancement of high-performance crystalline OLEDs.