Abstract: Realizing efficient red/near-infrared (NIR) electroluminescence (EL) by precisely modulating molecular aggregations of thermally activated delayed fluorescence (TADF) emitters is an attractive pathway, yet the molecular designs are elusive. Here, we propose a new approach to manage molecular aggregation via a mild-twist acceptor-donor-acceptor (A-D-A)-type molecular design. A proof-of-concept TADF molecule, QCN-PhSAC-QCN, was developed that furnishes a fast radiative rate and obvious aggregation-induced emission (AIE) feature. Its emission bands can be facilely shifted from intrinsic yellow to the red/NIR region via fine-tuning doping levels and molecular aggregates while maintaining elegant photoluminescence quantum yields benefiting from suppressed exciton annihilation processes. As a result, a QCN-PhSAC-QCN-based organic light-emitting diode (OLED) exhibits a record-setting external quantum efficiency (EQE) of 39.1% at a doping ratio of 10 wt.%, peaking at 620 nm. Moreover, its nondoped NIR OLED affords a champion EQE of 14.3% at 711 nm and retains outstanding EQEs as high as 5.40% and 2.35% at high current densities of 10 and 100 mA cm−2, respectively, which are the highest values among all NIR-TADF OLEDs at similar density levels. This work validates the feasibility of such mild-twist A-D-A-type molecular design for precisely controlling molecular aggregation while maintaining high efficiency, thus providing a promising pathway for high-performance red/NIR TADF OLEDs.

链接：https://onlinelibrary.wiley.com/doi/10.1002/adma.202307725