Hyperbranched Conjugated Polymer with Multiple Charge Transfer Enables High-Efficiency Nondoped Red...

Conjugated polymers featuring thermally activated delayed fluorescence (TADF) attract tremendous attention in both academic and industry communities due to their easy solution processing for fabricating large-area and low-cost high-performance polymer light-emitting diodes (PLEDs). However, current nondoped solution-processed PLEDs frequently encounter significant efficiency roll-offs and unreasonably high operating voltages at high brightness, especially for red-emitting polymers. Herein, we design hyperbranched conjugated polymers (HCPs) with D-A-D type TADF characteristics for high-performance red-emitting PLEDs. Multiple intramolecular charge transfer (ICT) channels induced by quasi-equivalent donors of the TADF core strongly boost the reverse intersystem crossing (RISC) process and singlet excitons radiative transition. Coupling with the efficient energy transfer process generated by structure advantages of HCPs, the strongly electron-withdrawing oxygen atoms located on the TADF cores further accelerate hole transportation from the host chains to the TADF cores. Under a rational regulation of the TADF core ratio, the related nondoped red-emitting device performs an outstanding performance with an EQE_max of 8.39% and exhibits no roll-off while the luminance is less than 100 cd/m² and only 3.3% decrease at 500 cd/m². Simultaneously, the EQE can maintain 7.4% under 1000 cd/m². Furthermore, the corresponding nondoped device exhibits a low turn-on voltage of around 2.5 V and achieves a luminance of 500 cd/m² at 3.5 V and even 1000 cd/m² at 3.9 V. To our knowledge, this is the best performance among all nondoped red PLEDs with high brightness obtained at low operating voltage.