Peripheral host engineering in TADF dendrimers: integrating radiative promotion and well-balanced bipolar transport for high-luminance, low-roll-off solution-processable OLEDs
摘要
Single-component solution-processed organic light-emitting diodes (OLEDs) that simultaneously achieve high luminance, high efficiency, and low efficiency roll-off represent a significant challenge. Herein, we report a series of thermally activated delayed fluorescence (TADF) dendrimers (m-CzBr, m-CzPhCz, m-CzCzPh and m-CzTPA) featuring a 4CzIPN emissive core tethered to diverse peripheral host units via flexible alkoxy linkers. The localized LUMO on the 4CzIPN core ensures efficient electron transport, while systematic peripheral host modulation precisely tunes photophysical properties, HOMO levels, and charge transport properties. This molecular design leads to a dramatic improvement in device performance, with external quantum efficiency (EQE) rising from 0.76% (m-CzTPA) to 26.5% (m-CzPhCz) and the maximum luminance (Lmax) increasing from 4407 to 59812 cd m−2. The optimized dendrimer, m-CzPhCz, integrates a high photo-luminescence quantum yield, satisfactory charge-transport capability, and highly balanced bipolar carrier transport. These synergistic characteristics facilitate the realization of solution-processed, non-doped TADF-OLEDs that exhibit high external quantum efficiency, together with record-breaking luminance and the smallest efficiency roll-off under high brightness. Impressively, the device achieves unprecedented EQE retention of 25.4% at 5000 cd m−2 and 24% at 10000 cd m−2.