Manipulating the photophysical properties of multi-donor molecules for fast reverse intersystem crossing in solution-processed OLED devices

Abstract

The slow reverse intersystem crossing (RISC) rate in thermally activated delayed fluorescence (TADF) emitters result in extended exciton lifetime and pronounced efficiency loss at high luminance level. To address this limitation, we have developed and characterized a series of novel compounds featuring triazine cores substituted with tert-butyl carbazole moieties at various positions and quantities. The objective here is to fine-tune the charge transfer properties, thereby enhancing the efficiency of the RISC process. Our studies reveal that through-space charge transfer is more effective than long-range through-bond charge transfer in minimizing the singlet-triplet energy gap and accelerating RISC. The optimized compound, 4tCzTrz, exhibits an exceptionally fast RISC rate of 1.02 × 10⁷ s⁻¹ and a high photoluminescence quantum yield of up to 100 %. Solution-processed organic light-emitting diodes (OLEDs) incorporating this molecule have achieved outstanding maximum external quantum efficiencies of around 20 %, whether used as an emitter directly or as a sensitizer to boost overall emission efficiency.