Highly efficient blue thermally activated delayed fluorescent OLEDs with record-low driving voltages utilizing high triplet energy hosts with small singlet–triplet splittings

The high driving voltage of blue organic light-emitting diodes (OLEDs) based on emitters with thermally activated delayed fluorescence (TADF) remains a constraint for their portable application. A major reason for this is that the high triplet (T(1)) of the host required to match the blue TADF emitters would always lead to inferiority in terms of carrier injection. Therefore, a suitable host should possess not only a high T(1) but also a relatively low singlet (S(1)) for improved carrier injection, indicating that small singlet–triplet splittings (ΔE(ST)s) are highly desired. Here, four carbazolyl benzonitrile derivatives are facilely prepared in a one-step approach with restrained conjugate lengths to maintain high triplet energies while their highly twisted structures spatially separate the frontier orbital distribution to achieve relatively low ΔE(ST)s. Meanwhile, the charge transporting mobilities of these hosts are effectively tuned by the different linker types of the host moieties. Consequently, high-triplet-energy hosts with favorable carrier injection/transporting abilities are realized, endowing blue TADF devices with a maximum external quantum efficiency of 21.5%, a maximum power efficiency of 42.0 lm W(–1) and an ultra-low onset voltage of 2.8 V. It is noteworthy that a driving voltage of 4.9 V is achieved at a practical luminance of 1000 cd m(–2), which is the lowest among the doped blue TADF OLEDs reported until now. This work suggests that manipulation of the molecular topologies not only leads to the flexible and feasible design of novel bipolar host materials, but also affords a promising method for fine-tuning physical properties and thus obtaining state-of-the-art device performances.