Weakly Conjugated Phosphine Oxide Hosts for Efficient Blue Thermally Activated Delayed Fluorescence Organic Light-Emitting Diodes

The development of host materials with high first-triplet state (T1) energy and high charge mobility is a key to achieve efficient true-blue organic light-emitting diodes (OLEDs), employing phosphorescence and thermally activated delayed fluorescence (TADF). An ether-bridged double triphenylphosphine oxide (TPPO) compound, bis­(2-(diphenylphosphino)­phenyl)­ether oxide (DPEPO), was reported to have a very high T1 energy of 3.3 eV but suffers from poor charge mobility. Here, five bridge-controlled multi-TPPO derivatives were studied through a combination of experiments and theory. We demonstrate that the push–pull electron capability of the bridge group governs the T1 energy and electron mobility of these materials. Replacing the ether bridge by a bis­(trifluoromethyl)­methylene group can reduce the energy barrier for intramolecular electron exchange and consequently enhance the electron mobility by two orders of magnitude without lowering the T1 energy. A blue TADF OLED employing this bis­(trifluoromethyl)­methylene-bridged compound achieves the same high external quantum efficiency but a much higher current density compared to the control device employing DPEPO. In contrast, a bridge group with strong electron-withdrawing capability, such as phosphine oxygen or sulfone, lowers the T1 energy of the compound by enhancing the electronic coupling between TPPO subunits and inhibits intermolecular electron transfer by trapping the electron charge around the bridge.