Manipulating the Electronic Excited State Energies of Pyrimidine-Based Thermally Activated Delayed Fluorescence Emitters to Realize Efficient Deep-Blue Emission

The development of efficient and robust deep-blue emitters is one of the key issues in organic light-emitting devices (OLEDs) for environmentally friendly, large-area displays or general lighting. As a promising technology that realizes 100% conversion from electrons to photons, thermally activated delayed fluorescence (TADF) emitters have attracted considerable attention. However, only a handful of examples of deep-blue TADF emitters have been reported to date, and the emitters generally show large efficiency roll-off at practical luminance over several hundreds to thousands of cd m^-2, most likely because of the long delayed fluorescent lifetime (_d). To overcome this problem, we molecularly manipulated the electronic excited state energies of pyrimidine-based TADF emitters to realize deep-blue emission and reduced _d. We then systematically investigated the relationships among the chemical structure, properties, and device performances. The resultant novel pyrimidine emitters, called Ac-XMHPMs (X = 1, 2, and 3), contain different numbers of bulky methyl substituents at acceptor moieties, increasing the excited singlet (E_S) and triplet state (E_T) energies. Among them, Ac-3MHPM, with a high E_T of 2.95 eV, exhibited a high external quantum efficiency (η_ext,max) of 18% and an η_ext of 10% at 100 cd m^-2 with Commission Internationale de l′Eclairage chromaticity coordinates of (0.16, 0.15). These efficiencies are among the highest values to date for deep-blue TADF OLEDs. Our molecular design strategy provides fundamental guidance to design novel deep-blue TADF emitters.