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A series of dicyano-imidazole-based molecules with thermally activated delayed fluorescence (TADF) properties were synthesized to obtain pure blue-emitting organic light-emitting diodes (OLEDs). The targeted molecules used dicyano-imidazole with a short-conjugated system as the electron acceptor to strong intermolecular π-π interactions, and provide a relatively shallow energy level of the lowest unoccupied molecular orbital (LUMO). The cyano group was selected to improve imidazole as an electron acceptor due to its prominent electron-transporting characteristics. Four different electron donors, that is, 9,9-dimethyl-9,10-dihydroacridine (DMAC), 10H-spiro(acridine-9,9'-fluoren) (SPAC), and 9,9-diphenyl-9,10-dihydroacridine (DPAC), were used to alternate the highest occupied molecular orbital (HOMO) energy level to tune the emission color further. The crowded molecular structure in space makes the electron donor and acceptor almost orthogonal, reducing the energy gap (ΔEST ) between the first excited singlet (S1 ) and the triplet (T1 ) states and introducing significant TADF property. The efficiencies of the blue-emissive devices with imM-SPAC and imM-DMAC obtained in this work are the highest among the reported imidazole-based TADF-OLEDs, which are 13.8 % and 13.4 %, respectively. Both of Commission Internationale de l'Eclairage (CIE) coordinates are close to the saturated blue region at (0.17, 0.18) and (0.16, 0.19), respectively. Combining these tailor-made TADF compounds with specific device architectures, electroluminescent (EL) emission from sky-blue to deep-blue could be achieved, proving their great potential in EL applications.

Recently, perovskites have attracted intense attention due to their high potential in optoelectronic applications. Employing perovskites as the emissive materials of light-emitting electrochemical cells (LECs) shows the advantages of simple fabrication process, low-voltage operation, and compatibility with inert electrodes, along with saturated electroluminescence (EL) emission. Unlike in previously reported perovskite LECs, in which salts are incorporated in the emissive layer, the ion-transport layer was separated from the emissive layer in this work. The layer of ionic transition metal complex (iTMC) not only provides mobile ions but also serves as an electron-injection/transport layer. Orthogonal solvents are used in spin coating to prevent the intermixing of stacked perovskite and iTMC layers. The blue iTMC with high ionization potential is effective in blocking holes from the emissive layer and thus ensures EL color saturation. In addition, the carrier balance of the perovskite/iTMC LECs can be optimized by adjusting the iTMC layer thickness. The optimized external quantum efficiency of the CsPbBr3 /iTMC LEC reaches 6.8 %, which is among the highest reported values for perovskite LECs. This work successfully demonstrates that, compared with mixing all components in a single emissive layer, separating the layer of ion transport, electron injection and transport from the perovskite emissive layer is more effective in adjusting device carrier balance. As such, solution-processable perovskite/iTMC LECs open up a new way to realize efficient perovskite LECs.