Most phosphorescent devices suffer from severe triplet−triplet annihilation (TTA), and the efficiency recording at high luminance is much lower than that at low luminance, making the practicality worse than expected. In this study, a series of donor−acceptor (D−A) molecules consisting of dicyano-imidazole and phenylcarbazole were synthesized and applied to the host materials. For electroluminescence applications, imM-m-Cz-based green-emitting organic light-emitting diodes show a maximum luminance of 1.68 × 10 5 cd m −2 at 11.2 V, which is 20% higher than that of the benchmark host 4,4′-bis(N-carbazolyl)-1,1′-biphenyl at 13.4 V; in addition, the turn-on voltage (V on ) is only 2.3 V. In terms of hole and electron mobility, imM-m-Cz shows one of the most balanced carrier mobilities in the reported literature (electron and hole mobilities of 3.64 × 10 −5 and 4.23 × 10 −5 cm 2 V −1 s −1 , respectively). The balanced carrier mobility can help expand the recombination region and thus reduce the formation of TTA. Furthermore, the high maximum luminance of about 2.80 × 10 5 cd m −2 obtained in an imM-m-Cz-based tandem device demonstrates a sufficiently high current density/luminance, and the peak efficiency achieves an even higher efficiency of 40.6% (1.51 × 10 5 cd A −1 and 98.6 lm W −1 ), which is among the highest reported properties based on imidazole-based host materials. Combining the balanced carrier mobility with the proper device design in this study, the efficiency roll-off under high luminance can be greatly reduced, and the practicality of the resulting phosphorescent device can be significantly improved.

A series of dicyano-imidazole-based molecules with thermally activated delayed fluorescence (TADF) properties were synthesized to obtain pure blue-emitting organic lightemitting 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 9,9diphenyl-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 (ΔE ST ) between the first excited singlet (S 1 ) and the triplet (T 1 ) 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.

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In recent years, owing to the demand for highefficiency phosphorescent organic light-emitting devices (PhOLEDs), many studies have been conducted on the development of bipolar host materials. A series of imidazolylphenylcarbazole-based host materials, i. e., im-CzP, im-CzPCz, im-CzPtBu, and im-OCzP, were synthesized to obtain highefficiency green and red-emitting PhOLEDs. With im-OCzP as the host, satisfactory peak efficiencies of 22.2 (77.0 cd A À 1 and 93.1 lm W À 1 ) and 14.1 % (9.0 cd A À 1 and 10.1 lm W À 1 ) could be obtained, respectively. To further improve the performance of the devices, an electron transport material, bis-4,6-(3,5-di-3pyridylphenyl)-2-methylpyrimidine (B3PyMPM) was selected to construct a co-hosted system. The efficiency of im-OCzP combined with B3PyMPM forming co-hosts could also achieve high values of 23.0 (80.0 cd A À 1 and 98.8 lm W À 1 ) and 16.5 % (10.2 cd A À 1 and 13.4 lm W À 1 ) for green and red PhOLEDs, respectively. These results exhibited that the proposed bipolar hosts have great flexibility in adjusting the carrier balance of EML in OLEDs, demonstrating their ingenious design and high potential.

Recently, perovskites have attracted intense attention due to their high potential in optoelectronic applications. Employing perovskites as the emissive materials of lightemitting 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 CsPbBr 3 /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.