Cationic Ir(III) Complexes with 4-Fluoro-4'-pyrazolyl-(1,1'-biphenyl)-2-carbonitrile as the Cyclometalating Ligand: Synthesis, Characterizations, and Application to Ultrahigh-Efficiency Light-Emitting Electrochemical Cells.

Light-emitting electrochemical cells (LECs) promise low-cost, large-area luminescence applications with air-stabilized electrodes and a versatile fabrication that enables the use of solution processes. Nevertheless, the commercialization of LECs is still encountering many obstacles, such as low electroluminescence (EL) efficiencies of the ionic materials. In this paper, we propose five blue to yellow ionic Ir complexes possessing 4-fluoro-4'-pyrazolyl-(1,1'-biphenyl)-2-carbonitrile (ppfn) as a novel cyclometalating ligand and use them in LECs. In particular, the device within di[4-fluoro-4'-pyrazolyl-(1,1'-biphenyl)-2-carbonitrile]-4,4'-di-tert-butyl-2,2'-bipyridyl iridium(III) hexafluorophosphate (DTBP) shows a remarkable photoluminescence quantum yield (PLQY) of 70%, and by adjusting the emissive-layer thickness, the maximal external quantum efficiency (EQE) reaches 22.15% at 532 nm under the thickness of 0.51 µm, showing the state-of-the-art value for the reported blue-green LECs.

Imidazolyl-Phenylcarbazole-Based Host Materials and Their Use for Co-host Designs in Phosphorescent OLEDs.

In recent years, owing to the demand for high-efficiency phosphorescent organic light-emitting devices (PhOLEDs), many studies have been conducted on the development of bipolar host materials. A series of imidazolyl-phenylcarbazole-based host materials, i. e., im-CzP, im-CzPCz, im-CzPtBu, and im-OCzP, were synthesized to obtain high-efficiency green and red-emitting PhOLEDs. With im-OCzP as the host, satisfactory peak efficiencies of 22.2 (77.0 cd A-1 and 93.1 lm W-1 ) and 14.1 % (9.0 cd A-1 and 10.1 lm W-1 ) could be obtained, respectively. To further improve the performance of the devices, an electron transport material, bis-4,6-(3,5-di-3-pyridylphenyl)-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-1 and 98.8 lm W-1 ) and 16.5 % (10.2 cd A-1 and 13.4 lm W-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.

Perovskite Light-Emitting Electrochemical Cells Employing Electron Injection/Transport Layers of Ionic Transition Metal Complexes.

Invited for the cover of this issue are Chin-Wei Lu, Zu-Po Yang, Hai-Ching Su, and co-workers at National Yang Ming Chiao Tung University and Providence University. The image depicts electron transport for light-emitting electrochemical cells. Read the full text of the article at 10.1002/chem.202103739.

Perovskite Light-Emitting Electrochemical Cells Employing Electron Injection/Transport Layers of Ionic Transition Metal Complexes.

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.

Dicyano-Imidazole: A Facile Generation of Pure Blue TADF Materials for OLEDs.

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.

Combinational Approach To Realize Highly Efficient Light-Emitting Electrochemical Cells.

Light-emitting electrochemical cells (LECs) show high technical potential for display and lighting utilizations owing to the superior properties of solution processability, low operation voltage, and employing inert cathodes. For maximizing the device efficiency, three approaches including development of efficient emissive materials, optimizing the carrier balance, and maximizing the light extraction have been reported. However, most reported works focused on only one of the three optimization approaches. In this work, a combinational approach is demonstrated to optimize the device efficiency of LECs. A sophisticatedly designed yellow complex exhibiting a superior steric hindrance and a good carrier balance is proposed as the emissive material of light-emitting electrochemical cells and thus the external quantum efficiency (EQE) is up to 13.6%. With an improved carrier balance and reduced self-quenching by employing the host-guest strategy, the device EQE can be enhanced to 16.9%. Finally, a diffusive layer embedded between the glass substrate and the indium-tin-oxide layer is utilized to scatter the light trapped in the layered device structure, and consequently, a high EQE of 23.7% can be obtained. Such an EQE is impressive and consequently proves that the proposed combinational approach including adopting efficient emissive materials, optimizing the carrier balance, and maximizing the light extraction is effective in realizing highly efficient LECs.

Hybrid White-Light-Emitting Electrochemical Cells Based on a Blue Cationic Iridium(III) Complex and Red Quantum Dots.

Solid-state white light-emitting electrochemical cells (LECs) show promising advantages of simple solution fabrication processes, low operation voltage, and compatibility with air-stable cathode metals, which are required for lighting applications. To date, white LECs based on ionic transition metal complexes (iTMCs) have shown higher device efficiencies than white LECs employing other types of materials. However, lower emission efficiencies of red iTMCs limit further improvement in device performance. As an alternative, efficient red CdZnSeS/ZnS core/shell quantum dots were integrated with a blue iTMC to form a hybrid white LEC in this work. By achieving good carrier balance in an appropriate device architecture, a peak external quantum efficiency and power efficiency of 11.2 % and 15.1 lm W-1, respectively, were reached. Such device efficiency is indeed higher than those of the reported white LECs based on host-guest iTMCs. Time- and voltage-dependent electroluminescence (EL) characteristics of the hybrid white LECs were studied by means of the temporal evolution of the emission-zone position extracted by fitting the simulated and measured EL spectra. The working principle of the hybrid white LECs was clarified, and the high device efficiency makes potential new white-emitting devices suitable for solid-state lighting technology possible.

Efficient and Saturated Red Light-Emitting Electrochemical Cells Based on Cationic Iridium(III) Complexes with EQE up to 9.4 .

Solid-state light-emitting electrochemical cells (LECs) have several advantages, such as low-voltage operation, compatibility with inert metal electrodes, large-area flexible substrates, and simple solution-processable device architectures. However, most of the studies on saturated red LECs show low or moderate device efficiencies (external quantum efficiency (EQE) <3.3 %). In this work, we demonstrate a series of five red-emitting cationic iridium complexes (RED1--RED5) with 2,2'-biquinoline ligands and test their electroluminescence (EL) characteristics in LECs. The Commission Internationale de l'Eclairage (CIE) 1931 coordinates for the LECs based on these complexes are all beyond the National Television System Committee (NTSC) red standard point (0.67, 0.33). The maximal EQE of the neat-film RED1-based LECs reaches 7.4 %. The reddest complex, RED3, is doped in the blue-emitting host complex, BG, to fabricate host-guest LECs. The maximal EQE of the host-guest LECs (1 wt % complex RED3) reaches 9.4 %, which is among the highest reported for the saturated red LECs.