Phosphorescent near‐infrared (NIR) organic light‐emitting devices (OLEDs) have drawn increasing attention for their promising applications in the fields such as photodynamic therapy and night‐vision readable displays. Here, three simple phosphorescent Pt(II) complexes are synthesized, and their intermolecular interactions are investigated in crystals and neat films by X‐ray single crystal diffraction and grazing‐incidence wide‐angle X‐ray scattering, respectively. The photophysical properties, molecular aggregation (including Pt–Pt interaction), molecular packing orientation, and electron transport ability are all influenced by the strong intermolecular hydrogen bonds. Consequently, the nondoped OLEDs based on tBu‐Pt and F‐Pt show electroluminescent emissions in NIR region with the highest external quantum efficiencies of 13.9% and 16.7%, respectively.

A cyclometalating ligand containing a 9-phenyl-9-phosphafluorene oxide (PhFlPO) moiety has been synthesized and used to construct asymmetric tris-heteroleptic cyclometalating Ir III complexes in combination with other ppy-type (Hppy = 2phenylpyridine) ligands containing a functional group with a different charge carrier injection/transporting character. Their photophysical properties, electrochemical behaviors, and electroluminescent (EL) performances have been characterized in detail. Timedependent density functional theory (TD-DFT) and natural transition orbital (NTO) calculation were carried out to gain insight into the photophysical properties of these complexes. The NTO results show that the characters of the lowest triplet excited states (T 1 ) can be delicately manipulated through the combination of different cyclometalating ligands. In addition, the strong electron injection/transporting (EI/ET) ability associated with the PhFlPO moiety can confer EI/ET properties to the asymmetric tris-heteroleptic cyclometalating Ir III complexes. Consequently, the solution-processed organic lightemitting diodes/devices (OLEDs) based on these asymmetric tris-heteroleptic Ir III phosphorescent complexes can exhibit outstanding electroluminescent (EL) performances with the maximum external quantum efficiency (η ext ) of 19.3%, current efficiency (η L ) of 82.5 cd A −1 , and power efficiency (η P ) of 57.3 lm W −1 for the yellow-emitting device. These results show the great potential of a PhFlPO moiety in developing phosphorescent emitters and functional materials with excellent EI/ET properties.

Organic light‐emitting diodes (OLEDs) are one of the most promising technologies for future displays and lighting. Compared with the blue and green OLEDs that have achieved very high efficiencies by using phosphorescent Ir(III) complexes, the red OLEDs still show relatively low efficiencies because of the lack of high‐performance red‐emitting Ir(III) complexes. Here, three highly efficient asymmetric red‐emitting Ir(III) complexes with two different cyclometalating ligands made by incorporating only one electron‐deficient triarylboron group into the nitrogen heterocyclic ring are reported. These complexes show enhanced photoluminescence quantum yields up to 0.96 and improved electron transporting capacity. In addition, the asymmetric structure can help to improve the solubility of Ir(III) complexes, which is crucial for fabricating OLEDs using the solution method. The photoluminescent and oxidation–reduction properties of these Ir(III) complexes are investigated both experimentally and theoretically. Most importantly, a solution‐processed red OLED achieves extremely high external quantum efficiency, current efficiency, and power efficiency with values of 28.5%, 54.4 cd A−1, and 50.1 lm W−1, respectively, with very low efficiency roll‐off. Additionally, the related device has a significantly extended operating lifetime compared with the reference device. These results demonstrate that the asymmetric diarylboron‐based Ir(III) complexes have great potential for fabricating high‐performance red OLEDs.

A new mechanism, namely radiative transition switch (RTS), has been proposed for aggregation-induced emission, which is of importance for developing highly efficient AIE-active emitters.

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