In Situ Solid‐State Generation of (BN)2‐Pyrenes and Electroluminescent Devices

New BN‐heterocyclic compounds have been found to undergo double arene photoelimination, forming rare yellow fluorescent BN‐pyrenes that contain two B? N units. Most significant is the discovery that the double arene elimination can also be driven by excitons generated electrically within electroluminescent (EL) devices, enabling the in situ solid‐state conversion of BN‐heterocycles to BN‐pyrenes and the use of BN‐pyrenes as emitters for EL devices. The in situ exciton‐driven elimination (EDE) phenomenon has also been observed for other BN‐heterocycles.     

Peripherally Heavy-Atom-Decorated Strategy Towards High-Performance Pure Green Electroluminescence with External Quantum Efficiency over 40 %

Heavy-atom integration into thermally activated delayed fluorescence (TADF) molecule could significantly promote the reverse intersystem crossing (RISC) process. However, simultaneously achieving high efficiency, small roll-off, narrowband emission and good operational lifetime remains a big challenge for the corresponding organic light-emitting diodes (OLEDs). Herein, we report a pure green multi-resonance TADF molecule BN-STO by introducing a peripheral heavy atom selenium onto the parent BN-Cz molecule. The organic light-emitting diode device based on BN-STO exhibited state-of-the-art performance with a maximum external quantum efficiency (EQE) of 40.1 %, power efficiency (PE) of 176.9 lm W⁻¹, well-suppressed efficiency roll-off and pure green gamut. This work reveals a feasible strategy to reach a balance between fast RISC process and narrow full width at half maximum (FWHM) of MR-TADF by heavy atom effect.     

Regulation of Multiple Resonance Delayed Fluorescence via Through-Space Charge Transfer Excited State towards High-Efficiency and Stable Narrowband Electroluminescence

B- and N-embedded multiple resonance (MR) type thermally activated delayed fluorescence (TADF) emitters usually suffer from slow reverse intersystem crossing (RISC) process and aggregation-caused emission quenching. Here, we report the design of a sandwich structure by placing the B−N MR core between two electron-donating moieties, inducing through-space charge transfer (TSCT) states. The proper adjusting of the energy levels brings about a 10-fold higher RISC rate in comparison with the parent B−N molecule. In the meantime, a high photoluminescence quantum yield of 91 % and a good color purity were maintained. Organic light-emitting diodes based on the new MR emitter achieved a maximum external quantum efficiency of 31.7 % and small roll-offs at high brightness. High device efficiencies were also obtained for a wide range of doping concentrations of up to 20 wt % thanks to the steric shielding of the B−N core. A good operational stability with LT₉₅ of 85.2 h has also been revealed. The dual steric and electronic effects resulting from the introduction of a TSCT state offer an effective molecular design to address the critical challenges of MR-TADF emitters.     

Optimizing Optoelectronic Properties of Pyrimidine‐Based TADF Emitters by Changing the Substituent for Organic Light‐Emitting Diodes with External Quantum Efficiency Close to 25 % and Slow Efficiency Roll‐Off

A series of green butterfly‐shaped thermally activated delayed fluorescence (TADF) emitters, namely PXZPM , PXZMePM , and PXZPhPM , are developed by integrating an electron‐donor (D) phenoxazine unit and electron‐acceptor (A) 2‐substituted pyrimidine moiety into one molecule via a phenyl‐bridge π linkage to form a D –π–A–π–D configuration. Changing the substituent at pyrimidine unit in these emitters can finely tune their emissive characteristics, thermal properties, and energy gaps between the singlet and triplet states while maintaining frontier molecular orbital levels, and thereby optimizing their optoelectronic properties. Employing these TADF emitters results in a green fluorescent organic light‐emitting diode (OLED) that exhibits a peak forward‐viewing external quantum efficiency (EQE) close to 25 % and a slow efficiency roll‐off characteristic at high luminance.     

Simple sulfone-bridged heterohelicene structure realizes ultraviolet narrowband thermally activated delayed fluorescence,circularly polarized luminescence,and room temperature phosphorescence

Due to narrowband emission and high quantum efficiencies, polycyclic aromatic heterocycles with multi-resonance thermally activated delayed fluorescence (MR-TADF) properties have recently gained considerable attention in the organic optoelectronic field. Albeit their great promise in the full visible region covering from blue to red, MR-TADF emitters with ultraviolet emission have been rarely reported. Through locking the two ortho-positions of a triphenylamine core by sulfone groups, a simple polycyclic aromatic heterocycle, BTPT, was facilely constructed, exhibiting 368 nm ultraviolet emission with a narrow full width at half maximum (FWHM) of 33 nm. Its neat film exhibited distinct TADF property with a main emission peak at 388 nm. Noteworthily, the enantiomeric crystals of BTPT not only demonstrated significant circularly polarized luminescence (CPL) with large luminescence dissymmetry factor in the 10^?3 order but also displayed obvious room temperature phosphorescence (RTP). The relationship between this innovative helical unit and unique photophysical properties, including ultraviolet MRTADF, CPL, and RTP, was reasonably revealed.

     

Synthesis and electronic absorption and fluorescence of 2-arylbenzothiazole derivatives

A series of new 2-arylbenzothiazoles have been prepared in high yields by Jacobson's cyclization condensation of 2-aminobenzenethiol with benzoyl chloride or benzaldehyde derivatives under three different routes. These compounds have been fully characterized by EA, IR, NMR and MS. The electronic absorption and fluorescence of these compounds have been systematically investigated for the first time. The relationships between their photophysical properties and structures have been discussed. The alteration of absorption and emission wavelengths can be elucidated by Hammett's substituent constants.     

Designing a Perylene Diimide/Fullerene Hybrid as Effective Electron Transporting Material in Inverted Perovskite Solar Cells with Enhanced Efficiency and Stability

Electron transport materials (ETM) play an important role in the improvement of efficiency and stability for inverted perovskite solar cells (PSCs). This work reports an efficient ETM, named PDI‐C₆₀, by the combination of perylene diimide (PDI) and fullerene. Compared to the traditional PCBM, this strategy endows PDI‐C₆₀ with slightly shallower energy level and higher electron mobility. As a result, the device based on PDI‐C₆₀ as electron transport layer (ETL) achieves high power conversion efficiency (PCE) of 18.6 %, which is significantly higher than those of the control devices of PCBM (16.6 %) and PDI (13.8 %). The high PCE of the PDI‐C₆₀‐based device can be attributed to the more matching energy level with the perovskite, more efficient charge extraction, transport, and reduced recombination rate. To the best of our knowledge, the PCE of 18.6 % is the highest value in the PSCs using PDI derivatives as ETLs. Moreover, the device with PDI‐C₆₀ as ETL exhibits better device stability due to the stronger hydrophobic properties of PDI‐C₆₀. The strategy using the PDI/fullerene hybrid provides insights for future molecular design of the efficient ETM for the inverted PSCs.     

Efficient phosphorescent polymer light-emitting diodes by suppressing triplet energy back transfer

Phosphorescent polymer light-emitting diodes (PhPLEDs) are promising devices in flat panel displays and solid state lighting sources since they can combine the advantages of the high efficiency of electrophosphorescence and low-cost, large-scale manufacture by using a solution process. However, their efficiencies are generally much lower than those of small-molecule-based devices fabricated by using a thermal deposition approach. One of the major reasons for their low efficiency is that energy is lost by back transfer to a polymer host. This tutorial review gives a brief introduction to the fundamentals of PhPLEDs, and then highlights recent progress in the main approaches to suppress triplet energy back transfer from the phosphor to the polymer host towards realizing highly efficient PhPLEDs. The suppressing mechanisms are discussed, and the achievement of high device efficiencies are demonstrated. Emphasis is placed on the relationships between molecular structure, the extent of suppressing triplet energy back transfer, and device performance.     

Iridium phosphors with peripheral triphenylamine encapsulation: highly efficient solution-processed red electrophosphorescence

The peripheral triphenylamine-encapsulated red-emitting iridium(III) complexes have been designed and synthesized. External quantum efficiency over 15% has been realized in single-layer polymer light-emitting diodes, which is the highest ever reported for solution-processed red phosphorescence.