Multiple resonance thermally activated delayed fluorescence (MR-TADF) molecule with a fused, planar architecture tends to aggregate at high doping ratios, resulting in broad full width at half maximum (FWHM), redshifting electroluminescence peaks, and low device efficiency. Herein, we propose a mono-substituted design strategy by introducing spiro-9,9'-bifluorene (SBF) units with different substituted sites into the MR-TADF system for the first time. As a classic steric group, SBF can hinder interchromophore interactions, leading to high device efficiency (32.2-35.9%) and narrow-band emission (~27 nm). Particularly, the shield-like molecule, SF1BN, seldom exhibits a broadened FWHM as the doping ratio rises, which differs from the C3-substituted isomer and unhindered parent emitter. These results manifest an effective method for constructing highly efficient MR-TADF emitters through a spiro strategy and elucidate the feasibility for steric modulation of spiro structure in π-framework.

Steric Modulation of Spiro Structure for Highly Efficient Multiple Resonance Emitters.

Afterglow materials are attracting widespread attention owing to their distinctive and long-lived optical emission properties which create exciting opportunities in various fields. Recent research has led to the discovery of many new afterglow materials featuring high photoluminescence quantum yields (PLQY) and lifetimes of up to several hours under ambient conditions. Afterglow materials are typically categorized according to their luminescence mechanism, such as long-persistent luminescence (LPL), room temperature phosphorescence (RTP), or thermally activated delayed fluorescence (TADF). Through rational design and novel synthetic strategies to modulate spin-orbit coupling (SOC) and populate triplet exciton states (T1), luminophores with long lifetimes and bright afterglow characteristics can be realized. Initial research towards afterglow materials focused mainly on pure inorganic materials, many of which possessed inherent disadvantages such as metal toxicity or low energy emissions. In recent years, organic-inorganic hybrid afterglow materials (OIHAMs) have been developed with high PLQY and long lifetimes. These hybrid materials exploit the tunable structure and easy processing of organic molecules, as well as enhanced SOC and intersystem crossing (ISC) processes involving heavy atom dopants, to achieve excellent afterglow performance. In this review, we begin by briefly discussing the structure and composition of inorganic and organic-inorganic hybrid afterglow materials, including strategies for regulating their lifetime, PLQY and luminescence wavelength. The specific advantages of organic-inorganic hybrid afterglow materials, including low manufacturing costs, diverse molecular/electronic structures, tunable structures and optical properties, and compatibility with a variety of substrates, are emphasized. Subsequently, we discuss in detail the fundamental mechanisms used by afterglow materials, their classification, design principles, and end applications (including sensing, anticounterfeiting, and photoelectric devices, among others). Finally, existing challenges and promising future directions are discussed, laying a platform for the design of afterglow materials for specific applications.

Recent advances in the design of afterglow materials: mechanisms, structural regulation strategies and applications.

ConspectusThe development of cutting-edge optoelectronic devices is rapidly changing science and technology. The organic light-emitting diodes (OLEDs), as one of the most applicable techniques of o...

Spiro Compounds for Organic Light-Emitting Diodes

We report three deep blue multiple resonant TADF emitters, m-ν-DABNA, 4F-ν-DABNA, and 4F-m-ν-DABNA by incorporating methyl groups and fluorine atoms in diboron based ν-DABNA core. The introduction of methyl groups at para positions to the boron atoms and fluorine atoms at ortho positions to the nitrogen atoms resulted in bandgap enhancement by electron donating and electron withdawing effects. All three emitters exhibit pure blue emissions with high photoluminescence quantum yield around ∼ 90%, small ΔEST (≤0.07 eV) values, and fast reverse intersystem crossing rate (kRISC). Fabricated OLEDs with these emitters show excellent external quantum efficiency over 33%. Among three materials, 4F-ν-DABNA and 4F-m-ν-DABNA exhibit the CIE y coordinate of 0.08 and 0.06, respectively. Our current material design approach guides a path for the development of deep blue TADF emitters for highly efficient narrowband OLEDs. 

Deep blue diboron embedded multi-resonance thermally activated delayed fluorescence emitters for narrowband organic light emitting diodes

The hyperfluorescence (HF) system has drawn great attention in display technology. However, the energy loss mechanism by low reverse intersystem crossing rate (kRISC) and the Dexter energy transfer (DET) channel is still challenging. Here, we demonstrate that this can be mitigated by the quadrupolar donor-acceptor-donor (D-A-D) type of thermally activated delayed fluorescence (TADF) sensitizer materials, DBA-DmICz and DBA-DTMCz. Further, the HF device with DBA-DTMCz and ν-DABNA exhibited 43.9% of high maximum external quantum efficiency (EQEmax) with the Commission Internationale de l'Éclairage coordinates of (0.12, 0.16). The efficiency values recorded for the device are among the highest reported for HF devices. Such high efficiency is assisted by hindered DET process through i) high kRISC, and ii) shielded lowest unoccupied molecular orbital with the presence of two donors in D-A-D type of skeleton. Our current study provides an effective way of designing TADF sensitizer for future HF technology. 

/pdf/efficient-pure-blue-hyperfluorescence-devices-utilizing-15su5gva.pdf

Efficient pure blue hyperfluorescence devices utilizing quadrupolar donor-acceptor-donor type of thermally activated delayed fluorescence sensitizers

Endowing imidazole derivatives with thermally activated delayed fluorescence and aggregation-induced emission properties for highly efficient non-doped organic light-emitting diodes

Herein disclosed is the first example of diarylation/annulation of benzoic acids via an iridium catalyst system. This protocol provides a step-economic and highly efficient pathway to 1-aryl, 1,3-diaryl, 1,7-diaryl and 1,3,7-triaryl spirobifluorenes from readily available starting materials. The applications of multi-aryl spirobifluorenes as pure hydrocarbon (PHC) hosts for red, green, and blue (RGB) phosphorescent organic light-emitting diodes (PhOLEDs) were explored. Due to high triplet energies, 1,3-diaryl spirobifluorenes exhibit the potential as the host material of blue PhOLEDs. 1,7-Diaryl spirobifluorene can serve as the host of green PhOLEDs. 1,3,7-Triaryl spirobifluorene is a high-performance host for red PhOLEDs, which exhibits a high external quantum efficiency (EQE) up to 27.3 %. This work not only exemplifies the great potential of multi-aryl spirobifluorenes as PHC hosts, but also offers a new approach for the synthesis of these PHC hosts.

Iridium(III)-Catalyzed Diarylation/Annulation of Benzoic Acids: Facile Access to Multi-Aryl Spirobifluorenes as Pure Hydrocarbon Hosts for High-Performance OLEDs

Here, we report a novel methyl-shield strategy to design ideal TADF hosts for the improvement of the performance of TSF-OLEDs. The methyl group on the xanthone acceptor acts like a shield to protect the luminance center from close intermolecular hydrogen bonding with adjacent molecules, thus alleviating exciton quenching, and meanwhile the small size of the methyl group almost does not disturb the π–π stacking between acceptors, thus maintaining fast electron-transport pathways. dMeACRXTO having two methyl shields is exploited as the host to achieve a record-high EQE of 32.3%, which represents the first report of an EQE above 30% in TSF-OLEDs.

A methyl-shield strategy enables efficient blue thermally activated delayed fluorescence hosts for high-performance fluorescent OLEDs.

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Endowing imidazole derivatives with thermally activated delayed fluorescence and aggregation-induced emission properties for highly efficient non-doped organic light-emitting diodes

Iridium(III)-Catalyzed Diarylation/Annulation of Benzoic Acids: Facile Access to Multi-Aryl Spirobifluorenes as Pure Hydrocarbon Hosts for High-Performance OLEDs

A methyl-shield strategy enables efficient blue thermally activated delayed fluorescence hosts for high-performance fluorescent OLEDs.