A modular approach to efficient thermally activated delayed fluorescence from metal-perturbed intraligand charge-transfer excited state of Au(Ⅰ)complexes

The efficient harvesting of triplet excitons is crucial to the realization of high-performance organic light-emitting diodes(OLEDs).Herein,we show that coordination of donor-acceptor(D-A)type molecules to a metal atom in a monodentate fashion can lead to thermally activated delayed fluorescence(TADF)emissions with wide color tunability only through varying the noncoordinating acceptor moiety.A panel of TADF gold(Ⅰ)complexes with emission maxima(λmax)of 545–645 nm from metal perturbed intraligand charge-transfer(MPICT)excited states have been developed.Synergetic effects of heavy atom-induced spin-orbit coupling(SOC),steric-induced donor-acceptor twisting and suppressed intramolecular motions lead to high emission efficiencies of 65%-85%in doped films with delayed fluorescence lifetime of as short as 2.0μs.Transient absorption spectroscopic studies on selected complexes determined the kISCto be 6.5×10^(9)s^(-1).Theoretical calculations confirmed the participation of minor d orbital into the lowest excited state,which led to an SOC value of 5.19 cm^(-1)between the lowest-lying singlet and triplet excited states.The yellow to deep red solution-processed OLEDs based on the new gold(Ⅰ)complexes incorporated with various D-A ligands demonstrated promising performances.This study validates a modular design for TADF metal complexes,which will broaden the choices of metal centers and allow for facile color tuning via simple ligand synthesis.

Thermally activated delayed fluorescence carbazole-triazine dendrimer with bulky substituents

Carbazole-triazine dendrimers with a bulky terminal substituent were synthesized,and the thermally activated delayed fluorescence(TADF)property was investigated.Compared to unsubstituted carbazole dendrimers,dendrimers with bulky terminal substituents showed comparable to better photoluminescence quantum yields(PLQY)in neat films.Phenylfluorene(PF)-substituted dendrimers showed the highest PLQY of 81%,a smallΔEst of 0.06 eV,and the fastest reverse intersystem crossing(RISC)rate of∼1×10^(5 )s^(−1) compared to other dendrimers.Phosphorescence measurements of dendrimers and dendrons(fragments)indicate that the close proximity of the triplet energy of phenylfluorene-substituted carbazole dendrons(^(3)LE)to that of phenylfluorene-substituted dendrimers(^(1)CT,^(3)CT)contributes to RISC promotion and improves TADF efficiency.Terminal modification fine-tunes the energy level and suppresses intermolecular interactions,and this study provides a guideline for designing efficient solution-processable and non-doped TADF materials.

Achieving high-performance phosphorescent organic light-emitting diodes using thermally activated delayed fluorescence with low concentration

We fabricated phosphorescent organic light-emitting diodes(Ph OLEDs) using thermally activated delayed fluorescence(TADF) material 10,10’-(4,4’-sulfonylbis(4,1-phenylene)) bis(9,9-dimethyl-9,10-dihydroacridine)(DMAC-DPS) with low concentration, which showed better performance compared with 1,3-bis(carbazole-9-yl) benzene(m CP) based devices. When the concentration of DMAC-DPS was 1 wt%, the driving voltage of the device was only 3.3 V at 1 000 cd/m2, and the efficiency and lifetime of the device were effectively improved compared with those of m CP based devices. The result indicated that DMAC-DPS could effectively improve the performance of phosphorescent devices. We believe that the better device performance can be attributed to the optimization of the energy transfer process in the emitter layer and lifetime of triplet excitons by DMAC-DPS. The study may provide a simple and effective strategy to achieve high-performance OLEDs.

Improved stability of blue TADF organic electroluminescent diodes via OXD-7 based mixed host

Thermally activated delayed fluorescence(TADF)organic light-emitting diodes(OLEDs)have been demonstrated in applications such as displays and solid-state lightings.However,weak stability and ineffi-cient emission of blue TADF OLEDs are two key bottlenecks limiting the development of solution processable displays and white light sources.This work presents a solution-processed OLED using a blue-emitting TADF small molecule bis[4-(9,9-dimethyl-9,10-dihydroacridine)phenyl]sulfone(DMAC-DPS)as an emitter.We comparatively investigated the effects of single host poly(Nvinylcarbazole)(PVK)and a co-host of 60%PVK and 30%2,2′-(1,3-phenylene)-bis[5-(4-tert-butylphenyl)-1,3,4-oxadiazole](OXD-7)on the device performance(the last 10%is emitter DMAC-DPS).The co-host device shows lower turn-on voltage,similar maximum luminance,and much slower external quantum efficiency(EQE)rolloff.In other words,device stability improved by doping OXD-7 into PVK,and the device impedance simultaneously and significantly reduced from 8.6103 to 4.2103 W at 1000 Hz.Finally,the electroluminescent stability of the co-host device was significantly enhanced by adjusting the annealing temperature.

Carbon Dots-in-Zeolite via In-Situ Solvent-Free Thermal Crystallization:Achieving High-Efficiency and Ultralong Afterglow Dual Emission

Organic afterglow materials are highly desirable for optoelectronic applications,but they usually suffer from complex preparation process,low quantum efficiency,and short lifetime due to the ultrafast deactivation of the highly active excited states involved.Here,we succeeded in achieving solventfree thermal syntheses of high-efficiency afterglow CDs@zeolite composite materials by simply grinding the solid raw materials of zeolite and precursor CDs at room temperature,followed by thermal crystallization.This method afforded maximum embedding of CDs into growing zeolite crystals,as well as strong host–guest interaction to surpass the nonradiative transition of CDs,thus producing composite materials with ultralong dual emission of thermally activated delayed fluorescence and room temperature phosphorescence with a record high lifetime of 1.7 and 2.1 s,respectively,and the quantum yield of 90.7%.Furthermore,in a preliminary experiment,we applied the composite materials in alternatingcurrent light-emitting diode supplementary lighting,which exhibited a promising potential in optoelectronic applications.

Copper(Ⅰ) complexes with planar chirality realize efficient circularly polarized electroluminescence

Chiral organometallic emitters hold great promise in potential and practical applications of circularly polarized organic lightemitting diodes(CP-OLEDs).However,developing luminescent earth-abundant organometallic complexes concurrently exhibiting circularly polarized luminescence(CPL)and high quantum efficiency remains a formidable challenge.In this study,we introduced a typical planar chiral skeleton of a[2.2]paracyclophane moiety into earth-abundant copper(I)complexes with the goal of realizing efficient CPL and thermally activated delayed fluorescence(TADF)simultaneously.Two pairs of proof-of-theconcept copper(I)enantiomers,R_(p)/S_(p)-MAC^(*)-Cu-CzP and R_(p)/S_(p)-MAC^(*)-Cu-CNCzP,were developed using planar chiral[2.2]paracyclophane-based donor ligands in a carbene-metal-amide(CMA)motif.Both panels of enantiomers not only exhibited significant mirror-image CPL signals but also displayed distinct TADF nature with fast reverse intersystem crossing rates of up to 10^(8)s^(-1).The resultant OLEDs based on the MAC^(*)-Cu-Cz P enantiomers manifested efficient circularly polarized electroluminescence with excellent external quantum efficiencies of 13.2%and ultraslow efficiency roll-off(7.7%at 10,000 nits).This article not only demonstrates one of the best performances for CP-OLEDs based on earth-abundant organometallic complexes but also represents the first example of CP-OLEDs from CMA complexes to our knowledge.