High Maximum External Quantum Efficiency Research Articles

Strongly Luminescent Tetradentate Palladium(II)‐TADF Emitters. Blue TADF And TADF‐Sensitized OLEDs with External Quantum Efficiencies Over 23%

AbstractDue to the low‐lying Pd(4d)‐orbitals, luminescent palladium(II) complexes usually show 3IL phosphorescence (IL = intraligand) with excited state lifetimes in the range of hundreds of microseconds, which limits their application in blue organic light‐emitting diodes (OLEDs). Here, a molecular design strategy for the development of strongly luminescent Pd(II)‐based thermally activated delayed fluorescence (TADF) emitters with fast radiative decay rate constants and reverse intersystem crossing rate (kRISC) constants is presented. The synthesized tetradentate [Pd(N*C*C^N)] TADF emitters show sky‐blue to yellow (λmax = 484–565 nm) emission with excited state lifetimes in the range of 0.9−8.7 µs and high photoluminescence quantum yield of up to 77% in CH2Cl2 solution. In 5 wt.% 2,8‐bis(diphenylphosphoryl)dibenzo[b,d]furan (PPF) thin films, these [Pd(N*C*C^N)] TADF complexes display blue to sky‐blue (476−496 nm) emission with quantum yields close to unity. Variable‐temperature emission lifetime measurements, femtosecond time‐resolved spectroscopy, and density functional theory (DFT) and time‐dependent DFT (TDDFT) calculations together reveal ultrafast kRISC rate constants of these [Pd(N*C*C^N)] TADF emitters. Using these Pd(II)‐TADF emitters as dopants, sky‐blue TADF and blue TADF‐sensitized OLEDs with small efficiency roll‐offs achieved high maximum external quantum efficiencies (EQEs) of 24.8% and 23.1%, respectively.

Dielectric Regulation for Efficient Top-Emission Perovskite Light-Emitting Diodes with Suppressed Efficiency Roll-off.

Perovskite light-emitting diodes (PeLEDs) have shown incalculable application potential in the fields of next-generation displays and light communication owing to the rapidly increased external quantum efficiencies (EQEs). However, most PeLEDs obtain a maximum EQE at small current density (J) region and suffer from severe efficiency roll-off in different extents. Herein, it is demonstrated that the dopant with large dipole moment like KBF4 facilitates the effective dielectric regulation of perovskite emissive layer. The increased dielectric constant lowers the exciton binding energy and suppresses the Auger recombination of the 2D/3D segregated perovskite structure, which improves the photoluminescence quantum yield remarkably at an excitation intensity up to 103mWcm-2. Accordingly, the top-emission PeLED that delivers a high maximum EQE above 20% is fabricated and can retain EQE>10% at an extremely high J of 708mAcm-2. These results represent one of the most efficient top-emission PeLEDs with ultra-low efficiency roll-off, which provide a viable methodology for tuning the dielectric response of perovskite films for improved high radiance performance of perovskite electroluminescence devices.

A Breakthrough in Solution-Processed Ultra-Deep-Blue HLCT OLEDs: A Record External Quantum Efficiency Exceeding 10% Based on Novel V-Shaped Emitters.

It is always a great challenge to achieve high-efficiency solution-processed ultra-deep-blue organic light-emitting diodes (OLEDs) with the Commission Internationale de l'Eclairage (CIE) 1931 chromaticity coordinates matching the blue primary of Rec. International Telecommunication Union-Radiocommunication BT.2100, which specifies high dynamic range television image parameters. Inspired by hybrid local and charge transfer (HLCT) excited state emitters improving exciton utilization through high-lying reverse intersystem crossing, here, a series of high-performance blue emitters by a V-shaped symmetric donor (D)-π-acceptor (A)-π-D design strategy are developed. Here, the large torsions and unstable bonds of D-A structures can be improved through π bridges, and also the conjugation length and donor groups can be easily adjusted. The obtained emitters merit excellent photophysical and electrochemical properties, thermal stability, solution processibility, and HLCT excited state excellence. Results suggest that the OLEDs based on the obtained blue emitters all achieve high maximum external quantum efficiency (EQEmax ) of more than 8% with very low efficiency roll-off. In particular, the device based on 4',5'-bis(4-(9H-carbazol-9-yl)phenyl)spiro[fluorene-9,2'-imidazole] exhibits a satisfactory ultra-deep-blue emission (CIEx , y = 0.1579, 0.0387) and a record-high EQEmax (10.40%) among solution-processed HLCT OLEDs, which is very close to the record EQEmax of devices by vacuum vapor deposition technology.

Efficient and Bright Organic Radical Light-Emitting Diodes with Low Efficiency Roll-Off.

Organic radicals have been of interest due to their potential to replace nonradical-based organic emitters, especially for deep red/near-infrared (NIR) electroluminescence (EL), based on the spin-allowed doublet fluorescence. However, the performance of the radical-based EL devices is limited by low carrier mobility that causes a large efficiency roll-off at high current densities. Here, we report highly efficient and bright doublet EL devices by combining a thermally activated delayed fluorescence (TADF) host that supports both electron and hole transport and a tris(2,4,6-trichlorophenyl)methyl-based radical emitter. Steady-state and transient photophysical studies reveal the optical signatures of doublet luminescence mechanisms arising from both host and guest photoexcitation. The host system presented here allows balanced hole and electron currents, and we report a high maximum external quantum efficiency (EQE) of 17.4% at 707nm peak emission with substantially improved efficiency roll-off: over 70% of the maximum EQE (12.2%) is recorded at 10mA cm-2 , and even at 100mA cm-2 , nearly 50% of the maximum EQE (8.4%) is maintained. Charge recombination is primarily at the radical guest sites, but there is evidence from magneto-EL for host recombination and later energy transfer to the radical guest. We consider this is an important step to the practical application of organic radicals to NIR light-emitting devices. This article is protected by copyright. All rights reserved.

B-N/B-O Contained Heterocycles as Fusion Locker in Multi-Resonance Frameworks towards Highly-efficient and Stable Ultra-Narrowband Emission.

Fusing condensed aromatics into multi-resonance (MR) frameworks has been an exquisite strategy to modulate the optoelectronic properties, which, however, always sacrifices the small full width at half maxima (FWHM). Herein, we strategically embed B-N/B-O contained heterocycles as fusion locker into classical MR prototypes, which could enlarge the π-extension and alleviate the steric repulsion for an enhanced planar skeleton to suppress the high-frequency stretching/ scissoring vibrations for ultra-narrowband emissions. Sky-blue emitters with extremely small FWHMs of 17-18 nm are thereafter obtained for the targeted emitters, decreased by (1.4-1.9)-fold compared with the prototypes. Benefiting from their high photoluminescence quantum yields of >90 % and fast radiative decay rates of >108 s-1 , one of those emitters shows a high maximum external quantum efficiency of 31.9 % in sensitized devices, which remains 25.8 % at a practical luminance of 1,000 cd m-2 with a small FWHM of merely 19 nm. Notably a long operation half-lifetime of 1,278 h is also recorded for the same device, representing one of the longest lifetimes among sky-blue devices based on MR emitters.

B−N/B−O Contained Heterocycles as Fusion Locker in Multi‐Resonance Frameworks towards Highly‐efficient and Stable Ultra‐Narrowband Emission

AbstractFusing condensed aromatics into multi‐resonance (MR) frameworks has been an exquisite strategy to modulate the optoelectronic properties, which, however, always sacrifices the small full width at half maxima (FWHM). Herein, we strategically embed B−N/B−O contained heterocycles as fusion locker into classical MR prototypes, which could enlarge the π‐extension and alleviate the steric repulsion for an enhanced planar skeleton to suppress the high‐frequency stretching/ scissoring vibrations for ultra‐narrowband emissions. Sky‐blue emitters with extremely small FWHMs of 17–18 nm are thereafter obtained for the targeted emitters, decreased by (1.4–1.9)‐fold compared with the prototypes. Benefiting from their high photoluminescence quantum yields of >90 % and fast radiative decay rates of >108 s−1, one of those emitters shows a high maximum external quantum efficiency of 31.9 % in sensitized devices, which remains 25.8 % at a practical luminance of 1,000 cd m−2 with a small FWHM of merely 19 nm. Notably a long operation half‐lifetime of 1,278 h is also recorded for the same device, representing one of the longest lifetimes among sky‐blue devices based on MR emitters.

Engineering the Macrocyclic Donor Structures towards Deep-Blue Thermally Activated Delayed Fluorescence Emitters.

Deep-blue thermally activated delayed fluorescence (TADF) molecules present promising potential in organic light-emitting diodes (OLEDs), especially for display applications. Here, an efficient molecular engineering approach to modifying the donor or acceptor features of the D-π-A-configured TADF molecules for deep-blue emission is reported. By introducing oxygen and sulfone as a bridge unit onto the macrocyclic donor, two emitters, c-ON-MeTRZ and c-NS-MeTRZ, are synthesized and characterized, respectively. The reduced donor strength of c-ON-MeTRZ and c-NS-MeTRZ as compared to that of the model molecule c-NN-MeTRZ leads to blue-shifted emissions with high photoluminescence quantum yields (PLQYs) and retains TADF characters, while the new emitter c-NN-MePym with the most blue-shifted emission only exhibits a pure fluorescent nature because of the electron-accepting feature of pyrimidine that is insufficient for inducing the TADF property. In the presence of macrocyclic donors, these new emitters show high horizontal dipole ratios (Θ// = 85-89%), which are beneficial for improving the light out-coupling efficiency. Deep-blue TADF OLEDs incorporating c-ON-MeTRZ as an emitter doped in the mCPCN host achieves a high maximum external quantum efficiency (EQEmax) of 30.2% together with 1931 Commission Internationale de I'Eclairage (CIE) coordinates of (0.14, 0.13), while the counter device employing c-NS-MeTRZ as a dopant gives EQEmax of 15.4% and CIE coordinates of (0.14, 0.09). The EQEmax of c-ON-MeTRZ- and c-NS-MeTRZ-based devices can be significantly improved to 34.4 and 29.3%, respectively, with a polar host DPEPO, which stabilizes the charge transfer (CT) S1 state to give lower ΔEST for improving the reverse intersystem crossing process. The efficient TADF character, high PLQYs, and high anisotropic emission dipole ratios work together to render the superior electroluminescence (EL) efficiencies. Based on the detailed characterizations of physical properties, theoretical analyses, and comprehensive study on the corresponding devices, a clear structure-property-performance relationship has been successfully established to verify the effective molecular design strategy of modulating the macrocyclic donor characters for efficient deep-blue TADF emitters.

Modifications of Pyridine-3,5-dicarbonitrile Acceptor for Highly Efficient Green-to-Red Organic Light-Emitting Diodes.

The strategy of acceptor modification is a powerful technique for tuning the emission color of thermally activated delayed fluorescence (TADF) emitters. In this study, we have successfully designed and synthesized three TADF emitters with donor-acceptor (D-A) structures using a 4-(diphenylamino)-2,6-dimethylphenyl (TPAm) donor and various pyridine-3,5-dicarbonitrile (PC) acceptor units. As a result, three compounds named TPAmbPPC, TPAm2NPC, and TPAmCPPC exhibited greenish-yellow to orange-red emissions with high photoluminescent quantum yields (76-100%) in thin films. Remarkably, a greenish-yellow device based on TPAmbPPC and TPAm2NPC showed a high maximum external quantum efficiency (EQEmax) of 39.1 and 39.0%, respectively. Furthermore, benefiting from the suitable steric hindrance between the acceptor and donor, the nondoped organic light-emitting diodes (OLEDs) based on TPAmbPPC demonstrated an exceptional EQEmax of 21.6%, indicating its promising potential as an efficient emitter for the application of OLED applications. Furthermore, orange-red OLED devices based on TPAmCPPC exhibited a high EQEmax of 26.2%, a CE of 50.1 cd A-1, and a PE of 52.4 lm W-1.

Judicious Heteroatom Doping Produces High Performance Deep Blue/Near UV Multiresonant Thermally Activated Delayed Fluorescence OLEDs.

We present two multi-resonant thermally activated delayed fluorescence (MR-TADF) emitters and show how further borylation of a deep blue MR-TADF emitter, DIDOBNA-N, both blue shifts and narrows the emission producing a new near-UV MR-TADF emitter, MesB-DIDOBNA-N. DIDOBNA-N emits bright blue light (lPL = 444nm, FWHM = 64nm, FPL = 81%, td = 23 ms, 1.5 wt% in TSPO1). The deep blue organic light-emitting diode (OLED) based on this twisted MR-TADF compound shows a very high maximum external quantum efficiency (EQEmax) of 15.3% for a device with CIEy of 0.073. The fused planar MR-TADF emitter, MesB-DIDOBNA-N shows efficient and narrowband near UV emission (lPL = 402nm, FWHM = 19nm, FPL = 74.7%, td = 133 ms, 1.5 wt% in TSPO1). The best OLED with MesB-DIDOBNA-N, doped in a co-host, shows the highest efficiency reported for a near UV OLED at 16.2%. With a CIEy coordinate of 0.049, this device also shows the bluest EL reported for a MR-TADF OLED to date. This article is protected by copyright. All rights reserved.

Phenoxazine and phenothiazine embedded Multi-Resonance emitters for highly efficient Pure-Red OLEDs with improved color purity

Multi-resonance (MR) emitters based on boron-nitrogen doped polycyclic aromatic hydrocarbons are the cutting-edge light-emitting materials for organic light-emitting diodes (OLEDs) due to their high photoluminescence quantum yield and narrowband emission spectra. Among all the widely-reported MR molecules, emitters showing pure-red emission are the least developed. The difficulty in designing pure-red MR emitters lies in the limit of the weak charge transfer nature of the MR framework, as well as the large molecular weight which may bring difficulty in vacuum sublimation process. Herein, through introducing the strong electron donating phenoxazine and phenothiazine moiety into the double-boron-based MR molecular skeleton, two novel MR emitters namely PXZBNO and PTZBNO were designed and synthesized. These two emitters exhibited pure-red emission with emission maxima up to 627 nm, small full-width at half-maximum (FWHM) of 45 nm. Red OLEDs based on PTZBNO demonstrated very high maximum external quantum efficiency (EQEmax) of 34.5%, together with very small efficiency roll-off. Meanwhile, PXZBNO-based purity pure-red OLEDs exhibited high color purity with color coordinates of (0.69, 0.31), which is approaching BT. 2020 standard.

Discrete Mononuclear Platinum(II) Complexes Realize High-Performance Red Phosphorescent OLEDs with EQEs of up to 31.8% and Superb Device Stability.

Designing mononuclear platinum(II) complexes that do not rely on intermolecular aggregation for high-performance red organic light-emitting diodes remains a formidable challenge. In this work, three robust red-emitting Pt(II) complexes w ere created by utilizing a rigid 4-coordination configuration, where the ligands w ere formed by linking electron-donor of triphenylamine (TPA) moieties with electron-acceptor of pyridine, isoquinoline, and/or δ-carboline units. The thermal stability, electrochemical, and photophysical properties of the complexes w ere thoroughly examined. The complexes display efficient red phosphorescence, with high photoluminescence quantum yields and short excited lifetimes. The OLEDs doped with these complexes exhibit high maximum external quantum efficiencies (EQEs) of up to 31.8% with minimal efficiency roll-off even at high brightness. Significantly, the devices demonstrated exceptional long operational lifetime, with a T90 lifetime of over 14000 hours at initial luminance of 1000cd m-2 , indicating the potential for these complexes to be practically utilized. This article is protected by copyright. All rights reserved.

Fluorine Polymer‐Modified Dion‐Jacobson Perovskites Enabling Sky‐Blue Perovskite Light‐Emitting Diodes with an Efficiency of 16.55%

AbstractQuasi‐2D Dion‐Jacobson (DJ) perovskites are promising candidates for fabricating high‐performance blue‐emitting perovskite light‐emitting diodes (PeLEDs) because of their strong quantum/dielectric confinement and high stability. However, obtaining high‐efficiency blue PeLEDs based on DJ perovskites remains a major challenge. Herein, sky‐blue DJ perovskites are synthesized by using 1,8‐diamino‐3,6‐dioxaoctane as an organic diamine and high‐quality perovskite films are prepared by incorporating poly(vinylidene fluoride‐co‐hexafluoropropylene) (PVDF‐HFP) as an additive, aiming to improve the photoluminescence quantum yield and electron carrier mobility of the film used as an emissive layer in PeLEDs. Finally, sky‐blue PeLEDs using PVDF‐HFP‐modified DJ perovskite films are demonstrated to show a high maximum external quantum efficiency of 16.55%. A promising strategy is provided to design high‐quality perovskite films for constructing high‐performance blue PeLEDs.

Charge Transfer Excited State Promoted Multiple Resonance Delayed Fluorescence Emitter for High-Performance Narrowband Electroluminescence.

Multiple resonance thermally activated delayed fluorescence (MR-TADF) emitters are promising candidates for narrowband organic light-emitting diodes, but their electroluminescent performance is typically hindered by the slow reverse intersystem crossing rate (kRISC). Herein, we present an effective strategy to introduce a multichannel reverse intersystem crossing (RISC) pathway with large spin-orbit coupling by orthogonally linking an electron-donating unit to the MR framework. Through delicate manipulation of the excited-state energy levels, an additional intersegmental charge transfer triplet state could be "silently" induced without perturbing the MR character of the lowest excited singlet state. The proof-of-concept emitter CzBN3 not only affords 23-fold increase of kRISC compared with its prototypical MR skeleton but also realizes close-to-unity photoluminescence quantum yield, large radiative rate constant, and very narrow emission spectrum. These merits enable high maximum external quantum efficiency (EQEmax) of up to 37.1% and alleviated efficiency roll-off in the sensitizer-free device (EQE1000 = 30.4%), and a further boost of efficiency (EQEmax/1000 = 42.3/34.1%) is realized in the hyperfluorescent device. The state-of-the-art electroluminescent performance validates the superiority of our molecular design strategy.

41‐3: Efficient Pure Blue Hyperfluorescence OLEDs with Donor‐Acceptor‐Donor Type Thermally Activated Delayed Fluorescence Sensitizer

In a hyperfluorescecne (HF) system, minimization of energy loss channel consisted of slow reverse intersystem crossing (RISC) and fast Dexter energy transfer (DET) is still challenging. Here, we report that such energy loss channels can minimize by utilizing quadrupolar donor‐acceptor‐donor (D‐A‐D) type TADF as sensitizer materials. We synthesized DBA‐DmICz and DBA‐DTMCz as D‐A‐D type TADF materials, which could suppress the DET process through fast RISC rate and shielded lowest unoccupied molecular orbital structure. The fabricated HF device with DBA‐DTMCz and v‐DABNA as a final dopant exhibited 43.9% of high maximum external quantum efficiency (EQEmax) with the CIE coordinates of (0.12, 0.16).

Improving the stability and color purity of a BT.2020 blue multiresonance emitter by alleviating hydrogen repulsion.

Stable deep blue multiresonance emitters with small full width at half maximum (FWHM) are attractive for wide color-gamut organic light-emitting diodes (OLEDs). However, the steric repulsion from the spatially close hydrogens would twist the multiresonance skeletons, causing spectral broadening and molecular instability issues. Here, we strategically introduce a mesitylboron locking unit into a carbazole-embedded multiresonance model emitter, alleviating the hydrogen repulsions and also strengthening the para-positioned weak carbon-nitrogen bond in anionic states. An emission peaking at 452 nm with an FWHM of merely 14 nm and nearly BT.2020 blue chromaticity coordinates are obtained in toluene, affording a high maximum external quantum efficiency of 33.9% in a sensitizing device. Moreover, an impressive LT97 (time to decay to 97% of the initial luminance) of 178 hours at a constant current density of 12 mA/cm2 was achieved in a stable device with a small y coordinate of 0.057, nearly 20 times longer than the model emitter with even a substantially red-shifted emission.

Management of Host–Guest Triplet Exciton Distribution for Stable, High‐Efficiency, Low Roll‐Off Solution‐Processed Blue Organic Light‐Emitting Diodes by Employing Triplet‐Energy‐Mediated Hosts

AbstractHigh‐quality hosts are indispensable for simultaneously realizing stable, high efficiency, and low roll‐off blue solution‐processed organic light‐emitting diodes (OLEDs). Herein, three solution processable bipolar hosts with successively reduced triplet energies approaching the T1 state of thermally activated delayed fluorescence (TADF) emitter are developed and evaluated for high‐performance blue OLED devices. The smaller T1 energy gap between host and guest allows the quenching of long‐lived triplet excitons to reduce exciton concentration inside the device, and thus suppresses singlet‐triplet and triplet‐triplet annihilations. Triplet‐energy‐mediated hosts with high enough T1 and better charge balance in device facilitate high exciton utilization efficiency and uniform triplet exciton distribution among host and TADF guest. Benefited from these synergetic factors, a high maximum external quantum efficiency (EQEmax) of 20.8%, long operational lifetime (T50 of 398.3 h @ 500 cd m−2), and negligible efficiency roll‐off (EQE of 20.1% @ 1000 cd m−2) are achieved for bluish‐green TADF OLEDs. Additionally introducing a narrowband emission multiple‐resonance TADF material as terminal emitter to accelerate exciton dynamic and improve exciton utilization, a higher EQEmax of 23.1%, suppressed roll‐off and extended lifetime of 456.3 h are achieved for the sky‐blue sensitized OLEDs at the same brightness.

Deepening Insights into Aggregation Effect of Intermolecular Charge‐Transfer Aggregates for Highly Efficient Near‐Infrared Non‐Doped Organic Light‐Emitting Diodes over 780 nm

AbstractThough urgently needed, high‐efficiency near‐infrared (NIR) organic light‐emitting diode (OLED) is still rare due to the energy‐gap law. Formation of intermolecular charge‐transfer aggregates (CTA) with nonadiabatic coupling suppression can decelerate non‐radiative decay rates for high‐efficiency NIR‐OLEDs. However, the aggregation effect of CTA is still not fully understood, which limits the rational design of CTA. Herein, two CTA molecules with a same π‐framework but different terminal substituents are developed to unveil the aggregation effect. In highly ordered crystalline states, the terminal substituents substantially affect the molecular packing motifs and intermolecular charge‐transfer states, thus leading to distinct photophysical properties. In comparison, in amorphous states, these two CTA demonstrate similar photophysical behaviors and properties due to their similar molecular packing and intermolecular interactions as evidenced by molecular dynamics simulations. Importantly, the formations of amorphous CTA trigger multifunction improvements such as aggregation‐induced NIR emission, aggregation‐induced thermally activated delayed fluorescence, self‐doping and self‐host features. The non‐doped OLEDs demonstrate NIR emissions centered at 788 and 803 nm, and high maximum external quantum efficiencies of 2.6% and 1.5% with small efficiency roll‐off, respectively. This study provides deeper insight into the aggregation effect of CTA and lays a foundation for the development of high‐efficiency NIR non‐doped OLEDs.

Tetradentate C∧C∧N∧N Ligand-Containing Gold(III) Complexes with Orange to Deep-Red Thermally Activated Delayed Fluorescence (TADF) and Their Application in Organic Light-Emitting Devices

A new class of thermally activated delayed fluorescence (TADF) tetradentate C∧C∧N∧N ligand-containing gold(III) complexes containing acridinyl moieties has been designed and synthesized. These complexes exhibit orange-red to deep-red emission with photoluminescence quantum yields (PLQYs) of up to 0.76 in solid-state thin films. Short excited-state lifetimes of ≤2.0 μs and large radiative decay rate constants (kr) in the order of 105 s-1 have also been found in the complexes. High-performance solution-processed and vacuum-deposited organic light-emitting devices (OLEDs) based on these complexes have been fabricated, demonstrating high maximum external quantum efficiencies (EQEs) of 12.2 and 12.7%, respectively, which are among the best values ever reported for red-emitting gold(III)-based OLEDs. In addition, satisfactory operational half-lifetime (LT50) values of up to 34,058 h have been attained in these red-emitting devices. It is found that the operational stability is strongly dependent on the choice of functional groups on the acridinyl moieties, of which the incorporation of -O- and -S- linkers can effectively prolong the LT50 value by an order of magnitude. The TADF properties of the complexes are substantiated by the hypsochromic shift in emission energies and the remarkable enhancement in the emission intensity upon increasing temperature. The TADF properties have also been supported by temperature-dependent ultrafast transient absorption studies, with the direct observation of reverse intersystem crossing (RISC) and the determination of the activation parameters for the very first time, together with their excited-state dynamics.

Orbital Symmetry Engineering in Fused Polycyclic Heteroaromatics toward Extremely Narrowband Green Emissions with an FWHM of 13nm.

Multiresonance (MR) molecules generally face spectral broadening issues with redshifted emissions. Thus, green emitters with full widths at half maximum (FWHMs) of <20nm are rarely reported, despite being highly desired. Herein, by properly fusing indolo(3,2,1-jk)carbazole (ICZ) and naphthalene moieties, green MR emitters are reported, which have FWHMs of merely 13nm (0.064eV) and 14nm (0.069eV) in dichloromethane, accompanied by high photoluminescence quantum yields of >95%, which represent not only the smallest FWHMs among all green MR emitters but also the first green emitters based on ICZ MR derivatives. Theoretical studies reveal that the orbital interactions between the antisymmetric sites of the segments play an important role in extending the conjugation length in the fusion architectures while simultaneously maintaining a small FWHM. The corresponding organic light-emitting diodes exhibit green emission peaks at 508-509nm and the first green electroluminescence FWHM of <20nm ever reported. Benefiting from the preferential horizontal dipole orientation, a high maximum external quantum efficiency of up to 30.9% is obtained, which remains at 28.9% and 23.2% under luminances of 1000 and 10000 cdm-2 , respectively, outperforming most reported green devices based on narrowband emitters.

Triazolotriazine-based mixed host for pure-red phosphorescent organic light-emitting diodes exhibiting ultra-low efficiency roll-off

The development of high-performance pure-red phosphorescent organic light-emitting diodes (Ph-OLEDs) especially with low efficiency roll-off at high brightness is still an appealing yet challenging task. Despite success of well-documented 1,3,5-triazine (TRZ)-based thermally activated delayed fluorescence (TADF) hosts in green Ph-OLEDs, the limited electron-withdrawing ability of the TRZ acceptor makes the TADF hosts unsuitable enough for usage in the assembly of high-performance red Ph-OLEDs. Herein, pure-red Ph-OLEDs with ultra-low efficiency roll-off at luminance above 10000 cd m−2 are achieved by developing two triazolotriazine-based TADF hosts (23aIC-TAZTRZ and 32aIC-TAZTRZ) with balanced bipolar transporting property, good morphological stability and high photoluminescence quantum yield in neat film. Particularly, the phosphor-doped 23aIC-TAZTRZ and 32aIC-TAZTRZ emitting layers display high horizontal orientation factors (Θ//) of 84% and 85%, respectively. Ph-OLEDs utilizing 50 wt% 23aIC-TAZTRZ and 50 wt% 32aIC-TAZTRZ as the mixed host exhibit pure-red emission with Commission Internationale de l’Eclairage (CIE) coordinate of [0.66, 0.34], high maximum external quantum efficiency (EQEmax) of 27.4% and ultra-low efficiency roll-off at 10000 cd m−2 (EQE10000 = 23.9%). This work not only discloses the potential of triazolotriazine acceptor for the construction of efficient TADF hosts, but also provides alternative candidates to TRZ-based hosts for the assembly of high-performance red Ph-OLEDs.