High EQE Research Articles

Dual Emission and Low-Temperature Afterglow in Xanthone-Dibenzoazepine for High EQE Host-Guest OLEDs with Low-Efficiency Roll-Off.

Research has been driven to demonstrate organic light-emitting diodes (OLEDs) with high efficiency, and in the quest for new materials, thermally activated delayed fluorescence (TADF) emitters have been employed. Preparation of donor-acceptor (D-A) π-conjugates is a useful guideline for developing TADF emitters. TADF emitters have shown excellent progress and high maximum external quantum efficiency (EQEmax) for OLEDs in the recent past; however, they suffer with substantial roll-off resulting in a decrease in their efficiency. In order to have efficient OLED emitters with less efficiency roll-off, we designed a xanthone-amine derivative with twisted electron-rich dibenzoazepine having limited rotation at the donor-acceptor bond. Xan-Azepine shows solvent polarity-dependent fluorescence in the range of 441- 597 nm having a lifetime below 10 ns. At 77 K in Me-THF, a triplet at 557 nm was observed having a decay lifetime of 0.75 s and an afterglow for about 6 s. In powder, it shows dual emission, i.e., fluorescence (490 and 6 ns) and phosphorescence (530 nm and 192 μs) at ambient conditions. The energy difference between the singlet and triplet energy levels of Xan-Azepine is found to be 0.18 eV in the powder sample. Its blend in 4,4'-bis(N-carbazolyl)-1,1'-biphenyl (CBP) showed delayed fluorescence with a lifetime of 118 μs at 300 K, while it reduced to 84 μs at 150 K. These observations suggest the TADF nature of Xan-Azepine in its CBP blend. OLED devices of Xan-Azepine showing a turn-on voltage of 2.8 V and a EQEmax of 12% were successfully fabricated. In the doped films of Xan-Azepine (5 wt %) with CBP, a maximum luminescence of 5980 Cd/m2 at a current density of 70 mA/cm2 was obtained, resulting in devices with low-efficiency roll-off (2.75%).

PEDOT:PSS-Free Quantum-Dot Light-Emitting Diode with Enhanced Efficiency and Stability.

Although high-performance quantum-dot light-emitting diodes (QLEDs) have been achieved, their stability is still limited due to the use of unstable PEDOT:PSS as the hole injection layer (HIL). Here, we developed a PEDOT:PSS-free QLED by using a binary PTAA:F4-TCNQ HIL. Because the PTAA, with a highest occupied molecular orbital (HOMO) level of ∼5.20 eV, can facilitate hole injection from ITO to the hole transport layer, and the F4-TCNQ can act as the electron acceptor dopant to improve the hole density and hole mobility of PTAA, the PTAA:F4-TCNQ HIL can exhibit excellent hole injection capability. As a result, the PEDOT:PSS-free QLED can exhibit a high EQE of 24.19% and an impressive brightness of 367,200 cd/m2, which are significantly higher than those of conventional QLEDs. Moreover, due to the improvement of device performance and the removal of PEDOT:PSS, the PEDOT:PSS-free QLED can also exhibit a high T95 operational lifetime of 4206 h at 1000 cd/m2 and an excellent T80 shelf lifetime of 207.41 h at 136400 cd/m2, which are about 1.6- and 3.3-fold those of conventional QLEDs, respectively. We believe that the demonstrated PEDOT:PSS-free QLED, with higher performance and stability, will promote the practical application of QLEDs in displays.

New blue emitters based on anthracene through charge transfer control

We designed new moieties with varying electron-donating effects and sizes based on diphenylamine and introduced them into anthracene to synthesize three types of emitting materials. All three materials exhibited high thermal stability with glass transition temperatures above 175°C, confirming their potential as OLED emitters. Devices doped with N9,N9,N10,N10-tetraphenylanthracene-9,10-diamine (TAD), where diphenyl amine is substituted on both sides, and N9,N10-di([1,1′-biphenyl]-4-yl)-N9,N10-bis(dibenzo[b,d]furan-2-yl)anthracene-9,10 diamine (ABFA), with a fused side group of diphenyl amine and dibenzofuran, showed EQEs of 1.28 % and 3.57 % respectively. Due to the intramolecular charge transfer (ICT), they exhibited ELmax values at 517 nm and 538 nm. On the other hand, the device doped with N,N′-(anthracene-9,10-diylbis(4,1-phenylene))bis(N-([1,1′-biphenyl]-4-yl)dibenzo[b,d]furan-2-amine) (APBFA), which has optimized side groups that suppress ICT and intermolecular packing, achieved a relatively high EQE of 4.48 % and showed blue emission with CIE coordinates of (0.146, 0.142).

Superior Hole Injection Material PEGDT/TPF/PVDF with p-Doping Capability for Highly Efficient Solution-Processed Organic Light-Emitting Diode.

The ability to charge injection is a key factor in determining the performance of the organic light-emitting diode (OLED) devices. Improving the work function of the anode surface via interface modification, thus lowering the hole injection barrier, stands as a crucial strategy for enhancing the performance of the OLED device. Herein, we propose an innovative p-doping hole injection material, namely, PEGDT/TPF/PVDF that exhibits excellent performance in OLED devices with the value of maximum current efficiency at 56.4 Cd A-1, maximum luminescence at 25,564 Cd m-2, and a high EQE of 19.8%. The results for PEGDT/TPF/PVDF showed good conductivity, excellent film-forming property, and high transmittance over 98% in the spectrum range of 500-700 nm. Changes in the hole-injection energy barriers observed from the surface of the anode suggest a modified anode with PEGDT/TPF/PVDF deepened the work function at a value of 0.2 eV, which dramatically improves the hole-injection properties. This work not only provides novel structural materials with exceptional hole-injection properties but also proposes a promising alternative to PEDOT/PSS.

High EQE of 43.76% in solution-processed OLEDs operating at a wavelength of 626 nm

Simultaneously achieving high-efficiency, deep-red emission, and solution-processed organic light-emitting diodes (OLEDs) remains a huge challenge. In this work, a thermally activated delayed fluorescent (TADF) material of CzPXZ that exhibits aggregation-induced emission property and a deep-red phosphorescent emitter of Ir(dmppy)(piq)2(od) are developed to build effective energy transfer pathways by dissolving them in a non-polar organic solvent. The electroluminescent emission peaks of CzPXZ:Ir(III)-based OLEDs are located at deep-red 626 nm, demonstrating efficient energy transfer from CzPXZ to the Ir(III) complex. Furthermore, an optimized DPEPO hole-blocking layer is utilized in such Ir(III)-doped OLEDs to enhance the radiative recombination. Therefore, a high external quantum efficiency of 43.76% is achieved for CzPXZ:Ir(III)-based OLEDs. This work sheds light on the great potential of energy transfer from AIE-TADF to red phosphorescent emitters for high-efficiency, solution-processed, deep-red OLEDs.

Creating highly efficient stretchable OLEDs with nanowavy structures for angle-independent narrow band emission

Stretchable organic light-emitting diodes (SOLEDs) have been the challenging class of OLEDs as they have limited processability to fabricate a design that can withstand external deformation. Herein, we demonstrated the highly efficient top-emitting geometrical stretchable OLED (GSOLED) by incorporating the prestretched elastomer with optical adhesive film. The experimental and theoretical characterizations verified the enhancement of device efficiencies with the light extraction phenomenon brought by nanowavy corrugated structures. Furthermore, GSOLED shows stability in stretchable conditions and displays narrower emission spectrum with improved color purity. The full width at half maximum (FWHM) of 21 nm shows narrowband emission with a high current efficiency and EQE of 221 cd A−1 and 39.50%. This work marks a significant step forward, providing unprecedented insights into the factors influencing device performance in current and future material systems for stretchable organic light-emitting diodes.

Suppression of efficiency roll-off in solution-processed OLEDs using pyrimidine-based iridium complexes modified with sterically hindered groups

Three bis-cyclometalated iridium complexes Ir1-Ir3 were successfully synthesized through mild reaction conditions. All complexes exhibit emission peaks at 507-509 nm, with excellent photoluminescence quantum efficiencies (PLQY) ranging from 69% to 97%. Self-quenching is significantly reduced because the steric spacers lead to minimum bimolecular interactions. Accordingly, the electroluminescence device based on complex Ir3 exhibits a maximum luminous efficiency of 39.6 cd A−1, a high EQE of 13.1% with an efficiency roll-off of 4.2% at 1000 cd m−2, which is much smaller than that (10.8%) of the Ir1-based device. Moreover, its devices exhibit excellent stability even at elevated doping concentrations, suggesting a notable reduction in intermolecular interactions caused by the steric pinene spacer.

White Organic Light-Emitting Diodes with External Quantum Efficiency of 20.77% at 10000cdm-2 and Ultra-High Color Stability by Controlling Exciton Distribution.

Although brightness and efficiency have been continually improved, the inability to achieve superior efficiency, color stability, and low-efficiency roll-off simultaneously in white organic light-emitting diodes (OLEDs) remains a knotty problem restricting the commercial application. In this paper, emission balance for two different horizontal orientation emitting molecules is maintained by using hole transport materials and bipolar host materials to control carriers' recombination and exciton diffusion. Impressively, the obtained devices exhibit extremely stable white emission with small chromaticity coordinates variation of (0.0023, 0.0078) over a wide brightness range from 1000 to 50000cdm-2. Meanwhile, the optimal white OLED realizes the power efficiency, current efficiency, and external quantum efficiency up to 70.68lmW-1, 85.53cdA-1, and 24.33%, respectively at the practical brightness of 1000cdm-2. Owing to reduced heterogeneous interfaces and broadening recombination region, this device exhibits a high EQE over 20% under high luminance of 10000cdm-2, demonstrating slight efficiency roll-off. The operating mechanism of the device is analyzed by versatile experimental and theoretical evidences, which concludes precise manipulation of charges and excitons is the key points to achieve these excellent performances. This work provides an effective strategy for the design of high-performance white OLEDs.

Peripheral carbazole units-decorated MR emitter containing B−N covalent bond for highly efficient green OLEDs with low roll-off

Boron−nitrogen doped multiple resonance (BN-MR) emitters, characterized by B−N covalent bonds, offer distinctive advantages as pivotal building blocks for facile access to novel MR emitters featuring narrowband spectra and high efficiency. However, there remains a scarcity of exploration concerning synthetic methods and structural derivations to expand the library of novel BN-MR emitters. Herein, we present the synthesis of a BN-MR emitter, tCz[B−N]N, through a one-pot borylation reaction directed by the amine group, achieving an impressive yield of 94%. The emitter is decorated by incorporating two 3,6-di-t-butylcarbazole (tCz) units into a B−N covalent bond doped BN-MR parent molecule via para-C−π−D and para-N−π−D conjugations. This peripheral decoration strategy enhances the reverse intersystem crossing process and shifts the emission band towards the pure green region, peaking at 526 nm with a narrowband full-width at half maximum (FWHM) of 41 nm. Consequently, organic light emitting diodes (OLEDs) employing this emitter achieved a maximum external quantum efficiency (EQEmax) value of 27.7%, with minimal efficiency roll-off. Even at a practical luminance of 1000 cd∙m−2, the device maintains a high EQE value of 24.6%.

Chiral Co-Assembly with Narrowband Multi-Resonance Characteristics for High-Performance Circularly Polarized Organic Light-Emitting Diodes.

A promising kind of ternary chiral co-assemblies with high PLQY, large dissymmetry factor (glum), and narrowband multi-resonance characteristics are achieved by codoped-thermal annealing treatments of achiral luminescent polymer F8BT, chiral inducers R/S-5011, and achiral FRET acceptor DBN-ICZ. The optimized co-assemblies (F8BT)0.9-(R/S-5011)0.1-(DBN-ICZ)0.005 display narrowband yellow emission with full-width half maximum (FWHM) of 37 nm, PLQY of 79%, and intense CPL signals with |glum| of up to 0.26. Meaningfully, solution-processed CP-OLEDs by using those ternary chiral co-assemblies as emitting layer are successfully fabricated, which display yellow circularly polarized electroluminescence (CPEL) with EQEmax of 4.6% and gEL of up to 0.16. The corresponding Q-factor could reach up to 7.36 × 10-3, which is the highest of all the reported CP-OLEDs. Moreover, the devices also exhibit excellent comprehensive device performance with low Von of 7.0 V, high Lmax of about 25000 cd m-2, extremely low efficiency roll-off with EQE of 4.3% at 10000 cd m-2, as well as narrowband EL with FWHM of only 39 nm. The proposed ternary co-assembly strategy in fabricating CP-OLED provides the possibility to achieve high comprehensive device performance such as balancing high EQE and large gEL value, as well as narrowband emission, high brightness and low efficiency roll-off simultaneously.

Self-Assembled Chiral Polymers Exhibiting Amplified Circularly Polarized Electroluminescence.

Circularly polarized electroluminescence (CPEL) is highly promising in realm of 3D display and optical data storage. However, designing a groundbreaking chiral material with high comprehensive CPEL performance remains a formidable challenge. In this work, a pair of chiral polymers with self-assembled behavior is designed by integrating a chiral BN-moiety into polyfluorene backbone, named R-PBN and S-PBN, respectively. The chiral polymers show narrowband emission centered at 490 nm with full-width half maximum (FWHM) of 29 nm and high photoluminescence quantum yield (PLQY) of 79 %. After thermal annealing treatment, the chiral polymers undergo self-assembly, exhibiting amplified circularly polarized luminescence (CPL) with asymmetry factor (|glum|) of up to 0.11. Moreover, the solution-processed nondoped CP-OLEDs based on the chiral polymers as emitting layers exhibit maximum external quantum efficiency (EQEmax) of 9.8 %, intense CPEL activities with |gEL| of up to 0.07, and small FWHM of 36 nm, simultaneously. This represents the first case of self-assembled chiral polymers that combines high EQE, large gEL value and narrowband emission.

Self‐Assembled Chiral Polymers Exhibiting Amplified Circularly Polarized Electroluminescence

Circularly polarized electroluminescence (CPEL) is highly promising in realm of 3D display and optical data storage. However, designing a groundbreaking chiral material with high comprehensive CPEL performance remains a formidable challenge. In this work, a pair of chiral polymers with self‐assembled behavior is designed by integrating a chiral BN‐moiety into polyfluorene backbone, named R‐PBN and S‐PBN, respectively. The chiral polymers show narrowband emission centered at 490 nm with full‐width half maximum (FWHM) of 29 nm and high photoluminescence quantum yield (PLQY) of 79%. After thermal annealing treatment, the chiral polymers undergo self‐assembly, exhibiting amplified circularly polarized luminescence (CPL) with asymmetry factor (|glum|) of up to 0.11. Moreover, the solution‐processed nondoped CP‐OLEDs based on the chiral polymers as emitting layers exhibit maximum external quantum efficiency (EQEmax) of 9.8%, intense CPEL activities with |gEL| of up to 0.07, and small FWHM of 36 nm, simultaneously. This represents the first case of self‐assembled chiral polymers that combines high EQE, large gEL value and narrowband emission.

Spirobifluorene Trimers: High Triplet Pure Hydrocarbon Hosts for Highly Efficient Blue Phosphorescent Organic Light‐Emitting Diodes

AbstractPure aromatic hydrocarbon materials (PHCs) represent a new generation of host materials for phosphorescent OLEDs (PhOLEDs), free of heteroatoms. They reduce the molecular complexity, can be easily synthesized and are an important direction towards robust devices. As heteroatoms can be involved in bonds dissociations in operating OLEDs through exciton induced degradation processes, developing novel PHCs appear particularly relevant for the future of this technology. In the present work, we report a series of extended PHCs constructed by the assembly of three spirobifluorene fragments. The resulting positional isomers present a high triplet energy level, a wide HOMO/LUMO difference and improved thermal and morphological properties compared to previously reported PHCs. These characteristics are beneficial for the next generation of host materials for PhOLEDs and provide relevant design guidelines. When used as a host in blue‐emitting PhOLEDs, which are still the weakest link of the field, a very high EQE of 24 % and low threshold voltage of 3.56 V were obtained with a low‐efficiency roll‐off. This high performance strengthens the position of PHC strategy as an efficient alternative for OLED technology and opens the way to a more simple electronic.

Spirobifluorene Trimers: High Triplet Pure Hydrocarbon Hosts for Highly Efficient Blue Phosphorescent Organic Light-Emitting Diodes.

Pure aromatic hydrocarbon materials (PHCs) represent a new generation of host materials for phosphorescent OLEDs (PhOLEDs), free of heteroatoms. They reduce the molecular complexity, can be easily synthesized and are an important direction towards robust devices. As heteroatoms can be involved in bonds dissociations in operating OLEDs through exciton induced degradation processes, developing novel PHCs appear particularly relevant for the future of this technology. In the present work, we report a series of extended PHCs constructed by the assembly of three spirobifluorene fragments. The resulting positional isomers present a high triplet energy level, a wide HOMO/LUMO difference and improved thermal and morphological properties compared to previously reported PHCs. These characteristics are beneficial for the next generation of host materials for PhOLEDs and provide relevant design guidelines. When used as a host in blue-emitting PhOLEDs, which are still the weakest link of the field, a very high EQE of 24 % and low threshold voltage of 3.56 V were obtained with a low-efficiency roll-off. This high performance strengthens the position of PHC strategy as an efficient alternative for OLED technology and opens the way to a more simple electronic.

36‐1: Invited Paper: Submicron Narrow‐Band Phosphors in Luminescent Color Filters & Next Generation MiniLED and MicroLED Displays

Both phosphors and quantum dots are currently used in liquid crystal displays (LCDs), with GE's KSF narrow red phosphor demonstrating the best possible red color point, reliability, and efficiency. Next generation miniLED and microLED based displays require excellent color quality (gamut) and high brightness which will require color conversion materials with high EQE and narrow emission peaks. Here we describe recent advancements in submicron narrow‐band phosphors which are being implemented in next‐generation miniLED displays, and being considered for enabling full‐color microLED and luminescent color filter displays of the future due to their excellent optical performance and robust nature.

P‐257: Late‐News Poster: Highly Efficient Geometrically Stretchable Organic Light Emitting Diodes with Angle Independent Narrow‐Band Emission

Herein, we demonstrated the first highly efficient geometrical stretchable top‐emitting organic light emitting diode by incorporating the pre‐stretched optical adhesive (OA) film. The enhancement of device efficiencies with light extraction phenomenon brought by the nanowavy corrugated structures of OA substrate. GSOLED shows stability in stretchable conditions and displays narrowband emission with color purity. The device shows very high current efficiency and EQE of 221 cd A ‐1 and 51 %.

P‐203: Highly‐Pure Color and Stable Green Hyperfluorescence Device through Host Adjustment

In this study, we report a fluorescent green emitter based on 4,4‐dfluoro‐4‐bora‐3a,4a‐diaza‐s‐indacene (BODIPY) backbone and its hyperfluroescence (HF) device. Our HF device shows high EQE of 20.0%, emission peak at 532 nm with narrow FWHM of 29 nm and Commission Internationale de l'Eclairage (CIE) of (0.27, 0.68). Moreover, with consideration of good host materials the device realized a long lifetime (LT90) of 210 h at an initial luminance of3,000 cd/m2.

Drag force shear manipulating ligand distribution at perovskite buried interface enables efficiently suppressed EQE roll-off of perovskite light-emitting diodes

Effectively manipulating the ligand distribution at the perovskite buried interface is critical for achieving high-performance nanocrystal-based perovskite light-emitting diodes (PeLEDs). However, it is challenging to realize it due to the non-exposed feature of the buried interface. Here, the drag force shear (DFS) is utilized to successfully regulate the ligand distribution at the perovskite buried interface which can effectively suppress the EQE roll-off of devices. By manipulating the ligand distribution at the perovskite buried interface, it is revealed that a more ligand preservation could result in an improved defect passivation leading to higher EQE, while the carrier injection barrier is increased simultaneously making devices suffer from severe EQE roll-off and decreased luminance, and vice versa. With the help of optimizing the ligand distribution by manipulating the DFS, the balance between carrier injection and interfacial defect passivation is successfully achieved. Resultantly, an enhanced EQE of 17.24 % with substantially suppressed EQE roll-off is reached, culminating in a remarkable luminance of 61,900 cd/m2. This work presents an efficient approach to control ligand distribution at the perovskite buried interface and offers valuable insights for realizing high luminance and low EQE roll-off of PeLEDs.

Ultrahigh Responsivity In2O3 UVA Photodetector through Modulation of Trimethylindium Flow Rate

Oxygen vacancies (Vo) can significantly degrade the electrical properties of indium oxide (In2O3) thin films, thus limiting their application in the field of ultraviolet detection. In this work, the Vo is effectively suppressed by adjusting the Trimethylindium (TMIn) flow rate (fTMIn). In addition, with the reduction of the fTMIn, the background carrier concentration and the roughness of the film decrease gradually. And a smooth In2O3 thin film with roughness of 0.44 nm is obtained when the fTMIn is 5 sccm. The MSM photodetectors (PDs) are constructed based on In2O3 thin films with different fTMIn to investigate the opto-electric characteristics of the films. The dark current of the PDs is significantly reduced by five orders from 100 mA to 0.28 μA with the reduction of the fTMIn from 50 sccm to 5 sccm. In addition, the photo response capacity of PDs is dramatically enhanced. The photo-to-dark current ratio (PDCR) increases from 0 to 2589. Finally, the PD with the fTMIn of 5 sccm possesses a record-high responsivity of 2.53 × 103 AW−1, a high detectivity of 5.43 × 107 Jones and a high EQE of 9383 × 100%. Our work provides an important reference for the fabrication of high-sensitivity UV PDs.

Performance improvement of blue light micro-light emitting diodes (< 20 μm) by neutral beam etching process

In this study, micro-light emitting diodes array (μLEDs) with dimensions of 5 μm and 15 μm chip size were fabricated using Neutral Beam Etching (NBE) processes. Size-dependent issues of μLEDs processed by traditional inductively coupled plasma-reactive ion etching (ICPRIE) were alleviated by NBE technology, which exhibited lower equivalent resistance, turn-on voltage, and Ideality factor as compared with those of μLEDs by ICPRIE. Additionally, higher light output power of μLEDs processed by NBE with both 5 μm and 15 μm resulted in higher EQE 7.6 % and 7.7 % than those of μLEDs processed by ICPRIE. Furthermore, the size effect led to a decrease in EQEmax values of the ICPRIE sample by 0.4 %, but only a 0.1 % decay in NBE. Overall, samples fabricated by the NBE process exhibited superior optoelectronic characteristics. Finally, non-radiative recombination behaviors on the mesa sidewall were verified by cathodoluminescence analysis, showing significant decay in ICPRIE samples but not in NBE samples. These results demonstrated the potential of the NBE process for fabricating small chip sizes blue-light μLEDs required for high-brightness, high-efficiency, and high-resolution μLED displays.