Performance Of Organic Light-emitting Diodes Research Articles

Achieving Deep‐Blue Through‐Space Charge‐Transfer Emitter by Designing the Donor‐π‐Donor‐σ‐Acceptor Molecular Structure

AbstractIn the realm of organic light‐emitting diode (OLED), through‐space charge transfer (TSCT) thermally activated delayed fluorescence (TADF) emitters have demonstrated remarkable achievements. Nevertheless, realizing both deep‐blue emission and high efficiency by the TSCT strategy remains a persistent challenge. Here, the novel donor‐π‐donor‐σ‐acceptor (D‐π‐D‐σ‐A) type deep‐blue TSCT emitter, namely D‐tCz‐BO, is formulated to investigate its performance in OLED. D‐tCz‐BO show a narrow deep‐blue emission and efficient TADF character (λPL = 448, FWHM = 54 nm, ΦPL = 82%, and ΔEST = 0.09 eV). More importantly, the OLED based on D‐tCz‐BO as the emitter showed a maximum external quantum efficiency (EQEmax) of 20.5%, with a Commission Internationale de l'Eclairage (CIE) coordinate of (0.14, 0.12). This represents one of the best deep‐blue TSCT‐TADF emitters to date.

Rational Design of Coumarin-Based Hybridized Local and Charge-Transfer Blue Emitters for Solution-Processed Organic Light-Emitting Diodes.

Hybridized local and charge-transfer (HLCT) with the utilization of both singlet and triplet excitons through the "hot excitons" channel have great application potential in highly efficient blue organic light-emitting diodes (OLEDs). The proportion of charge-transfer (CT) and locally excited (LE) components in the relevant singlet and triplet states makes a big difference for the high-lying reverse intersystem crossing process. Herein, three novel donor (D)-acceptor (A) type HLCT materials, 7-([1,1'-biphenyl]-4-yl(9,9-dimethyl-9H-fluoren-2-yl)amino)-3-phenyl-1H-isochromen-1-one (pPh-7P), 7-([1,1'-biphenyl]-4-yl(9,9-dimethyl-9H-fluoren-2-yl)amino)-3-methyl-1H-isochromen-1-one (pPh-7M), and 6-([1,1'-biphenyl]-4-yl(9,9-dimethyl-9H-fluoren-2-yl)amino)-3-methyl-1H-isochromen-1-one (pPh-6M), were rationally designed and synthesized with diphenylamine derivative as donor and oxygen heterocyclic coumarin moiety as acceptors. The proportions of CT and LE components were fine controlled by changing the connection site of diphenylamine derivative at C6/C7-position and the substituent at C3-position of coumarin moiety. The HLCT characteristics of pPh-7P, pPh-7M, and pPh-6M were systematically demonstrated through photophysical properties and density functional theory calculations. The solution-processed doped OLEDs based on pPh-6M exhibited deep-blue electroluminescence with the maximum emission wavelength of 446 nm, maximum luminance of 8755 cd m-2, maximum current efficiency of 5.83 cd A-1, and maximum external quantum efficiency of 6.54%. The results reveal that pPh-6M with dominant 1LE and 3CT components has better OLED performance.

Effective donor and acceptor modifications of carbazole-benzonitrile thermally activated delayed fluorescence molecules enabling high-performance OLEDs

Carbazole-benzonitrile derivatives (CzBNs) have great potential to enable thermally activated delayed fluorescence (TADF) molecules with both high efficiency and good stability simultaneously. However, the device performances of most CzBN-based organic light-emitting diodes (OLEDs) still lag behind other types of TADF molecules. In this work, we proposed a design strategy to construct efficient CzBN-TADF molecules through acceptor and donor modifications. The cyano-modified acceptor enables the extension of the lowest unoccupied molecular orbital while mostly preserving the overlapped area with the highest occupied molecular orbital. The optimized distributions of frontier molecular orbitals contribute to tiny singlet-triplet energy gaps while maintaining a high radiative decay rate. The incorporation of tert-butyl units in the donor groups further enhances the TADF property of resulted tPCNBN molecule due to suppressed non-radiative decay and reduced exciton self-quenching. Accordingly, OLEDs based on tPCNBN present the best device performances, such as a maximum external quantum efficiency of 33.1 % at 400 cd m−2, which is still as high as 26.3 % at a high luminance of 4000 cd m−2, demonstrating relatively low efficiency roll-off. These results confirm the effectiveness of the proposed design strategy in developing efficient and stable CzBN-TADF materials and devices.

Understanding of complex spin up-conversion processes in charge-transfer-type organic molecules

Despite significant progress made over the past decade in thermally activated delayed fluorescence (TADF) molecules as a material paradigm for enhancing the performance of organic light-emitting diodes, the underlying spin-flip mechanism in these charge-transfer (CT)-type molecular systems remains an enigma, even since its initial report in 2012. While the initial and final electronic states involved in spin-flip between the lowest singlet and lowest triplet excited states are well understood, the exact dynamic processes and the role of intermediate high-lying triplet (T) states are still not fully comprehended. In this context, we propose a comprehensive model to describe the spin-flip processes applicable for a typical CT-type molecule, revealing the origin of the high-lying T state in a partial molecular framework in CT-type molecules. This work provides experimental and theoretical insights into the understanding of intersystem crossing for CT-type molecules, facilitating more precise control over spin-flip rates and thus advancing toward developing the next-generation platform for purely organic luminescent candidates.

Solution-processed orange organic light-emitting diodes based on phosphorescent iridium(III) complexes with coumarin 6 as the main ligand

Four ionic orange phosphorescent iridium(III) complexes (Ir1, Ir2, Ir3, Ir4) were successfully synthesized using coumarin 6 as the cyclometalated ligand and 2,2′-bipyridine (bpy) derivatives with different number and position of methyl groups as the auxiliary ligand. The effects of substituents in the auxiliary ligands on their properties were systematically investigated. These four complexes exhibited orange emission at wavelengths of 590, 588, 587, and 586 nm, respectively, with excellent solubility and remarkable photophysical properties in different solvents. Furthermore, they were further applied in the organic light-emitting diodes (OLEDs) based on solution method. The maximum luminance of the devices based on Ir1/Ir2/Ir3/Ir4 reached 1907.0/932.6/760.8/519.3 cd/m2, with corresponding maximum current efficiency (CE), power efficiency (PE), and external quantum efficiency (EQE) values of 1.56/1.71/1.97/1.52 cd/A, 0.33/0.32/0.35/0.27 lm/W, and 0.77/0.82/0.90/0.72 %, respectively. Although there is room for improvement in the performance of OLEDs, this strategy inspires us to modulate the novel photoluminescent and electroluminescent properties of iridium(III) complexes through rational modifications of their ancillary ligands.

Effect of the Glass Transition Temperature of Organic Materials on Exciton Recombination Region of Deep Blue OLED under Thermal Stress

The carrier transport and the exciton recombination region, which are strongly affected by temperature, are essential to organic light‐emitting diodes (OLEDs) under thermal stress. A different charge carrier transport materials with different glass transition temperature (Tg) is selected to investigate their effect on the thermal stability of OLEDs. By calculating the carrier mobility at different annealing temperatures and comparing the simulated values by the Arrhenius equation, the effect of the thermal stress on the performance of OLEDs is analyzed. Then, using the luminescent dye as a probe adjacent to the emitting layer and charge transporting layer to identify the exciton recombination region at different temperatures and driving voltages, it is revealed that replacing the functional material with low Tg with a high Tg one could effectively increase the thermal stability of the device to 100 °C. The optimized devices have a reduced turn‐on voltage, and the electron mobility is increased by more than one order of magnitude, which was conducive to exciton recombination. The work promotes the application of OLEDs in extreme environments by improving their thermal stability.

Recent progress in multi-resonance thermally activated delayed fluorescence emitters with an efficient reverse intersystem crossing process.

Multi-resonance thermally activated delayed fluorescence (MR-TADF) emitters have become an active research topic at the forefront of organic light-emitting diodes (OLEDs) owing to their excellent photophysical properties such as high efficiency and narrow emission characteristics. However, MR-TADF materials always exhibit slow reverse intersystem crossing rates (kRISC) due to the large energy gap and small spin-orbit coupling values between singlet and triplet excited states. In order to optimize the RISC process, strategies such as heavy-atom-integration, metal perturbation, π-conjugation extension and peripheral decoration of donor/acceptor units have been proposed to construct efficient MR-TADF materials for high-performance OLEDs. This article provides an overview of the recent progress in MR-TADF emitters with an efficient RISC process, focusing on the structure-activity relationship between the molecular structure, optoelectronic feature, and OLED performance. Finally, the potential challenges and future prospects of MR-TADF materials are discussed to gain a more comprehensive understanding of the opportunities for efficient narrowband OLEDs.

High-performance solution-deposited ambipolar Ir(III) complex phosphors with aggregation-induced phosphorescence enhancement behavior based on N-P=O resonant variation skeleton

Ir(III) complex phosphors with both ambipolar feature and aggregation-induced phosphorescence enhancement (AIPE) property are promising to furnish high electroluminescent performance for solution-deposited phosphorescent organic light-emitting diodes. However, the molecular design...

Performance enhancement of blue organic light-emitting devices by inserting BPhen: Alq3 as an n-doping electron transport layer

An n-doping electron transport layer (ETL) that consists of 4-7-diphenyl-1, 10-phenanlhroline (BPhen) and tris(8-hydroxyquinoline) aluminum (Alq3) was applied to enhance the performance of blue organic light-emitting diodes (OLEDs). The resulting n-doping OLED afforded a maximum luminance efficiency of 8.24 cd/A, which was higher than the devices using either BPhen or Alq3 as ETL by 56.9 % and 91.2 %, respectively. In addition, this device was found to possess a higher maximum power efficiency of 5.17 Lm/W compared to the blue OLEDs without such n-doping ETL concentrations. By performing the hole- and electron- ‘only’ devices and the density functional theory (DFT) calculations, we show that the enhancement of the device performance can be attributed to increased electron injection/transport at ETL interfaces and hence improved carrier balance in emission layer (EML).

Twisted vibration of Aza-azulene promotes ultra-fast triplet-singlet up-conversion for extremely stable red electroluminescence

The fast triplet-singlet up-conversion based on thermally activated delayed fluorescence (TADF) molecules is a unique effort to improve the utilization of triplet excitons. We construct two TADF molecules using nonbenzenoid aromatic aza-azulene as donor and triazine as acceptor. The distortion structural resonance of aza-azulene enhances the reverse intersystem crossing (RISC) process, resulting in efficient inter/intramolecular charge transfer (CT) emission. The rate constant of RISC (kRISC) is 9.0 × 106 and 8.4 × 106 s−1 in solid states. Efficient Förster Energy Transfer (FRET) and/or Dexter Energy Transfer (DET) between these molecules and dopants make them suitable host materials to improve the performances of red phosphorescent organic light-emitting diodes (OLEDs). Especially, the top-emitting device achieves an external quantum efficiency (EQE) of 51.3% and a current efficiency of 68.2 cd/A at 1000 cd m−2 with a long device lifetime of LT95 = 52,350 and LT50 = 536,200 h.

Unraveling Degradation Processes and Strategies for Enhancing Reliability in Organic Light-Emitting Diodes

Organic light-emitting diodes (OLEDs) have emerged as a promising technology for various applications owing to their advantages, including low-cost fabrication, flexibility, and compatibility. However, a limited lifetime hinders the practical application of OLEDs in electronic devices. OLEDs are prone to degradation effects during operation, resulting in a decrease in device lifetime and performance. This review article aims to provide an exciting overview of OLED degradation effects, highlighting the various degradation mechanisms. Subsequently, an in-depth exploration of OLEDs degradation mechanisms and failure modes is presented. Internal and external processes of degradation, as well as the reactions and impacts of some compounds on OLED performance, are then elucidated. To overcome degradation challenges, the review emphasizes the importance of utilizing state-of-the-art analytical techniques and the role of these techniques in enhancing the performance and reliability of OLEDs. Furthermore, the review addresses the critical challenges of lifetime and device stability, which are crucial for the commercialization of OLEDs. This study also explores strategies to improve OLEDs’ lifetime and stability, such as using barrier layers and encapsulation techniques. Overall, this article aims to contribute to the advancement of OLED technology and its successful integration into diverse electronic applications.

Effect of hole-transport layer thickness on the performance of organic light-emitting diodes

In this study, we investigated the influence of hole-transport layer thickness (0, 5, 10, 15, 20, 25, 30, 35 and 40 nm), N,N′-bis(naphthalen-1-yl)-N,N′-bis(phenyl)-2,2′-dimethylbenzidine (α-NPD) on the performance of thermally evaporated multilayer organic light-emitting diodes (OLEDs) with tris(8-hydroxy-quinolinato)aluminium (Alq3) as electroluminescent material. A device with 5 nm α-NPD thickness showed a current density ∼30 times higher than without any α-NPD layer. However, the current density decreased as the α-NPD thickness increased beyond 5 nm. In contrast to the current density, the device efficiency improved as α-NPD layer thickness increased to 30 nm, after which a drop in efficiency was observed. The current efficiency of the device with 30 nm α-NPD thickness was 10 times higher than the device with 5 nm α-NPD thickness. The results indicated that hole-injection in OLEDs was more efficient with thin 5 nm α-NPD, while optimal efficiency was at 30 nm of α-NPD thickness.

Realizing high efficiency and luminance in green, yellow and blue organic light emitting diode by deoxyribonucleic acid

Although the effect of the electron blocking layer (EBL) material, deoxyribonucleic acid (DNA), on the electroluminescence (EL) performance of organic light-emitting diodes (OLEDs) has been studied, the process of DNA regulation of exciton recombination region within the device is still unclear. Herein, devices with and without EBL were fabricated using different DNA spin-coating speeds, and the photoelectric performance of device were measured. By using DNA compounded with cetyltrimethyl ammonium (CTMA) as the EBL and hole buffer layer, so-called BioLEDs. The DNA-based green Alq3 BioLEDs achieve higher luminance (39 000 cd m−2) and higher current efficiency (8.4 cd A−1), which are increased by 49% and 54%, respectively, compared to the reference OLEDs without the addition of DNA. Similarly, the maximum luminance and efficiency of yellow Rubrene BioLEDs is increased by 64% (from 12 120 to 19 820 cd m−2) and 74% (from 1.36 to 2.36 cd A−1), the luminance and efficiency of blue TCTA BioLEDs is increased by 101% and 245%. Specifically, we found that as the thickness of DNA-CTMA increases, the exciton recombination region moves towards the interface between the emitting layer (EML) and the hole transport layer (HTL). By better confining excitons within the EML, the current efficiency of the BioLEDs is effectively improved. Accordingly, we provide a possible idea for achieve high performance DNA-based BioLEDs by adding DNA-CTMA EBL and hole buffer layers. Meanwhile, as the DNA thickness increases, the exciton recombination region moves towards the EML/HTL interface, thereby enhancing the efficiency of the DNA-based BioLEDs.

Marching Toward Long‐Wavelength Narrowband Emissive Multi‐Resonance Delayed Fluorescence Emitters for Organic Light Emitting Diodes

AbstractOver the past decade, thermally activated delayed fluorescence (TADF) emitters have garnered tremendous impetus because of their ability to harvest 100% excitons for the light emission in organic light emitting diodes (OLEDs). However, despite their superior external quantum efficiencies (> 35%), the broad emission spectra with associated full‐width‐at‐half maximum (FWHM > 70 nm) present a limiting factor that must be solved. Recently, multiple‐resonance TADF (MR‐TADF) materials based on the heteroatom doped polyaromatic hydrocarbons have gained astonishing attention owing to their remarkable narrowband emission (FWHM < 30 nm). However, emission of the majority of reported MR‐TADF emitters falls in the blue/green region, which inevitably jeopardizes their application in full‐color OLEDs. Therefore, there is an urgent need to develop the new molecular designs for expanding the color‐gamut of MR‐TADF emitters, i.e., λem > 550 nm without compromising the narrowband emission. To the best of current knowledge, no detailed reviews focusing on the different design strategies for producing long‐wavelength (> 550 nm) MR‐TADF emitters have been reported to date. To this end, a review highlighting the recent design advances for constructing long‐wavelength MR‐TADF emitters is presented, and their photophysics and OLED performance is discussed. Finally, the current status and future prospects of long‐wavelength MR‐TADF materials are discussed.

A Rising Star: Luminescent Carbene-Metal-Amide Complexes.

Coinage metal (gold, silver, and copper) complexes are attractive candidates to substitute the widely studied noble metal complexes, such as, iridium(III) and platinum(II), as luminescent materials in organic light-emitting diodes (OLEDs). However, the development of coinage metal complexes exhibiting high emission quantum yields and short exciton lifetimes is still a formidable challenge. In the past few years, coinage metal complexes featuring a carbene-metal-amide (CMA) motif have emerged as a new class of luminescent materials in OLEDs. Thanks to the coinage metal-bridged linear geometry, coplanar conformation, and the formation of excited states with dominant ligand-to-ligand charge transfer character and reduced metal d-orbital participation, most CMA complexes have high radiative rates via thermally activated delayed fluorescence. Currently, the family of CMA complexes have rapidly evolved and remarkable progresses in CMA-based OLEDs have been made. Here, a Concept article on CMA complexes is presented, with a focus on molecular design principles, the correlation between molecular structure/conformation and optoelectronic properties, as well as OLED performance. The future prospects of CMA complexes are also discussed.

(Invited) Making Stacks of Nitrogenated Polycyclic Aromatic Hydrocarbons with Hydrogen Bonds

Architectures constituted of stacked aromatics play a crucial role in the development of function in biomacromolecules. Recreating this feature on synthetic systems would not only allow understanding and reproducing biological functions but also developing new functions. For instance, the performance of organic field-effect transistors, light-emitting diodes, and solar cells critically depends on the charge transport efficiency of stacks of organic semiconductors. Among different packing configurations, lamellar π-stacking has been identified as an optimal configuration for electronic transport, because of the efficient intermolecular electronic coupling.Nitrogenated polycyclic aromatic hydrocarbons and nanographenes have attracted considerable attention in recent years. Besides the effect of nitrogen doping on the electronic structure, sp2 nitrogens can be engaged in hydrogen bonding interactions as acceptors. We have developed the synthesis of novel architectures constituted of stacked nitrogenated polycyclic aromatic hydrocarbons held together by hydrogen bonds, which include new families of pseudorotaxanes, rotaxanes, foldamers and supramolecular polymers. The synthesis and self-assembling properties of these systems will be discussed together with their charge transporting properties.

Synthetic Strategy for the Development of Conjugated Polyelectrolytes as Cathode Interfacial Layers: Toward Sustainable Organic Devices

AbstractThe use of conjugated polyelectrolytes (CPEs) as interfacial layers (ILs) to increase the efficiency of organic light‐emitting diodes (OLEDs), organic solar cells (OSCs), and organic transistors is a well‐established strategy. Here, the rational process is reported that led to develop the bifunctional poly[(2,7‐(9,9’‐bis(6’‐diethoxylphosphorylhexyl)‐fluorene)‐alt‐(2,7‐(9,9′‐bis(6″‐trimethylammonium bromide)hexyl)‐fluorene)] (PF‐NBr‐EP). PF‐NBr‐EP is successfully incorporated as a cathode IL (CIL) in diverse electronic and optoelectronic devices. The properties of two fluorene‐based CPEs containing, respectively, phosphonate (EP) and ammonium (NBr) moieties used as building blocks for the synthesis of the PF‐NBr‐EP copolymer and their mixtures are investigated to evaluate the combined effect of the two moieties and therefore to gain insight into the behavior of PF‐NBr‐EP chemical structure in the devices. Additionally, the performance of OLEDs and OSCs is analyzed based on established active layers, incorporating all these neat and mixed CILs.

Prolonging blue TADF-OLED lifetime through ytterbium doping of electron transport layer

Balanced charge carrier transport and broad carrier recombination zone are essential features for reducing triplet exciton concentration and suppressing triplet-mediated annihilation processes, which affect the performance and stability of blue-emitting organic light-emitting diodes (OLEDs) based on thermally activated delayed fluorescence (TADF) phenomenon. Doping of organic layers is among the most effective methods to control these features. Herein, the impact of ytterbium (Yb) doping of electron transport layer on the TADF-OLED performance, and particularly the lifetime, was thoroughly assessed. It was found that the lower doping concentrations of Yb (<10wt%) cause electron trapping and reduced current density, whereas higher Yb concentrations facilitate electron transport in the device. Although the introduction of Yb somewhat deteriorated device efficiency, it extended operational lifetime of blue-emitting device by 2 orders of magnitude (up to 46 hours at 1000 cd/m2). This was shown to occur as a result of Yb-assisted non-radiative triplet exciton quenching at the electron transport and emission layer interface, thus diminishing detrimental exciton annihilation processes.

RGB Thermally Activated Delayed Fluorescence Emitters for Organic Light-Emitting Diodes toward Realizing the BT.2020 Standard.

With the surging demand for ultra-high-resolution displays, the International Telecommunication Union (ITU) announce the next-generation color gamut standard, named ITU-R Recommendation BT.2020, which not only sets a seductive but challenging milestone for display technologies but also urges researchers to recognize the importance of color coordinates. Organic light-emitting diodes (OLEDs) are an important display technology in current daily life, but they face challenges in approaching the BT.2020 standard. Thermally activated delayed fluorescence (TADF) emitters have bright prospects in OLEDs because they possess 100% theoretical exciton utilization. Thus, the development of TADF emitters emitting primary red (R), green (R), and blue (B) emission is of great significance. Here, a comprehensive overview of the latest advancements in TADF emitters that exhibit Commission Internationale de l'Éclairage (CIE) coordinates surpassing the National Television System Committee (NTSC) and approaching BT.2020 standards is presented. Rational strategies for molecular designs, as well as the resulting photophysical properties and OLED performances, are discussed to elucidate the underlying mechanisms for shifting the CIE coordinates of both donor-acceptor and multiple resonance (MR) typed TADF emitters toward the BT.2020 standard. Finally, the challenges in realization of the wide-color-gamut BT.2020 standard and the prospects for this research area are provided.

Neoteric Advances in Oxygen Bridged Triaryl Boron-based Delayed Fluorescent Materials for Organic Light Emitting Diodes.

Since their first demonstration, thermally activated delayed fluorescence (TADF) materials have been emerged as the most promising emitters because of their promising applications in optoelectronics, typified by organic light-emitting diodes (OLEDs). In which, the rigid oxygen bridged boron acceptor-featured (DOBNA) emitters have gained tremendous impetus for OLEDs, which is ascribed to their excellent external quantum efficiency (EQE). However, these materials often displayed severe efficiency roll-off and poor operational stability. Therefore, there needs to be a comprehensive understanding of the aspect of the molecular design and structure-property relationship. To the best of our knowledge, there is no detailed review on the structure-function outlook of DOBNA-based emitters emphasizing the effect of the nature of donor units, their number density, and substitution pattern on the physicochemical properties, excited state dynamics and OLED performance were reported. To fill this gap, herein we presented the recent advancements in DOBNA-based acceptor featured TADF materials by classifying them into several subgroups based on the molecular design i. e. donor-acceptor (D-A), D-A-D, A-D-A, and multi-resonant TADF (MR-TADF) emitters. The detailed design concepts, along with their respective physicochemical and OLED performances were summarized. Finally, the prospective of this class of materials in forthcoming OLED displays is also discussed.