Organometal Halide Perovskite Quantum Dot Light‐Emitting Diodes

Organometal halide perovskites quantum dots (OHP‐QDs) with bright, color‐tunable, and narrow‐band photoluminescence have significant advantages in display, lighting, and laser applications. Due to sparse concentrations and difficulties in the enrichment of OHP‐QDs, production of large‐area uniform films of OHP‐QDs is a challenging task, which largely impedes their use in electroluminescence devices. Here, a simple dip‐coating method has been reported to effectively fabricate large‐area uniform films of OHP‐QDs. Using this technique, multicolor OHP‐QDs light‐emitting diodes (OQ‐LEDs) emitting in blue, blue‐green, green, orange, and red color have been successfully produced by simply tuning the halide composition or size of QDs. The blue, green, and red OQ‐LEDs exhibited, respectively, a maximum luminance of 2673, 2398, and 986 cd m^?2 at a current efficiency of 4.01, 3.72, and 1.52 cd A^?1, and an external quantum efficiency of 1.38%, 1.06%, and 0.53%, which are much better than most LEDs based on OHP films. The packaged OQ‐LEDs show long‐term stability in air (humidity ≈50%) for at least 7 d. The results demonstrate the great potential of the dip‐coating method to fabricate large‐area uniform films for various QDs. The high‐efficiency OQ‐LEDs also demonstrate the promising potential of OHP‐QDs for low‐cost display, lighting, and optical communication applications.     

Highly Efficient,Bright, and Stable Colloidal Quantum Dot Short‐Wave Infrared Light‐Emitting Diodes

Unbalanced charge injection is deleterious for the performance of colloidal quantum dot (CQD) light‐emitting diodes (LEDs) as it deteriorates the quantum efficiency, brightness, and operational lifetime. CQD LEDs emitting in the infrared have previously achieved high quantum efficiencies but only when driven to emit in the low‐radiance regime. At higher radiance levels, required for practical applications, the efficiency decreased dramatically in view of the notorious efficiency droop. Here, a novel methodology is reported to regulate charge supply in multinary bandgap CQD composites that facilitates improved charge balance. The current approach is based on engineering the energetic potential landscape at the supra‐nanocrystalline level that has allowed to report short‐wave infrared PbS CQD LEDs with record‐high external quantum efficiency in excess of 8%, most importantly, at a radiance level of ≈5 W sr^?1 m², an order of magnitude higher than prior reports. Furthermore, the balanced charge injection and Auger recombination reduction has led to unprecedentedly high operational stability with radiance half‐life of 26 068 h at a radiance of 1 W sr^?1 m^?2.     

Achieving Highly Efficient Fluorescent Blue Organic Light‐Emitting Diodes Through Optimizing Molecular Structures and Device Configuration

Based on the results of first‐principles calculations of the electronic properties of blue light‐emitting materials, the molecular structures of oligofluorenes are optimized by incorporating electron‐withdrawing groups into the molecules to balance hole and electron injection and transport for organic light‐emitting diodes (OLEDs). The result is a remarkable improvement in the maximum external quantum efficiency (EQE) of the undoped device from 2.0% to 4.99%. Further optimization of the device configurations and processing procedures, e.g., by changing the thickness of the emitting layer and through thermal annealing treatments, leads to a very high maximum EQE of 7.40% for the undoped sky‐blue device. Finally, by doping the emitter in a suitable host material, 4,4’‐bis(carbazol‐9‐yl)biphenyl (CBP), at the optimal concentration of 6%, pure blue emission with extremely high maximum EQE of 9.40% and Commission Internationale de l’Eclairage (CIE) coordinates of (0.147, 0.139) is achieved.     

Low Roll‐Off Perovskite Quantum Dot Light‐Emitting Diodes Achieved by Augmenting Hole Mobility

The external quantum efficiencies (EQEs) of perovskite quantum dot light‐emitting diodes (QD‐LEDs) are close to the out‐coupling efficiency limitation. However, these high‐performance QD‐LEDs still suffer from a serious issue of efficiency roll‐off at high current density. More injected carriers produce photons less efficiently, strongly suggesting the variation of ratio between radiative and non‐radiative recombination. An approach is proposed to balance the carrier distribution and achieve high EQE at high current density. The average interdot distance between QDs is reduced and this facilitates carrier transport in QD films and thus electrons and holes have a balanced distribution in QD layers. Such encouraging results augment the proportion of radiative recombination, make devices with peak EQE of 12.7%, and present a great device performance at high current density with an EQE roll‐off of 11% at 500 mA cm^?2 (the lowest roll‐off known so far) where the EQE is still over 11%.     

Light Extraction Efficiency Enhancement of Colloidal Quantum Dot Light‐Emitting Diodes Using Large‐Scale Nanopillar Arrays

A colloidal quantum dot light‐emitting diode (QLED) is reported with substantially enhanced light extraction efficiency by applying a layer of large‐scale, low‐cost, periodic nanopillar arrays. Zinc oxide nanopillars are grown on the glass surface of the substrate using a simple, efficient method of non‐wetting templates. With the layer of ZnO nanopillar array as an optical outcoupling medium, a record high current efficiency (CE) of 26.6 cd/A is achieved for QLEDs. Consequently, the corresponding external quantum efficiency (EQE) of 9.34% reaches the highest EQE value for green‐emitting QLEDs. Also, the underlying physical mechanisms enabling the enhanced light‐extraction are investigated, which leads to an excellent agreement of the numerical results based on the mode theory with the experimental measurements. This study is the first account for QLEDs offering detailed insight into the light extraction efficiency enhancement of QLED devices. The method demonstrated here is intended to be useful not only for opening up a ubiquitous strategy for designing high‐performance QLEDs but also with respect to fundamental research on the light extraction in QLEDs.     

Efficient Nondoped Blue Fluorescent Organic Light‐Emitting Diodes (OLEDs) with a High External Quantum Efficiency of 9.4% @ 1000 cd m−2 Based on Phenanthroimidazole−Anthracene Derivative

Organic light‐emitting diodes (OLEDs) can promise flexible, light weight, energy conservation, and many other advantages for next‐generation display and lighting applications. However, achieving efficient blue electroluminescence still remains a challenge. Though both phosphorescent and thermally activated delayed fluorescence materials can realize high‐efficiency via effective triplet utilization, they need to be doped into appropriate host materials and often suffer from certain degree of efficiency roll‐off. Therefore, developing efficient blue‐emitting materials suitable for nondoped device with little efficiency roll‐off is of great significance in terms of practical applications. Herein, a phenanthroimidazole?anthracene blue‐emitting material is reported that can attain high efficiency at high luminescence in nondoped OLEDs. The maximum external quantum efficiency (EQE) of nondoped device is 9.44% which is acquired at the luminescence of 1000 cd m^?2. The EQE is still as high as 8.09% even the luminescence reaches 10 000 cd m^?2. The maximum luminescence is ≈57 000 cd m^?2. The electroluminescence (EL) spectrum shows an emission peak of 470 nm and the Commission International de L'Eclairage (CIE) coordinates is (0.14, 0.19) at the voltage of 7 V. To the best of the knowledge, this is among the best results of nondoped blue EL devices.     

Over 30% External Quantum Efficiency Light‐Emitting Diodes by Engineering Quantum Dot‐Assisted Energy Level Match for Hole Transport Layer

In the study of hybrid quantum dot light‐emitting diodes (QLEDs), even for state‐of‐the‐art achievement, there still exists a long‐standing charge balance problem, i.e., sufficient electron injection versus inefficient hole injection due to the large valence band offset of quantum dots (QDs) with respect to the adjacent carrier transport layer. Here the dedicated design and synthesis of high luminescence Zn_1?x Cd_xSe/ZnSe/ZnS QDs is reported by precisely controlled shell growth, which have matched energy level with the adjacent hole transport layer in QLEDs. As emitters, such Zn_1?xCd_xSe‐ based QLEDs exhibit peak external quantum efficiencies (EQE) of up to 30.9%, maximum brightness of over 334 000 cd m^?2, very low efficiency roll‐off at high current density (EQE ≈25% @ current density of 150 mA cm^?2), and operational lifetime extended to ≈1 800 000 h at 100 cd m^?2. These extraordinary performances make this work the best among all solution‐processed QLEDs reported in literature so far by achieving simultaneously high luminescence and balanced charge injection. These major advances are attributed to the combination of an intermediate ZnSe layer with an ultrathin ZnS outer layer as the shell materials and surface modification with 2‐ethylhexane‐1‐thiol, which can dramatically improve hole injection efficiency and thus lead to more balanced charge injection.     

Alternating‐Current MXene Polymer Light‐Emitting Diodes

MXenes (Ti₃C₂) are 2D transition‐metal carbides and carbonitrides with high conductivity and optical transparency. However, transparent MXene electrodes suitable for polymer light‐emitting diodes (PLEDs) have rarely been demonstrated. With the discovery of the excellent electrical stability of MXene under an alternating current (AC), herein, PLEDs that employ MXene electrodes and exhibit high performance under AC operation (AC MXene PLEDs) are presented. The PLED exhibits a turn‐on voltage, current efficiency, and brightness of 2.1 V, 7 cd A^?1, and 12 547 cd m^?2, respectively, when operated under AC with a frequency of 1 kHz. The results indicate that the undesirable electric breakdown associated with heat arising from the poor interface of the MXene with a hole transport layer in the direct‐current mode is efficiently suppressed by the transient injection of carriers accompanied by the alternating change of the electric polarity under the AC, giving rise to reliable light emission with a high efficiency. The solution‐processable MXene electrode can be readily fabricated on a flexible polymer substrate, allowing for the development of a mechanically flexible AC MXene PLED with a higher performance than flexible PLEDs employing solution‐processed nanomaterial‐based electrodes such as carbon nanotubes, reduced graphene oxide, and Ag nanowires.     

Recent Progress in High‐Efficiency Blue‐Light‐Emitting Materials for Organic Light‐Emitting Diodes

Organic light‐emitting diodes (OLEDs) are increasingly used in displays replacing traditional flat panel displays; e.g., liquid crystal displays. Especially, the paradigm shifts in displays from rigid to flexible types accelerated the market change from liquid crystal displays to OLEDs. However, some critical issues must be resolved for expansion of OLED use, of which blue device performance is one of the most important. Therefore, recent OLED material development has focused on the design, synthesis and application of high‐efficiency and long‐life blue emitters. Well‐known blue fluorescent emitters have been modified to improve their efficiency and lifetime, and blue phosphorescent emitters are being investigated to overcome the lifetime issue. Recently, thermally activated delayed fluorescent emitters have received attention due to the potential of high‐efficiency and long‐living emitters. Therefore, it is timely to review the recent progress and future prospects of high‐efficiency blue emitters. In this feature article, we summarize recent developments in blue fluorescent, phosphorescent and thermally activated delayed fluorescent emitters, and suggest key issues for each emitter and future development strategies.     

Highly Efficient Quantum Dot Light‐Emitting Diodes by Inserting Multiple Poly(methyl methacrylate) as Electron‐Blocking Layers

This work presents a new device architecture integrating multiple poly(methyl methacrylate) (PMMA) electron‐blocking layers (EBL) in quantum dot light‐emitting diodes (QD‐LEDs). The device utilizes red‐emitting CdSe/ZnS QD with a novel structure where multiple PMMA EBLs are sandwiched between a pair of QD layers. A systematic optimization of QD‐LED structures has shown that a device including two PMMA and three QD layers performs the best, achieving a current efficiency of 17.8 cd A^?1 and a luminance of 194 038 cd m^?2. Numerical simulation of a simplified model of the proposed QD‐LED structure verifies that the structure consisting of two PMMA and three QD layers provides significant improvement in electroluminescent intensity. The simulation provides further insight into the origin of the effect of the PMMA EBL by showing that the addition of PMMA EBL reduces the electron leakage from the active QD region and enhances electron confinement, leading to an increased electron concentration in the QD active layers and a higher radiative recombination rate. The experimental and theoretical studies presented in this work demonstrate that multiple layers of PMMA can act as efficient EBLs in the fabrication of QD‐LEDs of improved performance.     

Energy Level Modification with Carbon Dot Interlayers Enables Efficient Perovskite Solar Cells and Quantum Dot Based Light‐Emitting Diodes

Controlling the transport and minimizing charge carrier trapping at interfaces is crucial for the performance of various optoelectronic devices. Here, how electronic properties of stable, abundant, and easy‐to‐synthesized carbon dots (CDs) are controlled via the surface chemistry through a chosen ratio of their precursors citric acid and ethylenediamine are demonstrated. This allows to adjust the work function of indium tin oxide (ITO) films over the broad range of 1.57 eV, through deposition of thin CD layers. CD modifiers with abundant amine groups reduce the ITO work function from 4.64 to 3.42 eV, while those with abundant carboxyl groups increase it to 4.99 eV. Using CDs to modify interfaces between metal oxide (SnO₂ and ZnO) films and active layers of solar cells and light‐emitting diodes (LEDs) allows to significantly improve their performance. Power conversion efficiency of CH₃NH₃PbI₃ perovskite solar cells increases from 17.3% to 19.5%; the external quantum efficiency of CsPbI₃ perovskite quantum dot LEDs increases from 4.8% to 10.3%; and that of CdSe/ZnS quantum dot LEDs increases from 8.1% to 21.9%. As CD films are easily fabricated in air by solution processing, the approach paves the way to a simplified manufacturing of large‐area and low‐cost optoelectronic devices.     

Extremely Efficient White Organic Light‐Emitting Diodes for General Lighting

Highly power‐efficient white organic light‐emitting diodes (OLEDs) are still challenging to make for applications in high‐quality displays and general lighting due to optical confinement and energy loss during electron‐photon conversion. Here, an efficient white OLED structure is shown that combines deterministic aperiodic nanostructures for broadband quasi‐omnidirectional light extraction and a multilayer energy cascade structure for energy‐efficient photon generation. The external quantum efficiency and power efficiency are raised to 54.6% and 123.4 lm W^?1 at 1000 cd m^?2. An extremely small roll‐off in efficiency at high luminance is also obtained, yielding a striking value of 106.5 lm W^?1 at 5000 cd m^?2. In addition to a substantial increase in efficiency, this device structure simultaneously offers the superiority of angular color stability over the visible wavelength range compared to conventional OLEDs. It is anticipated that these findings could open up new opportunities to promote white OLEDs for commercial applications.     

Binaphthyl‐Containing Green‐ and Red‐Emitting Molecules for Solution‐Processable Organic Light‐Emitting Diodes

Strong intermolecular interactions usually result in decreases in solubility and fluorescence efficiency of organic molecules. Therefore, amorphous materials are highly pursued when designing solution‐processable, electroluminescent organic molecules. In this paper, a non‐planar binaphthyl moiety is presented as a way of reducing intermolecular interactions and four binaphthyl‐containing molecules ( BNCM s): green‐emitting BBB and TBT as well as red‐emitting BTBTB and TBBBT , are designed and synthesized. The photophysical and electrochemical properties of the molecules are systematically investigated and it is found that TBT , TBBBT , and BTBTB solutions show high photoluminescence (PL) quantum efficiencies of 0.41, 0.54, and 0.48, respectively. Based on the good solubility and amorphous film‐forming ability of the synthesized BNCM s, double‐layer structured organic light‐emitting diodes (OLEDs) with BNCM s as emitting layer and poly(N‐vinylcarbazole) (PVK) or a blend of poly[N,N′‐bis(4‐butylphenyl)‐N,N′‐bis(phenyl)benzidine] and PVK as hole‐transporting layer are fabricated by a simple solution spin‐coating procedure. Amongst those, the BTBTB based OLED, for example, reaches a high maximum luminance of 8315 cd · m⁻² and a maximum luminous efficiency of 1.95 cd · A⁻¹ at a low turn‐on voltage of 2.2 V. This is one of the best performances of a spin‐coated OLED reported so far. In addition, by doping the green and red BNCM s into a blue‐emitting host material poly(9,9‐dioctylfluorene‐2,7‐diyl) high performance white light‐emitting diodes with pure white light emission and a maximum luminance of 4000 cd · m⁻² are realized.     

Transparent InP Quantum Dot Light‐Emitting Diodes with ZrO2 Electron Transport Layer and Indium Zinc Oxide Top Electrode

Because of outstanding optical properties and non‐vacuum solution processability of colloidal quantum dot (QD) semiconductors, many researchers have developed various light emitting diodes (LEDs) using QD materials. Until now, the Cd‐based QD‐LEDs have shown excellent properties, but the eco‐friendly QD semiconductors have attracted many attentions due to the environmental regulation. And, since there are many issues about the reliability of conventional QD‐LEDs with organic charge transport layers, a stable charge transport layer in various conditions must be developed for this reason. This study proposes the organic/inorganic hybrid QD‐LEDs with Cd‐free InP QDs as light emitting layer and inorganic ZrO₂ nanoparticles as electron transport layer. The QD‐LED with bottom emission structure shows the luminescence of 530 cd m^?2 and the current efficiency of 1 cd/A. To realize the transparent QD‐LED display, the two‐step sputtering process of indium zinc oxide (IZO) top electrode is applied to the devices and this study could fabricate the transparent QD‐LED device with the transmittance of more than 74% for whole device array. And when the IZO top electrode with high work‐function is applied to top transparent anode, the device could maintain the current efficiency within the driving voltage range without well‐known roll‐off phenomenon in QD‐LED devices.     

Electric‐Field‐Assisted Charge Generation and Separation Process in Transition Metal Oxide‐Based Interconnectors for Tandem Organic Light‐Emitting Diodes

The charge generation and separation process in transition metal oxide (TMO)‐based interconnectors for tandem organic light‐emitting diodes (OLEDs) is explored using data on electrical and spectral emission properties, interface energetics, and capacitance characteristics. The TMO‐based interconnector is composed of MoO₃ and cesium azide (CsN₃)‐doped 4,7‐diphenyl‐1,10‐phenanthroline (BPhen) layers, where CsN₃ is employed to replace the reactive metals as an n‐dopant due to its air stability and low deposition temperature. Experimental evidences identify that spontaneous electron transfer occurs in a vacuum‐deposited MoO₃ layer from various defect states to the conduction band via thermal diffusion. The external electric‐field induces the charge separation through tunneling of generated electrons and holes from MoO₃ into the neighboring CsN₃‐doped BPhen and hole‐transporting layers, respectively. Moreover, the impacts of constituent materials on the functional effectiveness of TMO‐based interconnectors and their influences on carrier recombination processes for light emission have also been addressed.