Stable White Light‐Emitting Biocomposite Films

The demonstration of reliable and stable white light‐emitting diodes (LEDs) is one of the main technological challenges of the LED industry. This is usually accomplished by incorporation of light‐emitting rare‐earth elements (REEs) compounds within an external polymeric coating of a blue LED allowing the generation of white light. However, due to both environmental and cost issues, the development of low‐cost REE‐free coatings, which exhibit competitive performance compared to conventional white LED is of great importance. In this work, the formation of an REE‐free white LED coating is demonstrated. This biocomposite material, composed of biological (crystalline nanocellulose and porcine gastric mucin) and organic (light‐emitting dyes) compounds, exhibits excellent optical and mechanical properties as well as resistance to heat, humidity, and UV radiation. The coating is further used to demonstrate a working white LED by incorporating it within a commercial blue LED.     

Three‐Dimensional Branched Nanowire Heterostructures as Efficient Light‐Extraction Layer in Light‐Emitting Diodes

A facile method to fabricate three‐dimensional branched ZnO/MgO nanowire heterostructures and their application as the efficient light‐extraction layer in light‐emitting diodes are reported. The branched MgO nanowires are produced on the hydrothermally‐grown ZnO nanowires with a small tapering angle towards the tip (≈6°), by the oblique angle flux incidence of MgO. The structural evolution during the growth verifies the formation of the MgO nanoscale islands with strong (111) preferred orientation on very thin (5–7 nm) MgO (110) layer. The MgO nanobranches, then grown on the islands, are polycrystalline consisting of many grains oriented in specific directions of <200> and <220>, supported by the nucleation theory. The LEDs with the branched ZnO/MgO nanowire arrays show a remarkable enhancement in the light output power by 21% compared with that of LEDs with pristine ZnO nanowires. Theoretical calculations using a finite‐difference time‐domain method reveal that the nanostructure is very effective in breaking the wave‐guiding mode inside the ZnO nanowires, extracting more light especially in radial direction through the MgO nanobranches.     

High‐Performance,Phosphorescent, Top‐Emitting Organic Light‐Emitting Diodes with p–i–n Homojunctions

High‐performance, green, orange, and red top‐emitting organic light‐emitting diodes (TOLEDs) with p–i–n homojunction are demonstrated. An excellent ambipolar host, 2,5‐bis(2‐(9H‐carbazol‐9‐yl)phenyl)‐1,3,4‐oxadiazole (o‐CzOXD), which has good thermal and morphological stabilities, a high triplet energy level, and equally high electron and hole mobilities, is chosen as the organic host material for the homojunction devices. By electrical doping, the carrier injection and transporting characteristics are greatly improved. The optical structure is optimized in view of light emission of different colors to enhance the color purity and improve the view characte­ristics. As a result, high efficiency p–i–n homojunction TOLEDs with saturated intrinsic emission of the emitting materials and angular independence of the emission are realized. The performances of these p–i–n homojunction TOLEDs are even higher than the multi‐layer heterojunction bottom‐emitting devices using the same emitting layers.     

White Light‐Emitting Diode From Sb‐Doped p‐ZnO Nanowire Arrays/n‐GaN Film

A whole interfacial transition of electrons from conduction bands of n‐type material to the acceptor levels of p‐type material makes the energy band engineering successful. It tunes intrinsic ZnO UV emission to UV‐free and warm white light‐emitting diode (W‐LED) emission with color coordinates around (0.418, 0.429) at the bias of 8–15.5 V. The W‐LED is fabricated based on antimony (Sb) doped p‐ZnO nanowire arrays/Si doped n‐GaN film heterojunction structure through one‐step chemical vapor deposition with quenching process. Element analysis shows that the doping concentration of Sb is ≈1.0%. The I–V test exhibits the formation of p‐type ZnO nanowires, and the temperature‐dependent photoluminescence measurement down to 4.65 K confirms the formation of deep levels and shallow acceptor levels after Sb‐doping. The intrinsic UV emission of ZnO at room temperature is cut off in electroluminescence emission at a bias of 4–15.5 V. The UV‐free and warm W‐LED have great potential application in green lights program, especially in eye‐protected lamp and display since television, computer, smart phone, and mobile digital equipment are widely and heavily used in modern human life, as more than 3000 h per year.     

Light‐Emitting Paper

A solution‐based fabrication of flexible and light‐weight light‐emitting devices on paper substrates is reported. Two different types of paper substrates are coated with a surface‐emitting light‐emitting electrochemical cell (LEC) device: a multilayer‐coated specialty paper with an intermediate surface roughness of 0.4 μm and a low‐end and low‐cost copy paper with a large surface roughness of 5 μm. The entire device fabrication is executed using a handheld airbrush, and it is notable that all of the constituent layers are deposited from solution under ambient air. The top‐emitting paper‐LECs are highly flexible, and display a uniform light emission with a luminance of 200 cd m^?2 at a current conversion efficacy of 1.4 cd A^?1.     

Quasi‐2D Inorganic CsPbBr3 Perovskite for Efficient and Stable Light‐Emitting Diodes

Metal halide perovskites are rising as a competitive material for next‐generation light‐emitting diodes (LEDs). However, the development of perovskite LEDs is impeded by their fast carriers diffusion and poor stability in bias condition. Herein, quasi‐2D CsPbBr₃ quantum wells homogeneously surrounded by inorganic crystalline Cs₄PbBr₆ of large bandgap are grown. The centralization of carriers in nanoregion facilitates radiative recombination and brings much enhanced luminescence quantum yield. The external quantum efficiency and luminescence intensity of the LEDs based on this nanocomposite are one order of magnitude higher than the conventional low‐dimensional perovskite. Meanwhile, the use of inorganic nanocomposite materials brings much improved device operation lifetime under constant electrical field.     

Role of Excess FAI in Formation of High‐Efficiency FAPbI3‐Based Light‐Emitting Diodes

Introducing extensively excess ammonium halides when forming perovskites has recently been demonstrated as an effective approach to improve the performance of perovskite light‐emitting diodes (PeLEDs). Here, Cs_0.17FA_0.83PbI_2.5Br_0.5 is used as a model system to elucidate the impact of introducing excess formamidinium iodide (FAI) on the crystallization process of the perovskite film and operation of the corresponding PeLED. The excess FAI ratio is varied from 0 to 120 mol% and the crystallization process of the perovskite through in situ absorbance, in situ photoluminescence, and ex situ X‐ray diffraction measurements is systematically monitored. The results suggest that excess FAI triggers formation of a compact wide‐bandgap intermediate phase in the as‐deposited film, which then transforms to isolated and highly crystalline perovskite grains upon annealing. Using excitation correlation photoluminescence spectroscopy it is found that excess FAI results in a lower density of deep trap states and therefore a reduction of nonradiative losses in the material. This leads to a greatly enhanced maximum external quantum efficiency (EQE) from 0.25% (stoichiometric) to 12.7% (90 mol% excess). Furthermore, the FAI‐excess perovskite film is optimized with Pb(SCN)₂ and 5‐ammonium valeric acid iodide additives and achieve a record radiance of 965 W Sr^?1 m^?2 for near‐infrared PeLEDs and a high EQE of 17.4%.     

Amine‐Free Synthesis of Cesium Lead Halide Perovskite Quantum Dots for Efficient Light‐Emitting Diodes

Cesium lead halide perovskite quantum dots (PQDs) have attracted significant interest for optoelectronic applications in view of their high brightness and narrow emission linewidth at visible wavelengths. A remaining challenge is the degradation of PQDs during purification from the synthesis solution. This is attributed to proton transfer between oleic acid and oleylamine surface capping agents that leads to facile ligand loss. Here, a new synthetic method is reported that enhances the colloidal stability of PQDs by capping them solely using oleic acid (OA). Quaternary alkylammonium halides are used as precursors, eliminating the need for oleylamine. This strategy enhances the colloidal stability of OA capped PQDs during purification, allowing us to remove excess organic content in thin films. Inverted red, green, and blue PQD light‐emitting diodes (LED) are fabricated for the first time with solution‐processed polymer‐based hole transport layers due to higher robustness of OA capped PQDs to solution processing. The blue and green LEDs exhibit threefold and tenfold improved external quantum efficiency (EQE), respectively, compared to prior related reports for amine/ammonium capped cross‐linked PQDs. The brightest blue LED based on all inorganic CsPb(Br_1?xCl_x)₃ PQDs is also reported.     

Candle Light‐Style Organic Light‐Emitting Diodes

In response to the call for a physiologically‐friendly light at night that shows low color temperature, a candle light‐style organic light emitting diode (OLED) is developed with a color temperature as low as 1900 K, a color rendering index (CRI) as high as 93, and an efficacy at least two times that of incandescent bulbs. In addition, the device has a 80% resemblance in luminance spectrum to that of a candle. Most importantly, the sensationally warm candle light‐style emission is driven by electricity in lieu of the energy‐wasting and greenhouse gas emitting hydrocarbon‐burning candles invented 5000 years ago. This candle light‐style OLED may serve as a safe measure for illumination at night. Moreover, it has a high color rendering index with a decent efficiency.     

Small Molecules in Light‐Emitting Electrochemical Cells: Promising Light‐Emitting Materials

Light‐emitting electrochemical cells (LECs) are solid‐state lighting devices that convert electric current to light within electroluminescent organic semiconductors, and these devices have recently attracted significant attention. Introduced in 1995, LECs are considered a great breakthrough in the field of light‐emitting devices for their applications in scalable and adaptable fabrication processes aimed at producing cost‐efficient devices. Since then, LECs have evolved through the discovery of new suitable emitters, understanding the working mechanism of devices, and the development of various fabrication methods. LECs are best known for their simple architecture and easy, low‐cost fabrication techniques. The key feature of their fabrication is the use of air stable electrodes and a single active layer consisting of mobile ions that enable efficient charge injection and transport processes within LEC devices. More importantly, LEC devices can be operated at low voltages with high efficiencies, contributing to their widespread interest. This review provides a general overview of the development of LECs and discusses how small molecules can be utilized in LEC applications by overcoming the use of traditional lighting materials like polymers and ionic transition metal complexes. The achievements of each study concerning small molecule LECs are discussed.     

High‐Efficiency and Stable Quantum Dot Light‐Emitting Diodes Enabled by a Solution‐Processed Metal‐Doped Nickel Oxide Hole Injection Interfacial Layer

Stabilization is one critical issue that needs to be improved for future application of colloidal quantum dot (QD)‐based light‐emitting diodes (QLEDs). This study reports highly efficient and stable QLEDs based on solution‐processsed, metal‐doped nickel oxide films as hole injection layer (HIL). Several kinds of metal dopants (Li, Mg, and Cu) are introduced to improve the hole injection capability of NiO films. The resulting device with Cu:NiO HIL exhibits superior performance compared to the state‐of‐the‐art poly(3,4‐ethylenedioxythiophene):poly(styrene‐sulfonate) (PEDOT:PSS)‐based QLEDs, with a maximum current efficiency and external quantum efficiency of 45.7 cd A^?1 and 10.5%, respectively. These are the highest values reported so far for QLEDs with PEDOT:PSS‐free normal structure. Meanwhile, the resulting QLED shows a half‐life time of 87 h at an initial luminance of 5000 cd m^?2, almost fourfold longer than that of the PEDOT:PSS‐based device.     

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.     

High‐Efficient Deep‐Blue Light‐Emitting Diodes by Using High Quality ZnxCd1‐xS/ZnS Core/Shell Quantum Dots

High‐quality violet‐blue emitting Zn_xCd_1‐xS/ZnS core/shell quantum dots (QDs) are synthesized by a new method, called “nucleation at low temperature/shell growth at high temperature”. The resulting nearly monodisperse Zn_xCd_1‐xS/ZnS core/shell QDs have high PL quantum yield (near to 100%), high color purity (FWHM) <25 nm), good color tunability in the violet‐blue optical window from 400 to 470 nm, and good chemical/photochemical stability. More importantly, the new well‐established protocols are easy to apply to large‐scale synthesis; around 37 g Zn_xCd_1‐xS/ZnS core/shell QDs can be easily synthesized in one batch reaction. Highly efficient deep‐blue quantum dot‐based light‐emitting diodes (QD‐LEDs) are demonstrated by employing the Zn_xCd_1‐xS/ZnS core/shell QDs as emitters. The bright and efficient QD‐LEDs show a maximum luminance up to 4100 cd m^?2, and peak external quantum efficiency (EQE) of 3.8%, corresponding to 1.13 cd A^?1 in luminous efficiency. Such high value of the peak EQE can be comparable with OLED technology. These results signify a remarkable progress, not only in the synthesis of high‐quality QDs but also in QD‐LEDs that offer a practicle platform for the realization of QD‐based violet‐blue display and lighting.     

Work‐Function Engineering of Graphene Anode by Bis(trifluoromethanesulfonyl)amide Doping for Efficient Polymer Light‐Emitting Diodes

Graphene has been considered to be a potential alternative transparent and flexible electrode for replacing commercially available indium tin oxide (ITO) anode. However, the relatively high sheet resistance and low work function of graphene compared with ITO limit the application of graphene as an anode for organic or polymer light‐emitting diodes (OLEDs or PLEDs). Here, flexible PLEDs made by using bis(trifluoromethanesulfonyl)amide (TFSA, [CF₃SO₂]₂NH) doped graphene anodes are demonstrated to have low sheet resistance and high work function. The graphene is easily doped with TFSA by means of a simple spin‐coating process. After TFSA doping, the sheet resistance of the TFSA‐doped five‐layer graphene, with optical transmittance of ≈88%, is as low as ≈90 Ω sq^?1. The maximum current efficiency and power efficiency of the PLED fabricated on the TFSA‐doped graphene anode are 9.6 cd A^?1 and 10.5 lm W^?1, respectively; these values are markedly higher than those of the PLED fabricated on pristine graphene anode and comparable to those of an ITO anode.     

Blue‐Light‐Emitting Oligoquinolines: Synthesis,Properties, and High‐Efficiency Blue‐Light‐Emitting Diodes

The synthesis, photophysics, cyclic voltammetry, and highly efficient blue electroluminescence of a series of four new n‐type conjugated oligomers, 6,6′‐bis(2,4‐diphenylquinoline) (B1PPQ), 6,6′‐bis(2‐(4‐tert‐butylphenyl)‐4‐phenylquinoline) (BtBPQ), 6,6′‐bis(2‐p‐biphenyl)‐4‐phenylquinoline) (B2PPQ), and 6,6′‐bis((3,5‐diphenylbenzene)‐4‐phenylquinoline) (BDBPQ) is reported. The oligoquinolines have high glass‐transition temperatures (T_g ≥ 133 °C), reversible electrochemical reduction, and high electron affinities (2.68–2.81 eV). They emit blue photoluminescence with 0.73–0.94 quantum yields and 1.06–1.42 ns lifetimes in chloroform solutions. High‐performance organic light‐emitting diodes (OLEDs) with excellent blue chromaticity coordinates are achieved from all the oligoquinolines. OLEDs based on B2PPQ as the blue emitter give the best performance with a high brightness (19 740 cd m^–2 at 8.0 V), high efficiency (7.12 cd A^–1 and 6.56 % external quantum efficiency at 1175 cd m^–2), and excellent blue color purity as judged by the Commission Internationale de L'Eclairage (CIE) coordinates (x = 0.15,y = 0.16). These results represent the best efficiency of blue OLEDs from neat fluorescent organic emitters reported to date. These results demonstrate the potential of oligoquinolines as emitters and electron‐transport materials for developing high‐performance blue OLEDs.     

Self‐Heating in Light‐Emitting Electrochemical Cells

Electroluminescent devices become warm during operation, and their performance can, therefore, be severely limited at high drive current density. Herein, the effects of this self‐heating on the operation of a light‐emitting electrochemical cell (LEC) are systematically studied. A drive current density of 50 mA cm^?2 can result in a local device temperature for a free‐standing LEC that exceeds 50 °C within a short period of operation, which in turn induces premature device degradation as manifested in the rapidly decreasing luminance and increasing voltage. Furthermore, this undesired self‐heating for a free‐standing thin‐film LEC can be suppressed by the employment of a device architecture featuring high thermal conductance and a small emission‐area fill factor, since the corresponding improved heat conduction to the nonemissive regions facilitates more efficient heat transfer to the ambient surroundings. In addition, the reported differences in performance between small‐area and large‐area LECs as well as between flexible‐plastic and rigid‐glass LECs are rationalized, culminating in insights that can be useful for the rational design of LEC devices with suppressed self‐heating and high performance.     

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.     

Optimization of Orange‐Emitting Electrophosphorescent Copolymers for Organic Light‐Emitting Diodes

Orange‐emitting phosphorescent copolymers containing iridium complexes and bis(carbazolyl)fluorene groups in their side chains are employed as the emissive layer in multilayer organic light‐emitting diodes (OLEDs). The efficiency of the OLED devices is optimized by varying characteristics of the copolymers: the molecular weight, the iridium loading level, and the nature and length of the linker between the side chains and the polymer backbone. A maximum efficiency of 4.9 ± 0.4%, 8.8 ± 0.7 cd A⁻¹ at 100 cd m⁻² is achieved with an optimized copolymer.