White Organic Light‐Emitting Devices for Solid‐State Lighting

White organic light‐emitting devices (WOLEDs) have advanced over the last twelve years to the extent that these devices are now being considered as efficient solid‐state lighting sources. Initially, WOLEDs were targeted towards display applications for use primarily as liquid‐crystal display backlights. Now, their power efficiencies have surpassed those of incandescent sources due to improvements in device architectures, synthesis of novel materials, and the incorporation of electrophosphorescent emitters. This review discusses the advantages and disadvantages of several WOLED architectures in terms of efficiency and color quality. Hindrances to their widespread acceptance as solid‐state lighting sources are also noted.     

Multiphotoluminescence from a Triphenylamine Derivative and Its Application in White Organic Light‐Emitting Diodes Based on a Single Emissive Layer

White organic light‐emitting diode (WOLED) technology has attracted considerable attention because of its potential use as a next‐generation solid‐state lighting source. However, most of the reported WOLEDs that employ the combination of multi‐emissive materials to generate white emission may suffer from color instability, high material cost, and a complex fabrication procedure which can be diminished by the single‐emitter‐based WOLED. Herein, a color‐tunable material, tris(4‐(phenylethynyl)phenyl)amine (TPEPA), is reported, whose photoluminescence (PL) spectrum is altered by adjusting the thermal annealing temperature nearly encompassing the entire visible spectra. Density functional theory calculations and transmission electron microscopy results offer mechanistic understanding of the PL redshift resulting from thermally activated rotation of benzene rings and rotation of 4‐(phenylethynyl) phenyl)amine connected to the central nitrogen atom that lead to formation of ordered molecular packing which improves the π–π stacking degree and increases electronic coupling. Further, by precisely controlling the annealing time and temperature, a white‐light OLED is fabricated with the maximum external quantum efficiency of 3.4% with TPEPA as the only emissive molecule. As far as it is known, thus far, this is the best performance achieved for single small organic molecule based WOLED devices.     

Correlation of recombination zone and device performances of phosphorescent white organic light-emitting diodes

We demonstrate a general method for tuning the color performance of white organic light-emitting diodes (WOLEDs) by inserting 0.5 nm thick red emitting layer in different location of blue phosphorescent emitting layer. The Commission Internationale de L'Eclairage (CIE) coordinates of WOLEDs were dependent on the position of red emitting layer and they were correlated with recombination zone of the blue phosphorescent emitting layer. Red shift of white CIE was observed as the location of red emitting layer get close to recombination zone of blue emitting layer. In addition, CIE of WOLEDs was kept stable between 100 cd/m² and 10,000 cd/m².     

Single-Molecular White-Light Emitters and Their Potential WOLED Applications

White organic light-emitting diodes (WOLEDs) are superior to traditional incandescent light bulbs and compact fluorescent lamps in terms of their merits in ensuring pure white-light emission, low-energy consumption, large-area thin-film fabrication, etc. Unfortunately, WOLEDs based on multilayered or multicomponent (red, green, and blue (RGB)) emissive layers can suffer from some remarkable disadvantages, such as intricate device fabrication and voltage-dependent emission color, etc. Single molecules, which can emit white light, can be used to replace multiple emitters, leading to a simplified fabrication process, stable and reproducible WOLEDs. Recently, the performance of WOLEDs by using single molecules is catching up with that of the state-of-the-art devices fabricated by multicomponent emitters. Therefore, an increasing attention has been paid on single white-light-emitting materials for efficient WOLEDs. In this review, different mechanisms of white-light emission from a single molecule and the performance of single-molecule-based WOLEDs are collected and expounded, hoping to light up the interesting subject on single-molecule white-light-emitting materials, which have great potential as white-light emitters for illumination and lighting applications in the world.     

Purely Organic Thermally Activated Delayed Fluorescence Materials for Organic Light‐Emitting Diodes

The design of thermally activated delayed fluorescence (TADF) materials both as emitters and as hosts is an exploding area of research. The replacement of phosphorescent metal complexes with inexpensive organic compounds in electroluminescent (EL) devices that demonstrate comparable performance metrics is paradigm shifting, as these new materials offer the possibility of developing low‐cost lighting and displays. Here, a comprehensive review of TADF materials is presented, with a focus on linking their optoelectronic behavior with the performance of the organic light‐emitting diode (OLED) and related EL devices. TADF emitters are cross‐compared within specific color ranges, with a focus on blue, green–yellow, orange–red, and white OLEDs. Organic small‐molecule, dendrimer, polymer, and exciplex emitters are all discussed within this review, as is their use as host materials. Correlations are provided between the structure of the TADF materials and their optoelectronic properties. The success of TADF materials has ushered in the next generation of OLEDs.     

Organic Light‐Emitting Transistors: Materials,Device Configurations,and Operations

Organic light‐emitting transistors (OLETs) represent an emerging class of organic optoelectronic devices, wherein the electrical switching capability of organic field‐effect transistors (OFETs) and the light‐generation capability of organic light‐emitting diodes (OLEDs) are inherently incorporated in a single device. In contrast to conventional OFETs and OLEDs, the planar device geometry and the versatile multifunctional nature of OLETs not only endow them with numerous technological opportunities in the frontier fields of highly integrated organic electronics, but also render them ideal scientific scaffolds to address the fundamental physical events of organic semiconductors and devices. This review article summarizes the recent advancements on OLETs in light of materials, device configurations, operation conditions, etc. Diverse state‐of‐the‐art protocols, including bulk heterojunction, layered heterojunction and laterally arranged heterojunction structures, as well as asymmetric source‐drain electrodes, and innovative dielectric layers, which have been developed for the construction of qualified OLETs and for shedding new and deep light on the working principles of OLETs, are highlighted by addressing representative paradigms. This review intends to provide readers with a deeper understanding of the design of future OLETs.     

Toward Environmentally Robust Organic Electronics: Approaches and Applications

Recent interest in flexible electronics has led to a paradigm shift in consumer electronics, and the emergent development of stretchable and wearable electronics is opening a new spectrum of ubiquitous applications for electronics. Organic electronic materials, such as π‐conjugated small molecules and polymers, are highly suitable for use in low‐cost wearable electronic devices, and their charge‐carrier mobilities have now exceeded that of amorphous silicon. However, their commercialization is minimal, mainly because of weaknesses in terms of operational stability, long‐term stability under ambient conditions, and chemical stability related to fabrication processes. Recently, however, many attempts have been made to overcome such instabilities of organic electronic materials. Here, an overview is provided of the strategies developed for environmentally robust organic electronics to overcome the detrimental effects of various critical factors such as oxygen, water, chemicals, heat, and light. Additionally, molecular design approaches to π‐conjugated small molecules and polymers that are highly stable under ambient and harsh conditions are explored; such materials will circumvent the need for encapsulation and provide a greater degree of freedom using simple solution‐based device‐fabrication techniques. Applications that are made possible through these strategies are highlighted.     

OLEDs: Degradation Mechanisms in Small‐Molecule and Polymer Organic Light‐Emitting Diodes (Adv. Mater. 34/2010)

Degradation in organic light‐emitting diodes (OLEDs) is a complex problem. Depending upon the materials and the device architectures used, the degradation mechanism can be very different. In this Progress Report, using examples in both small molecule and polymer OLEDs, the different degradation mechanisms in two types of devices are examined. Some of the extrinsic and intrinsic degradation mechanisms in OLEDs are reviewed, and recent work on degradation studies of both small‐molecule and polymer OLEDs is presented. For small‐molecule OLEDs, the operational degradation of exemplary fluorescent devices is dominated by chemical transformations in the vicinity of the recombination zone. The accumulation of degradation products results in coupled phenomena of luminance‐efficiency loss and operating‐voltage rise. For polymer OLEDs, it is shown how the charge‐transport and injection properties affect the device lifetime. Further, it is shown how the charge balance is controlled by interlayers at the anode contact, and their effects on the device lifetime are discussed.     

Degradation Mechanisms in Small‐Molecule and Polymer Organic Light‐Emitting Diodes

Degradation in organic light‐emitting diodes (OLEDs) is a complex problem. Depending upon the materials and the device architectures used, the degradation mechanism can be very different. In this Progress Report, using examples in both small molecule and polymer OLEDs, the different degradation mechanisms in two types of devices are examined. Some of the extrinsic and intrinsic degradation mechanisms in OLEDs are reviewed, and recent work on degradation studies of both small‐molecule and polymer OLEDs is presented. For small‐molecule OLEDs, the operational degradation of exemplary fluorescent devices is dominated by chemical transformations in the vicinity of the recombination zone. The accumulation of degradation products results in coupled phenomena of luminance‐efficiency loss and operating‐voltage rise. For polymer OLEDs, it is shown how the charge‐transport and injection properties affect the device lifetime. Further, it is shown how the charge balance is controlled by interlayers at the anode contact, and their effects on the device lifetime are discussed.     

Thermally Activated Delayed Fluorescence Materials Towards the Breakthrough of Organoelectronics

The design and characterization of thermally activated delayed fluorescence (TADF) materials for optoelectronic applications represents an active area of recent research in organoelectronics. Noble metal‐free TADF molecules offer unique optical and electronic properties arising from the efficient transition and interconversion between the lowest singlet (S₁) and triplet (T₁) excited states. Their ability to harvest triplet excitons for fluorescence through facilitated reverse intersystem crossing (T₁→S₁) could directly impact their properties and performances, which is attractive for a wide variety of low‐cost optoelectronic devices. TADF‐based organic light‐emitting diodes, oxygen, and temperature sensors show significantly upgraded device performances that are comparable to the ones of traditional rare‐metal complexes. Here we present an overview of the quick development in TADF mechanisms, materials, and applications. Fundamental principles on design strategies of TADF materials and the common relationship between the molecular structures and optoelectronic properties for diverse research topics and a survey of recent progress in the development of TADF materials, with a particular emphasis on their different types of metal‐organic complexes, D‐A molecules, and fullerenes, are highlighted. The success in the breakthrough of the theoretical and technical challenges that arise in developing high‐performance TADF materials may pave the way to shape the future of organoelectronics.     

25th Anniversary Article: Organic Field‐Effect Transistors: The Path Beyond Amorphous Silicon

Over the past 25 years, organic field‐effect transistors (OFETs) have witnessed impressive improvements in materials performance by 3–4 orders of magnitude, and many of the key materials discoveries have been published in Advanced Materials. This includes some of the most recent demonstrations of organic field‐effect transistors with performance that clearly exceeds that of benchmark amorphous silicon‐based devices. In this article, state‐of‐the‐art in OFETs are reviewed in light of requirements for demanding future applications, in particular active‐matrix addressing for flexible organic light‐emitting diode (OLED) displays. An overview is provided over both small molecule and conjugated polymer materials for which field‐effect mobilities exceeding > 1 cm² V^–1 s^–1 have been reported. Current understanding is also reviewed of their charge transport physics that allows reaching such unexpectedly high mobilities in these weakly van der Waals bonded and structurally comparatively disordered materials with a view towards understanding the potential for further improvement in performance in the future.     

High‐Brightness Blue and White LEDs based on Inorganic Perovskite Nanocrystals and their Composites

Inorganic metal halide perovskite nanocrystals (NCs) have been employed universally in light‐emitting applications during the past two years. Here, blue‐emission (≈470 nm) Cs‐based perovskite NCs are derived by directly mixing synthesized bromide and chloride nanocrystals with a weight ratio of 2:1. High‐brightness blue perovskite light‐emitting diodes (PeLEDs) are obtained by controlling the grain size of the perovskite films. Moreover, a white PeLED is demonstrated for the first time by blending orange polymer materials with the blue perovskite nanocrystals as the active layer. Exciton transfer from the blue nanocrystals to the orange polymers via Förster or Dexter energy transfer is analyzed through time resolved photoluminescence. By tuning the ratio between the perovskite nanocrystals and polymers, pure white light is achieved with the a CIE coordinate at (0.33,0.34).     

有机半导体照明(有机照明)研究进展

采用有机发光二极管(OLEDs)的有机半导体照明(有机照明)是绿色环保、健康安全的新型面光源,有望在固态照明领域得到广泛的应用。有机照明的发展是随着有机发光材料的不断进步而进步的。有机发光材料从最初的荧光材料发展到磷光材料以及最近提出的热活化延迟荧光材料,其性能在不断地提升。基于这些材料的白光OLEDs的性能也在不断提升。最早的白光器件基于荧光小分子材料,但是由于只能利用单线态激子发光,效率很低。随后磷光材料的引入使得白光器件的效率大幅度提升,但是由于蓝色磷光材料本身的稳定性问题,全磷光白光器件的寿命较短。为了结合荧光和磷光的优点,人们提出了荧光/磷光杂化的白光器件,这是目前最有前景的一类白光器件结构。目前针对有机照明的研究,已从早期只关注效率突破阶段,进入到综合提高效率和寿命阶段。从荧光白光、磷光白光以及荧光/磷光混合白光3个方面对有机照明的研究状况、发展趋势进行了介绍。     

Highly Efficient Thermally Activated Delayed Fluorescence via J‐Aggregates with Strong Intermolecular Charge Transfer

The development of high‐efficiency and low‐cost organic emissive materials and devices is intrinsically limited by the energy‐gap law and spin statistics, especially in the near‐infrared (NIR) region. A novel design strategy is reported for realizing highly efficient thermally activated delayed fluorescence (TADF) materials via J‐aggregates with strong intermolecular charge transfer (CT). Two organic donor–acceptor molecules with strong and planar acceptor are designed and synthesized, which can readily form J‐aggregates with strong intermolecular CT in solid states and exhibit wide‐tuning emissions from yellow to NIR. Experimental and theoretical investigations expose that the formation of such J‐aggregates mixes Frenkel excitons and CT excitons, which not only contributes to a fast radiative decay rate and a slow nonradiative decay rate for achieving nearly unity photoluminescence efficiency in solid films, but significantly decreases the energy gap between the lowest singlet and triplet excited states (≈0.3 eV) to induce high‐efficiency TADF even in the NIR region. These organic light‐emitting diodes exhibit external quantum efficiencies of 15.8% for red emission and 14.1% for NIR emission, which represent the best result for NIR organic light‐emitting diodes (OLEDs) based on TADF materials. These findings open a new avenue for the development of high‐efficiency organic emissive materials and devices based on molecular aggregates.     

Indium Phosphide‐Based Quantum Dots with Shell‐Enhanced Absorption for Luminescent Down‐Conversion

It is shown that admixing small amounts of cadmium into the shell of InP/ZnSe core/shell quantum dots results in an increased absorption of blue light and a limited redshift of the band‐edge emission. These effects reflect the reduced bandgap of (Zn,Cd)Se alloys and their smaller conduction‐band offset with InP. Nevertheless, adjusting the InP core size enables InP/ZnSe and InP/(Zn,Cd)Se quantum dots with identical emission characteristics to be made. Processing both materials into remote phosphor disks, it is demonstrated that the shell‐enhanced absorbance of InP/(Zn,Cd)Se has the double benefit of suppressing self‐absorption and reducing the amount of quantum dots by weight needed to attain a given blue‐to‐red color conversion.     

Semiconductor‐Nanocrystals‐Based White Light‐Emitting Diodes

In response to the demands for energy and the concerns of global warming and climate change, energy efficient and environmentally friendly solid‐state lighting, such as white light‐emitting diodes (WLEDs), is considered to be the most promising and suitable light source. Because of their small size, high efficiency, and long lifetime, WLEDs based on colloidal semiconductor nanocrystals (or quantum dots) are emerging as a completely new technology platform for the development of flat‐panel displays and solid‐state lighting, exhibiting the potential to replace the conventionally used incandescent and fluorescent lamps. This replacement can cut the ever‐increasing level of energy consumption, solve the problem of rapidly depleting fossil fuel reserves, and improve the quality of the global environment. In this review, the recent progress in semiconductor‐nanocrystals‐based WLEDs is highlighted, the different approaches for generating white light are compared, and the benefits and challenges of the solid‐state lighting technology are discussed.     

Introduction of Red‐Green‐Blue Fluorescent Dyes into a Metal–Organic Framework for Tunable White Light Emission

The unique features of the metal–organic frameworks (MOFs), including ultrahigh porosities and surface areas, tunable pores, endow the MOFs with special utilizations as host matrices. In this work, various neutral and ionic guest dye molecules, such as fluorescent brighteners, coumarin derivatives, 4‐(dicyanomethylene)‐2‐methyl‐6‐(p‐dimethylaminostyryl)‐4H‐pyran (DCM), and 4‐(p‐dimethylaminostyryl)‐1‐methylpyridinium (DSM), are encapsulated in a neutral MOF, yielding novel blue‐, green‐, and red‐phosphors, respectively. Furthermore, this study introduces the red‐, green‐, and blue‐emitting dyes into a MOF together for the first time, producing white‐light materials with nearly ideal Commission International ed'Eclairage (CIE) coordinates, high color‐rendering index values (up to 92%) and quantum yields (up to 26%), and moderate correlated color temperature values. The white light is tunable by changing the content or type of the three dye guests, or the excitation wavelength. Significantly, the introduction of blue‐emitting guests in the methodology makes the available MOF host more extensive, and the final white‐light output more tunable and high‐quality. Such strategy can be widely adopted to design and prepare white‐light‐emitting materials.     

Recent Advances in Alternating Current‐Driven Organic Light‐Emitting Devices

Organic light‐emitting devices (OLEDs), typically operated with constant‐voltage or direct‐current (DC) power sources, are candidates for next‐generation solid‐state lighting and displays, as they are light, thin, inexpensive, and flexible. However, researchers have focused mainly on the device itself (e.g., development of novel materials, design of the device structure, and optical outcoupling engineering), and little attention has been paid to the driving mode. Recently, an alternative concept to DC‐driven OLEDs by directly driving devices using time‐dependent voltages or alternating current (AC) has been explored. Here, the effects of different device structures of AC‐driven OLEDs, for example, double‐insulation, single‐insulation, double‐injection, and tandem structure, on the device performance are systematically investigated. The formation of excitons and the dielectric layer, which are important to achieve high‐performance AC‐driven OLEDs, are carefully considered. The importance of gaining further understanding of the fundamental properties of AC‐driven OLEDs is then discussed, especially as they relate to device physics.     

Chemical Degradation in Organic Light‐Emitting Devices: Mechanisms and Implications for the Design of New Materials

Degradation of the materials in organic light‐emitting devices (OLEDs) is the major impediment for the development of economically feasible, highly efficient and durable devices for commercial applications. Even though this chemical degradation is complex and the least understood of the different degradation modes in OLEDs, scientists were successful in providing insight into some of the responsible processes. In this progress report we will review recent advances in the elucidation of chemical degradation mechanisms: First possible reasons for defect formation and the most common and important methods to investigate those processes are covered before discussing the reactions and their products for the different types of materials present in a device. We summarize commonalities in the occurring mechanisms, and identify structural features and moieties that can be detrimental to operational stability. Some of the resulting implications on the development of new materials are presented and backed by concrete examples from literature.     

Triplet Harvesting with 100% Efficiency by Way of Thermally Activated Delayed Fluorescence in Charge Transfer OLED Emitters

Organic light‐emitting diodes (OLEDs) have their performance limited by the number of emissive singlet states created upon charge recombination (25%). Recently, a novel strategy has been proposed, based on thermally activated up‐conversion of triplet to singlet states, yielding delayed fluorescence (TADF), which greatly enhances electroluminescence. The energy barrier for this reverse intersystem crossing mechanism is proportional to the exchange energy (ΔE_ST) between the singlet and triplet states; therefore, materials with intramolecular charge transfer (ICT) states, where it is known that the exchange energy is small, are perfect candidates. However, here it is shown that triplet states can be harvested with 100% efficiency via TADF, even in materials with ΔE_ST of more than 20 kT (where k is the Boltzmann constant and T is the temperature) at room temperature. The key role played by lone pair electrons in achieving this high efficiency in a series of ICT molecules is elucidated. The results show the complex photophysics of efficient TADF materials and give clear guidelines for designing new emitters.