25th Anniversary Article: Organic Electronics Marries Photochromism: Generation of Multifunctional Interfaces,Materials, and Devices

Organic semiconductors have garnered significant interest as key components for flexible, low‐cost, and large‐area electronics. Hitherto, both materials and processing thereof seems to head towards a mature technology which shall ultimately meet expectations and efforts built up over the past years. However, by its own organic electronics cannot compete or complement the silicon‐based electronics in integrating multiple functions in a small area unless novel solutions are brought into play. Photochromic molecules are small organic molecules able to undergo reversible photochemical isomerization between (at least) two (meta)stable states which exhibit markedly different properties. They can be embedded as additional component in organic‐based materials ready to be exploited in devices such as OLEDs, OFETs, and OLETs. The structurally controlled incorporation of photochromic molecules can be done at various interfaces of a device, including the electrode/semiconductor or dielectric/semiconductor interface, or even as a binary mixture in the active layer, in order to impart a light responsive nature to the device. This can be accomplished by modulating via a light stimulus fundamental physico‐chemical properties such as charge injection and transport in the device.     

Organic Photodetectors for Next-Generation Wearable Electronics

Next-generation wearable electronics will need to be mechanically flexible and stretchable such that they can be conformally attached onto the human body. Photodetectors that are available in today's market are based on rigid inorganic crystalline materials and they have limited mechanical flexibility. In contrast, photodetectors based on organic polymers and molecules have emerged as promising alternatives due to their inherent mechanical softness, ease of processing, tunable optoelectronic properties, good light sensing performance, and biocompatibility. Here, the recent advances of organic photodetectors in terms of both optoelectronic and mechanical properties are outlined and discussed, and their application in wearable electronics including health monitoring sensors, artificial vision, and self-powering integrated devices are highlighted.     

Stretchable,Large‐area Organic Electronics

Stretchability will significantly expand the application scope of electronics, particularly large‐area electronics—displays, sensors, and actuators. If arbitrary surfaces and movable parts could be covered with stretchable electronics, which is impossible with conventional electronics, new classes of applications are expected to emerge. A large hurdle is manufacturing electrical wiring with high conductivity, high stretchability, and large‐area compatibility. This Review describes stretchable, large‐area electronics based on organic field‐effect transistors for applications to sensors and displays. First, novel net‐shaped organic transistors are employed to realize stretchable, large‐area sensor networks that detect distributions of pressure and temperature simultaneously. The whole system is functional even when it is stretched by 25%. In order to further improve stretchability, printable elastic conductors are developed by dispersing single‐walled carbon nanotubes (SWNTs) as dopants uniformly in rubbers. Further, we describe integration of printable elastic conductors with organic transistors to construct a rubber‐like stretchable active matrix for large‐area sensor and display applications. Finally, we will discuss the future prospects of stretchable, large‐area electronics with delineating a picture of the next‐generation human/machine interfaces from the aspect of materials science and electronic engineering.     

Wearable Electronics Based on Stretchable Organic Semiconductors

Wearable electronics are attracting increasing interest due to the emerging Internet of Things (IoT). Compared to their inorganic counterparts, stretchable organic semiconductors (SOSs) are promising candidates for wearable electronics due to their excellent properties, including light weight, stretchability, dissolubility, compatibility with flexible substrates, easy tuning of electrical properties, low cost, and low temperature solution processability for large-area printing. Considerable efforts have been dedicated to the fabrication of SOS-based wearable electronics and their potential applications in various areas, including chemical sensors, organic light emitting diodes (OLEDs), organic photodiodes (OPDs), and organic photovoltaics (OPVs), have been demonstrated. In this review, some recent advances of SOS-based wearable electronics based on the classification by device functionality and potential applications are presented. In addition, a conclusion and potential challenges for further development of SOS-based wearable electronics are also discussed.     

Metal‐Halide Perovskite Transistors for Printed Electronics: Challenges and Opportunities

Following the unprecedented rise in photovoltaic power conversion efficiencies during the past five years, metal‐halide perovskites (MHPs) have emerged as a new and highly promising class of solar‐energy materials. Their extraordinary electrical and optical properties combined with the abundance of the raw materials, the simplicity of synthetic routes, and processing versatility make MHPs ideal for cost‐efficient, large‐volume manufacturing of a plethora of optoelectronic devices that span far beyond photovoltaics. Herein looks beyond current applications in the field of energy, to the area of large‐area electronics using MHPs as the semiconductor material. A comprehensive overview of the relevant fundamental material properties of MHPs, including crystal structure, electronic states, and charge transport, is provided first. Thereafter, recent demonstrations of MHP‐based thin‐film transistors and their application in logic circuits, as well as bi‐functional devices such as light‐sensing and light‐emitting transistors, are discussed. Finally, the challenges and opportunities in the area of MHPs‐based electronics, with particular emphasis on manufacturing, stability, and health and environmental concerns, are highlighted.     

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.     

Stretchable Thin‐Film Electrodes for Flexible Electronics with High Deformability and Stretchability

Flexible and stretchable electronics represent today's cutting‐edge electronic technologies. As the most‐fundamental component of electronics, the thin‐film electrode remains the research frontier due to its key role in the successful development of flexible and stretchable electronic devices. Stretchability, however, is generally more challenging to achieve than flexibility. Stretchable electronic devices demand, above all else, that the thin‐film electrodes have the capacity to absorb a large level of strain (>>1%) without obvious changes in their electrical performance. This article reviews the progress in strategies for obtaining highly stretchable thin‐film electrodes. Applications of stretchable thin‐film electrodes fabricated via these strategies are described. Some perspectives and challenges in this field are also put forward.     

Charge Injection in Solution‐Processed Organic Field‐Effect Transistors: Physics,Models and Characterization Methods

A high‐mobility organic semiconductor employed as the active material in a field‐effect transistor does not guarantee per se that expectations of high performance are fulfilled. This is even truer if a downscaled, short channel is adopted. Only if contacts are able to provide the device with as much charge as it needs, with a negligible voltage drop across them, then high expectations can turn into high performances. It is a fact that this is not always the case in the field of organic electronics. In this review, we aim to offer a comprehensive overview on the subject of current injection in organic thin film transistors: physical principles concerning energy level (mis)alignment at interfaces, models describing charge injection, technologies for interface tuning, and techniques for characterizing devices. Finally, a survey of the most recent accomplishments in the field is given. Principles are described in general, but the technologies and survey emphasis is on solution processed transistors, because it is our opinion that scalable, roll‐to‐roll printing processing is one, if not the brightest, possible scenario for the future of organic electronics. With the exception of electrolyte‐gated organic transistors, where impressively low width normalized resistances were reported (in the range of 10 Ω·cm), to date the lowest values reported for devices where the semiconductor is solution‐processed and where the most common architectures are adopted, are ～10 kΩ·cm for transistors with a field effect mobility in the 0.1–1 cm²/Vs range. Although these values represent the best case, they still pose a severe limitation for downscaling the channel lengths below a few micrometers, necessary for increasing the device switching speed. Moreover, techniques to lower contact resistances have been often developed on a case‐by‐case basis, depending on the materials, architecture and processing techniques. The lack of a standard strategy has hampered the progress of the field for a long time. Only recently, as the understanding of the rather complex physical processes at the metal/semiconductor interfaces has improved, more general approaches, with a validity that extends to several materials, are being proposed and successfully tested in the literature. Only a combined scientific and technological effort, on the one side to fully understand contact phenomena and on the other to completely master the tailoring of interfaces, will enable the development of advanced organic electronics applications and their widespread adoption in low‐cost, large‐area printed circuits.     

Gate Dielectrics for Organic Field‐Effect Transistors: New Opportunities for Organic Electronics

In this contribution we review the motivations for, and recent advances in, new gate dielectric materials for incorporation into organic thin‐film transistors (OTFTs) for organic electronics. After a general introduction to OTFT materials, operating principles, and processing requirements for optimizing low‐cost organic electronics, this review focuses on three classes of OTFT‐compatible dielectrics: i) inorganic (high‐k) materials; ii) polymeric materials; and iii) self‐assembled mono‐ and/multilayer materials. The principal goals in this active research area are tunable and reduced OTFT operating voltages, leading to decreased device power consumption while providing excellent dielectric/insulator properties and efficient low‐cost solution‐phase processing characteristics.     

Controlling Molecular Doping in Organic Semiconductors

The field of organic electronics thrives on the hope of enabling low‐cost, solution‐processed electronic devices with mechanical, optoelectronic, and chemical properties not available from inorganic semiconductors. A key to the success of these aspirations is the ability to controllably dope organic semiconductors with high spatial resolution. Here, recent progress in molecular doping of organic semiconductors is summarized, with an emphasis on solution‐processed p‐type doped polymeric semiconductors. Highlighted topics include how solution‐processing techniques can control the distribution, diffusion, and density of dopants within the organic semiconductor, and, in turn, affect the electronic properties of the material. Research in these areas has recently intensified, thanks to advances in chemical synthesis, improved understanding of charged states in organic materials, and a focus on relating fabrication techniques to morphology. Significant disorder in these systems, along with complex interactions between doping and film morphology, is often responsible for charge trapping and low doping efficiency. However, the strong coupling between doping, solubility, and morphology can be harnessed to control crystallinity, create doping gradients, and pattern polymers. These breakthroughs suggest a role for molecular doping not only in device function but also in fabrication—applications beyond those directly analogous to inorganic doping.     

Inorganic Semiconductors for Flexible Electronics

This article reviews several classes of inorganic semiconductor materials that can be used to form high‐performance thin‐film transistors (TFTs) for large area, flexible electronics. Examples ranging from thin films of various forms of silicon to nanoparticles and nanowires of compound semiconductors are presented, with an emphasis on methods of depositing and integrating thin films of these materials into devices. Performance characteristics, including both electrical and mechanical behavior, for isolated transistors as well as circuits with various levels of complexity are reviewed. Collectively, the results suggest that flexible or printable inorganic materials may be attractive for a range of applications not only in flexible but also in large‐area electronics, from existing devices such as flat‐panel displays to more challenging (in terms of both cost and performance requirements) systems such as large area radiofrequency communication devices, structural health monitors, and conformal X‐ray imagers.     

Nanomaterial‐Enabled Stretchable Conductors: Strategies,Materials and Devices

Stretchable electronics are attracting intensive attention due to their promising applications in many areas where electronic devices undergo large deformation and/or form intimate contact with curvilinear surfaces. On the other hand, a plethora of nanomaterials with outstanding properties have emerged over the past decades. The understanding of nanoscale phenomena, materials, and devices has progressed to a point where substantial strides in nanomaterial‐enabled applications become realistic. This review summarizes recent advances in one such application, nanomaterial‐enabled stretchable conductors (one of the most important components for stretchable electronics) and related stretchable devices (e.g., capacitive sensors, supercapacitors and electroactive polymer actuators), over the past five years. Focusing on bottom‐up synthesized carbon nanomaterials (e.g., carbon nanotubes and graphene) and metal nanomaterials (e.g., metal nanowires and nanoparticles), this review provides fundamental insights into the strategies for developing nanomaterial‐enabled highly conductive and stretchable conductors. Finally, some of the challenges and important directions in the area of nanomaterial‐enabled stretchable conductors and devices are discussed.     

柔性电致变色器件研究进展

电致变色材料是一类重要的光电功能材料, 可以随周期性调整的电压改变颜色。这种可控的光学吸收率和透过率的调制在智能窗户、电致变色显示和防眩光后视镜等应用场合大显身手。近年来电致变色技术发展迅速, 但当前的研究大多集中在传统刚性电致变色器件, 通常以氧化铟锡(ITO)等导电玻璃为基底。这些刚性变色器件存在厚度大、共型性差、机械强度低、成本高等不可忽视的问题, 阻碍了电致变色技术及其商业化的发展。伴随着开发可穿戴设备和电子皮肤等其他未来技术的热潮, 柔性电致变色器件因其可折叠性、可穿戴性甚至可嵌入性而备受关注, 已跻身成为电致变色领域的研究热点。本综述从制备柔性电致变色器件的材料出发, 系统地概述了无机、有机、无机/有机复合及其他新型柔性电致变色器件最新进展和趋势, 着重介绍了可拉伸电致变色器件的国内外研究进展。同时讨论了现阶段柔性电致变色器件在性能提升和实际应用等方面遇到的挑战, 以及国内外研究者采取的应对措施。最后明确了柔性电致变色器件制备与提升性能的关键, 并对未来的发展趋势做出展望。     

Perovskite Materials for Light‐Emitting Diodes and Lasers

Organic–inorganic hybrid perovskites have cemented their position as an exceptional class of optoelectronic materials thanks to record photovoltaic efficiencies of 22.1%, as well as promising demonstrations of light‐emitting diodes, lasers, and light‐emitting transistors. Perovskite materials with photoluminescence quantum yields close to 100% and perovskite light‐emitting diodes with external quantum efficiencies of 8% and current efficiencies of 43 cd A^?1 have been achieved. Although perovskite light‐emitting devices are yet to become industrially relevant, in merely two years these devices have achieved the brightness and efficiencies that organic light‐emitting diodes accomplished in two decades. Further advances will rely decisively on the multitude of compositional, structural variants that enable the formation of lower‐dimensionality layered and three‐dimensional perovskites, nanostructures, charge‐transport materials, and device processing with architectural innovations. Here, the rapid advancements in perovskite light‐emitting devices and lasers are reviewed. The key challenges in materials development, device fabrication, operational stability are addressed, and an outlook is presented that will address market viability of perovskite light‐emitting devices.     

Recent Advances in White Organic Light‐Emitting Materials and Devices (WOLEDs)

WOLEDs offer new design opportunities in practical solid‐state lighting and could play a significant role in reducing global energy consumption. Obtaining white light from organic LEDs is a considerable challenge. Alongside the development of new materials with improved color stability and balanced charge transport properties, major issues involve the fabrication of large‐area devices and the development of low‐cost manufacturing technology. This Review will describe the types of materials (small molecules and polymers) that have been used to fabricate WOLEDs. A range of device architectures are presented and appraised.     

Flexible Electronics Based on Organic Semiconductors: from Patterned Assembly to Integrated Applications

Organic flexible electronic devices are at the forefront of the electronics as they possess the potential to bring about a major lifestyle revolution owing to outstanding properties of organic semiconductors, including solution processability, lightweight and flexibility. For the integration of organic flexible electronics, the precise patterning and ordered assembly of organic semiconductors have attracted wide attention and gained rapid developments, which not only reduces the charge crosstalk between adjacent devices, but also enhances device uniformity and reproducibility. This review focuses on recent advances in the design, patterned assembly of organic semiconductors, and flexible electronic devices, especially for flexible organic field-effect transistors (FOFETs) and their multifunctional applications. First, typical organic semiconductor materials and material design methods are introduced. Based on these organic materials with not only superior mechanical properties but also high carrier mobility, patterned assembly strategies on flexible substrates, including one-step and two-step approaches are discussed. Advanced applications of flexible electronic devices based on organic semiconductor patterns are then highlighted. Finally, future challenges and possible directions in the field to motivate the development of the next generation of flexible electronics are proposed.     

Large‐Area Organic Solar Cells: Material Requirements,Modular Designs,and Printing Methods

The printing of large‐area organic solar cells (OSCs) has become a frontier for organic electronics and is also regarded as a critical step in their industrial applications. With the rapid progress in the field of OSCs, the highest power conversion efficiency (PCE) for small‐area devices is approaching 15%, whereas the PCE for large‐area devices has also surpassed 10% in a single cell with an area of ≈1 cm². Here, the progress of this fast developing area is reviewed, mainly focusing on: 1) material requirements (materials that are able to form efficient thick active layer films for large‐area printing); 2) modular designs (effective designs that can suppress electrical, geometric, optical, and additional losses, leading to a reduction in the PCE of the devices, as a consequence of substrate area expansion); and 3) printing methods (various scalable fabrication techniques that are employed for large‐area fabrication, including knife coating, slot‐die coating, screen printing, inkjet printing, gravure printing, flexographic printing, pad printing, and brush coating). By combining thick‐film material systems with efficient modular designs exhibiting low‐efficiency losses and employing the right printing methods, the fabrication of large‐area OSCs will be successfully realized in the near future.     

Recent Progress on Stretchable Electronic Devices with Intrinsically Stretchable Components

Stretchable electronic devices with intrinsically stretchable components have significant inherent advantages, including simple fabrication processes, a high integrity of the stacked layers, and low cost in comparison with stretchable electronic devices based on non‐stretchable components. The research in this field has focused on developing new intrinsically stretchable components for conductors, semiconductors, and insulators. New methodologies and fabrication processes have been developed to fabricate stretchable devices with intrinsically stretchable components. The latest successful examples of stretchable conductors for applications in interconnections, electrodes, and piezoresistive devices are reviewed here. Stretchable conductors can be used for electrode or sensor applications depending on the electrical properties of the stretchable conductors under mechanical strain. A detailed overview of the recent progress in stretchable semiconductors, stretchable insulators, and other novel stretchable materials is also given, along with a discussion of the associated technological innovations and challenges. Stretchable electronic devices with intrinsically stretchable components such as field‐effect transistors (FETs), photodetectors, light‐emitting diodes (LEDs), electronic skins, and energy harvesters are also described and a new strategy for development of stretchable electronic devices is discussed. Conclusions and future prospects for the development of stretchable electronic devices with intrinsically stretchable components are discussed.     

Emerging Semitransparent Solar Cells: Materials and Device Design

Semitransparent solar cells can provide not only efficient power‐generation but also appealing images and show promising applications in building integrated photovoltaics, wearable electronics, photovoltaic vehicles and so forth in the future. Such devices have been successfully realized by incorporating transparent electrodes in new generation low‐cost solar cells, including organic solar cells (OSCs), dye‐sensitized solar cells (DSCs) and organometal halide perovskite solar cells (PSCs). In this review, the advances in the preparation of semitransparent OSCs, DSCs, and PSCs are summarized, focusing on the top transparent electrode materials and device designs, which are all crucial to the performance of these devices. Techniques for optimizing the efficiency, color and transparency of the devices are addressed in detail. Finally, a summary of the research field and an outlook into the future development in this area are provided.     

Organic FETs: Functional Organic Field‐Effect Transistors (Adv. Mater. 40/2010)

Functional organic field‐effect transistors (OFETs) have attracted increasing attention in the past few years due to their wide variety of potential applications. Research on functional OFETs underpins future advances in organic electronics. In this review, different types of functional OFETs including organic phototransistors, organic memory FETs, organic light emitting FETs, sensors based on OFETs and other functional OFETs are introduced. In order to provide a comprehensive overview of this field, the history, current status of research, main challenges and prospects for functional OFETs are all discussed