Roll‐to‐Roll Production of Transparent Silver‐Nanofiber‐Network Electrodes for Flexible Electrochromic Smart Windows

Electrochromic smart windows (ECSWs) are considered as the most promising alternative to traditional dimming devices. However, the electrode technology in ECSWs remains stagnant, wherein inflexible indium tin oxide and fluorine‐doped tin oxide are the main materials being used. Although various complicated production methods, such as high‐temperature calcination and sputtering, have been reported, the mass production of flexible and transparent electrodes remains challenging. Here, a nonheated roll‐to‐roll process is developed for the continuous production of flexible, extralarge, and transparent silver nanofiber (AgNF) network electrodes. The optical and mechanical properties, as well as the electrical conductivity of these products (i.e., 12 Ω sq^?1 at 95% transmittance) are comparable with those AgNF networks produced via high‐temperature sintering. Moreover, the as‐prepared AgNF network is successfully assembled into an A4‐sized ECSW with short switching time, good coloration efficiency, and flexibility.     

Roll‐to‐Roll Cohesive,Coated, Flexible,High‐Efficiency Polymer Light‐Emitting Diodes Utilizing ITO‐Free Polymer Anodes

This paper reports solution‐processed, high‐efficiency polymer light‐emitting diodes fabricated by a new type of roll‐to‐roll coating method under ambient air conditions. A noble roll‐to‐roll cohesive coating system utilizes only natural gravity and the surface tension of the solution to flow out from the capillary to the surface of the substrate. Because this mechanism uses a minimally cohesive solution, the roll‐to‐roll cohesive coating can effectively realize an ultra‐thin film thickness for the electron injection layer. In addition, the roll‐to‐roll cohesive coating enables the fabrication of a thicker polymer anode film more than 250 nm at one time by modification of the surface energy and without wasting the solution. It is observed that the standard sheet resistance deviation of the polymer anode is only 2.32 Ω/□ over 50 000 bending cycles. The standard sheet resistance deviation of the polymer anode in the different bending angles (0 to 180°) is 0.313 Ω/□, but the case of the ITO‐PET is 104.93 Ω/□. The average surface roughness of the polymer anode measured by atomic force microscopy is only 1.06 nm. Because the surface of the polymer anode has a better quality, the leakage current of the polymer light‐emitting diodes (PLEDs) using the polymer anode is much lower than that using the ITO‐PET substrate. The luminous power efficiency of the two devices is 4.13 lm/W for the polymer anode and 3.21 lm/W for the ITO‐PET. Consequently, the PLEDs made by using the polymer anode exhibited 28% enhanced performance because the polymer anode represents not only a higher transparency than the ITO‐PET in the wavelength of 560 nm but also greatly reduced roughness. The optimized the maximum current efficiency and power efficiency of the device show around 6.1 cd/A and 5.1 lm/W, respectively, which is comparable to the case of using the ITO‐glass.     

Roll‐to‐Roll Production of Graphene Hybrid Electrodes for High‐Efficiency,Flexible Organic Photoelectronics

Despite nearly two decades of research, the absence of ideal, flexible, and transparent electrodes has been the biggest bottleneck for realizing flexible and printable electronics via roll‐to‐roll (R2R) method. A fabrication of poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate):graphene:ethyl cellulose (PEDOT:PSS:G:EC) hybrid electrodes by R2R process, which allows for the elimination of strong acid treatment. The high‐performance flexible printable electrode includes a transmittance (T) of 78% at 550 nm and a sheet resistance of 13 Ω sq⁻¹ with excellent mechanical stability. These features arise from the PSS interacting strongly with the ethyoxyl groups from EC promoting a favorable phase separation between PEDOT and PSS chains, and the highly uniform and conductive G:EC enable rearrangement of the PEDOT chains with more expanded conformation surrounded by G:EC via the π–π interaction between G:EC and PEDOT. The hybrid electrodes are fully functional as universal electrodes for outstanding flexible electronic applications. Organic solar cells based on the hybrid electrode exhibit a high power conversion efficiency of 9.4% with good universality for active layer. Moreover, the organic light‐emitting diodes and photodetector devices hold the same level to or outperform those based on indium tin oxide flexible transparent electrodes.     

Micrometer‐ and Nanometer‐Sized Organic Single‐Crystalline Transistors

The use of micrometer and nanometer‐sized organic single crystals to fabricate devices can retain all the advantages of single crystals, avoid the difficulties of growing large crystals, and provide a way to characterize organic semiconductors more efficiently. Moreover, the effective use of such “small” crystals will be beneficial to nanoelectronics. Here we review the recent progress of organic single‐crystalline transistors based on micro‐/nanometer‐sized structures, namely fabrication methods and related technical issues, device properties, and current challenges.     

Stretchable Organometal‐Halide‐Perovskite Quantum‐Dot Light‐Emitting Diodes

Stretchable light‐emitting diodes (LEDs) and electroluminescent capacitors have been reported to potentially bring new opportunities to wearable electronics; however, these devices lack in efficiency and/or stretchability. Here, a stretchable organometal‐halide‐perovskite quantum‐dot LED with both high efficiency and mechanical compliancy is demonstrated. The hybrid device employs an ultrathin (<3 µm) LED structure conformed on a surface‐wrinkled elastomer substrate. Its luminescent efficiency is up to 9.2 cd A^?1, which is 70% higher than a control diode fabricated on the rigid indium tin oxide/glass substrate. Mechanical deformations up to 50% tensile strain do not induce significant loss of the electroluminescent property. The device can survive 1000 stretch–release cycles of 20% tensile strain with small fluctuations in electroluminescent performance.     

Roll‐to‐Roll Production of Layer‐Controlled Molybdenum Disulfide: A Platform for 2D Semiconductor‐Based Industrial Applications

A facile methodology for the large‐scale production of layer‐controlled MoS₂ layers on an inexpensive substrate involving a simple coating of single source precursor with subsequent roll‐to‐roll‐based thermal decomposition is developed. The resulting 50 cm long MoS₂ layers synthesized on Ni foils possess excellent long‐range uniformity and optimum stoichiometry. Moreover, this methodology is promising because it enables simple control of the number of MoS₂ layers by simply adjusting the concentration of (NH₄)₂MoS₄. Additionally, the capability of the MoS₂ for practical applications in electronic/optoelectronic devices and catalysts for hydrogen evolution reaction is verified. The MoS₂‐based field effect transistors exhibit unipolar n‐channel transistor behavior with electron mobility of 0.6 cm² V^?1 s^?1 and an on‐off ratio of ≈10³. The MoS₂‐based visible‐light photodetectors are fabricated in order to evaluate their photoelectrical properties, obtaining an 100% yield for active devices with significant photocurrents and extracted photoresponsivity of ≈22 mA W^?1. Moreover, the MoS₂ layers on Ni foils exhibit applicable catalytic activity with observed overpotential of ≈165 mV and a Tafel slope of 133 mV dec^?1. Based on these results, it is envisaged that the cost‐effective methodology will trigger actual industrial applications, as well as novel research related to 2D semiconductor‐based multifaceted applications.     

High‐Performance,Ultrathin, Ultraflexible Organic Thin‐Film Transistor Array Via Solution Process

Ultrathin organic thin‐film transistors (OTFTs) have received extensive attention due to their outstanding advantages, such as extreme flexibility, good conformability, ultralight weight, and compatibility with low‐cost and large‐area solution‐processed techniques. However, compared with the rigid substrates, it still remains a challenge to fabricate high‐performance ultrathin OTFTs. In this study, a high‐performance ultrathin 2,7‐dioctyl[1]benzothieno[3,2‐b][1]benzothiophene (C8‐BTBT) OTFT array is demonstrated via a simple spin‐coating method, with mobility as high as 11 cm² V⁻¹ s⁻¹ (average mobility: 7.22 cm² V⁻¹ s⁻¹), on/off current ratio of over 10⁶, switching current of >1 mA, and a good yield ratio as high as 100%. The ultrathin thickness at ≈380 nm and the ultralight weight at ≈0.89 g m⁻² enable the free‐standing OTFTs to imperceptibly adhere onto human skin, and even a damselfly wing without affecting its flying. More importantly, the OTFTs show good electrical characteristics and mechanical stability when conformed onto the curved surfaces and even folded in a book after 100 folding cycles. These results illustrate the broad application potential of this simply fabricated ultrathin OTFT in next‐generation electronics such as foldable displays and wearable devices.     

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.     

Freestanding Lamellar Porous Carbon Stacks for Low‐Temperature‐Foldable Supercapacitors

High‐performance supercapacitors (SCs) are important energy storage components for emerging wearable electronics. Rendering low‐temperature foldability to SCs is critically important when wearable devices are used in a cold environment. However, currently reported foldable SCs do not have a stable electrochemical performance at subzero temperatures, while those that are performing are not foldable. Herein, a freestanding pure‐carbon‐based porous electrode, namely, lamellar porous carbon stack (LPCS), is reported, which enables stable low‐temperature‐foldable SCs. The LPCS, which is fabricated with a simple vacuum filtration of a mixture of carbon fibers (CFs), holey reduced graphene oxides (HRGOs), and carbon nanotubes (CNTs), possesses a lamellar stacking of porous carbon thin sheets, in which the CFs act as the skeleton and the HRGOs and CNTs act as binders. The unique structure leads to excellent compression resilience, high foldability, and high electronic and ionic conductivity. SCs made with the LPCS electrodes and ionic liquid electrolyte show a high energy density (2.1 mWh cm^?2 at 2 mA cm^?2), low‐temperature long lifetime (95% capacity after 10 000 cycles at ?30 °C), and excellent low‐temperature foldability (86% capacity after 1000 folding cycles at ?30 °C).