Flexible and wearable electronics are attracting wide attention due to their potential applications in wearable human health monitoring and care systems. Carbon materials have combined superiorities such as good electrical conductivity, intrinsic and structural flexibility, light weight, high chemical and thermal stability, ease of chemical functionalization, as well as potential mass production, enabling them to be promising candidate materials for flexible and wearable electronics. Consequently, great efforts are devoted to the controlled fabrication of carbon materials with rationally designed structures for applications in next-generation electronics. Herein, the latest advances in the rational design and controlled fabrication of carbon materials toward applications in flexible and wearable electronics are reviewed. Various carbon materials (carbon nanotubes, graphene, natural-biomaterial-derived carbon, etc.) with controlled micro/nanostructures and designed macroscopic morphologies for high-performance flexible electronics are introduced. The fabrication strategies, working mechanism, performance, and applications of carbon-based flexible devices are reviewed and discussed, including strain/pressure sensors, temperature/humidity sensors, electrochemical sensors, flexible conductive electrodes/wires, and flexible power devices. Furthermore, the integration of multiple devices toward multifunctional wearable systems is briefly reviewed. Finally, the existing challenges and future opportunities in this field are summarized.

Advanced Carbon for Flexible and Wearable Electronics.

Ambipolar organic electronics offer great potential for simple and low-cost fabrication of complementary logic circuits on large-area and mechanically flexible substrates. Ambipolar transistors are ideal candidates for the simple and low-cost development of complementary logic circuits since they can operate as n-type and p-type transistors. Nevertheless, the experimental demonstration of ambipolar organic complementary circuits is limited to inverters. The control of the transistor polarity is crucial for proper circuit operation. Novel gating techniques enable to control the transistor polarity but result in dramatically reduced performances. Here we show high-performance non-planar ambipolar organic transistors with electrical control of the polarity and orders of magnitude higher performances with respect to state-of-art split-gate ambipolar transistors. Electrically reconfigurable complementary logic gates based on ambipolar organic transistors are experimentally demonstrated, thus opening up new opportunities for ambipolar organic complementary electronics.

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Reconfigurable Complementary Logic Circuits with Ambipolar Organic Transistors.

Exciting advancements have been made in the field of flexible electronic devices in the last two decades and will certainly lead to a revolution in peoples’ lives in the future. However, because of the poor sustainability of the active materials in complex stress environments, new requirements have been adopted for the construction of flexible devices. Thus, hierarchical architectures in natural materials, which have developed various environment-adapted structures and materials through natural selection, can serve as guides to solve the limitations of materials and engineering techniques. This review covers the smart designs of structural materials inspired by natural materials and their utility in the construction of flexible devices. First, we summarize structural materials that accommodate mechanical deformations, which is the fundamental requirement for flexible devices to work properly in complex environments. Second, we discuss the functionalities of flexible devices induced by nature-inspired stru...

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Nature-Inspired Structural Materials for Flexible Electronic Devices

Biomimetic skin-like materials, capable of adapting shapes to variable environments and sensing external stimuli, are of great significance in a wide range of applications, including artificial intelligence, soft robotics, and smart wearable devices. However, such highly sophisticated intelligence has been mainly found in natural creatures while rarely realized in artificial materials. Herein, we fabricate a type of biomimetic iontronics to imitate natural skins using supramolecular polyelectrolyte hydrogels. The dynamic viscoelastic networks provide the biomimetic skin with a wide spectrum of mechanical properties, including flexible reconfiguration ability, robust elasticity, extremely large stretchability, autonomous self-healability, and recyclability. Meanwhile, polyelectrolytes' ionic conductivity allows multiple sensory capabilities toward temperature, strain, and stress. This work provides not only insights into dynamic interactions and sensing mechanism of supramolecular iontronics, but may also promote the development of biomimetic skins with sophisticated intelligence similar to natural skins.

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A supramolecular biomimetic skin combining a wide spectrum of mechanical properties and multiple sensory capabilities.

DOI: 10.1002/admt.201800628 applications (e.g., soft robotics, medical devices).[1–6] Despite state-of-the-art bulkbased planar integrated-circuit devices, their rigid and brittle nature gives rise to the incompatibility with curvilinear and soft human bodies, restricting the development of newborn human-friendly interactive electronics. In contrast, the bendable and flexible wearable electronics could be conformally attached onto human bodies almost without discomfort and succeed in performing a great deal of sensing functionalities. Realization of such promising goals requires the flexible sensor platforms provided with crucial characteristics of light weight, ultrathinness, superior flexibility, stretchability, high sensitivity as well as rapid response.[7–10] Inspired by the perceptive features of human skins, the wearable sensor systems are capable of acquiring abundant information from the external environment with the assistance of sensing modules, such as pressure sensors, strain sensors, temperature sensors, etc.[11] A typical example is their application in prosthetics that could afford the capacity to perceive touch or temperature for the disabled.[12] Additionally, the wearable sensor systems are able to identify physical or chemical signals produced by the human body, providing promising opportunities to evaluate health states.[5,13–15] Conventional skin-like sensor platforms primarily comprise one or two sensing modules, data processing units, and power supplies. Their unitary functionality, however, cannot satisfy the increasing demands of IoTs. Recently, the rapid advances in novel sensing materials, fabrication strategies, and innovative electronic constitution contribute to the development of versatile integration of multimodal sensors, which could synchronously distinguish diverse stimuli from the complex environment and monitor multiple vital signs from the human body.[16,17] In spite of several attempts done in terms of such multimodal sensor systems, one of the cumbersome issues originates from the crosscoupling effect among different categories of signals simultaneously generated by various sensors. Furthermore, the skin-like multiple sensor systems usually suffer from the limited number of repeated use, resulting in their high use-cost. The development of separable versatile devices may address this issue with one layer realized by costeffective materials and fabrication manners for disposable use and the other composed of relatively expensive components for repeatable applications.[18] Additionally, the multiple bending or Skin-inspired wearable devices hold great potentials in the next generation of smart portable electronics owing to their intriguing applications in healthcare monitoring, soft robotics, artificial intelligence, and human–machine interfaces. Despite tremendous research efforts dedicated to judiciously tailoring wearable devices in terms of their thickness, portability, flexibility, bendability as well as stretchability, the emerging Internet of Things demand the skininterfaced flexible systems to be endowed with additional functionalities with the capability of mimicking skin-like perception and beyond. This review covers and highlights the latest advances of burgeoning multifunctional wearable electronics, primarily including versatile multimodal sensor systems, self-healing material-based devices, and self-powered flexible sensors. To render the penetration of human-interactive devices into global markets and households, economical manufacturing techniques are crucial to achieve large-scale flexible systems with high-throughput capability. The booming innovations in this research field will push the scientific community forward and benefit human beings in the near future.

Multifunctional Skin-Inspired Flexible Sensor Systems for Wearable Electronics

An organic flexible temperature-sensor array exhibits great potential in health monitoring and other biomedical applications. The actively addressed 16 × 16 temperature sensor array reaches 100% yield rate and provides 2D temperature information of the objects placed in contact, even if the object has an irregular shape. The current device allows defect predictions of electronic devices, remote sensing of harsh environments, and e-skin applications.

A Low-Operating-Power and Flexible Active-Matrix Organic-Transistor Temperature-Sensor Array.

Low-cost solution-shearing methods are highly desirable for deposition of organic semiconductor crystals over a large area. To enhance the rate of evaporation and deposition, elevated substrate temperature is commonly employed during shearing processes. However, the Marangoni flow induced by a temperature-dependent surface-tension gradient near the meniscus line shows negative effects on the deposited crystals and its electrical properties. In the current study, the Marangoni effect to improve the shearing process of 2,7-dioctyl[1]benzothieno[3,2-b][1]benzothiophene for organic field-effect transistor (OFET) applications is utilized and regulated. By modifying the gradient of surface tension with different combinations of solvents, the mass transport of molecules is much more favorable, which largely enhances the deposition rate, reduces organic crystal thickness, enlarges grain sizes, and improves coverage. The average and highest mobility of OFETs can be increased up to 13.7 and 16 cm2 V−1 s−1. This method provides a simple deposition approach on a large scale, which allows to further fabricate large-area circuits, flexible displays, or bioimplantable sensors.

Marangoni-Effect-Assisted Bar-Coating Method for High-Quality Organic Crystals with Compressive and Tensile Strains

Organic optical memory devices keep attracting intensive interests for diverse optoelectronic applications including optical sensors and memories. Here, flexible nonvolatile optical memory devices are developed based on the bis[1]benzothieno[2,3-d;2',3'-d']naphtho[2,3-b;6,7-b']dithiophene (BBTNDT) organic field-effect transistors with charge trapping centers induced by the inhomogeneity (nanosprouts) of the organic thin film. The devices exhibit average mobility as high as 7.7 cm2 V-1 s-1 , photoresponsivity of 433 A W-1 , and long retention time for more than 6 h with a current ratio larger than 106 . Compared with the standard floating gate memory transistors, the BBTNDT devices can reduce the fabrication complexity, cost, and time. Based on the reasonable performance of the single device on a rigid substrate, the optical memory transistor is further scaled up to a 16 × 16 active matrix array on a flexible substrate with operating voltage less than 3 V, and it is used to map out 2D optical images. The findings reveal the potentials of utilizing [1]benzothieno[3,2-b][1]benzothiophene (BTBT) derivatives as organic semiconductors for high-performance optical memory transistors with a facile structure. A detailed study on the charge trapping mechanism in the derivatives of BTBT materials is also provided, which is closely related to the nanosprouts formed inside the organic active layer.

A High-Performance Optical Memory Array Based on Inhomogeneity of Organic Semiconductors.

Charge carrier mobility is one of the important parameters to measure to compare the behavior of different organic transistors. A high carrier mobility is essential for the organic transistors to o...

Overestimation of Carrier Mobility in Organic Thin Film Transistors Due to Unaccounted Fringe Currents

Self-assembled monolayer (SAM) is usually applied to tune the interface between dielectric and active layer of organic field-effect transistors (OFETs) and other organic electronics, a time-saving, direct patterning approach of depositing well-ordered SAMs is highly desired. Here, a new direct patterning method of SAMs by stamp printing or roller printing with special designed stamps is introduced. The chemical structures of the paraffin hydrocarbon molecules and the tail groups of SAMs have allowed to use their attractive van der Waals force for the direct patterning of SAMs. Different SAMs including alkyl and fluoroalkyl silanes or phosphonic acids are used to stamp onto different dielectric surfaces and are characterized by water contact angle, atomic force microscopy, X-ray diffraction, and attenuated total reflectance Fourier transform infrared. The p-type dinaphtho[2,3-b:2′,3′-f]thieno[3,2-b]thiophene (DNTT) and n-type F16CuPc OFETs show competitive mobility as high as 3 and 0.018 cm2 V−1 s−1, respectively. This stamp printing method also allows to deposit different SAMs on certain regions of same substrate, and the complementary inverter consists of both p-type and n-type transistors whose threshold voltages are tuned by stamp printing SAMs and shows a gain higher than 100. The proposed stamp or roller printing method can significantly reduce the deposition time and compatible with the roll-to-roll fabrication.

Direct Patterning of Self-Assembled Monolayers by Stamp Printing Method and Applications in High Performance Organic Field-Effect Transistors and Complementary Inverters

Ke Pei

Papers

A Low-Operating-Power and Flexible Active-Matrix Organic-Transistor Temperature-Sensor Array.

Marangoni-Effect-Assisted Bar-Coating Method for High-Quality Organic Crystals with Compressive and Tensile Strains

A High-Performance Optical Memory Array Based on Inhomogeneity of Organic Semiconductors.

Overestimation of Carrier Mobility in Organic Thin Film Transistors Due to Unaccounted Fringe Currents

Direct Patterning of Self-Assembled Monolayers by Stamp Printing Method and Applications in High Performance Organic Field-Effect Transistors and Complementary Inverters