- Nano Review
- Open Access
Carbon Nanotube Flexible and Stretchable Electronics
© Cai and Wang. 2015
- Received: 27 May 2015
- Accepted: 13 July 2015
- Published: 12 August 2015
The low-cost and large-area manufacturing of flexible and stretchable electronics using printing processes could radically change people’s perspectives on electronics and substantially expand the spectrum of potential applications. Examples range from personalized wearable electronics to large-area smart wallpapers and from interactive bio-inspired robots to implantable health/medical apparatus. Owing to its one-dimensional structure and superior electrical property, carbon nanotube is one of the most promising material platforms for flexible and stretchable electronics. Here in this paper, we review the recent progress in this field. Applications of single-wall carbon nanotube networks as channel semiconductor in flexible thin-film transistors and integrated circuits, as stretchable conductors in various sensors, and as channel material in stretchable transistors will be discussed. Lastly, state-of-the-art advancement on printing process, which is ideal for large-scale fabrication of flexible and stretchable electronics, will also be reviewed in detail.
- Carbon nanotube network
- Thin-film transistor
- Flexible electronics
- Stretchable electronics
- Printed electronics
Unlike conventional microelectronics/nanoelectronics, whose emphasis is miniaturization for ultimate performance and integration density, macroelectronics focuses on large-area and low-cost applications and new form factors such as flexible and stretchable devices . Electronic devices that are fabricated on plastic or rubbery substrates such as flexible display, electronic paper, smart packages, skin-like sensors, wearable electronics, implantable medical implements, and many others could radically change people’s perspectives on electronics . The development of those new forms of electronics relies largely on the advancements in material science. Over decades, amorphous silicon, polysilicon, and organic semiconductors have been extensively studied as the channel materials for thin-film transistors (TFTs), one of the key components in macroelectronics [3–6]. In recent years, nanomaterials, including quantum dots , one-dimensional carbon nanotubes and nanowires [8, 9], as well as two-dimensional (2D) materials [10, 11] have attracted numerous research interests in this area because they offer significantly better performance than organic semiconductors and are easier to process than a-Si or polysilicon. In particular, carbon nanotubes (CNTs) hold great promise for high-performance flexible electronics due to their extremely high carrier mobility, superior mechanical flexibility, and stability .
A single-wall carbon nanotube (SWCNT) can be considered as a seamless cylinder formed by rolling up a graphene sheet along a vector C h = na 1 + ma 2 , where a 1 and a 2 are the basis vectors of the hexagonal crystal lattice of graphene. The indices (n, m) define the two structural parameters, diameter and chirality, of the nanotube. Theoretical calculations indicate that, depending on the indices, the nanotube can have different electrical attributes—metallic for n-m equals multiples of 3, and semiconducting for others. In addition, the bandgap of a semiconducting nanotube is known to be inversely proportional to its diameter .
The unique structure-property relation makes SWCNTs ideal candidates for molecular electronic devices—e.g., metallic nanotubes act as interconnects while semiconducting SWCNTs play the role of channel material for field-effect transistors (FETs) . Additionally, numerous studies have already revealed that individual SWCNTs exhibit very exciting electronic properties, which are well beyond their conventional material counterparts. For instance, the current carrying capability of metallic SWCNTs can reach 109 A/cm2 (much better than aluminum or copper) while semiconducting SWCNTs can exhibit field-effect mobilities up to 104 cm2V−1 s−1 (far exceeding silicon) [15–17]. Nevertheless, devices based on individual SWCNTs suffer from poor uniformity and reproducibility, mainly due to difficulties in reliable synthesis of SWCNTs with homogeneous structural attributes, as well as controllable assembly of SWCNTs over a large area [12, 18]. In addition, novel fabrication methods are needed to render the individual-SWCNT-based devices compatible with current industrial manufacturing processes. On the other hand, macroscale assemblies of SWCNTs, particularly random networks and thin-films, are believed to enable the most realistic applications of SWCNTs in electronics in the short term because they not only offer facile processing but also uniform and reproducible performance due to ensemble averaging [12, 19, 20]. Additionally, SWCNT networks are especially suitable for flexible and stretchable electronics because the lateral deformation of the curvy and entangled SWCNTs can accommodate practically large strains [21, 22]. In fact, there have already been lots of studies demonstrating the great promise of SWCNT networks as the channel materials and/or electrodes in various types of flexible/stretchable electronic devices, such as integrated circuits [23–28], sensors [22, 29–31], organic light-emitting diodes (OLEDs) [32, 33], supercapacitors [34–36], touch panels , and so on.
On the other end of the spectrum lies the solution-based process, where several methods have been reported including vacuum filtration , rod coating , drop coating [26, 44], and printing [45–47]. The solution process of CNTs is enabled by successfully dissolving them in suitable organic solvents or in aqueous solution with the assistance of certain types of surfactants [48, 49]. SWCNT thin films obtained by vacuum filtration and rod coating have been used for flexible, stretchable, and transparent electrodes [33, 50], while printed SWCNT networks have been demonstrated to act as both electrodes and channel materials for TFTs . One key advantage of solution-based process is low temperature and compatibility with various types of widely used polymeric materials, thus enabling the low-cost and large-scale deposition onto various flexible and stretchable substrates [12, 20]. More importantly, through the solution process, it is possible to selectively assemble the SWCNTs with the same electronic type or chirality obtained by post-growth purification and separation [51–53]. With the tremendous progress in SWCNT separation and purification, semiconductor-enriched SWCNTs (sSWCNTs) are now available in large quantities , which enables the wafer-scale fabrication of sSWCNT TFTs with high yield and uniform performance . The most significant advantage of using sSWCNT networks for TFT application lies in the unique combination of superior flexibility/stretchability, optical transparency, and low-temperature solution process, which are not possible with conventional polysilicon or amorphous silicon platforms [3, 4]. In addition, compared with organic semiconductors, sSWCNT networks not only offer drastically better air stability but also multiple orders of magnitude improvements in carrier mobility .
The realization of large area flexible/stretchable electronics also relies on the innovations in manufacturing techniques. Conventional microfabrication processes used in semiconductor industry is not desirable due to its high cost, limitation in sample size, and restrictions in substrate material. Alternatively, printing is a promising method with theoretically no restrictions in substrate material and size [55, 56]. In addition, as an additive process, printing produces minimum material waste and thereby enables eco-friendly and cost-effective manufacturing. Recently, several groups have reported printed flexible devices and circuits using solution-processed SWCNTs, representing a viable way to large-scale and low-cost flexible electronics based on SWCNTs [45–47, 57–66].
In this paper, we survey the recent progress on flexible and stretchable electronics with SWCNT networks as either electrodes or channel materials. This review is organized as follows. In “Carbon Nanotube Networks for Applications in Flexible Electronics” section, we briefly discuss progress made on the high-performance flexible electronics with sSWCNT networks as channel semiconductors. Herein, three examples are presented, namely, flexible TFTs, integrated circuits, and electronic skins. For more detailed and systematic discussion of sSWCNT-based flexible electronics, readers are referred to the recent review papers covering this topic [12, 67]. In “Carbon Nanotube Networks for Applications in Stretchable Electronics” section, we highlight several applications of SWCNT networks in stretchable electronics, including stretchable conductors and electrodes, sensors, and TFTs. In “Scalable Fabrication Process—Printing” section, we focus on the recently developed fabrication process that is most suitable for large-area flexible/stretchable electronics—printing. The state-of-the-art development of fully printed SWCNT-based TFTs and integrated circuits are discussed in detail. Lastly in “Conclusions” section, we conclude with the current remaining challenges and future prospects in this area.
Carbon Nanotube Networks for Applications in Flexible Electronics
Carbon Nanotube Networks for Applications in Stretchable Electronics
Mechanical flexibility by itself may not be sufficient for some applications. For instance, a surface with nonzero Gaussian curvature like a sphere or an irregular surface like the elbow could never be conformally covered with a system that is only flexible . Instead, stretchable electronics could fill in. One strategy to realize stretchable devices is based on thin films of conventional bulk semiconductors like Si and GaAs that are configured into wavy or buckling structures and bonded on elastomer substrates [74–76]. However, this buckling method is rather complicated to fabricate and may not be suitable for large area or mass production. Alternatively, systems that are intrinsically stretchable can be built by using organic materials or nanomaterials with relatively simple process .
Because of the extreme aspect ratio, carbon nanotubes are naturally highly curved and entangled in their macroscale assemblies, making them ideal materials for stretchable electronics [77, 78]. In situ scanning probe microscopic observations also reveal that, upon stretching and releasing process, carbon nanotubes form wavy structures, either in plane or out of plane [21, 22], that could accommodate further deformations. Generally speaking, metallic nanotubes can be used as stretchable interconnects and electrodes [22, 33–36, 79–85] while semiconducting nanotubes can take the role of channel materials for stretchable TFTs [27, 28, 68]. In the following section, we first discuss the carbon nanotube stretchable conductors and their applications and then shift focus to the stretchable transistors with semiconducting carbon nanotubes as channel materials.
In addition to the selection of suitable dielectric material, stable interface between different components also plays a critical role as minute interfacial sliding or delamination may lead to catastrophic failure of the entire device. However, the huge discrepancy in the mechanical and chemical properties of different components poses a great challenge in acquiring a stable interface that can survive large strains (>100 %) . For instance, the modulus of SWCNTs can reach 1 TPa , more than six orders of magnitude higher than that of common elastomer substrates like PDMS. As a result, the realization of highly stretchable and robust SWCNT transistors still needs intensive research efforts in material synthesis, structure design, and fabrication techniques.
Scalable Fabrication Process—Printing
Printing as a new manufacturing method for macroelectronics is attracting a great deal of research interests due to the promise of high-speed and large-scale production of electronic devices in novel form factors [55, 56]. Because no photolithographic patterning or vacuum-based deposition/etching equipment is needed, the cost of electronic devices can be substantially reduced. Additionally, printed electronics can be fabricated on many unconventional substrates, including plastics, papers, textiles, and even rubbers, thus enabling numerous beyond-silicon applications ranging from smart packaging to electronic paper and from large-area smart wallpaper to ubiquitous wearable electronics . Organic semiconductors have been the mainstay in printed electronics for a long time , whereas nanomaterials, among which are quantum dots , nanotubes , nanowires , and two-dimensional (2D) nanomaterials [10, 11], are new members of printable functional inks. In fact, many nanomaterials have already significantly outperformed organic semiconductors. For example, the field-effect mobility of printed TFTs using sSWCNTs is generally higher than 1 cm2V−1 s−1, which marks the upper limit for organic semiconductors. So far, several printing methods have been used to fabricate SWCNT-based devices, such as ink-jet printing [45–47, 59, 65], screen printing , and gravure printing [60–63, 66]. In the following section, we summarize the state-of-the-art development of printed electronics using carbon nanotubes. Although there are several other studies of printed electrical interconnects based on carbon nanotubes [81, 80], we focus on the use of carbon nanotubes as channel semiconductors though.
Gate dielectric layer plays a crucial role and poses a major challenge in printing top-gated TFTs on flexible substrates. The widely adopted printable dielectrics are polymers which have rather low dielectric constant, resulting in a large operating voltage. In addition, it is very difficult to get an ultrathin dielectric film with good uniformity and clean interface through printing processes; any pinhole or interfacial trap would lead to poor device characteristics. Besides, the realization of flexible TFTs requires the dielectric material to be highly compliant, posing a greater challenge in selecting suitable materials. Two of the promising printable dielectric material platforms that have been studied extensively are ion gels [46, 59] and organic-inorganic hybrid dielectrics [58, 60, 61, 66]. Due to the formation of electrical double layers at the gate/dielectric and dielectric/semiconductor interfaces, ion gel offers very large gate capacitance, which is, in principle, independent of the film thickness . Hybrid dielectrics consisting of polymers and inorganic nanoparticles are also excellent platforms for printed and mechanically compliant TFTs because they not only possess high dielectric constant and mechanical flexibility/stretchability but could also enable low-cost and scalable solution-based processing .
Tremendous progress has been made in SWCNT-based flexible and stretchable electronics. Nonetheless, almost no SWCNT-based flexible electronic product is commercially available at this moment . Several challenges remain to be overcome before SWCNT-based electronic devices and systems can be made ready for the applications in consumer markets.
In the material aspect, although semiconductor-enriched SWCNTs are already commercially available in large quantities, there is still large inhomogeneity in terms of chirality and nanotube length. It is expected that high purity and good homogeneity of the starting material is beneficial for uniform device performance. Additionally, longer nanotubes are desired to reduce the number of tube-to-tube junctions, which could lead to further improvement in device mobility. However, the dissolution and separation of long nanotubes (>10 μm) are not easy. Furthermore, the effects of surfactants on device electrical characteristics require more thorough investigation. The surfactants used to disperse SWCNTs are difficult to remove and can act as barriers for electronic conduction, thus increase the contact and channel resistance. In the future, new surfactant-free methods need to be explored to effectively dissolve SWCNTs without damaging or shortening them. Recent studies of dispersing SWCNTs using superacids or salt-ammonia solutions show promise in this direction [96, 97]. Other problems confronting researchers include methods to obtain air-stable n-type conduction in SWCNTs and improve the uniformity, yield, and stability of SWCNT-based devices.
At the fabrication process end, although printing has been demonstrated to be a promising method for large-scale and low-cost manufacturing, the printed devices are still far inferior to their counterparts fabricated using conventional microfabrication processes in terms of electrical performance and uniformity. This is mainly caused by the low resolution (typically >50 μm) and poor reproducibility of current printing methods. Future work on printed SWCNT devices should also focus on improving the metal contacts and developing new dielectric materials. Stretchable electronics are relatively new and have attracted significant research interests. Despite the excellent stretchability of both sSWCNT networks and SWCNT thin-film electrodes, the realization of compliant dielectrics and robust interfaces appears to be the bottleneck in this field. Furthermore, fully printed stretchable systems have yet to be realized. Finally, graphene and other 2D semiconducting materials are also showing increasing potential for flexible/stretchable electronics [10, 11, 98, 99]. Incorporating SWCNTs with other forms of nanomaterials may lead to some exciting results .
This work was partially funded by Michigan State University and the National Science Foundation under Grant ECCS-1549888.
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