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Printed Thin Film Transistors: Research from China Sichao Tong, Jia Sun, and Junliang Yang ACS Appl. Mater. Interfaces, Just Accepted Manuscript • DOI: 10.1021/acsami.7b16413 • Publication Date (Web): 01 Mar 2018 Downloaded from http://pubs.acs.org on March 1, 2018

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ACS Applied Materials & Interfaces

Printed Thin Film Transistors: Research from China Sichao Tong, Jia Sun and Junliang Yang* Hunan Key Laboratory for Super-microstructure and Ultrafast Process, School of Physics and Electronics, Central South University, Changsha 410083, Hunan, China * Corresponding author. Email: [email protected]; Tel: +86-731-88660256 (J. L. Yang)

ABSTRACT:

Thin

film

transistors

(TFTs)

have

experienced

tremendous

development during the past decades and show great promising applications in flat displays, sensors, radio frequency identification tags, logic circuit, and so on. The printed TFTs are the key components for rapid development and commercialization of printed electronics. The researchers in China play important roles to accelerate the development and commercialization of printed TFTs. In this review, we comprehensively summarize the research progress of printed TFTs on rigid and flexible substrates from China. The review will focus on printing techniques of TFTs, printed TFTs components including semiconductors, dielectrics and electrodes, as well as fully-printed TFTs and printed flexible TFTs. Furthermore, perspectives on the remaining challenges and future developments are proposed as well.

KEYWORDS: printed electronics, flexible electronics, printed thin film transistors, inkjet printing, transfer printing, screen printing, gravure printing

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1. INTRODUCTION Printed electronics are emerging as an alternative to conventionally processed silicon electronics for great potential applications in wearable electronics1, 2, healthcare devices3, 4, displays5, human-machine interfaces6, and so on. As the next generation electronics, printed flexible electronics technology owns significant advantages, including superior intrinsic mechanical flexibility, satisfying light-weight and large-scale ceaseless preparation7, 8. To date, low-cost and high-efficient printing techniques are popularly used to deposit organic or inorganic materials on flexible substrates such as polymer films and paper, realizing flexible electronic devices. Printed electronics have been attracted increasing attention in organic light emitting diodes (OLED)9, neuromorphic devices10,

11

, capacitive energy storage

devices12, gas sensing13, 14, thin film transistor liquid crystal display (TFT-LCD)

15, 16

,

photodetectors17 and so on. Due to the unique advantages and great potential prospect of printing techniques, printing electronics has been chosen as a revolutionary project to accelerate the development of electronics industry in developed and developing countries and regions. Thus more and more research are being studied on printable materials, devices, technologies and equipments, as well as further extending to the applications such as communication, new energy resources, information display, radio frequency identification tag (RFID) and transducer. According to a report by the consulting company IDTechEx in 2012, the market of printed electronics was $ 9.46 billion in 2012, and it will be $ 63.28 billion by 202218. The 7th Framework program of the European Union (EU) and the United States of America (USA) continuously invest to the research on printed electronics, and has achieved significant progress on fundamental study and printed electronics industry19,20. Furthermore, regional industry associations and many enterprises are taking huge efforts to accelerate the development and commercialization of printed and flexible electronics, for example, Organic and Printed Electronics Association (OE-A) in EU, Flex Tech Alliance in USA, Japan Advanced Printed Electronics Technology Research Association (JAPERA) in Japan, Victorian Organic Solar Cell Consortium (VICOSC) in Australia. In mainland China, there is few research groups focused on printed electronics 2


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before 2010. Printed electronics gradually attract much attention in mainland China just after Printable Electronics Research Center was founded in 2010 in Suzhou Institute of Nano-tech and Nano-bionics (SINANO). Then, Tianjin University and Beijing Institute of Graphic Communication jointly built Printable Electronics Research Center in 2011. In the same year, Innovation Alliance of Printed Electronics (IAPE) in mainland China was founded as well, which is devoted itself to combine information electronics with printing industry and accelerate the development of printed electronics. In 2013, Changzhou Institute of Printed Electronics Industry was founded, which invested over $ 8 million for accelerating the commercialization of printed electronics from fundamental study. Because of rapid development of printed electronics in China, the 5th International Conference on Flexible and Printed Electronics (ICFPE 2014) was held in Beijing. Meanwhile, many companies focused on materials, equipment, products of printed electronics are founded as well, such as Kunshan Hisense, Beijing NanoTop, Changzhou Enfucell, Hunan NanoUp, etc. Recently, government dramatically increases the investment on printed electronics. In the 13th 5-year plan, the National Key Research and Development Program of China will invest over $ 3 billion for the research on printed display and printed thin film transistors (TFTs). The great application prospects and huge market would make government and companies continuously increase the investment on both fundamental and applied study in China for accelerating the commercialization of printed electronics. TFTs is one of the most important printed electronic devices, which is constituted by a semiconductor layer, a dielectric layer and electrodes for forming multilayer devices.14, 15 For obtaining high-performance printed TFTs, there are lots of research focused on printable semiconductor/dielectric/electrode materials, surface and interface properties, as well as printing techniques. The semiconductor material is crucial for the performance of TFTs. Up to now, varieties of semiconductor materials, including organic and inorganic, are used as the channel materials in TFTs and fabricated

by

printing

techniques,

for

examples,

fullerene

(C60)21,

poly(3-hexylthiophene) (P3HT)22, carbon nanotubes (CNTs)23, graphene24, indium 3



gallium zinc oxide (IGZO)25. The dielectric materials also play a key role in TFTs due to the carriers transport at the interface between the dielectric and the semiconductor, as well as the determination on the range of threshold voltage (Vth) and the energy consumption26-28. Furthermore, electrodes are another key component in TFTs, and their patterning and conductivity are the important topics in printed TFTs29, 30. With the in-depth research on materials, device structure, manufacturing processes, TFTs gradually realize the fabrication on flexible substrates with printing techniques. In this review, we comprehensively summarize and discuss the research progress on printed TFTs on rigid and flexible substrates from China. It does not include normal solution-processed or printable TFTs or only flexible TFTs, but is focused on printed TFTs on both rigid and flexible substrates. In section 2, we will introduce printing techniques employed in fabricating TFTs, including inkjet printing, transfer printing, screen printing and gravure printing. In section 3, we mainly focus on the state-of-the-art strategies for realizing printed TFTs components on rigid substrate. It includes printed semiconductor materials (printed organic semiconductors, printed inorganic semiconductor and printed carbon-based semiconductors), printed dielectric materials and printed electrodes. In section 4, recent progress on printed TFTs on polymer and paper substrates for forming flexible TFTs will be reviewed. Finally, perspectives on the future developments and remaining challenges in printed TFTs will be discussed.

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2. PRINTING TECHNIQUES Printing is an attractive strategy for processing large-scale electronic devices with low cost and high output, especially for large-area flexible electronics31, 32. As compared with fabrication process of traditional complementary compound semiconductor transistors using lithographic patterning and vacuum deposition, printing process would dramatically decrease the cost and increase the production efficiency33, 34. Several printing techniques have been employed to fabricate TFTs, including inkjet printing, transfer printing, screen printing and gravure printing[35, 3635, 36. The schematic is shown in Figure 1, and the characteristic parameters are summarized in Table 1. They are discussed in details below.

Figure 1. Schematic of printing techniques for fabricating TFTs: inkjet printing, transfer printing, screen printing, gravure printing and other printing techniques. Table 1. The characteristic parameters of printing techniques for fabricating TFTs. Techniques Inkjet printing

Resolution (µm) 0.4 ~ 50

Speed (m min-1)

Wet film thickness (µm)

1 ~ 100

0.3 ~ 20

Viscosity (mPa s) 1 ~ 40

Transfer printing

0.1 ~ 90

-

-

-

Screen printing

50 ~ 100

10 ~ 100

3 ~ 100

500 ~ 50000

Gravure printing

20 ~ 75

20 ~ 1000

0.1 ~ 5

1 ~ 200

Slot-die coating

50 ~ 100

1 ~ 10

0.1 ~ 5

1 ~ 200

5



Knife coating

50 ~ 100

1 ~ 10

0.1 ~ 5

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1 ~ 200

2.1. Inkjet printing Inkjet printing is a non-contact technique for micro-scale process and direct jetting solutions with small particle size on flexible or rigid substrates. Because inkjet printing can directly produce patterned films without any masks, it is considered as an alternative to lift-off process37, 38. Actually, inkjet printing is a convenient patterning technique. It generally includes an ink chamber and could quantitatively deposit solution from the ink chamber at designated areas through jet ejection. Owing to its inherent advantageous characteristics including the precise control on the volume of depositing solution and location, easily pattering, efficient use of materials and minimal contamination resulted from non-contact deposition process, inkjet printing has been regarded as the most potential technology for commercially fabricating electronic and optoelectronic devices with low cost and high-output. Government and many companies have invested huge money focusing on inkjet printing for organic light-emitting diodes (OLED), quantum light-emitting diodes (QLED) and TFTs, such as Samsung, LG, BOE, Visionox. Normally, inkjet printing has three modes, i.e., piezoelectric, acoustic and thermal. As compared with lithographic techniques, the resolution is low, which would limit its application. Normally, the resolution is about 20 µm, and it would be improved to 400 nm with suitable inkjet printer and inks39. The characteristics of drop ejection, the evaporation behavior of solvent, the viscosity of ink and the diameter of nozzle are the important parameters to influence the resolution. Meanwhile, the coffee-ring effect is also a great challenge for fabricating homogeneous and compact thin films, which is caused by the outward fluid flow inside of liquid materials and the pinning of the contact line40, 41. There are many remarkable techniques for improving the quality of inkjet-printed thin films. (i) ink engineering: using lower surface tension materials (surfactant42, dodecanethiol43) or a higher boiling point solvent44, a gelatinization polymer45 or by modulating nanoparticle properties46. (ii) Substrate treatment: improving wettability47, reducing surface temperature48, introducing 6


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electro-wetting process49. (iii) Equipment development, such as customized diameter of nozzle and accurate xyz motion stage50. The above methods can effectively improve the controllability of shape, thickness and morphology in dried droplet, as well as the resolution of printed thin films. In a word, inkjet printing is a digital mastering for patterning and is a wide adaptation for materials and easy preparation technique, which would be a printing strategy for commercially fabricating TFTs.

2.2. Transfer printing Transfer printing is also a promising method for mass production. It can perfectly match with low-temperature preparation process and flexible substrates, as well as exhibit good compatibility with other deposition technology. Originally, flexible substrates could not be used directly in high-temperature chemical vapor deposition (CVD)-grown nanotubes. Motivating by the demands of growing materials on flexible substrates under the high temperature condition, transfer printing technique was developed to transfer materials from growth substrates (donor substrate) to designed substrates (acceptor substrate)51. Through transfer printing mediator, original patterning structures can be transferred from donor substrate onto acceptor substrate via controlling surface interaction properties of chemical or physical. The major physical or chemical interactions generally correlate with capillary and van der Waals force. There are three typical steps involved in transfer printing process. (i) The materials grown on the donor substrate are transferred onto the transfer mediator by pressure, illumination, temperature, etc. (ii) The transfer mediator with transferred materials is closely attached to the acceptor substrate surface with well controlling. (iii) The transfer mediator is moved away and leaves materials onto the acceptor substrate surface. A suitable transfer mediator is a very important factor in transfer printing technique for obtaining a high yield, excellent fidelity and easy controllability52. Organic polymer films poly(dimethylsilox-ane) (PDMS) and polymethyl methacrylate (PMMA) and metals foils such as Cu and Cr have been used as the transfer mediator in transfer printing process53-55. Recently, a highly oriented one-dimensional nanostructure network was successful transferred to Si substrate by 7



using one-step transfer printing, in which the PDMS film was used as transfer mediator56. With the development of transfer printing, all kinds of transfer printing methods emerge, such as contact printing57, nanoimprinting58, 59, laser transfer printing60 and two-step transfer printing (TTP)61, which tremendously expand transfer printing technique in the application of fabricating electronic devices. Contact printing is a typical technique to fabricate oriented nanowire (NW) arrays. The transformation and rearrangement of materials from the donor substrate could be realized by directional shear force62. While both of nanoimprinting and laser transfer printing can precisely produce patterns up to nanometer scale in large-area, in which the materials could be transfer onto flexible substrate by the assist of pressure and laser radiation, respectively58-60. Furthermore, TTP can be compatible with other printing process and successfully achieve patterning and super flexible microelectrode arrays on curved substrates61. In summary, transfer printing is a good technique to process electronic devices on flexible and rigid substrate with high resolution, and it is widely used for fabricating micro- and nanoscale patterns.

2.3. Screen printing Screen printing is being widely used in Si-based solar cells for processing Ag or Al electrodes and in printed circuit board (PCB) for depositing a protecting layer for etching63, 64. It usually involves specially prepared inks, a reusable and devisable screen mask and a squeegee. The replicated screen mask is usually made by a porous mesh, such as polymer materials or stainless steel, of which the configuration is photo-chemically or manually defined on the mesh. By squeezing inks through the mask onto the substrate surface, large-area film with patterning can be obtained65. Because of the simplicity of the process, screen printing can be suited for variety of flexible or rigid substrates with suitable inks. Furthermore, it can be matched with roll-to-roll (R2R) printing process with a rotary screen printing, which is one of screen printing techniques with the high edge resolution, mass-production and precisely controlled wet thickness66. In industry production, the thickness of screen 8


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printed films is generally lager than 0.5 µm67. Screen printing is capable of printing homogeneity and smooth films, but it is limited by the finest feature size in the range of 75 µm to hundreds of micrometers. Thus, screen printing is not a perfect choice for the films requiring accuracy control on thickness or nanostructure size of designing. The use of screen printing in TFTs is mainly to deposit electrodes such as metal68 and polymer69.

2.4. Gravure printing Gravure printing is a common printing method in our daily life, which is extensively used in processing newsprint, banner and textile printing. In recent years, gravure printing technology is being increasingly used in fabricating large-scale electronic and optoelectronic devices, such as patterning electrodes70, photodetectors17 and solar cells71-74, etc. In gravure printing, a gravure cylinder with tiny engraved cavities is rolled on a moving paper or polymer substrate. Before the ink is transferred from the cavities onto the accepted substrate, the excess ink material is removed by a blade, ensuring that the ink material is only existing in the cavities. The patterning and thickness of the film can be optimized by the shape and depth of the cavities. R2R gravure printing can produce high-quality film with high throughout, in which the printing speed can be up to 900 m/min66. Hence, gravure printing is regarded as the fastest method with excellent reliability and repeatability. The main disadvantage is that the different patterns need new engraved cylinders to be designed. The cost of cylinders would be compensated by large-scale and high-speed fabricating process.

2.5. Others printing techniques Some other printing techniques could be used to fabricate TFTs as well, for example, slot-die coating75 and knife coating76, 77. The schematic diagrams are shown in Figure 1. In slot-die coating, the ink is provided by the meniscus via a slot and a pump. The film thickness is controlled by the web speed and the ink supplying. Meanwhile, the film thickness is dependent on the coating window as well, which is bound up with the ink properties, the web surface properties and the coating 9



geometry66. The knife coating is an evolving form of doctor blading, and it is more adapt to the mass production in industry. Slot-die coating and knife coating can easily process large-area and uniform film with high throughout, but it is difficult to pattern the film using these two printing techniques. Noteworthy, offset printing is the most commonly printing technique today and covers more than 40% of traditional printing market. However, it is barely reported in printed TFTs. Usually, the offset printing employs three plates to transfer the pattern onto the acceptor substrate. A pattern is sculptured on an offset plate, which is special treated in order that the ink is adsorbed onto pattern areas. Due to the special treatment, the required ink only “assemble” onto the pattern area, while all of required area without pattern rejects the ink. Then, the pattern areas with ink are transferred and form the pattern on the surface of flexible substrate. For full color printing, an offset printing process should be reprinted four times in four printing units with fundamental color. Offset printing is a large-scale and high-speed fabricating process, and it has an advantage on patterning. However, because of (i) a sizeable investment in equipment and (ii) technical difficulty for exploiting printable electronic materials, there are barely reports on offset printed TFTs.

3. PRINTED TFTs ON RIGID SUBSTRATE TFTs are a multilayer structural electronic device, and it is constituted of a semiconductor layer, a dielectric layer and source (S)/drain (D)/gate (G) electrodes. As a bias voltage is applied on gate electrode, the charge carriers inject from the source electrode and move to the interface between semiconductor layer and dielectric layer. Then, a current will be generated as a bias voltage is applied between the electrodes (S/D). According to the position of electrodes (S/D/G), TFTs is normally be classified as four device configurations, as shown in Figure 2, which include Bottom Gate/Bottom Contact, Bottom Gate/Top Contact, Top Gate/Top Contact and Top Gate/Bottom Contact. Because of a better contact and carriers charge transferring path, the Bottom Gate/Top Contact and Top Gate/Bottom Contact structural TFTs normally 10


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exhibit better performance parameters than that with other two structures78. Moreover, the intrinsic properties of semiconductor/dielectric/electrode materials, the interface energy levels and thin film quality play key roles in the performance parameters of TFTs. All kinds of organic and inorganic semiconductor, dielectric and electrode materials have been used to fabricate TFTs via printing techniques79, 80. This section will mainly give a review on the research progress of printed TFTs on rigid substrate.

Figure 2. Schematic diagram of four types of TFTs. (a) Bottom Gate/Bottom Contact structure, (b) Bottom Gate/Top Contact structure, (c) Top Gate/Top Contact structure, (d) Top Gate/Bottom Contact structure.

In order to accurately evaluate TFTs performance with different materials, structure and preparation technology, there are four performance parameters, i.e., mobility (µ), current on/off ratio (Ion/Ioff), Vth and subthreshold slope (SS), which can be obtained from the curves of output characteristics (ISD-VSD) and transfer characteristics (ISD-VG). The µ is the drift velocity of carriers under an applied electric field, showing the move ability of electrons or holes in semiconductor. It is the most important parameter in TFTs. As the TFTs work in the linear region, the mobility can be expressed as following equation:

11



=

Where L is the channel length, W is the channel width, Ci is the unit-area capacitance of insulating layer, Vsd is the voltage between S/D electrodes, ⁄ is the curve slope of transfer characteristics. As the TFTs work in the saturation region, the mobility is expressed in the equation:

2 =

Where the ISD is the current between S/D electrodes. The mobility is dependent on semiconductor purity, crystal quality, grain size, contact resistance of electrodes, channel size, devices structure, etc. Generally speaking, the mobility of TFTs based on organic or inorganic compound semiconductors approaches or exceeds the value of amorphous silica (~1 cm2 V-1s-1), the TFTs would show the potential in practical applications. The Ion/Ioff is defined as the specific value of ISD in the “on” and “off” states, which is a very important parameter for TFTs’ application in display and logical circuit. Actually, the Ioff is the leakage current, and further effect the power dissipation. A high Ion/Ioff means the good stability, excellent anti-interference ability and high load-driving ability. In logic circuit chip, the Ion/Ioff usually is up to 106. The Vth is the lowest voltage to operate TFTs, meaning that TFTs with low Vth can be used in a low voltage condition. The Vth can be calculated in both of output characteristics curve and transfer characteristics curve with slight difference. Universally, the Vth is dependent on the charge-trapping density between semiconductor and dielectric, the contact resistance of S/D electrodes, and built-in electric field. The SS is a parameter to estimate how quickly the current change from “on” state to “off” state, reflecting the voltage span of current variation. It can be calculated according to the following equation:

=

According to equation, a low SS means a quick speed from “on” to “off” states 12


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with a small voltage span. Admittedly, the SS is influenced by the interface quality between semiconductor and dielectric.

3.1. Printed semiconductor layer 3.1.1. Organic semiconductor Semiconductor layer is the core component in TFTs. Organic semiconductor is one of the most important semiconductor materials, which can realize specific electrical and chemical properties by customized functional groups in organic materials and designed for printable TFTs79, 81-83. Generally, thermal evaporation or spin-coating techniques are used to deposit organic semiconductors for studying TFTs device performance. But, it is desirable to develop simple, low-cost and scalable manufacturing techniques in potential industrial products. Hence, many researchers including Chinese researchers tried themselves to develop organic semiconductor, including soluble organic polymer semiconductor and small molecular semiconductor, in large-scale, high-throughput and flexible electronic devices by printing technology.

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(a)

PDVT-8

P3HT

PBDTT PDPPTzBT

PQTBTz-C12

PDFDT

DPP-DTT

NDI2OD-DTYM2 C8H17 C8H17

O

C10H21

S S 0.75

0.25

N O C10H21

F

N

LGC-D148

O C10H21

S

S

S

S S

N

F

O N

C10H21

C8H17

C8H17

(b)

Si

Cn-BTBT Si

TIPS-PEN PCBM 14


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Figure 3. The typical soluble organic semiconductors applied in printed TFTs. (a) polymers, (b) small molecules.

Polymer semiconductor own the customer designed properties and the advantages of solution processibility and perfect matching with flexible substrate. Many typical semiconductor polymer materials have been widely used in printed electronics (Figure 3a), such as P3HT, poly[2,5-bis(alkyl)pyrrolo[3,4-c]pyrrole -1,4-(2H,5H)-dione-alt-5,5’-di(thiophen-2-yl)-2,2’-(E)-2-(2-(thio-phen-2-yl)vinyl)-thi ophene]

(PDVT-8),

conjugated

polymer

(PBDTT),84

diketopyrrolopyrrole-

thiazolothiazole copolymer (PDPPTzBT),85 fluorinated difluorobenzothiadiazoledithienosilole

(PDFDT),86

polymer

poly(didodecylquaterthiophene-alt-

didodecylbithiazole (PQDBTz-C12),87 diketopyrrolopyrrole polymer (DPP-DTT),88 diketopyrrolopyrrole-based conjugated polymer (LGC-D148)89, core-expanded naph-thalene

diimide

fused

with

2-(1,3-dithiol-2-ylidene)malonitrile

groups

(NDI2OD-DTYM2)90, and so on. P3HT is a classical polymer semiconductor used in polymer electronics and optoelectronics. Lin et al comprehensively compared the films morphology of inkjet-printed and spin-coated P3HT, as shown in Figure 4a91. Although inkjet-printed P3HT thin film is a little rough, the mobility of inkjet-printed P3HT TFTs (0.8×10-3 cm2 V-1s-1) could be comparable to the value of spin-coated TFTs (1×10-3 cm2V-1s-1) (Figure 4b). Meanwhile, self-assembled monolayer (SAM) was used to adjust interfacial properties of organic semiconductor/dielectric interface or organic semiconductor/electrodes interface for improving the performance parameters of organic TFTs fabricated via inkjet printing92, 93. Chen et al. found that the appropriate surface treatment would be helpful to produce uniform P3HT thin film via inkjet printing, resulting in great improvement in electric characteristics94. By inserting

octyltrichlorosilane

(OTS),

phenethy-ltricholosilane

(PETS)

and

phenyltrichlorosilane (PTS) between P3HT and dielectric layer as the interface modification, the mobilities of inkjet-printed P3HT TFTs could be improved from 2.37×10-3 cm2V-1s-1 to 3.52×10-3, 8.07×10-3 and 7.95×10-3 cm2V-1s-1, respectively94. In addition, PDVT-8 was used as the active layer in organic TFTs fabricated by inkjet 15



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printing95. Yang et al demonstrated the effect of additive polystyrene (PS) on PDVT-8 domain size, domain purity and molecular packing, which could further improve the charge mobility and result in a mobility of about 0.58 cm2V-1s-1, a Ion/Ioff of about 5×104 and a Vth of about -9 V96.

Figure 4. (a) AFM image and transfer characteristic of spin-coated P3HT thin film and TFTs, respectively. (b) AFM image and transfer characteristic of inkjet-printed P3HT thin film and TFTs, respectively. Reprinted with permission from ref 91. Copyright 2016 Royal Society of Chemistry. (c) AFM images of inkjet-printed TIPS-pentacene thin films on SiO2/Si substrates by PETS, PTS, PVP coating and UV-ozone treatment. Reprinted with permission from ref 97. Copyright 2015 AIP Publishing LLC.

For improving the performance of printed TFTs, some new polymer semiconductors were designed and synthesized. For example, Wang et al reported a novel polymer material, namely PDPPTzBT, and its TFTs could be fabricated through inkjet printing pure solvents with a high-resolution, low-cost and high-yields. PDPPTzBT TFTs exhibited an average hole mobility of 1.20 cm2V-1s-1 in atmospheric conditions85. Li et al reported a conjugated alternating donor-acceptor (D-A) polymer with a relatively strong donor moiety, dithienylthieno[3,2-b]thiophene (DTT) and a comparatively weaker acceptor moiety, n-alkyl diketopyrrolo-pyrrole (DPP), and it was further used to fabricate p-type TFTs via inkjet printing DPP-DPP semiconductor layer, exhibiting a high mobility up to 10.5 cm2V-1s-1 and an Ion/Ioff 10698. 16


of higher than

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Organic small molecular semiconductor is normally processed by thermal deposition because of its insolubility, such as pentacene, phthalocyanine compounds. Recently, more and more soluble organic small molecular semiconductors have been synthesized via introducing suitable soluble groups for printed electronics, for example,

2,7-dioctyl[1]benzothieno[3,2-b][1] benzothiophene (C8BTBT) and

[6,6]-phenyl-C61-butyric acid methyl ester (PCBM), as shown in Figure 3b83, 99. The group 6,13-bis(triisopropyl-silylethynyl) (TIPS) is added into pentacene, it could form a excellently soluble, high-performance TIPS-pentacene100,

101

. For fabricating

TIPS-pentacene thin film with homogeneity thickness and high-quality morphology via inkjet printing, surface energies were tuned via SAM, ultraviolet (UV)-ozone treatment and a polymeric dielectric (Figure 4c)97. Wang et al demonstrated that the crystal growth of TIPS-pentacene could be controlled by inkjet printing, in which crystal orientation of TIPS-pentacene was adjusted by surface-modified Au because there is a slightly higher dispersive surface energy than the dielectric substrate102. Thus, it could produce high-quality TIPS-pentacene thin film with large grain size and more convergent crystalline microstructure. Furthermore, high-quality inkjet-printed TIPS-pentacene thin film and accordingly high-performance TFTs could be achieved via modifying the dielectric surface properties, in which inserting SAM, e.g. phenethyltrichlorosilane

(PETS),

perfluorodecyltrichlorosilane (PDTS)97,

phenyltrichlorosilane

(PTS)

and

103

. In addition, UV-ozone treatment on

substrate could also control the morphology, crystallization behavior and device performance of TIPS-pentacene via inkjet printing. The UV irradiation accelerates the formation of uniform and large strip-like crystals (Figure 4c), leading to the mobility of TIPS-pentacene TFTs fabricated via inkjet printing up to 0.48 cm2 V-1s-1104. The performance parameters of TFTs with printed organic semiconductor on rigid substrate are summarized in Table 2. For printable organic semiconductors, both polymers and small molecules are faced with low mobility and/or high-cost, as well as poor long-term stability, which are big challenges for the actual application of printed organic TFTs. Fortunately, with the development of chemical design, a series of novel organic semiconductors 17



with customized properties have been synthesized for TFTs, which would be hopeful for the development of printable organic TFTs.

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Printed Carbon-based Semiconductor

Printed Organic Semiconductor

Table 2. The performance parameters of printed TFTs on rigid substrate.

Printed Inorganic Semiconductor

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47


Device Architectures (Semiconductor, Dielectric, D/S/G Electrodes)

Printed Materials

P3HT, SiO2, Au/Au/Si P3HT, SiO2, Au/Au/Si P3HT(CNPs), SiO2, Au/Au/Si PDVT-8(PS), SiO2, Au/Au/Si PDVT-8(PS), SiO2, Au/Au/Si PDPPTzBT, SiO2, Au/Au/Si PDPPT-DTT, SiO2, Au/Au/Si DPP-DTT, SiO2, Au/Au/Si TIPS-pentacene, SiO2, Au/Au/Si TIPS-pentacene, SiO2, Au/Au/Si TIPS-pentacene, SiO2, --/--/Si TIPS-pentacene, SiO2, Au/Au/Si SWCNTs, PMPA-ODAa, Au/Au/Ag SWCNTs, EMIM-TFSIb(PS-PMMA), Au/Au/Si SWCNTs,SiO2, Au/Au/Si SWCNTs, SiO2, Au/Au/Si SWCNTs, HfO2, Au/Au/Si SWCNTs, HfO2, Au/Au/Si SWCNTs, HfO2, Au/Au/Si SWCNTs, HfO2, Au/Au/Si SWCNTs, HfO2, Au/Au/Si SWCNTs, HfO2, Au/Au/Si SWCNTs, SiO2(PMMA), Au/Au/Si SWCNTs, SiO2(OTS), Au/Au/Si Graphene, SiO2, Au/Au/Si IGZO, SiO2, Au/Au/Si IGZO, SiO2, MoNb/MoNb/Si IGZO, SiO2, Al/Al/Si IGZO, SiO2, ITO/ITO/Si IGZO, SiO2, ITO/ITO/Si IGZO, SiO2, ITO/ITO/Si IZO, SiO2, Ti(Au)/Ti(Au)/Si Zn2GeO4, SiO2, Ti(Al)/Ti(Al)/Si In2Ge2O7, SiO2, Ti(Al)/Ti(Al)/Si

P3HT P3HT P3HT(CNPs) PDVT-8(PS) PDVT-8(PS) PDPPTzBT PDPPT-DTT DPP-DTT TIPS-pentacene TIPS-pentacene TIPS-pentacene TIPS-pentacene SWCNTs, Ag SWCNTs, EMIM-TFSI (PS-PMMA), SWCNTs SWCNTs SWCNTs SWCNTs SWCNTs SWCNTs SWCNTs SWCNTs SWCNTs, Au SWCNTs, Au Graphene IGZO IGZO IGZO IGZO IGZO IGZO IZO Zn2GeO4 In2Ge2O7

Printing Techniques

Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Slot-die coating Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Transfer printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Transfer printing Transfer printing

19


Device Performance Mobility (cm2 V-1 s-1) 0.002 0.00807 0.0123 1.39 ~ 1.63 0.51 ~ 0.65 1.80 3.76 1.50 ~ 3.50 0.140 0.077 0.1-0.8 0.48 ~269 ~1 ~42.1 3.54 ~29.8 17.6~ 37.7 ~22.6 30 -57 85 91 ~2.3 1.5 6.2 4.93 10.2 1.41 5.7 8 25.01 11.67

Ion/Ioff

Vth (V)

~103 ~103 2.1 (3.0 ~5.0) × 104 (3.0 ~7.0) × 104 ~108 -55 ~ 60 ~2.5×104 25.8 5 ~104 ~106 ~103 ~107 3 × 105 ~106 104~ 107 ~106 ~106 104 ~106 6.5 × 106 3.1 × 106 -106 107 107 2.10× 108 4.30× 107 7.90× 104 104~105 2.51 × 103 1.59 × 103

----4 ~ -8 -7 ~ -11 ---1 ~ 1 1.1 -0.9 -21 -0.25 ----2~ 2 -2~ 2 -2~ 2 ---2.6 2.1 --8.5 -8 -1 1.2 -6 22

Ref. 91 94 105 95 96 85 75 98 97 102 103 104 106 107 108 109 110 111 112 113 114 115 116 116 117 118 119 120 121 122 123 124 125 125


Printed Electrodes

Printed Dielectri c Layer

Printed Inorganic Semiconductor

Device Architectures (Semiconductor, Dielectric, D/S/G Electrodes) InOx, Al2Ox:Nd(PVA), ITO/ITO/Al:Nd

Fully-pri nted TFT

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47

Device Performance \ Printed Materials

In2O3(PS) Si NWs

ZnO NWs, SiO2, Ti(Al)/Ti(Al)/Si

ZnO NWs

Zn3As2 NWs, SiO2, Ni(Au)/Ni(Au)/Si

Zn3As2 NWs

WSe2, SiO2, Au/Au/Si

WSe2

pentacene, PVP(TiO2), Au/Au/ITO

IGZO, SiO2(ZrOx), ITO/ITO/PEDOT: PSS pentacene, SiO2, PPOD/PPOD/Si F16CuPc, SiO2, PPOD/PPOD/Si CuPc, SiO2, PPOD/PPOD/Si TIPS-pentacene (PS), PVP, Ag/Ag/Al IGZO, Al2Ox:Nd, AlNd/AlNd/Ag TIPS-pentacene (PS), PVP, Ag/Ag/Al IGZO, Al2O3, Ag/Ag/Al TIPS-pentacene (PS), PVP, Ag/Ag/Ag TIPS-pentacene, SiO2 (OTS), Ag/Ag/Si SWCNTs, Al2O3, Ag/Ag/ITO SWCNTs, Al2O3, Ag/Ag/ITO TIPS-pentacene (NDI2OD-DTYM2), SiO2, graphene/graphene/--

Inkjet printing

TTF-TCNQ Ca2Nb3O10(PMMA) PMSQ

graphene

InGaO, ZrOx, ITO/ITO/ITO SWCNTs, Al2O3, Ag/Ag/ITO

SWCNTs, Ag, ITO

Ion/Ioff

Vth(V)

109

-6

Ref. 126

127

13.7 0.101

3.5 × 10 1.0 × 107

-4.0 -11

90

105

0.25

128

305.5

10

--

129

Inkjet printing

1

3 × 105

--

130

Inkjet printing

PEDOT: PSS PPOD PPOD PPOD Ag Ag Ag Ag Ag Ag Ag, ITO Ag, ITO

Mobility (cm2 V-1 s-1) 4.9

Inkjet printing Transfer printing Gravure printing and transfer printing Transfer printing

Inkjet printing Inkjet printing Inkjet printing

PVP(TiO2)

SWCNTs, PMSD(EMIT-TFSI), Au InGaO, ZrOx, ITO

SWCNTs, PMSD(EMIT-TFSI), Au/Au/Ag

Printing Techniques

InOx, ITO

In2O3(PS), SiO2, Au/Au/Si Si NWs(PBTTTc), SiO2, Ni(Au)/Ni(Au)/Si

pentacene, SiO2(TTF-TCNQ), Au/Au/Si IGZO, Ca2Nb3O10(PMMA), Al/Al/Si IGZO, PMSQ, Al/Al/Si

Page 20 of 62

0.4 2.4 1.8 0.49

5

5

3.59 × 10 104 2.5 × 102 3

3.0 × 10 3

----6.6

56

32 131 132 133

69

Screen printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing Slot-die coating,

0.2 0.18 0.00449 0.007 0.10~ 0.28 4.28 0.3 0.29 0.1 0.08 6.6 ~34.0

10 2 × 106 4 × 105 2.6 × 103 -106 104 105 -104 105 107

0.3 -17 29.1 -10.2 0.59~ 0.71 -2 ---4.2 ---

Inkjet printing

0.2

105

--

40

Inkjet printing

0.5

103

--

141

Inkjet printing

11.7

--

--

142

Inkjet printing

6.6

105

--

140

a

PMPA-ODA: poly (pyromellitic dianhydride-co-4, 4’-oxydianiline) EMIM-TFSI: 1-ethyl-3-methylimidazolium bis(tri-fluoromethylsulfonyl) imide c PBTTT: poly(2,5-bis(3-alkylthiophen-2-yl)thieno[3,2-b]-thiophene) b

20


134 134 134 135 136 35 137 138 139 140 140

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3.1.2. Carbon-based semiconductor As typical representatives of 1-dimensions (1D) and 2-dimensions (2D) materials, CNTs and graphene are attracting much interesting in electronic devices duo to their high electronic conductivity and mechanical strength. The CNTs-based transistor with a hole mobility up to 79 000 cm2V-1s-1 was demonstrated143. Single-walled carbon nanotubes (SWCNTs) are thought to one of the most promising semiconductor for creating high-performance printed TFTs due to their outstanding electrical, chemical and mechanical properties144, 145. It demonstrated that SWCNTs TFTs fabricated via inkjet printing on Si substrates showed a Ion/Ioff of 104114. Furthermore, due to electric-double-layer effect and good performance of SWCNTs, Feng et al reported inkjet-printed

SWCNTs

TFTs

using

a

poly(pyromellitic

dianhydride-co-4,4’-oxydianiline) as the dielectric layer, leading to a very high mobility up to 269 cm2V-1s-1106. Because of metallic pollution to semiconducting CNTs, as well as the adsorption of oxygen, water and solvent molecules, the performance of CNTs TFT would be seriously encumbered. In order to over-come these issues, a number of methods are developed to improve the performance of TFTs, including chemical doping by active metals146, organic reducing reagents147, aromatic extraction148, surfactant extraction149, amine extraction150, surface alignment151, and so on. Wang et al found that diazonium salts could preferentially react with metallic species of several commercial SWCNTs in solutions, and inkjet-printed TFTs exhibited excellent electrical properties with the mobility and Ion/Ioff up to 3.54 cm2 V-1 s-1 and 3×105, respectively109. Meanwhile, Xu et al reported a simple, efficient and robust way to convert the polarity of sorted SWCNTs via using printable polarity conversion inks as an electron doping agent (Figure

such

5a),

as

poly{(9,9-dioctylfluorene)-2,7-diyl-alt-[3,6-dithiene-2-yl-2,5-di(2-ethylhexyl)pyrrolo[ 3,4-]

pyrrole-1,4-dione-5,5’’-diyl}

(PFO-DPP),

poly[(9,9-dioctylfluorenyl-2,7-diyl)-alt-co-(6,6’-{2,2’:6’,2’’-terpyridine})] (PFO-TP), isoindigo-based

poly(9,9-dioctylfluorene)

derivative

(PFIID),

poly[(9,9-dioctylfluorenyl-2,7-diyl)-co-(1,4-benzo-2,1-3-thiadiazole)] (PFO-BT) and 21



poly[2,7-(9,9-dioctylfluorene)-alt-4,7-bis(thiophen-2-yl)benzo-2,1,3-thiadiazole] (PFO-DBT)113. By the deposition of ethanolamine inks on the active region via inkjet printing, the inkjet-printed p-type SWCNT TFTs could be converted into n-type, and exhibit an effective electron mobility of 30 cm2V-1s-1 and an Ion/Ioff of 106 (Figure 5b and c).

Figure 5. (a) Photographs of high-purity SWCNTs by (1) PFO-DPP, (2) PFO-TP, (3) PFIID, (4) PFO-BT and (5) PFO-DBT and printable polarity conversion inks at the beginning (6) and after 6 months (7). (b) Optical images of a printed SWCNTs inverter after the deposition of polarity conversion thin film (on the active region of the upper device) and the silver interconnect. (c) Typical transfer curves of p-type and n-type TFTs. Reprinted with permission from ref 113. Copyright 2017 American Chemical Society. (d) The cross-sectional and the horizontal views of wrapping configurations of P-DPPb5T on SWCNTs with different chirality. Reprinted with 22


Page 22 of 62

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permission from ref 111. Copyright 2016 Royal Society of Chemistry.

Polymer wrapping becomes an effective strategy to selectively differentiate SWCNTs after regioregular poly(3-dodecylthiophene) (rr-P3DDT) was used as wrapping material152. Then, polymer sorted SWCNTs was directly used to print TFTs via solution process method. A new nonlinear DPP-based semiconducting copolymer (P-DPPb5T) was proved to be high-efficiency for wrapping SWCNTs with large diameter and was applied in inkjet-printed TFTs (Figure 5d)

111

. The sorted

inkjet-printed SWCNTs TFTs exhibited good homogeneity with low Vth of (±2 V) and SS (122-161 mV dec-1), high mobility (17.6-37.7 cm2 V-1 s-1) and high Ion/Ioff (104-107). The inkjet-printed SWCNTs TFTs, being modified by poly(9,9-dioctylfluorene) (PFO) derivative with large conjugated planar surface, exhibited superior performance with a high hole mobility (~29.8 cm2 V-1 s-1) and Ion/Ioff (~106), as well as small SS (142-163 mV/dec) at low Vth of ±2V110. Besides, other polymer materials such as (9,9-dioctylfluorene-co-bithiophene) (F8T2) have been used in high-performance CNTs TFTs fabricated via printing technology as well108, 112. Reduced graphene oxide (rGO) is thought as a promising material for building high-performance TFTs because of its excellent electrical properties and great chemical stability153, 154. Zhang et al demonstrated an array of rGO TFTs, in which high-quality stripe and square shaped rGO thin films were fabricated by transfer printing, resulting in bipolar transport with a hole mobility of 2.3 cm2V-1s-1 and an electron mobility of 0.84 cm2V-1s-1117. The performance parameters of TFTs with printed carbon-based semiconductor on rigid substrate are summarized in Table 2. In general, CNTs and graphene semiconductors are suitable for high-mobility, low-cost and stability TFTs due to their electrical characteristics, solubility, and chemical/physical stability. But, pure carbon materials own the poor device performance because of strong adsorption capacity between carbon atoms and gaseous molecules. For improving the printability of CNTs and graphene semiconductors with little metallic and amorphous carbon, polymer wrapped CNTs and functionalized graphene are appearing and applied in TFTs, which have been 23



Page 24 of 62

proved to be good approach for improving performance of printed carbon-based TFTs.

3.1.3. Inorganic semiconductor Inorganic semiconductor exhibits the advantages of high carrier mobility and excellent air-stability, and several research groups have been focusing on inorganic TFTs155-159. The printed inorganic TFTs are mainly composed of n-type semiconductors, such as binary (ZnO, In2O3, SnO2, Ga2O3), ternary (ZIO, ITO, ZTO, IGO), quaternary compounds (IZTO, IGZO), as well as some p-type semiconductors including CuI, CuO, NiO, WSe2 and CuInSe28, 121, 160, 161. Wang

et

al

reported

an

inkjet-printed

IGZO

TFTs

with

bottom-gate/bottom-contact device architecture, in which the thickness of inkjet-printed IGZO thin film obviously influence TFTs performance. Under an optimized IGZO thickness at 55 nm, inkjet-printed TFTs showed a mobility of 1.41 cm2V-1s-1, a Vth of 1 V and a Ion/Ioff of 4.3×107122. Xie et al found that the performance of IGZO TFTs could be enhanced by a preheating process at 300 oC, leading to the mobility enhancement of over10 times from 0.31 cm2V-1s-1 to 4.93 cm2V-1s-1120. Printing techniques is a solution process. However, printable inorganic semiconductor normally needs to be annealed at a high temperature over 400 oC, which does not match with flexible substrate. So, low-temperature treatment techniques were introduced to fabricate inorganic TFTs 162. Inkjet-printed IGZO TFTs were fabricated at low temperature by laser beam annealing treatment, as shown in Figure 6a and b. With laser scanning at 1 mm/s for 40 times, the 30 nm IGZO TFTs baked at 200 oC, showed a mobility of 1.5 cm2V-1s-1, a Vth of 8.5 V, and an Ion/Ioff of ~106 (Figure 6c) 118

.

Furthermore,

by

hydrophobic

treatment

on

substrate

surface

using

hexamethyldisilazane (HMDS) and OTS assembly, the resolution of printed array could be reduced from over 80 µm down to 45 µm and 35 µm, resulting from the increase of the contact angles up to 52° and 102°, respectively (Figure 6d)

119

.

Meantime, by adding poly(4-vinylphenol) (PVP) to adjust the viscosity of inks, a uniform and printed IGZO TFTs array could be fabricated, leading to the highest 24


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mobility of about 6.2 cm2V-1s-1and Ion/Ioff of ~ 107 (Figure 6e). In addition, sensors and detectors based on inkjet-printed compound TFTs have been reported by Du and co-workers as well121, 123.

Figure 6. (a) Schematic diagram of TFTs with laser beam annealing treatment. (b) SEM image of original TFT. (c) Transfer characteristics of inkjet-printed IGZO TFTs. Reprinted with permission from ref 118. Copyright 2017 Minerals, Metals & Materials Society. (d) The static contact angles of deionized water on HMDS- and OTS-assembled Si/SiO2 substrates. (e) Photographs of inkjet-printed dot arrays on HMDS-treated SiO2. Reprinted with permission from ref 119.Copyright 2017 Royal Society of Chemistry.

Except for printed inorganic TFTs discussed above, other types of inorganic TFTs fabricated via printing process have attracted much attention as well. Liu et al reported TFTs based on highly ordered horizontally-aligned nanowire arrays of Zn2GeO4 and In2Ge2O7 by transfer printing technique, which exhibited effective mobility of 25.44 cm2V-1s-1 and 11.9 cm2V-1s-1, respectively125. Another typical example of inkjet-printed InOx TFTs was fabricated by coffee-ring defined short channels, in which the channel length is as small as ~3.5 µm. Meanwhile, the spreading of InOx semiconductor precursor ink could be well-controlled by an ultrathin polyvinyl acetate (PVA) layer modified the surface of S/D electrodes. The short channel InOx TFTs showed a maximum mobility of 4.9 cm2V-1s-1 and a Ion/Ioff of larger than 109126. Furthermore, it was reported that p-type CuI TFTs could be fabricated via inkjet printing at a low-temperature of 60 °C, and exhibited a mobility 25



Page 26 of 62

up to be 1.86 cm2V-1s-1 and a Ion/Ioff of 101-102163. Besides, Zn3As2 nanowire arrays TFTs were fabricated via transfer printing, which exhibited a typical p-type semiconductor characteristics with a mobility up to 305 cm2V-1s-1 and a high Ion/Ioff of 10×107129.

The

performance

parameters

of

TFTs

with

printed

inorganic

semiconductor on rigid substrate are summarized in Table 2. Up to now, inorganic semiconductor, especially IGZO, is potentially to replace amorphous silicon TFTs in display applications. However, for printed electronics on flexible substrate, it is very important to develop compatible, low-temperature treatment process during or after printing. Thus, specific inks with low-temperature treatment and instant annealing technique have been proposed and successfully used in printed high-performance TFTs, which would accelerate the actual application of printed inorganic TFTs.

3.2. Printed dielectric layer As one of the core constituents in TFTs, the dielectric layer also plays a significance role on the device performance. Recently, some printable dielectric materials were developed for TFTs, such as inorganic oxide164, polymers165, ion-gel166, solid-state

electrolyte167,

and

so

on168.

Wu

et

al

reported

that

poly(methylsilsesquioxane) (PMSQ) could play as the gate insulator in IGZO TFTs by printable dielectric ink132. The top-gate/top-contact IGZO TFTs with inkjet-printed PMSQ dielectric layer showed a mobility of 0.75 cm2V-1s-1 and an Ion/Ioff of 2×104. Although polymer dielectric materials show good printable characteristics, the permittivity is relatively lower than that of conventional inorganic materials. Thus, the composites of printable high-permittivity (high-k) inorganic nanoparticles (NPs) and printable polymers are good choices for high-performance dielectric materials in TFTs, which possess high-k constant, excellent stability and printability. A nanocomposite combining high-k TiO2 NPs and PVP was used as the gate dielectric layer for enhancing the permittivity and reducing Vth in inkjet-printed organic TFTs133. The IGZO TFTs with nanocomposite dielectric material exhibited a mobility of ~0.49 cm2V-1s-1 and low voltage operation of -6V. Besides, a dispersing Ca2Nb3O10 26


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nanosheets in acetone diluted PMMA solution was fabricated as the dielectric layer via inkjet printing, and it was found that 2D structural nanosheets are more suitable for the dielectric layer than 1D materials because of their proper lamellar geometry, as shown in Figure 7a-c131. However, in any composite of a low-k polymer and a high-k inorganic dielectric, the low-k property will dominate unless the high-k material is at a very high volume fraction. The IGZO TFTs based on printed nanocomposite layer as the gate dielectrics exhibited a mobility of 2.4 cm2V-1s-1and an Ion/Ioff over 104.

Figure 7. Schematic showing metal element permeability of fillers with different shapes. (a) spherical filler, (b) 2D flake filler and (c) top view of b. Reprinted with permission from ref131. Copyright 2014 Elsevier Ltd.

Meanwhile, a printed modification layer between semiconductor layer and dielectric layer is a feasible route to enhance TFTs performance as well. Li et al proved that tetracene-based TFTs with atetrathiafulvalene-tetracyanoquinodimethane (TTF-TCNQ) nanoweb buffer layer deposited via inkjet-printing exhibited mobility up to 0.4 cm2V-1s-1, which was improved up to two orders of magnitudes as compared to OTS modification32. The performance parameters of TFTs with printed dielectric layer on rigid substrate are summarized in Table 2. As compared with reported printed semiconductor layer in TFTs, there are much less reports on printed dielectric layer because of the few printable high-k dielectric 27



materials and it is hard to print high-quality dielectric thin film. It would be one of main breakthroughs for the development of printed TFTs.

3.3. Printed electrodes Printed electrodes have the advantages of patterning with mask-free and mass production with low cost, as well as the compatibility with flexible substrate, e.g. polymer169 or paper170. The inks based on conducting nanoparticle, conductive polymer and organometallic solutions can be directly deposited by printing technology171,

172

. However, due to the poor interface adhesive strength and the

compatibility of electrodes with the semiconductor or dielectric layer, the integration of electrodes via printing techniques in TFTs still shows great challenge. Conductive polymers poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) and polyaniline (PANI) show the potential application as the electrodes in printed and flexible TFTs173. Gao et al deposited the conductive PEDOT:PSS via screen printing as the gate electrode in IGZO TFTs, in which the channel width and length is 500 µm and 50 µm, respectively69. The IGZO TFTs showed a mobility of 0.2 cm2V-1s-1, an Ion/Ioff of 10 and a Vth of 0.3 V. Recently, a novel polymer material, i.e., pyrolyzed poly(l,3,4-oxadiazole) (PPOD), was synthesized as the electrode in organic TFTs134. The TFTs based on pentacene, CuPc and fluorinated copper phthalocyanine (F16CuPc) semiconductors were fabricated with inkjet-printed PPOD electrodes, in which all of them have a clearer PPOD electrode/semiconductor contact edge than that of Au electrodes, resulting in the enhancement of mobility from 0.09 cm2V-1s-1, 1.2 × 10-3 cm2V-1s-1 and 3.34 × 10-4 cm2V-1s-1 to 0.18 cm2V-1s-1, 7.0 × 10-3 cm2V-1s-1 and 4.94 × 10-3 cm2V-1s-1, respectively (Figure 8a).

28


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Figure 8. (a) AFM images of organic semiconductors pentacene, CuPc and F16CuPc on inkjet-printed PPOD electrodes and SiO2 substrate, respectively. Reprinted with permission from ref 134. Copyright 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (b) Optical microscope image of an array of inkjet-printed Ag dots. (c) Schematic diagram of short channels via adjusting the printed ink, in which DS is drop spacing, R is track spreading width, D is moving distance of the printer, L is channel length. Reprinted with permission from ref 35. Copyright 2014 Royal Society of Chemistry. (d) SEM image of inkjet-printed graphene electrodes with the optimized conditions. Reprinted with permission from ref 40. Copyright 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

However, conductive polymers normally exhibit low conductivity and poor air-stability as compared with metal electrodes. In order to fabricate high-quality electrodes, conducting metal nanoparticle and organometallic solutions are developed to be printable inks for processing the electrodes in printed electronics. Generally speaking, Au is a very satisfying material to be electrode in TFTs because of its excellent stable and good conductivity, as well as excellent Ohmic contact with most semiconductors, but it is too expensive93, 174. Thus, printable Ag electrodes have been greatly developed due to the low cost and high conductivity138, 175-177. Ning et al deposited Ag S/D electrodes via inkjet printing directly on an amorphous IGZO layer to complete the fabrication of IGZO TFTs137. It was found that the Ag nanoparticles connect to the adjacent interface together and diffuse into amorphous IGZO, resulting 29



in the improvement contact between the electrodes and the semiconductor, and further enhancing the TFTs performance. In addition, several types of silver inks were inkjet-printed on IGZO thin film for completing TFTs, and it was found that Ag salt ink is much better than Ag nanoparticle ink to produce high-performance TFTs. The IGZO TFTs with printing Ag S/D electrodes showed a mobility of 4.28 cm2V-1s-1 and an Ion/Ioff of 106136. Meanwhile, some approaches were proposed for fabricating short channels with printing electrodes. Tang et al fabricated inkjet-printed Ag S/D electrodes with accurate control and produced the short channels with the width down to 20 µm by controlling ink wetting on a PVA surface, leading to form good interface contacts between organic semiconductor and electrodes (Figure 8b and c)35. Furthermore, delicate and continuous inkjet-printed S/D electrodes for the short channels with the width down to ~15 µm were reported, in which the surface wettability of polymer gate dielectric layer was reduced by a SAM modification135. Apart from the discussion above, printed ITO and reduced rGO electrodes were reported as well. The inkjet-printed graphene patterns acted as S/D electrodes in TFTs were developed, showing excellent performance with an Ion/Ioff of ~105 and a mobility of ~0.2 cm2V-1s-1 for carbon-based TFTs (Figure 8d)40. The performance parameters of TFTs with printed electrodes on rigid substrate are summarized in Table 2. In summary, printed metal electrodes is mature and already applied in flexible electronics, such as RFID, logic circuits, display, OLED, etc. Reducing the cost of noble metals electrode and enhancing the stability of metal electrode are the next goal of printed metal electrode. In addition, conductor polymer still has some challenges, for example, stability and conductivity, in actual application in printed TFTs.

3.4. Fully-Printed TFTs At the moment, most reports are focused on one or two components’ printing in TFTs178, inks179 or elimination of coffee rings180. Some researchers try to fully employ printing technology to fabricate TFTs, for example, fully-inkjet-printed TFTs181. Fully-printing fabrication would become a research hotspot from both fundamental and application aspects in TFTs area. However, there are a series of challenges to 30


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realize fully-printed TFTs: (i) high-quality printable inks for electrode conductors, semiconductors and dielectrics, (ii) interface properties and contacts for printed multi-layers, (iii) matching between printing techniques and printing layers, as well as inks and substrate. Some progress was achieved for fully-printed TFTs as well. For example, fully inkjet-printed TFTs with the construction of SWCNTs semiconductor, PDMS and EMIT-TFSI gate dielectric and Au gate electrode, showing a mobility of ~0.5 cm2V-1s-1 and an Ion/Ioff of more than 103 in both of top-gated and bottom-gated devices141. In addition, an array of inkjet-printed metal oxide TFTs was demonstrated for the first time with the assistance of surface-energy patterns prepared by printing pure solvent to etch the ultrathin hydrophobic layer. The surface-energy patterns not only restrained the spreading of inks but also provided a facile way to regulate the morphology of metal oxide films without optimizing ink formulation. The fully-printed InGaO TFTs in the array exhibited excellent electron transport characteristics with a maximum mobility of 11.7 cm2V-1s-1, negligible hysteresis, good uniformity and stability under bias stress. The new route lights a general way toward fully inkjet-printed inorganic TFTs arrays142. Recently, Wang et al showed an ITO gate electrode and Ag electrodes deposited by inkjet printing technology. The TFTs based on inkjet-printed, dip-coated and drop-casted SWCNTs semiconductor were fabricated, and a high mobility of 34 cm2V-1s-1 and an Ion/Ioff of 107 could be achieved by integration dip-coating method and drop-casting technique on Si substrates with lithographed inter-digitated Au S/D electrodes. Meanwhile, the fully inkjet-printed TFTs also possessed a mobility as high as 6.6 cm2V-1s-1 and an Ion/Ioff up to 105. Furthermore, an inkjet-printed inverter on glass substrate was fabricated, which can be operated at 10 Hz and the voltage gain is up to 112. However, the printed ITO electrode arrays require high annealing temperature up to 500°C, which is not suitable for conventional flexible polymer or paper substrates140. The performance parameters of TFTs fabricated via fully-printing process on rigid substrate are summarized in Table 2. As compared with printing one or two components in TFTs, it is a huge 31



Page 32 of 62

challenge for realizing fully-printed TFTs because of multilayers and interface contacts. The state-of-the-art TFTs show high-performance parameters but own poor scalability for mass-production via fully printing process. The high-quality printable inks, interface properties and contacts, and matchable printing techniques are the key factors for realizing fully-printed TFTs with high reliability, repeatability and manufacturability.

4. PRINTED TFTs ON FLEXIBLE SUBSTRATE The flexible substrate is the first requirement to achieve flexible electronics, and it is very important to specially designed printable inks. The flexible substrate, e.g. polymer and paper, is different from conventional rigid substrate, and it normally can’t withstand high temperature process. Polyimide (PI) is the polymer that can bear the highest temperature, of which the glass-transition temperature (Tg) is about 360 C182. Thus, it is necessary to consider annealing temperature of inks at the o

designing process, or use instant sintering technology or instant high temperature treatment with low damage to the flexible substrate. In this section, the research progress of printed TFTs on flexible substrates will be discussed.

4.1. Polymer substrates Polymers are the most commonly used flexible substrates in flexible electronics including flexible TFTs98, 183. Comparing with conventional rigid substrates, flexible polymer substrates have a much lower Tg. Thus, it is very important to consider the o

fabrication temperature of printing technology. PI has a Tg up to 360 C, which is much o

higher than the Tg of other polymer substrates, such as PET (120 C), polycarbonate o

o

o

(PC, 155 C), polyethersulfone (PES, 230 C), poly(ethylene napthalate) (PEN, 150 C) and polyetheretherketone (PEEK, 250 C), etc2, 114, 182. Especially, transparent flexible o

substrates are attracting much attention because they are used to fabricate semi-transparent flexible electronics184, 185. Because these flexible polymer substrates can’t

endure

high-temperature

processing

or

treatment,

low-temperature

post-processing methods are developed, such as photonic sintering186, microwave 32


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sintering187, etc. Meanwhile, low-temperature treated inks are necessary to be developed as well188, 189. In addition, the wettability between flexible substrates and inks should be especially considered, which directly determines the quality of deposited thin film190.

4.1.1. Partly printed TFTs on flexible substrate Organic semiconductor is the most common and compatible materials applied in printed and flexible electronics. Xiao et al proposed a transfer printing method to fabricate P3HT TFTs on PET substrate, and it was found that P3HT semiconductor could be separated and demonstrated clear patterns on the PDMS as the transfer mediator191. The flexible P3HT TFTs showed a mobility of 5× 10-3~ 2.2× 10-2 cm2V-1s-1 and an Ion/Ioff of 10. Meanwhile, a novel organic semiconductor NDI2OD-DTYM2 was synthesized and introduced into organic TFTs fabricated by inkjet printing on PET substrate, which exhibited a mobility of 0.07~ 0.45 cm2V-1s-1 and excellent ambient stability90. With the development of ultra-flexibility and sensitivity such as electronic-skin, TFTs fabricated on ultra-flexible substrate is emerging. Deng et al reported CuPc NWs as semiconductor grown on Si substrate, and were then transfer-printed on flexible and transparent PDMS substrate. They were further used for fabricating flexible transistors with a mobility of 2.0 cm2V-1s-1 and an Ion/Ioff up to 104192. The flexible transistors on PDMS substrate (thickness ~100 µm) can be bent with a very small curvature from 12 to 3 mm, and the performance parameters just changed little after being bent in 450 deformation cycles. Furthermore, another CuPc NWs transistors fabricated on PDMS substrate via transfer printing was demonstrated as well, in which 260 µm thick transistors could retain the device performance after being bent in 700 cycles with small curvature of 5 mm. The above CuPc NWs transistors even could be applied to the action recognition of a human palm, exhibiting excellent flexibility, stability and reproducibility, of which the current could retain to the initial value with several cycles. (Figure 9a) 193.

33



Figure 9. (a) The flexible TFTs array was used to action recognition of hand palm with repeatedly crumpled. Reprinted with permission from ref 193.Copyright 2014 Royal Society of Chemistry. (b) The optical images of SWCNT TFTs, inverter arrays and logic circuits on PET fabricated via inkjet-printing. The right image is enlarged pictures of TFTs, inverters and a five-stage ring oscillator, in which T1 and T2 is transistor 1 and 2, respectively. Reprinted with permission from ref 194. Copyright 2014 Royal Society of Chemistry. (c) The photograph of TFTs array with 105 printed TFTs on PET substrate. The bottom image is enlarged pictures of one printed TFTs (scale bar: 500 µm). Reprinted with permission from ref 36. Copyright 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Furthermore, Su et al reported the inkjet-printed SWCNTs as semiconductor and rGO patterns as S/D/G electrodes on PET substrate for constructing TFTs, which showed excellent performance with an Ion/Ioff of ~104 and a mobility of ~8 cm2V-1s-1195. In addition, inkjet-printed biosensor based on graphene TFTs on Kapton substrate was reported by Xiang et al196. The flexible carbon-based CMOS logic circuits can be fabricated by using p-type and n-type CNTs TFTs197-200. However, because of the adsorption of oxygen and water, it is very difficult to construct air-stable n-type CNTs TFTs at low-temperature (≤150 °C). Recently, Xu et al reported inkjet-printed TFTs and logic circuits on PET substrate, in which the top-gate TFTs were constituted by the aerosol inkjet printed SWCNTs as the channel material and silver lines as top electrodes194. Furthermore, 34


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the inverters and five-stage ring oscillators based on flexible and printed top-gate TFTs with a mobility of 46.2 cm2V-1s-1and an Ion/Ioff of 105 were demonstrated (Figure 9b)194. Meanwhile, Zhang et al constructed flexible CMOS circuits based on aerosol inkjet printed p-type and n-type CNTs TFT, in which both of them showed a mobility up to 15 cm2V-1s-1 and an Ion/Ioff of ~105171. Aerosol inkjet printed p-type and n-type CNTs TFTs provide a selectable way to fabricate high-performance logic circuits with large area and good stability. Flexible electrode is also very important to achieve flexible electronics. Recently, an ultrashort channel of 2 µm was successfully deposited by inkjet-printed conducting PEDOT:PSS with modified water-dissolvable PVA on PET substrate, in which the printed channel length and edges could be precisely controlled by pinning effect201. The research hotspot of printed and flexible electrodes is still focused on metal materials because of the low conductivity and stability of organic conducting materials202, 203. Chen et al reported transfer-printed Ag electrodes with laser sintering treatment on PET, which possess good conductivity and excellent flexural endurance even after being bent 2000 times. The pentacene TFTs showed a mobility of 0.053 cm2V-1s-1 and an Ion/Ioff of 1.1× 102172. Peng et al demonstrated a laser sintered Ag electrodes for parylene-C TFTs on PEN by screen printing, showing a mobility of 0.33 cm2V-1s-1, an Ion/Ioff of 106 and Vth of -3.2 V204. For achieving high-performance and low-cost electronics, printed and flexible Cu electrodes were reported by Yu (Figure 9c)36. The IGZO TFTs with vertically printed S/D/G Cu electrodes showed a high mobility of 15.3 cm2V-1s-1 and an Ion/Ioff of 4.22 × 106 even under 1000 folding tests. The performance parameters of partly-printed TFTs on flexible substrates are summarized in Table 3.

35



Table 3. The performance parameters of printed TFTs on flexible substrates

Printed semiconductor


Printed electrodes

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47

Page 36 of 62

Substrate

P3HT, P4VPa, Au/Au/ITO

PET

NDI2OD-DTYM2, PAN(PMSQ), Ag/Ag/Au

PET

Printing Techniques

Printed Materials P3HT

Device Performance Flexibility

Mobility (cm2 V-1 s-1)

Ion/Ioff

Vth (V)

Transfer printing

0.005~ 0.022

10

--

The device can be bended

Ref. 191

Inkjet printing

0.07~ 0.45

(4~6) × 101

-0.6 ~ 10.5

--

90

PDMS PDMS

NDI2OD-DTYM2, Ag CuPc NWs CuPc NWs

Transfer printing Transfer printing

2.0 0.02

~104 ~103

---

192

PET

SWCNTs, graphene

Inkjet printing

~8

~106

0.25

PEN PET PET PET Kapton

SWCNTs SWCNTs, Ag SWCNTs, Ag SWCNTs, Ag Graphene, Ag

Inkjet printing Inkjet printing Inkjet printing Inkjet printing Inkjet printing

0.4 1.5 15 46.2

~104 106 4 10 ~ 106 ~105

--1 ~ 1 ---

450 bendings 700 bendings A5 sized PET substrate. -2000 bendings ---

PET

PEDOT(PSS)

Inkjet printing

0.37~ 0.91

0.92× 103

1.94

--

201

PET PEN PET PEN

Ag Ag Ag Ag

0.053 0.37 10 0.33

1.1× 102 ~105 ~103 106

----3.2

2000 bendings ----

172

IGZO, SiO2(PVP), Gu/Gu/Gu

PET

Gu

9-17

105~ 107

--

1000 bendings

36

DNTT, Parylene-C, Ag/Ag/Ag

Paper

Ag

Transfer printing Inkjet printing Inkjet printing Screen printing Inkjet and screen printing Screen printing

0.33

--

-1.22

65

DNTT, Parylene-C, Ag/Ag/Ag

Paper

Ag

Screen printing

0.297

105

--

-10000 bendings

CuPc, NWs, Ni3Si4, Au/Au/Au CuPc, NWs, Ni3Si4, Au/Au/Au SWCNTs, PMMPA, graphene/graphene/graphene SWCNTs, PI, Au/Au/Au SWCNTs, HfO2, Au/Au/Ag SWCNTs, HfO2, Au/Au/Ag SWCNTs, HfO2, Au/Au/Ag Graphene, --, Ag/Ag/Ag PDQTb, PMMA, PEDOT(PSS)/PEDOT(PSS)/PEDOT(PSS) pentacene, PMMA, Ag/Ag//PEDOT TIPS-pentacene (PS), PVC, Ag/Ag/ Ag SWCNTs, HfO2, Au/Au/Ag DNTTc, Parylene-C, Ag/Ag/Ag

36


193 195 114 205 171 194 196

202 203 204

206

Page 37 of 62


Substrate

Printing Techniques

Printed Materials

Device Performance Flexibility

Mobility (cm2 V-1 s-1)

Ion/Ioff

Vth (V)

~108

0.8

Radius:3 mm Ultra-flexibl e

Ref.

207

IGZO, SiNx, Ti(ITO)/Ti(ITO)/Ti(ITO)

PI

--

Transfer printing

15.9

P3HT (PAN), PAN(PS), --/--/--

--

--

Transfer printing

0.0026

Inkjet printing

0.005

1.75× 106

3

--

209

Inkjet printing

0.0251

6.29× 104

-7.8

--

210

Inkjet printing

0.0123

2.1

--

--

105

Inkjet printing

0.16

--

--

--

81

Inkjet printing

0.26

3.1× 105

-0.17

--

211

Inkjet and screen printing

3.5

--

0.8

--

212

Inkjet printing

91

1.23

--

Inkjet printing

150

2.5

--

P3HT, P(VDF-HFP), PEDOT:PSS/PEDOT:PSS/PEDOT:PSS P3HT(CNP), PVP, PEDTO(PSS)/PEDOT(PSS)/PEDOT(PSS) IGZO, SiNx, Ti(ITO)/Ti(ITO)/Ti(ITO) Fully-printed TFTs

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47


PI PI PI

P3HT, PHPMA(PEI), Ag/Ag/Ag

PET

TIPS-pentacene (PS), PVP, Ag/Ag/ Ag

PEN

Parylene(C8BTBT), CYTOP, Au/Au/Au

PEN

Graphene, BN, PEDOT:PSS/PEDOT:PSS/PEDOT:PSS

Textile

P3HT, P(VDF-HFP), PEDOT:PSS P3HT(CNP), PVP, PEDTO(PSS) P3HT(CNP), PVP, PEDTO(PSS) P3HT, PHPMA(PEI), Ag TIPS-pentacene (PS), PVP, Ag Parylene(C8BTBT), CTYOP, Au Graphene, BN, PEDOT:PSS

-2.5

Radius:4 mm Radius:4 mm

Graphene, BN, Ag/Ag/Ag

PET

Graphene, BN, Ag

SWCNTs( PVP), Ion gel, Ag/Ag/ Ag

PET

SWCNTs( PVP), Ion gel, Ag

Inkjet and transfer printing

0.1~0.8

104~ 106

--

Kapton

CNTs, PVP(pMSSQ), Ag

Inkjet printing

4.1

104

--

102~ 104

--

1000 bendings --

--

--

--

CNTs, PVP(pMSSQ), Ag/Ag/Ag

CNTs, PVA, Au/Au/Au PBS CNTs, PVA, Au Transfer printing 17~37 rGO, high GO, high rGO/high rGO, high GO, high rGO, PEN Inkjet printing 350 rGO/SWCNTs SWCNTs a P4VP: poly(4-vinylphenol) b PDQT: poly [3,6-bis(40-dodecyl[2,20]bithiophenyl-5-yl)-2,5-bis(2-hexyldecyl)-2,5-dihy-dropyrrolo[3,4-c]pyrrole-1,4-dione] c DNTT: dinaphtho[2,3-b:2',3'-f]thieno[3,2-b]thiophene

37


--

208

213

213

2

214

215 216


Page 38 of 62

4.1.2. Fully-printed TFTs on flexible substrate With the emergence of novel functional materials and new printing techniques, the performance of fully-printed flexible TFTs has been steadily improved22, 217. Wu et al demonstrated fully inkjet-printed organic TFTs on PI using double-layer dielectric

structures,

in

which

fluoride-co-hexafluoropropylene)

inkjet-printed

(P(VDF-HFP)),

and

P3HT,

poly(vinylidene

PEDOT:PSS

acted

as

semiconductor, gate dielectric and electrodes, respectively209. The Vth of fully inkjet-printed P3HT TFTs could be adjusted between -13 V and 10 V by changing the composition of printed dielectric layers, leading to a mobility of 5× 10-3 cm2V-1s-1, an Ion/Ioff of 1.75 × 106 and Vth of -3 V. However, fully inkjet-printed organic TFT normally

exhibit

low

mobility. Subsequently,

it

is

possible

to

achieve

high-performance, fully inkjet-printed organic TFTs on PI with incorporating P3HT and CNTs semiconductor. It was found that the mobility and Ion/Ioff of fully-printed TFTs with blending P3HT and carbon NPs were dramatically enhanced, and the Vth was reduced as well210. In addition, P3HT blended with carbon NPs could improve contact resistance and channel resistance in fully inkjet-printed TFTs on PI, resulting in the obvious improvement on mobility from 3.5× 10-4 cm2V-1s-1 to 1.2× 10-2 cm2V-1s-1105. Meanwhile, some novel materials were designed for printed flexible TFTs as well. Huang et al developed a self-healing polymer blends with poly(2-hydroxypropyl methacrylate) and poly(ethyleneimine) (PHPMA/PEI), which could be acted as dielectric layer in TFTs, and exhibited surprisingly high effective thin film capacitance (1400 nF cm-2 at 120 nm thickness and 20-100 Hz) and self-healing property(Figure 10a)

81

. The organic TFTs on PET constructing with inkjet-printed

P3HT, PHPMA/PEI and Ag acted as semiconductor, gate dielectric and electrodes showed a mobility up to 0.16 cm2V-1s-1. Meantime, fully inkjet-printed TFTs on PEN substrate based on small molecule semiconductor TIPS-pentacene were reported as well211. The TFTs fabricated by inkjet printing is consisted of TIPS-pentacene semiconductor layer, PVP dielectric layer and Ag electrodes. The printed flexible 38


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TIPS-pentacene TFTs exhibited a mobility up to 0.26 cm2V-1s-1, an Ion/Ioff of 3.1×105 and Vth of -0.17 V. For small molecule semiconductor, C8BTBT is a good candidate for

fabricating

high-performance

TFTs218.

Liu

et

al

demonstrated

an

ultra-high-resolution printing technique, leading to the room-temperature printing of narrow Au lines and gaps down to 1 µm212. The organic TFTs on PEN, constituting by inkjet-printed parylene and C8BTBT semiconductor layer, screen-printed fluorous polymer (CYTOP) dielectric layer and inkjet-printed Au electrodes, possessed a mobility up to 3.5 cm2V-1s-1.

Figure 10. (a) The healing process images of self-healing polymer film. Reprinted with permission from ref 81. Copyright 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (b) The photograph images of fully-printed SCNT TFTs on PET substrate. (c) The photograph images of Ag electrodes on PET substrate produced by nanoimprinting technique before and after fabrication of Cu film. Reprinted with permission from ref 2. Copyright 2012 Royal Society of Chemistry. (d) Transfer characteristic curves of printed TFTs with a bend radius of 1 mm over 1000 cycles. The inset is the optic image of printed TFTs being wrapped by a cylinder. (e) Variation of the tensile strains on top of the dielectric film fabricated on PET as a function of bending curvature. The inset is the testing schematic diagram, in which r is the bending curvature and the t is the substrate thickness. Reprinted with permission from ref 214. Copyright 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (f) The photograph of printed TFTs on polyester textile. (g) The optic image of TFTs array on flexible textile. Reprinted with permission from ref 213. Copyright 2017 Springer Nature. 39



Carbon nanomaterial is becoming one of the popular materials in last several years for making printable inks in printed TFTs on flexible substrate219. Zhao et al fabricated fully-printed SWCNTs/PVP TFTs on PET via a combination of nanoimprinting, inkjet printing and aerosol inkjet printing, in which nanoimprinting was used for depositing Ag S/D electrodes, inkjet printing was used for depositing SWCNTs/PVP semiconductor layer and ion gel dielectric layer, and aerosol inkjet printing was used for depositing Ag gate electrode (Figure 10b and c)2. The optimum inks were developed by tuning the additives, leading to fully-printed TFTs with a mobility of 1.5 cm2V-1s-1 and an Ion/Ioff of over 4×103. In addition, Cao et al reported a fully-printed CNTs TFTs on Kapton film with an aerosol inkjet printing technique, including semiconducting CNTs, PVP blended with poly(methyl silsesquioxane) (pMSSQ) dielectric and Ag S/D/G electrodes. The CNTs TFTs showed a mobility of 4.1 cm2V-1s-1 and an Ion/Ioff of ~104. Especially, it demonstrated minimal variations in performance for over 1000 cycles of aggressive bending tests (Figure 10d and e)214. Shi et al demonstrated a single-step transfer printing to achieve fully-printed CNTs transistors on poly(butyl succinate (PBS), which is composed of transfer-printed CNTs, PVA and Au acted as the semiconductor, dielectric and electrodes, respectively. The fully-printed CNTs TFTs showed a mobility up to 27 ± 10 cm2V-1s-1 and an Ion/Ioff of 102~104215. Furthermore, Liu et al reported all-carbon-based TFTs fabricated by aerosol inkjet printing on PEN substrate, in which low-concentration rGO (0.5 mg mL-1) was used to fabricate semiconductor channel, high-concentration GO (10 mg mL-1) was used to fabricate dielectric layer due to low-conductive, high-concentration rGO (10 mg mL-1) was used to fabricate S/D electrodes because of highly-conductive, and multi-walled CNTs was acted as gate electrode216. Based on reasonably choosing carbon materials, the all-carbon-based TFTs with fully-printing process on flexible substrate showed an excellent mobility up to 350 cm2V-1s-1 under 1 V bias voltage. Except for polymer films, textile is also applied in printable and flexible electronic220-222. Tian et al reported all inkjet-printed TFTs on PET and textile 40


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substrates with the heterojunction based on graphene semiconductor layer and hexagonal-boron nitride (h-BN) dielectric layer. The inkjet-printed TFTs with Ag S/D/G electrodes on PET and PEDOT:PSS S/D/G electrodes on textile were realized, reaching a mobility of ~91 cm2V-1s-1 at bias voltage of 5 V. The TFTs on textile could sustain up to ∼4% strain and be bent with the radius of 4 mm213. The performance parameters of fully-printed TFTs on flexible substrates are summarized in Table 3. In a word, some progress of fully-printed TFTs on flexible substrate has been achieved, and fully-printed TFTs on flexible substrate could be used to construct logic circuits. However, there are still some issues for realizing fully-printed TFTs on flexible substrate with high reliability, repeatability and manufacturability.

41



4.2. Paper substrate Paper substrate offers the advantages of inexpensive, light weight, biodegradable, and flexible, which are promising for novel platforms with inexpensive, portable and simple TFTs223, 224. However, because of its rough and porous nature, a spreading form with wavy boundaries and an inadequate electrical property are appeared, hindering the achievement of high-performance TFTs. For obtaining ideal substrate, several strategies that converting hydrophilic paper to hydrophobic paper are developed, for example, using photo-paper, modifying papers by organosilanes, reducing surface roughness

225-227

. Huang et al reported a mass-production of

paper-based Ag nanowires by printing-filtration-press (PFP) on different paper substrates, showing that all kinds of paper could be adopted in flexible electronics (Figure 11a)68. However, it is not easy to achieve fully-printed TFTs on paper substrate. Peng et al used screen printing for depositing Ag gate electrode on standard paper, and further for depositing organic TFTs with a mobility of 0.56 cm2V-1s-1 and an Ion/Ioff as high as 109, respectively65. Moreover, one of important features of paper based electronics can be easily degraded and burnt. Peng et al successfully fabricated high-performance parylene-C TFTs on standard paper substrate under room temperature, owning a high mobility of 0.30 cm2V-1s-1 and an high Ion/Ioff of 105. The bending stability of organic TFTs is reasonably good, and the devices current only drops from 20 µA to 3 µA even after 10000 bending cycles with 4.4% bending strain. Satisfactory, paper-based organic TFTs could be burned out by fire within 3 s, leaving only silver and ash content of paper (Figure 11b) 206. The performance parameters of partly-printed TFTs on paper substrates are summarized in Table 3 as well.

42


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Figure 11. (a) The images of various paper substrates (above) and corresponding images of screen printed Ag nanowires electrodes (below). Reprinted with permission from ref 68. Copyright 2014 Royal Society of Chemistry. (b) The photographs of burning process of organic TFTs on paper with different times. Reprinted with permission from ref 206. Copyright 2013 Elsevier B.V.

5. CONCLUSION AND OUTLOOK Printed TFTs have attracted significant attention over the last few years due to the great advantages including low-cost, high-throughput fabrication process and additive manufacturing intrinsic, as well as the flexibility, showing the potential applications in wearable electronics, healthcare devices, displays, human-machine interfaces, and so on. The research progress from China suggests that there are many researchers are focusing on printed TFTs, including printable inks, printed technologies for dielectrics, semiconductors and electrodes, stability, and flexibility, as well as fully-printed TFTs. These researches dramatically accelerate the development of printed TFTs and their actual application in displays and sensors. However, there are still many challenges for further improving the performance of printed TFTs and their commercialization. Firstly, it is urgent to develop high-performance and stable printable materials, as well as green printable inks. As compared to conventional metal electrodes fabricated via thermal or electron beam deposition, printed metal electrodes normally show low conductivity and bad stability. 43



Meanwhile, it normally uses toxic solvents such as chlorobenzene and chloroform to make organic semiconductor inks. Secondly, much improvement on performance is required for fully printed TFTs. There are lots of good results for TFTs with only one or two printed components in dielectrics, semiconductors and electrodes. But the performance is normally very poor for fully printed TFTs. The biggest challenge is to exactly control the interface and nanostructures of printed functional multilayers, which would be determined by printing parameters and ink rheological behavior. Thirdly, the resolution of printed TFTs is still very low as compared to conventional transistor fabrication. Normally, the best resolution is about 20 µm at moment. The resolution is limited by printing technology itself. Recently, it was reported from University of Southern California that the resolution of modified inkjet printing up to 400 nm could be achieved. Hopefully, this printing technique can be used to widely fabricate high-performance TFTs. Finally, printing is large-scale or mass-production fabrication technique. It is important to increase the yields of printed TFTs. In other words, it is very important to retain the repeatability and stability of printing process. The research results in laboratory for small-area printed TFTs looks very good. But large-area printed TFT arrays often have the big issues in repeatability. Thus, it eagerly requires lots of research and technology development in printed TFTs. The development of printed TFTs is still at the early stages, and there is a long way to extensively push their commercialization. Through the joint efforts of government, institutions, universities and companies, printed TFTs would exhibit a prosperous development and booming market.

ACKNOWLEDGEMENTS This work was supported by the National Natural Science Foundation of China (51673214), the National Key Research and Development Program of China (2017YFA0206600), and the Hunan Provincial Natural Science Foundation of China (2015JJ1015).

44


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Printed Thin Film Transistors - American Chemical Society

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