2010 Stretchable, Large-Area Organic Electronics

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Stretchable, Large-area Organic Electronics

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By Tsuyoshi Sekitani and Takao Someya*
sensors,[17–19] actuators,[20,21] and other

Stretchability will significantly expand the application scope of electronics, electronic functions such as a memory[22]
are emerging and being used to create
particularly large-area electronics—displays, sensors, and actuators. If
intelligent surfaces. Thus, as the advance-
arbitrary surfaces and movable parts could be covered with stretchable ment of large-area electronic devices makes
electronics, which is impossible with conventional electronics, new classes of them elastic, it will be possible to place
applications are expected to emerge. A large hurdle is manufacturing elec- flexible sheet-type devices on curved
trical wiring with high conductivity, high stretchability, and large-area com- surfaces.
patibility. This Review describes stretchable, large-area electronics based on One of the examples of stretchable,
large-area sensors is an electric artificial
organic field-effect transistors for applications to sensors and displays. First,
skin (E-skin). Skin-like sensitivity will be a
novel net-shaped organic transistors are employed to realize stretchable, crucial property for future robots to enable
large-area sensor networks that detect distributions of pressure and them to work in an unstructured environ-
temperature simultaneously. The whole system is functional even when it is ment. Flexible, large-area pressure matrices
stretched by 25%. In order to further improve stretchability, printable elastic made of organic electronic devices have
been developed and proposed for E-skin
conductors are developed by dispersing single-walled carbon nanotubes
applications for future generations of robots
(SWNTs) as dopants uniformly in rubbers. Further, we describe integration of (Fig. 1).[17] These devices are inherently
printable elastic conductors with organic transistors to construct a rubber-like flexible and a bendability down to a 2 mm
stretchable active matrix for large-area sensor and display applications. radius has been shown, which is sufficient
Finally, we will discuss the future prospects of stretchable, large-area for robot finger applications. Similar to real
electronics with delineating a picture of the next-generation human/machine human skin, however, stretchability is
crucial. Without stretchability, it is not
interfaces from the aspect of materials science and electronic engineering.
possible to put E-skin on the joints of arms
or curved surfaces.
The first step in the development of stretchable electronics is
1. Introduction the manufacturing of stretchable wirings that exhibit good
mechanical robustness and electronic performance, simulta-
neously. While rigid and/or crystallized materials usually exhibit
The realization of stretchability in electronics is one of the most
good electronic performance and controllability or stability, their
interesting challenges in materials science and engineering. It is
mechanical robustness is poor. Soft materials, on the other hand,
expected that stretchability will open up a new class of
[1–22] show good mechanical properties, but poor electronic properties.
applications in large-area electronics because it will make
Indeed, the highest conductivity for conducting rubbers contain-
it possible to spread electronics over arbitrary curved surfaces and
ing carbon particles is 0.1 S cm1, which is too low for application
movable parts. In the last decade, large-area electronic devices
as wiring of integrated circuits.
have become thin and lightweight, allowing solar cells[7] or
Various types of high-conductivity stretchable materials have
displays to now be easily placed on roofs or walls, respectively.
been developed, such as three-dimensional microstructures in
This development is expected to continue, with displays
poly(dimethylsiloxane) (PDMS) including wavy thin metals,[23–44]
becoming bendable and rollable.[8–16] This emerging technology
metal-coated net-films,[18] graphene films,[45] and a single-walled
is often referred to as flexible electronics. Subsequently, large-area
carbon nanotube (SWNT)-fluorinated copolymer composite.[46]
These stretchable materials exhibit good conductivity and
[*] Prof. T. Someya, Dr. T. Sekitani mechanical stretchability by exploiting structures such as waves
Department of Electrical and Electronic Engineering and Information and nets. Various manufacturing processes have been employed
Systems
The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656 to form three-dimensional microstructures described above,
(Japan) including vacuum evaporation, photolithographic patterning, and
Prof. T. Someya mechanical punching and/or cutting.
Institute for Nano Quantum Information Electronics (INQIE) In order to apply stretchable wirings to large-area electronics,
The University of Tokyo, 4-6-1 Komaba, Meguro-ku, Tokyo 153-8505 scalability of manufacturing processes is very important. One of
(Japan) the most attractive solutions is the use of direct printing
E-mail: someya@ee.t.u-tokyo.ac.jp
technologies with printable inks that have high conductivity and
DOI: 10.1002/adma.200904054 stretchability. For this purpose, an printable elastic conductor has
2228 ß 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Adv. Mater. 2010, 22, 2228–2246
www.advmat.de
Tsuyoshi Sekitani received the
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B.S. degree from Osaka
University, Japan, and the Ph.D.
degree in applied physics from
the University of Tokyo, Japan, in
1999 and 2003, respectively.
From 1999 to 2003, he was with
the Institute for Solid State
Physics (ISSP), University of
Tokyo. From 2003 to 2009, he
was a Research Associate at the
Quantum-Phase Electronics
Center, University of Tokyo. Since 2009, he has been a
Research Associate of the Department of Electrical and
Electronic Engineering, University of Tokyo.
Takao Someya received the Ph.D.

degree in electrical engineering
from the University of Tokyo in
1997. In 1997, he joined the
Institute of Industrial Science
(IIS), University of Tokyo, as a
Research Associate. He was
appointed to be a Lecturer of the
Research Center for Advanced
Science and Technology
(RCAST), University of Tokyo, in
1998, and an Associate Professor
of RCAST in 2002. From 2001 to 2003, he worked for the
Nanocenter (NSEC) of Columbia University and Bell Labs,
Lucent Technologies, as a Visiting Scholar. From 2003 to 2009,
he was an Associate Professor of the Department of Applied
Figure 1. a) An image of an electronic artificial skin, E-skin. Organic Physics and Quantum-Phase Electronics Center, University of
transistors are employed to realize a flexible active matrix, which is used
to read out pressure images from the sensors. The device is bendable since
Tokyo. Since 2009, he has been a Professor of Electrical and
all the layers are made of soft materials. b) A picture of 16 16 sensor cells Electronic Engineering, University of Tokyo. His current
manufactured by integrating organic transistors and pressure sensors on a research interests include organic transistors, flexible
rubbery pressure-sensitive sheet. The periodicity of a sensor cell is 2.54 mm. electronics, plastic integrated circuits, large-area sensors, and
Adapted from [17]. Copyright 2004, National Academy of Sciences. plastic actuators.
been developed using a nanocomposite comprising SWNTs and

fluorinated copolymers.[47] realize a truly rubber-like active matrix and electronic applications
The second step toward stretchable electronics is the such as sensors and displays. All the materials and manufactur-
integration of active devices with stretchable wirings on rubber ing processes described in this Review, including the elastic
substrate. The integrations can be classified in two different conductors used for electrical wiring, organic transistors as active
approaches based on materials. The one is stretchable electronics components, and mechanical processes, are compatible with a
based on silicon or other high-performance materials. The recent large-area, cost-effective process.
progresses of the former category is reviewed by Rogers and his The contents of this Review are as follows; i) introduction, ii)
co-workers.[39] The other is based on organic electronics, whose perforated stretchable sensors, iii) stretchable organic transistor
electronic performances may be low, yet manufacturing costs active matrix using elastic conductors, iv) stretchable active matrix
would be potentially ultralow. organic light-emitting diode display, and v) future prospects.
This Review focuses on organic materials and devices for the
development of stretchable large-area electronics. First, a
perforated organic transistor active matrix is fabricated using 2. Perforated Organic Transistor Active Matrix
mechanical processes. Second, a truly rubber-like transistor active
for Stretchable, Large-area Sensors
matrix using SWNTs-based elastic conductors with extraordina-
rily high conductivity and stretchability is described. The elastic Let us first start describing stretchable, flexible, large-area E-skin
conductors can be finely patterned using high-definition printing films integrated with organic semiconductor-based thermal, and
technologies.[47] Then, this paper also presents the integration of pressure sensors. A plastic film with organic transistor-based
an organic transistor active matrix with elastic conductors to electronic circuits is processed to form a net-like structure, which
Adv. Mater. 2010, 22, 2228–2246 ß 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim 2229
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contact geometry are manufactured with fine shadow masks. The

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magnified image of a transistor is shown in Figure 2d. The base

(substrate) is a 75 mm-thick polyimide film. To form the gate
electrodes, the surface of this base film is coated with a
50 nm-thick gold (Au) layer with a 5 nm-thick chromium
adhesion layer in a vacuum evaporator using shadow masks.
Then, polyimide precursors are spin-coated and cured at 180 8C
for 1 h to form 750 nm-thick gate dielectric layers. A 50 nm-thick
layer of pentacene is deposited to form a channel layer, and a
60 nm-thick gold layer is evaporated through shadow masks to
form the source and drain electrodes of the transistors. The
channel length (L) and width (W) are 50 mm and 1800 mm,
respectively. The periodicity is 4 mm.
2.1.2. Sensor Array

Pressure sensor arrays are formed using a pressure sensitive
rubber containing carbon particles and a silicone rubber matrix.
Such a pressure-sensitive rubber sheet is now commercially
available, with a thickness of 500 mm (PCR Technical Co. Ltd,
Japan). The electrical resistance between the top and bottom
surfaces of the rubber sheet is a function of the mechanical
pressure. When pressure is applied to the rubber sheet, the
resistance decreases from 1 MV at 100 Pa to 100 V at 104 Pa.
Thermal sensors based on organic diodes are manufactured on
an ITO-coated poly(ethylene naphthalate) (PEN) film with a
resistivity 98 V/&. A 30 nm-thick p-type semiconductor of copper
phthalocyanine (CuPc) and 50 nm-thick 3,4,9,10-perylene-
tetracarboxylic-diimide (PTCDI) are deposited in a vacuum
sublimation system. Cathode electrodes are formed by depositing
Figure 2. a) A stretchable organic transistor active matrix network of 150 nm-thick layers of gold. The periodicity is 4 mm and the size
pressure and thermal sensors. A plastic film with organic transistors, of cathode electrodes is 0.19 mm2.
pressure sensitive rubber, and thermal sensors is processed mechanically
to form unique net-shaped structures, which makes the film device 2.1.3. Integration and Mechanical Process
stretchable by 25%. b) Magnified view of the stretched net-structure.
Organic transistors are positioned at intersection areas. c) A circuit Films with organic transistors and diodes are separately
diagram of the pressure and thermal sensor matrix is shown. A word line, transferred to the vacuum chamber without exposure to air after
denoted as WL, is connected to gate electrodes, while a bit line, denoted as the manufacturing process and both surfaces are uniformly
BL, is connected to drain electrodes. The circuit diagram of the thermal coated by a 2-mm-thick passivation layer of poly-
sensor matrix can be obtained when resistances are replaced with diodes.
d) A magnified picture of one organic transistor. The dashed line represents
chloro-para-xylylene, i.e., parylene (Daisankasei Co., Ltd.;
the area of the pentacene channel. e) A picture of 3 3 sensor cells. The diX-SR). For electronic interconnections, spots of parylene are
struts work as electrical wiring for the bit-lines and word-lines. Adapted removed from the electrodes using a CO2-laser drilling machine.
from [18]. Copyright 2005, National Academy of Sciences. These films are mechanically processed by a numerically
controlled (NC) cutting plotter or drilling machine to form
makes E-skin films stretchable by 25% (Fig. 2). This net-like net-shaped structures, as shown in Figure 2. Alternatively, a NC
pressure sensor matrix was stretched over the surface of an egg punching machine will improve the throughput and make it
and pressure images were obtained.[18] Organic transistors using possible to manufacture the net shape by a roll-to-roll process.
high-performance organic semiconductors[48–50] were used as active The periodicity is 4 mm and the width of the bridges is
matrix formation to read out the information from various sensors. 0.3–0.5 mm. Then these net films are laminated together with
microdispenser-patterned silver paste (Musashi Engineering,
Inc., Shotmaster 300) to complete the thermal sensor arrays.
2.1. Fabrication Process Similarly, a pressure sensitive rubber sheet and a copper electrode
suspended by a polyimide film are separately cut to form
net-shaped structures and these two films are laminated on the
2.1.1. Organic Transistors
top of the transistor film to complete the pressure sensor arrays.
Manufactured film devices contain multiple thermal and The last step is to laminate the pressure and thermal sensor arrays
pressure sensors, which are read out with organic transistor checkerwise, as shown in Figure 3. The effective sensing area is
active matrices. The cross-sectional structures of both types of 44 mm 44 mm. A parylene passivation layer is required for this
sensors are shown schematically in Figure 2. First, 12 12 process because the parylene layer that is put on the organic
(144) matrices of pentacene field-effect transistors with a top semiconductor layers works as a flexible gas barrier. Thus, the
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The plastic surface was uniformly coated with
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a 100 nm-thick gold layer and mechanically
processed to form a net-shaped structure. The
resistance of this structure remained
unchanged up to 1.5 N with 25% stretching.
Compared with previous stretchable conduc-
tors,[40,41] the present scheme could make it
possible to interconnect to transistors.
The major part of the strain occurs at the
bases of the current bridges, while it is quite
small in the transistor regions. Indeed, when
tension is applied to the device, mechanical
and electronic failure always occur around one
of the bases of the bridges. A serious concern
may be the mechanical weakness of the
stretchable film device. We tested its mechan-
ical resistance by repeatedly performing a 20%
extension and release of the stress and found
that the device showed no significant electro-
nic degradation even after 1000 cycles (Fig. 3a).
Its mechanical resistance is therefore suffi-
cient for many applications requiring a single
expansion, for example for a permanent
application on a curved surface. A better
mechanical resistance might be required
for applications such as the joints of arms.
This could be obtained if the strain near the
bases of the bridges could be suppressed by
optimizing the structural parameters such as
the thickness of the base films and the width of
the bridges.
Figure 3. a) Resistance of 100 nm-thick Au-coated PEN film with net-shaped structure as 2.2.2. Net-shaped Organic Transistors
function of 20%-stretching cycles. Resistance was irreversibly changed after 2000 cycles.
b) The circuit diagram of one pressure cell (SENCEL) comprising pressure sensitive rubber Organic transistors are characterized in an
and organic transistors. The current (IDS) changes when mechanical pressure is applied to the ambient environment with a semiconductor
pressure sensitive rubber. c) Cross-sectional illustration of the pressure sensor with organic parameter analyzer. The field-effect mobility in
transistors. VDD represents the operation voltage and is the same as VDS in (b). d) The drain the saturation regime is 1 cm2 Vs1, depend-
current, IDS, (at VDS ¼ VGS ¼ 40 V) with and without the application of pressure is monitored as
a function of the stretchability. The dotted-line represents the tension for device failure.
ing on the applied gate bias voltage VGS, which
e) Demonstration of a pressure sensor active matrix on an arbitrary curved surface. Pressure is consistent with our previous reports.[17]
sensor matrix spread over an egg. f) The current of each SENCEL measured by applying a The on/off ratio exceeds 105 when the off
voltage bias of VDS ¼ 20 V and VGS ¼ 20 V under the application of local pressure, and the current is defined as the minimum IDS at the
correct spatial distribution of the pressure obtained by current intensity. Adapted from [18]. positive gate bias.
Copyright 2005, National Academy of Sciences.
device lifetime is drastically enhanced from a couple of days 2.3. Sensing of Pressure and Temperature Distributions
without parylene to at least a number of weeks with parylene.
Furthermore, the parylene layer can prevent mechanical damage
2.3.1. Pressure Sensor
to the transistors or diodes during mechanical testing.
We characterized the pressure sensor matrix with organic
transistors at various temperatures. The circuit diagram of an
2.2. Electrical and Mechanical Performance individual sensor cell (SENCEL) can be seen in Figure 3b; the gate
electrodes of each line are connected to a word line (VWL), while
the drain electrodes of each line are connected to a bit line (VBL).
2.2.1. Net-shaped Electrical Wiring
The device works well in a wide temperature range (30 to 80 8C).
When the device is stretched, the many small square-holes of the The drain current (IDS) at VDS ¼ VGS ¼ 40 V is measured at
net are deformed into diamonds, as shown in Figure 2b. To 30 kPa (300 gf cm2). Since the resistance of the rubbery sheet
investigate the mechanical properties of the net-like structure becomes less than 1 kV at 30 kPa, the transconductance of the
with the application of tension, we prepared a test film sample. integrated device is very close to that of the transistor. The
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performance of the present switching transistors depends on temperature by applying voltages individually to each SENCEL,
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the temperature, but this effect can be compensated for by with VDS ¼ 20 V for each bit line and VGS ¼ 20 V for each word
simultaneously monitoring the temperature at the same position. line, under pressure from a rubber block. Figure 3f shows the
Tension is then applied to the pressure sensor matrix. As results of the current level obtained for each SENCEL when the
shown in Figure 3d, the magnitude of the drain current, IDS, with rubber block is positioned on two sensor cells. As can be seen,
and without the application of pressure remains practically the position and pressure are clearly obtained using the
unchanged when the tension increases up to 25%-stretching, perforated organic transistor active matrix.
while a device is not functional due to electronic disconnections at
the bridge wiring at more than 30%. Such a robust sensor 2.3.2. Thermal Sensor
performance against tension is realized in the present device The complete devices, including the diode-based thermal
because the tension induced in the transistors or sensors is much sensors, were characterized at temperatures between 30 and
less than that on the wiring, as mentioned above. We should note 100 8C. The temperature dependence of the transistor is much
here that conductive rubber, which is inherently stretchable, is smaller than that of the diode-based thermal sensors. The
formed into a net: When tension is applied to the device, the saturation current, IDS, (at VDS ¼ VGS ¼ 40 V) of a transistor
bridges of conductive rubber just become longer, with the sensor measured at 80 8C is only 50% larger than that obtained at 30 8C,
performance remaining practically unchanged. while the current (at a bias voltage of 1 V) of the diodes at 80 8C is
The device was put on the surface of an egg, as shown in larger than that at 30 8C by a factor of 7 (Fig. 4a). More
Figure 3e. A pressure spatial map is obtained at room importantly, the on/off ratio of the transistors depends much less
on temperature and exceeds 105 even at 80 8C. Furthermore, no
significant damage is found after the removal of heating up to
80 8C, indicating that the present devices have good heat-resistance.
2.4. Simultaneous Sensing of Pressure and Temperature
As shown in Figure 4b, the perforated pressure sensors and

thermal sensors are laminated so that they are positioned
alternately at each hole. This staggered configuration enables the
Figure 4. a) One cell of a thermal sensor network device consisting of

diode-based thermal sensors and organic transistors is characterized at
various temperatures from 30 to 80 8C. b) Illustration and picture of
integration of pressure and thermal sensor matrices. c,d) The saturation
current, IDS, (at VDS ¼ VGS ¼ 40 V) measured for a sensor cell (SENCEL)
at various temperatures under the application of pressure (30 kPa) and its
release (0 kPa). A copper block (15 mm 37 mm) whose temperature is
maintained at 50 8C is positioned at the centre of the array, as marked by
the dotted line. The sensing area is 44 mm 44 mm. e) Image of stretch- Figure 5. The manufacturing process for printable elastic conductors and
able E-skin on the arm of a robot. Adapted from [18]. Copyright 2005, pictures of the materials. Adapted from [47]. Copyright 2009, Nature
National Academy of Sciences. Publishing Group.
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sheets to detect pressure and temperature simultaneously In this regard, we have demonstrated truly rubber-like
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without sensor interference. When a mechanical pressure of integrated circuits that integrate a variety of materials ranging
about 30 kPa is applied to the laminated sensors using a metal from rigid and semi-rigid elastomers to gels.[46,47] In particular,
rectangular bar at 50 8C, we successfully and simultaneously we succeeded in the fabrication of a highly elastic conductor and
obtain the spatial distributions of the pressure and temperature gel, which could be used as stretchable wires and contacts in
(Figs. 4c and d). This indicates feasibility of using a perforated elastic integrated circuits. By taking advantage of a novel process
organic transistor active matrix to read out sensor information. that can uniformly disperse finer bundles of SWNTs in a rubber
Figure 4e shows a demonstration of the perforated thermal and matrix without shortening the length of nanotubes, the
pressure sensors spread over the surface of a robot’s arm, and SWNT-rubber composite gel becomes increasingly viscous, and
working as E-skin. consequently this material can be finely patterned using direct
printing technologies. Furthermore, the newly fabricated printed
elastic conductor requires no additional coating or mechanical
processing. It can be stretched by 118% and has an extraordinarily
3. Rubber-like Stretchable Organic Transistor high conductivity of 102 S cm1. To the best of our knowledge,
Active Matrix Using Elastic Conductors this is the highest value reported thus far for a stretchable,
printable conductor. The content of SWNTs[51,52] that were used
Although we can demonstrate the feasibility of the stretchable
as dopants could be increased up to 20 wt % without sacrificing
organic transistor active matrix with a net-shaped structure,
the mechanical flexibility or softness of the copolymer. The elastic
issues still remain in relation to the perforated configurations. For
conductors are chemically stable and stick well to base plastic
example, it cannot be stretched biaxially or in all directions, and
films. These elastic conductors were integrated with printed
the stretchability is limited to 25 30% because the wiring
organic transistors to fabricate a truly rubber-like active matrix,
materials on plastic films are not inherently stretchable.
which could be stretched by 70% without mechanical or electrical
damage. Furthermore, we integrated such printed elastic
Figure 7. a) Picture of 1.5-mm-wide elastic conductor stretched by 100%.

Figure 6. a) A picture of the printed elastic conductors on a PDMS sheet. b) The printed elastic conductors patterned using screen printing. The
Printed elastic conductors patterned by screen printing can be stretched by linewidth and spacing are both 100 mm. The elastic conductors are
100% without electrical or mechanical damage. A linewidth is 100 mm. chemically stable and adhere to the PDMS rubber sheet. The picture
Insets show a scanning electron microscopic (SEM) image of the surface of was taken before stretching. c) Micrograph with 100%-stretching. d and
a printed elastic conductor. The picture was taken without stretching. b) A e) Micrographs of the printed elastic conductors taken after stretchin-
magnified SEM image of the elastic conductor. Finer or exfoliated bundles g-release from 100% and 200% stretching. The elastic conductors were not
of SWNTs were uniformly dispersed in the rubber, and formed well- damaged electrically or mechanically after stretching by 100%, but stretch-
developed conducting networks. Adapted from [47]. Copyright 2009, nature ing by 200% caused delamination. Adapted from [47]. Copyright 2009,
publishing group. Nature Publishing Group.
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conductors with organic transistors and organic light-emitting A schematic representation of the manufacturing process is
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diodes (LEDs)[53–55] to realize a truly rubber-like active matrix shown in Figure 5. As a chemically stable and highly conductive
organic LED display. A 16 16-grid of transistors was used to dopant, super-growth (SG) SWNTs of high purity and with a high
drive the display and the effective size of the active matrix was aspect ratio (>99.98% in purity, >1 mm in length, and 3 nm in
10 cm2 10 cm2. The display could be stretched by 30–50% and diameter)[52] were used. Typically, a mixture of SG-SWNTs
spread over a hemisphere without any mechanical or electrical (30 mg), an ionic liquid (1-butyl-3-methylimidazolium bis(tri-
damage. Furthermore, it remained functional even when folded fluoromethanesulfonyl)imide, BMITFSI, 60 mg), and
in two or crumpled up, indicating good durability. 4-methyl-2-pentanone (20 mL) was stirred at 25 8C with a
magnetic stirrer (>700 rpm) for 16 h. The resulting swollen gel
3.1. Printable Elastic Conductor was processed on a high-pressure jet-milling homogenizer
(60 MPa; Nano-jet pal, JN10, Jokoh), giving a black paste-like
An elementary substance of SWNTs has been well-known to substance, referred to as ‘‘bucky gel.’’ Then, 4-methyl-2-
exhibit high conductivity like metals (>105 S cm1). However, pentanone (80 mL) and a fluorinated copolymer, vinylidene
typical SWNT-polymer composites exhibit very low conductivity fluoride-tetrafluoroethylene-hexafluoropropylene (50–1500 mg;
less than 101 S cm1 [56] because SWNTs are generally formed in Daiel-G912, Daikin; referred to as G912 henceforth), were
the state of strongly entangled bundles due to the strong successively added to this gel and the mixture was stirred at 25 8C
van-der-Waals bonds; therefore, it is very difficult to disperse for 16 h. It was then poured onto a glass plate by drop casting and
SWNTs uniformly into other materials including polymers and air-dried for 6 h to afford a SWNT-rubber composite gel (referred
rubbers. Fukushima et al.[57,58] and our previous works in to as SWNT paste henceforth; Fig. 5). The viscosity of this
Science[46] reported the methods to untangle SWNTs to finer paste was approximately 10 Pa s. Further, when the SWNT
bundles using compatible ionic liquids[59] and ultrasonic paste was air-dried for more than 12 h, an elastic conductor was
dispersion, and then realized elastic conductors. However, the formed.
material (SWNT-rubber composite gel) was
incompatible with printing due to low-viscosity
and reaggregation and, furthermore, it
required an additional rubber coating and
mechanical process to improve elasticity.
Recently, taking advantages of a novel process
using jet-milling, the SWNT-rubber composite
gel become increasingly viscous, and conse-
quently this material can be finely-patterned
using direct printing technologies.
Furthermore, a printed elastic conductor
requires no additional coating and mechanical
process, and can stretch by 118% and has an
extraordinarily high conductivity of 102 S
cm1. In this subsection, we describe the
manufacturing process of printable elastic
conductors.[47]
3.1.1. Manufacturing Process

The design strategy for elastic conductors
utilizes SWNTs as a conducting dopant due to
their chemical inertness and ability to improve
the mechanical properties of polymer
matrices. Furthermore, it has been reported
that bundles of SWNTs become much finer by
grinding with imidazolium ion-based ionic
liquids[57–59] and utilizing a jet-milling pro-
cess. By taking advantage of this method,
SWNTs were uniformly dispersed into a
fluorinated copolymer matrix to fabricate an
SWNT composite (in this paper simply
referred to as elastic conductors). In order to Figure 8. a) SEM (S4300, Hitachi High-Technologies) images of super-growth (SG) SWNTs
before and after jet milling at 60 MPa. These results indicate that the huge bundles of SG SWNTs
significantly improve the contractility, the with widths of approximately 80–100 mm become much finer, and form nanotube networks after
SWNT elastic conductors were finally coated jet milling. b) An atomic force microscopy (AFM) image where the surface of an elastic conductor
with a dimethylsiloxane-based rubber as a is very smooth, with an RMS value of 17.3 nm. Adapted from [47]. Copyright 2009, Nature
sealant. Publishing Group.
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The SWNT paste was patterned on rubber sheets made of a Figure 6b and the inset of Figure 6a show images of the surface
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silicone elastomer (polydimethylsiloxane, PDMS; Sylgard 184, of printed elastic conductors taken using a scanning electron
Dow-Corning) using screen printing through shadow masks. The microscope (SEM, S4300; Hitachi High-Technologies). The
patterned SWNT pastes were air-dried for more than 6 h to afford smooth surface confirms that the bundles of SWNTs were made
fine SWNT-based elastic conductors with a linewidth of 100 mm much finer through the ionic liquid and jet-milling processes. In
(Fig. 6). The resolution is currently limited by the adhesion fact, the SWNTs were significantly untangled or exfoliated by the
between the SWNT paste and PDMS substrate. The printed jet-milling process (Fig. 8). Furthermore, the uniformity of the
elastic conductors can be stretched by approximately 100% carbon-nanotube conducting network indicates the material
without mechanical damage or delamination from the PDMS compatibility of the carbon-nanotube, ionic liquid, and rubber
matrix (Fig. 7). Note that the stretchability can be enhanced by matrix (Fig. 9), which will be discussed later. This novel process,
sandwiching the printed elastic conductors between rubber including the ionic liquid and jet milling, significantly untangled
substrates because the encapsulation prohibits the delamination or exfoliated the bundles of SWNTs, and formed well-developed
of the elastic conductors. nanotube networks in a rubber, as shown in Figure 6b.
3.1.2. Electrical and Mechanical Characteristics
The electrical and mechanical properties of the printed elastic
conductors under tensile stress were investigated using a
precision mechanical stretching system (Autograph AG-X;
Shimazu). Figure 10 shows a plot of the conductivity as a
function of the stretchability as the SWNT content was changed
from 1.4 to 15.8 wt %. An SWNT content of 15.8 wt % produced
an extraordinarily high conductivity of 102 S cm1, along with a
stretchability of 29%. In contrast, the conductors with 1.4 wt %
SWNTs exhibited an extraordinarily high stretchability of 118%
and a conductivity of 9.7 S cm1. Importantly, the elastic
conductors did not show significant changes in conductivity or
Figure 9. a) The compatibility of the fluorinated copolymer, ionic liquid,

and organic solvent is one of the most important factors in realizing
printable elastic conductors. The molecular structures of fluorinated
copolymers, vinylidene fluoride–tetrafluoroethylene–hexafluoropropylene
(G912), and vinylidene fluoride (VDF)–hexafluoropropylene (HFP) with
VDF ratios (m) of 0.78 (G801) and 0.88 (Kyner) were used in this
experiment. G912 and G801 are soft rubbers, while Kyner is a hard resin.
The Mooney viscosities (ML1 þ 10 100 8C) of G912 and G801 are approxi-
mately 77 and 70, respectively. In the same figure, three types of ionic
liquids, BMITFSI, 1-methyl-3-butylimidazolium tetrafluoroborate:BMIBF4,
and 1-methyl-3-ethylimidazolium tetrafluoroborate:EMIBF4, are also
described. The organic solvent is 4-methyl-2 pentanon (Aldrich). The
copolymers (300 mg) were mixed with ionic liquids (300 mg) and 10 ml
of 4-methyl-2 pentanon was added. The resulting suspensions were stirred
at 30 8C for 12 h and then left standing for 3 days. When G912 was mixed
with BMIBF4 or EMIBF4, we observed a separation of phases, as shown by
the arrow. However, this did not occur when BMITFSI was used. In fact,
BMITFSI was highly compatible with the other copolymers, G801 and Figure 10. a) Electrical and mechanical characteristics of printed elastic
Kyner. b) Pictures of elastic conductors where Kyner and EMIBF4 were used conductors. The conductivities of the printed elastic conductors as a
in this process. The resulting material became porous and had an ash-like function of stretchability are shown, where typical elastic conductors with
color, which may be attributable to phase separation. Furthermore, fluori- 15.8, 5.1, and 1.4 wt % SWNTs are represented. The conductivity increases
nated copolymers are indispensable for film formation. Although the with the SWNT content, while the stretchability decreases. Furthermore,
material compatibility also depends on organic solvents, we used the conductivity does not change with stretching. b) The stretchability and
4-methyl-2 pentanon because G912 is highly resolvable into 4-methyl-2 conductivity are shown as functions of the SWNT content. Adapted from
pentanon. Adapted from [47]. Copyright 2009, Nature Publishing Group. [47]. Copyright 2009, Nature Publishing Group.
www.advmat.de
any sign of mechanical damage when fully stretched. For was as low as 0.1 S cm1, which is insufficient for electronic
REVIEW
comparison, a conventional conducting rubber containing carbon circuit applications. In fact, the low conductivity of electrical
particles was also tested. Although the stretchability of the wiring may result in low-speed response, large voltage depres-
conventional conducting rubber exceeded 150%, the conductivity sion, and large power consumption.
Figure 11 shows effect of the carbon-nanotube length on the
conductivity and stretchability. Elastic conductors with super-
growth (SG) SWNTs (>1 mm in length and 3 nm in diameter)
typically exhibited a conductivity in excess of 40 S cm1 when the
materials and content were optimized. The average conductivity
of films with commercially available HiPco SWNTs was lower
than that of films with SG SWNTs by a factor of 2 or 3. This result
indicates that a high aspect ratio of carbon nanotubes is important
to obtain higher conductivity.
Furthermore, the effects of the ionic liquid, BMITFSI, on the
conductivity were investigated. As shown in Figures 11b and c, an
appropriate BMITFSI content enhances the conductivity, as well
as the stretchability. We believe that this is because the ionic
liquids could prevent the nanotube bundles from aggregating,
resulting in a uniform dispersion of SWNTs in the rubber matrix.
The balance between conductivity and stiffness (stretchability)
Figure 12. a) Pictures of the top and side views of perforated elastic
conductors. The stretchability is much enhanced by the mechanical punch-
Figure 11. a) The conductivity of elastic conductors as a function of ing process because of three-dimensional deformation. b) The conductivity
stretchability, where two sample pf elastic conductors are compared: as a function of uniaxial stretching. Measurements were performed on
RED, elastic conductor manufactured with SG SWNTs (>1 mm in length three samples in ambient air: (1) elastic conductor, (2) perforated elastic
and 3 nm in diameter); and BLUE, commercially available HiPco SWNTs. conductor with PDMS coating, and (3) commercially available carbon-
The carbon-nanotube length is important, not only for conductivity, but particle-based conducting rubber. c) Changes in the conductance of
also for stability under stretching. b) The effects of BMITFSI on conduc- perforated elastic conductors under uniaxial stretching cycles. The stretch-
tivity. c) The stretchability and conductivity of elastic conductors as func- ability values were 25, 50, 70, 110, and 130%. Adapted from [46]. Copyright
tions of the ionic liquid content. Adapted from [46]. Copyright 2008, AAAS. 2008, AAAS.
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can be controlled by changing the BMITFSI content. also very essential. We performed material compatibility tests to
REVIEW
Such controllability over the mechanical and electrical character- determine which elastic polymers and ionic liquids would be
istics is important in practical applications of stretchable compatible with each other (Fig. 9). We examined three different
electronics. fluorinated copolymers: G912 and vinylidene fluoride–
hexafluoropropylene copolymers with composition ratios of
0.78:0.22 (Daiel-G801, Mw ¼ 150 000, Daikin; referred to as
3.1.3. Carbon-nanotube Dispersion and Material Compatibility
G801 henceforth) and 0.88:0.12 (KYNAR-FLEX2801,
There are three important factors that determine the conductivity Mw ¼ 30 000, Arkema; referred to as Kyner henceforth). G912
and stretchability of the printable elastic conductors. The first is is very soft and elastic, but this often results in the separation of
the mixing ratio of the SWNTs, ionic liquid (BMITFSI), and G912 and the ionic liquid phases. We employed BMITFSI, which
fluorinated copolymer matrix (G912). The SWNT content was is compatible with several fluorinated copolymers. In fact, when
changed from 1.4 to 15.8 wt % (Fig. 10) while the BMITFSI G912 and BMITFSI were used, the resulting SWNT rubber films
content was maintained at twice the SWNT content. When the were very smooth, flat, and uniform (Fig. 7), and thus exhibited
SWNT content was greater than 6 wt %, the conductivity was high conductivity and stretchability. In contrast, when Kyner
higher than 50 S cm1, while the stretchability was less than 40%. (which is a hard resin) was used, the resulting films exhibited a
In contrast, at less than 6 wt % of SWNTs, the stretchability was conductivity of only 21 S cm1 and were very fragile and not
higher than 50%, while the conductivity was
less than 40 S cm1. Importantly, we found
that the elastic conductors have very smooth
surfaces and high film quality over a wide
range of SWNT content. This is due to the
compatibility of the constituent materials, as
described later. Furthermore, Figure 10b
clearly indicates that the important para-
meters—conductivity and stretchability—
can be systematically controlled and tailored
to the demands of an electronic application,
although there is a trade-off between the two
parameters. One of the approaches for
enhancing the stretchability will be described
in Section 3.1.4.
The second factor is the method used to
exfoliate the bundles of SWNTs and make
them finer, so that they are uniformly
dispersed in the elastic fluorinated copolymer
matrix. Typical dispersing techniques such as
ultrasonication, grinder milling, and ball
milling can make the bundles finer, but at
the same time, they make the SWNTs shorter,
thus reducing conductivity. We used a jet
milling high-pressure homogenizer that
breaks materials into fragments with a high-
pressure jet. It is particularly worth noting that
a novel process allows us to uniformly disperse
finer bundles of SWNTs into a rubber matrix
without shortening the length of the nano-
tubes during the process (Fig. 8). The resulting
longer and finer bundles of SWNTs can form
well-developed conducting networks in rub-
bers, as shown in Figure 6, thus simulta-
neously leading to higher conductivity and
stretchability. This situation also realizes the
printability of this material since the SWNT
paste becomes increasingly viscous at more Figure 13. a) Images of a large-area stretchable active matrix comprising 19 37 printed organic
than 10 Pa s, which is well suited to high- transistors and wiring using the SWNT elastic conductor. The printed organic transistors function
as active components, while the SWNT elastic conductors function as word-lines and bit-lines for
definition screen printing.
interconnections among the transistors. A picture of the matrix was taken on a curved surface.
In addition to the mixing ratio and disper- b) The magnified image of one cell. SWNT elastic conductors were formed with a net-shaped
sing process, the compatibility of the materi- structure using a mechanical punching system and then coated with PDMS. c) Schematic
alsthe SWNTs, ionic liquids, and copolymersis illustrations of the stretchable active matrix. Adapted from [46]. Copyright 2008, AAAS.
www.advmat.de
stretchable. When G801 (which is also a soft rubber) was used, carbon particles (Kinugawa Rubber Industrial, Co. Ltd.) are also
REVIEW
the conductors exhibited a stretchability of 87% and conductivity shown in the figure. Although the stretchability of the
of 3 S cm1 with 1.8 wt % SWNTs, and a stretchability of 24% and commercial conducting rubber exceeded 150%, its conductivity
conductivity of 22 S cm1 at 15.7 wt % SWNTs. The results of was approximately 0.1 S cm1 for all strains, which is insufficient
the compatibility tests convinced us that, in a process that for electronic circuit applications. In contrast, the SWNT elastic
includes jet milling, a combination of G912 and BMITFSI is the conductor (G801 is used in this experiment) exhibited a high
best from both the electrical and mechanical performance conductivity of 57 S cm1, and did not show significant changes
points of view. in conductivity or mechanical damage when uniaxially stretched
by 38% or less. Furthermore, the perforated elastic conductor
exhibited a high conductivity of 57 S cm1, and could be
3.1.4. Perforated Elastic Conductors
uniaxially stretched up to 134%. However, its conductivity
One of the attractive approaches for achieving a better balance decreased moderately with the application of tensile strain. Even
between the conductivity and stretchability is the use of under such a large strain, the material showed good conductivity
mechanical punching to form a net-shaped structure, although (6 S cm1). We observed that the shapes of the holes of elastic
this manufacturing process is more complex. Perforated elastic conductors changed during stretching. The enhancement in the
conductors with a net-shaped structure were produced using a stretchability of the net-shaped structure was realized because
mechanical punching system (MP-8200Z, UHT Corporation). the interconnecting struts buckled and twisted out-of-plane upon
Stretch tests were performed using a high-
precision mechanical system. The shape of the
holes in the perforated films changed during
stretching. These perforated films enhanced
the stretchability because the interconnecting
struts buckled and twisted out-of-plane upon
tension. Figure 12a shows the top and side
views of perforated films under different
tensile strains; the photographs were taken
with a digital camera.
The maximum stretchability of a net-shaped
structure depends on the roundness of the
corners of the holes, as well as on their
geometries and the modulus of resilience. For
example, PEN films are semi-rigid and cannot
be stretched, while perforated PEN films with a
thickness of 150 mm and similar hole geome-
tries can be stretched up to 30 35%. Due to
similar mechanisms, the stretchability of the
net-shaped elastomer can be improved
significantly.
The degree of stretchability and the appar-
ent modulus depend on the direction of the
strain relative to the struts that form the
boundaries of the holes and the overall
geometry. In the net-shaped elastic conductors
with the PDMS coating, the struts are
0.6 1.0 mm in width and 150 250 mm in
thickness. The periodicity of the boundaries of
the holes is 5.04 mm, which is determined by
the periodicity of the organic transistors. By
reducing the width of the struts, we could
improve the mechanical performance of the
conductors, while the conductance decreased.
Therefore, the overall geometry of the system Figure 14. a,b) Typical transistor characteristics of the discrete transistors (before interconnec-
has to be designed carefully so that both the tion using SWNT elastic conductors). The channel width and length of the transistors were 2 mm
mechanical and electric performances meet and 150 mm, respectively. c) The transfer characteristics of typical transistors before and after
the requirements of the specific application. integrating SWNT elastic conductors, represented by red and green lines, respectively. The
Figure 12b shows the conductivity as a via-holes of the transistors were filled with Ag paste and connected to the SWNT elastic
conductors electrically and mechanically using SWNT paste. No damage or change was observed
function of uniaxial stretching. For compar- even after the integration. The typical characteristics of the organic transistors with the via holes
ison, the stretchability and conductivity of a filled with SWNT paste (blue line) are also shown for comparison. Adapted from [46]. Copyright
commercial conducting rubber containing 2008, AAAS.
www.advmat.de
tension. The deformations of perforated films with net-shaped contact pads for the gate, source, and drain electrodes using
REVIEW
structures will be modeled in a future study, in order to further the SWNT paste.
optimize their mechanical robustness and electronic
performance.
3.2.1. Integration Process
To investigate the reversibility of the elastic conductor, several
stretching cycles were applied. Measurements were performed at Figures 14a and b show the typical transistor characteristics of the
each stretching cycle using the four probe method. Figure 12c discrete transistors (before the interconnections using the SWNT
shows the normalized conductance as a function of the elastic conductors). The channel width and length of the
number of uniaxial stretching cycles. There was no significant transistors were 2 mm and 150 mm, respectively. Figure 14c
change in conductance even after 4000 25%-stretching cycles, shows the transfer characteristics of typical transistors before and
500 50%-stretching cycles, 20 50 70%-stretching cycles, or after integrating the SWNT elastic conductors, represented by red
1 2 110%-stretching cycles. A further increase in strain and green lines, respectively. The via holes of the transistors were
beyond 110% caused an irreversible change in conductance, filled with Ag paste and connected to the SWNTelastic conductors
although it remained greater than 1 S cm1. Similar to other electrically and mechanically through SWNT paste. No damage or
stretchable materials, either conducting or non-conducting, our change was observed even after the integration. The typical
elastic conductor exhibits irreversible mechanics after many characteristics of the organic transistors with the via holes filled
stretching cycles. However, our conductor with a conductivity of with SWNT paste (blue line) are also shown for comparison.
50 S cm1 can be stretched approximately 500 times at a high Images of the top view and cross section are shown. A large
level of strain (50%) without significant degradation. The decrease in the channel currents was observed when the SWNT
feasibility of such a robust conductor was
demonstrated unambiguously using a net-
shaped structure with a PDMS coating. In our
study, the electrical and mechanical character-
istics of the conductor did not deteriorate over
time (at least a year), because its components
were chemically stable.
Carbon-nanotube-based conducting materi-
als or carbon-nanotube/conducting-polymer
composites have also been produced by other
groups.[60–63] Especially, Spinks et al. and Shim
et al. reported composites with high conduc-
tivities of the order of 100 S cm1 by taking
advantage of highly-conductive polymers.[61,62]
Recently, Asaka and coworkers demonstrated
the fabrication of SWNT films comprising
millimeter-long SWNTs and an ionic liquid,
which also exhibited high conductivity of
169 S cm1 [63]. However, these materials
reported so far cannot be stretched.
3.2. Integration of Elastic Conductors with

Printed Organic Transistors
Taking full advantage of the SWNT elastic

conductor and paste, a 19 37 organic
transistor-based stretchable active matrix
(Fig. 13) was manufactured by combining
printing, vacuum evaporation, and mechanical
processes. The manufacturing process used
for the printed organic transistors can be seen
in our previous reports.[46,64,65] An array of
organic transistors was connected together by Figure 15. a) Transfer characteristics of 64 discrete transistors (before wiring, blue lines) and the
elastic conductors (bit lines for source electro- transistors that form an active matrix using SWNT elastic conductors (after wiring, red lines). The
channel width and length of the transistors were 6 mm and 150 mm, respectively. The changes in
des or word lines for gate electrodes). The
b) saturation currents, c) field-effect mobilities evaluated in the saturation regime, and d) on/off
transistor characteristics did not change after ratios are shown. The dashed lines represent average values. Histograms before and after wiring
the formation of the interconnections with the are also shown. The mobilities decreased by 50%, which may be due to the effect of the PDMS
fabricated elastic conductors. The SWNT coating on the transistors and partially due to air degradation during several process steps.
elastic conductors were connected to the Histograms of the performances are also shown. Adapted from [46]. Copyright 2008, AAAS.
www.advmat.de
paste was used as the material for filling the via holes since there were measured for the transistor positioned at the center of
REVIEW
was no path for vaporizing the organic solvent, although the the matrix, because that transistor was stretched to a greater
SWNT paste required an organic solvent for drying. This result extent than those at the corners. When the sheet was stretched by
clearly demonstrates that residual organic solvents affect the 70% or less, the changes in the transistor’s characteristics were
electrical characteristics. In contrast, excellent electrical char- negligibly small. Subsequently, the extension distortion was
acteristics were acquired using SWNT-based materials when the released, and recovery tests were performed to measure the
organic solvent was eliminated completely. transistor’s characteristics without strain (Fig. 17). After it was
stretched by 70% or less, the transistor’s characteristics without
strain did not change as compared to those measured before the
3.2.2. Device-to-device Uniformity After Integration
stretching tests. Furthermore, no changes in its electrical
Stand-alone organic transistors (before wiring using SWNT characteristics or mechanical damages were observed after 30
elastic conductors) and their active matrices (after wiring) were cycles at 70% stretching, thereby indicating the good electrical
characterized to evaluate the electrical functionalities of the functionalities and stability of the active matrix under stretching.
manufactured SWNT elastic conductors in a large-scale matrix. However, stretching by 70% or more resulted in irreversible
As shown in Figure 15, all the transistors were functional after degradation. This is mainly due to the exfoliation of the printed
interconnecting the organic transistors using
the SWNT elastic conductors. Figure 15a
shows the transfer characteristics of 64
discrete transistors (before wiring, blue lines)
and the transistors used to form an active
matrix with the SWNT elastic conductors (after
wiring, red lines). The channel width and
length of the transistors were 6 mm and
150 mm, respectively. The changes in the
saturation currents, field-effect mobilities
evaluated in the saturation regime, and on/
off ratios are shown in Figures 15b, c, and d,
respectively. The dashed lines represent aver-
age values. Histograms before and after wiring
are also shown. The mobilities decreased by
50%, which may be due to the effect of the
PDMS coating on the transistors and partially
due to air degradation during several process
steps. The on/off ratio also decreased from 107
to 106 after the interconnections were formed.
Such a reduction in the on/off ratio was
generally observed when transistors were
wired to each other using word lines and bit
lines since a small leakage current (typically
less than 100 pA) was added for every row and
column, even though all of the elastic
conductors were coated with PDMS. It will
be necessary to suppress such leakage currents
in order to increase the number of transistors.
One of the possible processes for suppressing
this leakage is forming an insulating paste by
screen printing.
3.3. Electrical and Mechanical

Performances
The sheet was stretched by increasing the

tensile strain, and the transistor characteristics
on the stretched sheet were examined (Fig. 16).
Figure 16. a) Pictures of stretching tests for the active matrix captured in the initial state before
In order to uniformly apply accurate strains stretching and under uniaxial and biaxial stretching. b) Transistor characteristics and c) channel
to a transistor active matrix, a small active currents measured under uniaxial stretching. The channel currents (IDS) were normalized with the
matrix comprising 10 10 cells was used. IDS measured before the experiments as the initial state. d) Transistor characteristics and
Furthermore, the electronic characteristics e) channel currents measured under biaxial stretching. Adapted from [46]. Copyright 2008, AAAS.
www.advmat.de
light emission during high-frequency opera-
REVIEW
tion. After manufacturing the organic LEDs
and organic driving cells independently on
separate PDMS sheets, the two sheets were
laminated together to construct a rubber-like
stretchable display.
4.1. Fabrication Process
4.1.1. Organic Transistor Active Matrix for

Driving Organic LED Display
A 16 16 organic transistor active matrix
was manufactured by vacuum evaporation,
chemical vapor deposition (CVD), and via-
hole formation using a CO2 laser. The driving
cell array, an enlarged view, and a cross-
sectional illustration of one cell are shown in
Figure 18. Details of the manufacturing
process can be seen in our previous report.[47]
An organic transistor active matrix was
mechanically processed and integrated with
printed elastic conductors on a silicone
rubber substrate. First, a 500 mm-thick poly-
dimethylsiloxane (PDMS; Sylgard 184,
Dow-Corning Toray Co. Ltd.) sheet was
Figure 17. a) Transistor characteristics and b) channel currents (IDS) after the release of uniaxial
prepared, and elastic conductors were pat-
stretching of up to 100%. c) Transistor characteristics and d) channel currents (IDS) after the
release of 100% biaxial stretching. The IDS values were normalized by the IDS measured before the terned on it using screen printing to form
experiments as the initial state. The change in transistor performance was negligibly small for a scanning-lines and ground-lines with line-
tensile strain of up to 80%, indicating the mechanical robustness of the present device under widths of 500 mm. It was transparent and had
stretching. Adapted from [46]. Copyright 2008, AAAS. a maximum stretchability of 120%. After
manufacturing the 16 16 organic driving
cell active matrix, the parts of the films not
supporting organic transistors or capacitors
Ag electrodes from the plastic substrates. The disconnection of were punched out using a mechanical punching system. It
the organic transistors from the SWNT elastic conductors was should be noted that in this process, the driving cells were still
considerably rare because of the good adhesion of the SWNT physically connected to the edges of the four corners. The
paste. perforated film with the 2T1C driving cells was stacked onto a
500 mm-thick rubber sheet made of PDMS that was prepared
beforehand. The perforated film with the 2T1C cells was placed
4. Rubber-like Organic Transistor Active Matrix on the PDMS sheet as a substrate, and then printed elastic
conductors were mechanically and electrically connected to the
Organic Light-emitting Diode Display
contact pads of the 2T1C cells on the bottom surface. The
Taking full advantage of the printable elastic conductors with printed elastic conductors functioned as scanning-lines and
large conductivity and stretchability, we manufactured a data-lines. Then, the perforated film was again mechanically
rubber-like stretchable active matrix organic LED display punched to isolate the 2T1C driving cells on the PDMS sheet.
comprising 16 16 driving cells with two organic transistors Therefore, the 16 16 driving cells were uniformly dispersed on
and one capacitor (2T1C), organic LEDs, elastic conductors, and the PDMS sheet. The periodicity was 5 mm. Again, elastic
pastes. Pictures of the sheet comprising the 2T1C organic conductors were patterned to form data-lines, which were
transistor driving cells and a magnified picture of one cell can be connected to the contact pads for the data-lines. Here, it should
seen in Figures 18a and b. A circuit diagram for a display cell be noted that the intersection points between the data-lines
with a 2T1C driving cell and an organic LED are shown in and the scanning- and ground-lines were electrically isolated
Figures 18c and d. Each driving cell comprises a select transistor using an insulating PDMS sheet. Then, the contact pads
(Trselect), driver transistor (Trdriver), capacitor (C), and printed for the organic LEDs were coated with droplets of Ag paste
elastic conductors. The select transistors allow each organic LED (E4110; EPO-TEK) using a microdispenser. This paste was dried
to be addressed for light emission, and the driver transistors at 80 8C for 3 h in air, and exhibited a conductivity higher than
control the luminance. Capacitors play a major role in stabilizing 103 S cm1.
www.advmat.de
deposited using a sputtering system to form

REVIEW
the anode electrodes. A 10 nm-thick layer

of 3-tert-butyl-9,10-di(2-naphthyl)anthracene
(TBADN):V2O3 and a 10 nm-thick layer of
TBADN were deposited by evaporation to act
as the hole-injection layer and hole transport
layer, respectively. A 70 nm-thick layer of
4,40 ,400 ,-tri(N-carbazolyl)triphenylamine(TCTA):
9,10-bis[N,N-di-(p-tolyl)-amino]anthracene
(TTPA) was formed by vacuum evaporation as
the emission layer. A 20 nm-thick layer of
TBADN and a 10 nm-thick layer of TBADN:
Lithium-quinolate were deposited to act as the
electron transport layer and electron injection
layer, respectively. A 100 nm-thick layer of Al
was deposited by evaporation to form the
cathode electrodes. Finally, the entire LED,
with the exception of the electrodes, was
encapsulated in a plastic barrier film. The
anode and cathode electrodes outside this
encapsulation layer were coated with a
5-nm-thick layer of Cr and a 100 nm-thick
layer of Au to improve their adhesion to the
printed elastic conductors.
A grid of 16 16 organic LEDs with a
periodicity of 5 mm was uniformly dispersed
on a PDMS sheet using a similar process to
act as a stretchable driving active matrix.
The cathode electrodes were connected to the
printed elastic conductors to act as the
bias-voltage lines for the organic LEDs,
while the anode electrodes were connected
to contact pads from the organic driving cells.
These isolated organic LEDs were electrically
interconnected using printed elastic conduc-
tors on a PDMS sheet.
A stretchable organic 2T1C driving cell
active matrix and stretchable organic LED
Figure 18. a) Pictures of the top and bottom surfaces of organic transistor arrays comprising array were manufactured independently, as
16 16 (512) driving cells. b) A picture of one organic driving cell comprising two organic described above. Finally, these two sheets were
transistors (2T) and one capacitor (1C). c) A circuit diagram of one display cell comprising a 2T1C laminated using PDMS, and the anode
driving cell and an organic light-emitting diode (LED). d) The cross-sectional illustration of one electrodes were connected to the contact pads
display cell. A rubber substrate with organic driving cells and a rubber substrate with organic LEDs
were manufactured independently on different substrates and laminated together using an
of the 2T1C driving cells using Ag paste
anisotropic conducting adhesive sheet or a simple conducting paste. Adapted from [47]. (Fig. 18d).
Copyright 2009, Nature Publishing Group.
4.1.2. Organic Light-emitting Diode (LED) Array on Transparent 4.2. Electrical Characteristics
Rubber
Organic LEDs were manufactured on a 125 mm-thick transparent
4.2.1 Organic LEDs on Rubber
plastic barrier film by vacuum evaporation. Figure 19a shows an
organic LED integrated with a printed elastic conductor on a The electrical and light-emitting characteristics were measured
PDMS rubber sheet. A printed elastic conductor with a 500 mm for the stand-alone organic LEDs before integration. The electrical
linewidth provides a bias voltage to the cathode of the organic characteristics were measured using a semiconductor parameter
LED. The size of one organic LED chip was 5 5 mm2, and the analyzer (B1500A; Agilent), while the light-emitting character-
effective size of the light-emitting area was 3 4 mm2. A istics (luminance) were measured using a luminance meter
schematic cross-sectional illustration is presented in (BM-9; Topcon Technohouse). Figure 19 shows the effective
Figure 19b. A 150 nm-thick indium tin oxide (ITO) layer was currents passing through the organic LEDs (IOLED) and the
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because the select transistors were not connected to ground,
REVIEW
while they could apply voltage VData to the gate electrodes of the
driver transistors. Therefore, when one select transistor is
addressed, the connected driver transistor is activated. In fact,
IOLED increased from several picoamperes or nanoamperes to
several milliamperes with increases in VScan and VData. The on/off
ratio of IOLED was found to be 106 when controlling VScan. This
result clearly indicates that driving cells with the 2T1C structure
can operate organic LEDs even though large-area organic LEDs
require large currents of the order of several hundred
microamperes to several milliamperes for light emission.
4.3. Luminance
Figure 21a shows pictures of a typical organic LED for various

bias voltages, where the luminance and IOLED are also
represented. These results indicate that our organic LEDs were
sufficiently bright to enable the construction of an organic LED
Figure 19. a) A picture of an organic LED on plastic. b) A cross-sectional display. Furthermore, the operational voltages and required
illustration of organic LEDs. The LEDs were manufactured on a transparent currents were low enough to be supplied by our 2T1C organic
plastic film, and then distributed uniformly on a rubber substrate using a driving cells.
mechanical process. c) The current density and luminance of a typical
stand-alone organic LED as a function of bias voltage. The experiments
The luminance of an organic LED integrated with Cu wiring
were performed in ambient air. d) Luminance of organic LEDs as a function was measured and compared with that of an organic LED
of the current passing though them. Adapted from [47]. Copyright 2009, integrated with elastic conductors (50 S cm1). Figure 21a shows
Nature Publishing Group. pictures of the luminance and corresponding bias voltage and
IOLED. All of the pictures are of the same organic LED, and the
data for this LED were obtained from experiments performed in
luminance as a function of the bias voltage. Figure 19d also shows
ambient air. This result clearly demonstrates that the electrical
the luminance as a function of the IOLED on the same organic
performance of the printed elastic conductor is sufficient for
LED. This result indicates that the luminance values of the LEDs
display applications.
are sufficiently high for display applications.
Figure 21b shows the light-emitting properties of the display
4.2.2. 2T1C Organic Transistor Driving Cells on Rubber cells at different VScan values, when VBias and VData were 30 V
and 40 V, respectively. The light-emitting properties of an
The electrical characteristics of a 2T1C driving cell with printed organic LED integrated with a driving cell and Cu wiring, an
elastic conductors were also investigated. Figure 20 shows the organic LED integrated with a driving cell and printed elastic
plots of the currents through a select transistor (Iselect), driver conductors (50 S cm1), and an organic LED integrated with a
transistor, and organic LEDs (IOLED) as functions of the driving cell and commercially available conventional conducting
scanning-line voltage (VScan) when the data-line voltages (VData) rubber (0.1 S cm1) are shown for comparison. The data in
were gradually changed from 5 to 50 V. The bias voltage for Figure 21 were obtained from a single organic LED and single
the organic LEDs (VBias) was constant at 30 V. Iselect is very small organic driving cell to evaluate the performance of the elastic
conductors. When printed elastic conductors were used, IOLED
decreased slightly by 8% to 1.2 mA, resulting in a high luminance
value of 364 cd m2, which is sufficient for display applications.
In contrast, when electrical conductors were formed with
conventional conducting rubber (0.1 S cm1), IOLED decreased
by 97% to 40 mA, producing a luminance of only 7.1 cd m2. This
indicates that printed elastic conductors with high conductivity
are crucial for stretchable display applications.
4.4. Demonstration
By integrating a driving cell active matrix and organic LEDs using

Figure 20. The electrical characteristics of a 2T1C organic driving cell. Iselect printed elastic conductors, we manufactured a 16 16 pixel
and IOLED are shown as functions of VScan when VBias is constant at 30 V stretchable active matrix organic LED display. Figure 22 shows a
and VData is varied from 5 to 50 V. Adapted from [47]. Copyright 2009, demonstration of this display, which can be spread over an
Nature Publishing Group. arbitrary curved surface. Bending or crumpling caused no
www.advmat.de
technologies,[66] and furthermore, printing

REVIEW
technologies of organic semiconductors and

electrodes with resolutions of 1 mm have been
reported.[67–69] Thus, combinations of these
state-of-the-art printing technologies will make
it possible to realize higher definition.
5. Future Prospects
We have realized elastic conductors with 102 S
cm1, which is the highest conductivity among
stretchable carbon-nanotube/rubber compo-
sites, thus far. However, conductivity is still
three orders of magnitude smaller than that of
metals. Although we employed jet-milling and
ionic liquid process, new methods for disper-
sing nanotubes are required for realizing
higher conductivity of elastic conductors.
Furthermore, one of the most important
challenges on elastic conductors is improve-
ment of robustness under stretching cycles. In
fact, robustness on 70%-stretching cycle is
now about 1000 when the SWNT content is
1 2 wt % (conductivity 10 S cm1). If we
can realize much finer nanotube conducting
networks, conductivity, stretchability, and
cycle-robustness will be much improved.
The stretchable materials and integration
technology mentioned above can also be used
to create other types of functional electronics
with an integrated, stretchable active matrix
and pressure sensors,[17,18] or a rubber-like
mechanical actuation system with an inte-
grated, stretchable active matrix and actuators
Figure 21. a) The luminance of an organic LED integrated with Cu wiring and compared with that that can create the sensation of touch
of an organic LED integrated with elastic conductors (50 S cm1). The luminance and corre-
sponding bias voltage and IOLED are represented. b) The luminance of a display cell as a function
electrically.[20,21] The combination of stretch-
of VScan. The luminance was investigated for three configurations of display cells: 1, an organic able sensors, actuators, and displays can be
LED integrated with a 2T1C driving cell and electrical wiring made of 1-mm-thick Cu; 2, an organic used to create real, tangible displays and
LED integrated with a 2T1C driving cell and electrical wiring made of printed elastic conductors friendly human-machine interfaces on all
(conductivity, 50 S cm1; length, 100 mm; linewidth, 500 mm; thickness, 100 mm); and 3, an kinds of surfaces. In this manner, the printable
organic LED integrated with a 2T1C driving cell and electrical wiring made of conventional elastic conductor allows for the construction of
1
conducting rubber (conductivity, 0.1 S cm ; length, 100 mm; linewidth, 1 mm; thickness,
electronic integrated circuits that can be spread
100 mm). The VBias and VData values were 30 V and 40 V, respectively. The IOLED and luminance
are also shown. The effective size of the light-emitting area was 3 mm 4 mm. All of the pictures over on any surface, including arbitrary curved
are of the same organic LED, and the data from this LED were taken from experiments performed surfaces and movable parts. This would
in ambient air. This result clearly demonstrates that the electrical performance of the printed significantly expand the areas where electro-
elastic conductor is sufficient for display applications. Adapted from [47]. Copyright 2009, Nature nics can be used. This is an important step
Publishing Group. toward the development of the infrastructure
for the imminent era of ambient electronics, in
mechanical or electrical damage because of the good conductivity which a multitude of electronic devices can be penetrated in daily
and mechanical durability of the printed elastic conductors, life for new classes of applications.
organic transistors, and organic LEDs manufactured on PDMS
rubber.
Miniaturization of display cells for a higher resolution is one of
the most important requirements. We successfully patterned
6. Conclusions
printable elastic conductors with linewidths of 100 mm using We outlined the fabrication of a large-area stretchable organic
screen printing. However, screen printing can be used to pattern transistor active matrix and how it could be used for electric
pastes to resolutions of 10 mm. Sirringhaus and coworkers applications. Perforated organic transistor active matrices have
reported that organic LEDs can be manufactured using printing been realized by employing mechanical processes. A net-shaped
www.advmat.de
Ltd., for the generous supply of fluorinated copolymer; and Daisankasei
REVIEW
Co., Ltd. for the high-purity parylene (diX-SR).
Received: November 26, 2009

Published online: March 12, 2010
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www.advmat.

Stretchable, Large-area Organic Electronics

By Tsuyoshi Sekitani and Takao Someya*

sensors,[17–19] actuators,[20,21] and other

Tsuyoshi Sekitani received the

Takao Someya received the Ph.D.

been developed using a nanocomposite comprising SWNTs and

contact geometry are manufactured with fine shadow masks. The

magnified image of a transistor is shown in Figure 2d. The base

2.1.2. Sensor Array

The plastic surface was uniformly coated with

2.4. Simultaneous Sensing of Pressure and Temperature

As shown in Figure 4b, the perforated pressure sensors and

Figure 4. a) One cell of a thermal sensor network device consisting of

Figure 7. a) Picture of 1.5-mm-wide elastic conductor stretched by 100%.

3.1.1. Manufacturing Process

Figure 9. a) The compatibility of the fluorinated copolymer, ionic liquid,

3.2. Integration of Elastic Conductors with

Taking full advantage of the SWNT elastic

3.3. Electrical and Mechanical

The sheet was stretched by increasing the

light emission during high-frequency opera-

4.1. Fabrication Process

4.1.1. Organic Transistor Active Matrix for

deposited using a sputtering system to form

the anode electrodes. A 10 nm-thick layer

because the select transistors were not connected to ground,

Figure 21a shows pictures of a typical organic LED for various

By integrating a driving cell active matrix and organic LEDs using

technologies,[66] and furthermore, printing

technologies of organic semiconductors and

Ltd., for the generous supply of fluorinated copolymer; and Daisankasei

Received: November 26, 2009

[1] F. Garnier, R. Hajlaoui, A. Yassar, P. Srivastava, Science 1994, 265, 1684.

1107. [51] S. Iijima, T. Ichihashi, Nature 1993, 363, 603.

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