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Chemical and Physical Sensing by Organic Field-Effect
Transistors and Related Devices
By Takao Someya, Ananth Dodabalapur, Jia Huang, Kevin C. See, and Howard E. Katz*

these transformations alter the electronic

Organic semiconductor films are susceptible to noncovalent interactions, input-output characteristics of the semi-
trapping and doping, photoexcitation, and dimensional deformation. While conductors and can be harnessed to detect
these effects can be detrimental to the performance of conventional circuits, chemical and physical stimuli that cause
these electronic modifications. Thus, OSCs
they can be harnessed, especially in field-effect architectures, to detect chem- are a promising platform for the construc-
ical and physical stimuli. This Review summarizes recent advances in the use tion of various types of sensors.[1] Such
of organic electronic materials for the detection of environmental chemicals, sensors would share the advantages of non-
pressure, and light. The material features that are responsible for the trans- responsive OSC devices, and could addi-
duction of the input signals to electronic information are discussed in detail. tionally be endowed with highly specific
functionality for well-resolved responses.
Semiconductors are defined by having
1. Introduction multiple degrees of conductivity, depending on the amount of
energy supplied to them. In the case of a field-effect transistor
1.1. Transduction in Organic Semiconductors (FET), the energy is in the form of a potential difference between
a gate electrode and a semiconductor interface. This “gate
Organic semiconductor (OSC) devices occupy an interesting voltage” (Vg) effectively switches the semiconductor between
level on the scale of device stability. On one hand, OSCs are a condition of having few mobile carriers and a condition
fairly unreactive and as solids are kinetically stable in the dark with many mobile carriers. Energy in the form of light or heat
to components of the atmosphere, including oxygen and water. can also greatly affect conductivity by altering the density and
Therefore, with proper packaging and attention to interface mobility of carriers. While mechanical work is relatively inef-
chemistry, OSCs are usable in various electronic components, fective at altering densities of carrier types, it can influence the
including light-emitting diode (LED) pixels and display back- application of gate voltage to a FET or the distribution of carriers
planes. They are also contemplated for use in more complex among molecules in an organic field-effect transistor (OFET).
circuits such as radiofrequency identification (RFID) tags and Environmental molecules (“analytes”) can have very special
distributed, adaptive circuits. These components share advan- effects on OFETs and other OSC devices. Noncovalent bonds
tages over silicon-based analogs, such as fabrication based such as hydrogen bonds and π interactions cause attractions
heavily on printing technology, compatibility with low-melting between analytes and OSCs that exceed simple van der Waals
and flexible substrates, and tunability of bandgaps and majority interactions. The interactions can occur on the surfaces of OSC
carrier types. On the other hand, OSCs are susceptible to non- films, between crystallites that make up a polycrystalline OSC
covalent interactions, trapping and doping, photoexcitation, solid, in the free volume of OSCs that are either amorphous or
dimensional deformation, and other mild and often reversible intentionally supplied with flexible side chains, or at interfaces
transformations. While not necessarily deactivating the devices, between OSCs and dielectrics or electrodes. Many analytes are
dipolar, and thus induce local fields that are superimposed
on the gate voltage, altering effective charge carrier mobili-
[∗] Prof. H. E. Katz, Dr. J. Huang, K. C. See ties. Even nonpolar analytes could conceivable alter mobilities
Department of Materials Science and Engineering through induced dipoles and disruption of molecular packing
and Department of Chemistry in the OSC. Furthermore, depending on the relative positions
Johns Hopkins University of OSC and analyte carrier energy levels, analytes can cause the
Baltmore, MD 21218 (USA)
E-mail: hekatz@jhu.edu
trapping of mobile carriers by localizing them on the analyte
Prof. T. Someya
molecules, or doping by donating or extracting electrons from
Department of Applied Physics the OSC matrix. The effects of doping and trapping on OSC
Tokyo University conductivity and interfacial potential barriers can be profound.
Tokyo (Japan)
Prof. A. Dodabalapur
Department of Electrical and Computer Engineering 1.2. Organic Transistor Sensor Device Physics
The University of Texas at Austin
Austin, TX 78712 (USA)
In most organic thin-film transistors, the charge transport
DOI: 10.1002/adma.200902760 mechanism is thermally activated hopping, following the

Adv. Mater. 2010, 22, 3799–3811 © 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim 3799
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Representative Set of Normalized Data

1.15
Normalized Base Line
1.10 Normalized Response
to 100 ppm of ethanol
Grain Boundary
1.05
Grain Body

Normalized ID
1.00

0.95
Ti/Au + + Ti/Au
+ + 0.90
Charge carriers trapped 0.85
SiO2 Injection through Schottky in grain boundaries
barrier or interface dipole 0.80

Si 0.75
0 50
Time (s)
Figure 1. Left: Schematic diagram of organic transistor chemical vapor sensor. Right: Typical large channel length device response upon exposure to
polar analyte. The semiconductor used is pentacene.

relation μ ≈ exp (−Ea/kT). The mobility in most OTFTs increases
with increasing gate bias, which is attributed to filling of the tail
states of the density of states (DOS). The gate dependence is
stronger at lower temperatures. Electric field effects also play
an important role in transport at low temperatures. These phe-
nomena are well-known for organic field-effect transistors made
from OSC films with grain boundaries, positional defects, or
impurities, where the band tail of localized states has a much
wider distribution at grain boundaries than within each grain
body, due to the increased disorder at grain boundaries[2,3] or
other inhomogeneities.
Figure 1 shows the schematic of an organic transistor
chemical vapor sensor. The sensor response is closely related
to charge transport in the device, which can be influenced by
charge injection from the metal contact to the semiconductor
(this is severe in small channel length devices) and charge
trapping at grain boundaries and interfaces. In a large scale
device (channel length much larger than the grain size in the
active semiconductor layer), charge transport is dominated by
the localized charges in tail states at grain boundaries due to
high disorder there, and therefore the sensing mechanism can
be described as analyte dipole-induced charge trapping at grain
boundaries, which generally leads to a decrease in device current
upon exposure to typical polar analytes, as shown in Figure 1,
left. In some cases, the analyte dipoles result in a transient
increase in channel conductivity, presumably because of more
charges being induced in the channel. For smaller lengths, there
are fewer grain boundaries, so that instead of the influence of
grain boundaries on electrical transport and chemical sensing,
these are now dominated by organic semiconductor-metal
interfaces. At smaller channel dimensions, especially when the
channel length is comparable to or smaller than the grain size
of polycrystalline organic molecules or conjugated polymers,
the charge transport is dominated by the injection through the
Schottky barrier and interface dipole at the metal-organic semi-
conductor contact as well as influenced by the local coverage of
in nanoscale OTFTs, the analyte molecules diffuse near the
source/drain contacts through the porous semiconductor layer
and modulate the charge carrier injection at the source and
drain contacts. The smaller the channel length, the stronger
this effect is. It is in this fashion that nanoscale organic transis-
tors exhibit a remarkably different behavior in charge transport
and chemical sensing from the micro-scale counterparts.
Thus, the key assumption in designing device responses to
chemical events in the OSC layer of an OFET is that charge
transport would be perturbed by the presence of an analyte mol-
ecule, by the mechanisms discussed above. Before proceeding
with device observations, it is necessary to check whether or
not this is reasonable. OFETs are often switched with 10–100 V
on the gate. At first glance, it is difficult to imagine how the
electric field associated with a typical covalent molecule could
confer such voltages, even immediately adjacent to the mole-
cule. Electrostatic modeling that we have performed suggests
that the incremental potentials around even a cluster of mod-
erately polar molecules are only a few tenths of a volt. How-
ever, the gate potential influencing charge carriers through
the thickness of the OSC film is much less than the switching
voltage, because much of the voltage drops across the gate
dielectric, and also because charge carriers in outer semicon-
ductor layers are screened from much of the gate voltage by as
much as 80–90% by those closer to the dielectric interface, as
S
S
S S
S
S
S
S
S
S
S

organic semiconductor material on the nanoscale channel, both S

of which overwhelm the intrinsic transport within the body

of grains. Correspondingly, during chemical sensing events Scheme 1. From top: α-6T, pentacene, and dihexyl-α-6T.

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R electrostatic modeling. We therefore conclude that the dipole
fields around potential analyte molecules may be sufficient
O N O
to lower the current passing through an OFET in its on state.
These local fields may be concentrated at grain boundaries,
where analytes are likely to bind, but could also exist in the bulk
of OSC films if analytes are able to intercalate among side chains
or inside defects in the grains. Receptor functional groups, by
N N N
increasing the binding constants, increase the channel volume
in which analyte molecules are affecting the carrier energies,
N Cu N
and result in larger current changes.
N In addition to dipole fields, strongly electron donating ana-
N N lyte molecules can act directly as traps or even dopants through
charge transfer interactions. This results in lowering or raising
O N O the current, respectively, via a different mechanism than that
R just discussed. For example, oxygen was found to lower the
electron density as well as the mobility of perylenetetracar-
Scheme 2. PTCDI (left) and copper phthalocyanine. boxylic diimide (PTCDI) thin films, presumably by “oxidizing”
the PTCDI radical anions.[6] The capability of various organic
C6H13 semiconductors to respond to particular analytes via multiple
S mechanisms increases the chances of “fingerprint” identifica-
C6H13
S tion of analytes by arrays of OSC devices.

C12H25

S S
S
2. Organic Field-Effect Transistors as
S
n S
S
Chemical Sensors
n
PQT12 2.1. Response of Unfunctionalized Vapor Sensors
C12H25

Scheme 3. 6PTTP6, P3HT, and PQT12.

The layout of an OFET vapor sensing experiment is shown in
Figure 2, illustrating the device configuration as well as the
delivery of analyte molecules from the sample reservoir to the
R various surfaces of the OFET that comprise a polycrystalline
O N O OSC film.
It is well recognized that current output levels of nonpackaged
OFETs made from nonpolar, unfunctionalized OSCs including
pentacene and α6T vary in the presence of polar vapors,
including water. A pentacene OFET had its mobility and on/
OC6H12OH off ratio vary by nearly an order of magnitude over extremes of
S O N O high and low humidity.[7] The sensitivity was greater for bottom
HOC6H12O
R
S
R = m-CH2C6H4OH contact devices compared to top contact, and for narrow devices

Scheme 4. Hydroxylated bithiophene oligomer and NTCDI

Air
shown by Horowitz.[4] Thus, it is conceivable that the effective
gate voltage governing some of the charge carriers is much less valve
than the applied voltage, and moderately polar molecules could Mix DMMP
deliver a local field sufficient to trap charge carriers. Using a
density of states argument, Tessler et al. also conclude that at VSD
moderate gate voltages, the channel can extend out for several Flow rate meter
monolayers.[5]
A direct observation has been made on the local potential
changes associated with binding a moderately polar molecule to a V Drain source
nonpolar OSC, α-sexithiophene (α-6T). NO2 chemisorption was
found to induce a change in film ionization potential of 650 mV,
Insulator
via a band bending mechanisim resulting from a diopolar field, Gate electrode
rather than doping. Methanol caused a Fermi level shift of
200 mV. These voltages are in the range for trap potentials Figure 2. Schematic of analyte gas (shown here as DMMP) delivery
in organic semiconductors and agree with our results from system with OFET under test.

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compared to wide one, indicating that near-contact regions
were particularly susceptible to moisture. Otherwise, the sen-
sitivity was attributed to grain boundary effects. Two nonpolar
oligomers were nearly as sensitive. Responses of dihexyl-α6T
to butanol have been extensively studied, and are on the order
of 50%, as the sum of contributions of on and off current,
and channel and contact resistances.[8] In this case, a granular
OSC film structure featuring numerous voids was thought to
be capable of absorption of vapor molecules by weak chemical
interactions. The PTCDI work cited above noted higher vapor
sensitivity in a film with greater free volume compared to one
with denser crystalline grains.[6] Copper phthalocyanine films
show varied responses to vapors of a range of polarities, from
toluene to ethyl acetate to methanol.[9] Response is higher to
the more polar vapors, and is also enhanced for thin semicon-
ductor films. The work was recently exgtended to include other
metal phthalocyanines, and a discriminating array was pro-
duced.[10] Pentacene, poly(3-hexylthiophene) (P3HT), and poly(3-
octylthiophene) respond to propanol, acetic acid, and related
polar vapors in distinct ways, possibly suitable for an electronic
nose platform for food analysis.[11] 5,5’-bis(4-hexylphenyl)-2,2’-
bithiophene (6PTTP6) shows considerable response to the
nerve gas stimulant dimethyl methylphosphonate, requiring
tens of minutes for the response to saturate.[12] The response is
much greater than it is to water at similar concentrations.
While the information gleaned from these studies may shed
useful mechanistic insight and may also be empirically useful
in constructing electronic noses, the responses cannot be traced
to well defined binding events between OSCs and analytes.
Except for nonspecific van der Waals forces, there is no antici-
pated attraction between volatile organic molecules and any of
the OSC molecules considered in the above reports. This is not
to say that the current changes are not reasonable; the above
discussion indicates that the adsorption of polar molecules, by
whatever mechanism, will introduce traps in OSC films and
alter currents. It is possible that molecules do stick to OSC films
at sites of high roughness at grain boundaries, or at other defect
sites marked by polar impurities or static electricity. However,
these nonspecific and poorly controlled binding events are not
well enough defined to serve as the basis for designing OSC
films with enhanced responses.
2.2. Effects of Analyte Binding Groups
In order to increase the binding strength, and therefore, the
number density and the resulting signal, of bound analyte
molecules in equilibrium with a vapor, and also to increase the
selectivity of molecular responses, a logical second generation
system would be an OSC film with binding groups covalently
attached to the molecules that make up the OSC film in the
OFETs. The capability of synthesizing OSC molecules with
binding groups that can be arbitrarily near the OFET charge
channels is one of the most attractive features of OSCs for use
in chemical sensors. Several years ago, it was shown that ether
oxygens groups on semiconducting polymer side chains altered
their responses to alcohol vapors.[13] The ether group made
a polythiophene OFET sensitive to ethanol, while a related
poly(alkylthiophene) OFET was not. Both polymers responded
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0.0
-0.2
-0.4
-0.6
Id-sat (A)
-0.8
Vg=-20v
Vg=-40v
-1.0
Vg=-60v
-1.2 Vg=-80v
-1.4
-1.6
0 5 10 15 20 25 30 35
Time (min)
Figure 3. Response of a single layer OSC oligomer blend on exposure
to DMMP vapor. The black solid vertical line indicates the time when
a vial with DMMP liquid was placed into the closed chamber and the
dashed vertical line indicates the time when the vial was removed and the
chamber was open to air.
to the more hydrophobic hexanol, though the ether derivative
showed a faster and more definitive response.
A focus of the Johns Hopkins University (JHU) group has
been to examine interactions between OFETs and the nerve
gas stimulant dimethyl methylphosphonate (DMMP), a fairly
polar and somewhat volatile organic liquid. As mentioned
above, response of an unfunctionalized OFET to this vapor
occurred over tens of minutes. By blending the hydroxylated
bithiophene oligomer 5,5’-bis(4-(6-hydroxyhexyloxy)phenyl)
bithiophene with 6PTTP6 in an approximately 1:1 ratio, the
response was made both larger (current decreasing to 25%
of its original value at the optimal gate voltage) and faster,
now on the time scale of a few minutes (Figure 3).[12] The
blend appeared to be a single phase by both x-ray diffrac-
tion and scanning electron microscopy, and behaved properly
as an OSC film in an OFET as evidenced by good saturation
behavior and a reasonable on/off ratio. It is logical to attribute
the more useful response to the greater ability of DMMP to
bind to a hydroxy-rich surface through hydrogen bonds than
to an all-alkyl surface through weaker interactions, and also
possibly to the larger changes in functional group dipole
moments upon polar binding, resulting in larger changes in
local electric fields.
This enhanced response to DMMP of hydroxylated OSCs
is not limited to hole-transporting OSCs alone. Islands of a
hydroxphenylated naphthalenetetracarboxylic diimide (NTCDI)
semiconductor deposited onto a nonpolar NTCDI also showed
stronger, more definitive, and more selective response to
DMMP than did the film of the nonpolar compound alone in
an OFET.[14] The island growth was probably due to the poor
wettability of the hydroxylated compound on the very nonpolar
surface of the base OSC layer.
A particularly dramatic demonstration of the selectivity
achievable with a relatively small side chain subunit was by the
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Torsi group, who showed that chiral amino acid or sugar deriva-
0 .0 0 8 B e fo re e x p o s u re to D M M P
tives attached to a OSC core subunit and deposited on top of an
E x p o s u re to D M M P v a p o r
unfunctionalized OSC made an OFET differentially responsive
to the two enantiomers of the chiral alcohol citronellol.[15] The 0 .0 0 6
idea was first proposed on the basis of quartz crystal microbal- (A)

1/2
(A)
ance response differences of a glucose-substituted conducting
0 .0 0 4
polymer to the two enantiomers of menthol.[16] Not only is

1/2
this a compelling model of the kind of selectivity possible

Id-sat
when somewhat sophisticated receptor groups are employed 0 .0 0 2
in OFETs, but it is also a convincing proof that the receptor
groups do mediate the interaction between the vapors and the
0 .0 0 0
OFET charge channel.
A special case of a “receptor” moiety is Cu tetraphenylpor- -1 0 0 -8 0 -6 0 -4 0 -2 0 0 20
phyrin (TPP) acting as a complexing agent for nitro compounds V g (V )
through donor-acceptor interactions. The addition of Cu TPP
to a P3HT film in an OFET made the device sensitive to a 0 .4 0
wider range of nitrated explosives, including 1,3,5-trinitro-1,3,5- 0 .3 5

d-sat,DMMP d-sat,0
triazacyclohexane (RDX), than was the original P3HT film (B )
0 .3 0
alone.[17] A combined coordination to the Cu and electron

/I
extraction by the RDX was believed responsible. 0 .2 5

0 .2 0
2.3. Response Models Normalized I R ^2 = 0 .9 7 1 2 5
0 .1 5

The changes in currents observed when OFETs are exposed to
analytes are a combination of effects on charge carrier mobility
(itself the combination of bulk and grain boundary mobilities)
and threshold voltage. Assuming mobility independent of gate
voltage and no short-channel effects, the saturation drain cur-
rent Isat of an OFET is given by Equation 1
 1/2
1/2 W FET versus gate voltage before and during DMMP vapor exposure. Vd
Isat = C : sat (Vg − Vt )
2L
When analyte molecules are adsorbed, changes occur in μsat
and Vt, noted as Δμ and ΔVt, so that the saturation drain cur-
rent Isat(analyte) of the OFET becomes Equation 2:
 1/2
1/2 W upper plot, to Equation 3, to obtain the lower plot. The fit gives
Isat(analyte) = C(: sat + : ) [Vg − (Vt + Vt )]
2L
Combining Equations 1 and 2, we can obtain the relation-
ship between Isat(analyte) and Isat, shown as Equation 3:
   2
: Vt
Isat(analyte) /Isat = 1 + 1−
: sat Vg − Vt
This equation is only valid when |ΔVt| < |Vg − Vt|, but it
expresses the gate voltage dependence of the sensor responses.
For hole-transporting OFET saffected by dipolar trapping mech-
anisms, the values of Vg, Vt, and ΔVt are all negative, while in
the case of doping analytes, it is possible for Δμ and ΔVt to
be positive. For n-channel OFETs, the signs are reversed. For
smaller values of |Vg|, the [1 − ΔVt/(Vg − Vt)] term is smaller,
which results in a smaller value of the ratio of the saturation
source drain currents Isat(DMMP)/Isat0, corresponding to more
noticeable sensor response when ΔVt is significant.
Figure 4 plots the square root of the saturation drain current of
a 6PTTP6 OFET versus gate voltages before and during DMMP
0 .1 0 du -0 .0 2 8 2 6
dv -1 5 .2 4 4 2 4
0 .0 5
0 .0 0
-1 0 0 -8 0 -6 0 -4 0 -2 0
V g (V )
Figure 4. A) The square root of the saturation drain current of a 6PTTP6
(1) is −100 V. B) The closed squares correspond to the ratio of saturation
source drain current Isat(DMMP)/Isat0 obtained from experiment; the solid
line is the least squares fitted curve according to Equation 3.
vapor exposure. We performed a least squares fit of those data,
together with the two values each of μ and Vt obtained from the
(2)
a reasonable prediction of the gate voltage dependence of the
sensitivity, except at the highest voltages, where contact resist-
ance may be playing a role, and at the lowest voltages, where
the mobility may be more gate voltage dependent.
This analysis assumes that the response is in fact arising
mainly from the channel and not from contact resistance. An
(3)
analysis of the butanol response experiment mentioned above
addressed this issue in detail.[8] To begin with, a dihexyl-α6T
OFET was used in which the contribution of contacts to the
total OFET resistance was several times less than the contribu-
tion of the channel, as determined by the dependence of the
total resistance on channel length. Then, the changes in resist-
ance on exposure to butanol were similarly attributed largely
to the channel, except for the case of short-channel devices.
Though not published in detail, we have made similar obser-
vations on our 6PTTP6 and NTCDI systems[12,14] with respect
to DMMP. Thus, it is certainly possible to design OFET-based
chemical sensors by tuning properties of the OSC films, as the
device responses need not be dominated by contact resistance
effects.

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2.4. Hybrid Organic/Inorganic Sensors
A new sensing device, which is illustrated in Figure 5, has
been recently demonstrated by the Texas group.[18] The device
is a four-terminal device that can be considered as two cou-
pled field-effect transistors (FETs). This device overcomes
some of the limitations of organic TFT sensors and can also
be of great help in understanding and evaluating trapping phe-
nomena in organic TFT sensors. The device can function as a
traditional chemical field-effect transistor (CHEMFET) wherein
the organic semiconductor acts as a gate to the silicon FET. In
a b
70
120
60 before analyte delivery
after analyte delivery 100
50
80
IDS(μA)
another mode of operation, the silicon FET can gate the organic
transistor which can act as a sensor. Ideally, the silicon FET is
a depletion mode n-channel device, since most organic transis-
tors are hole-conducting p-channel devices. The morphology
of the thin organic semiconductor film is polycrystalline with
a large number of grain boundaries. The grain boundaries can
serve as sites for the incorporation of receptors. The combina-
tion of the organic semiconductor and the receptor constitutes
the sensing interface.
When analytes bind to the sensing layer, charge injection or
extraction events will occur which will concomitantly modify
the conductivity of the channel of the Si FET
and result in a change in source-drain cur-
rent which can be readily and sensitively
before analyte delivery detected. In contrast to the case in a tradi-
after analyte delivery tional CHEMFET in which it is difficult to
restore channel conductivity after the sensing
event, the present device offers a pathway for

40
the charge to flow out of the gate through the
IDS(μamp)

60
30 97X 95X organic semiconductor. This ‘restoring’ of the
65X 40
20 45X sensor has been convincingly demonstrated
20 for vapor phase and aqueous analytes. In the
10
second sensing mode (which we describe as
0
0 organic transistor sensing) the conductivity
0 5 10 15 20 25 30 35 0 10 20 30
time (s) time (s)
of the organic semiconducting layer is modi-
d fied by the analyte-sensor interaction. To
c
7.20 facilitate this, field-induced charges will be
22
created in the organic semiconductor layer
7.15 20
Analyte delivery ends Analyte delivery begins by employing silicon as the gate. By varying
18
the gate potential, chemical information can
7.10 16
be extracted, again as shown for vapor phase
IDS (mA)

IDS(nA)

2.5%
7.05
14
57% analytes by Crone et al.[19]
12 The four-terminal device can also be
7.00 10
Analyte delivery ends implemented entirely with organic mate-
8 rials. In such a device, the silicon FET can
6.95 Analyte delivery begins 6 be replaced by another organic field-effect
0 5 10 15 20 25 30 0 10 20 30 40 50 channel. This device will therefore be two
time (s) time (s)
coupled organic field-effect devices pos-
sessing a common gate insulator. This will
be important in application where low cost
is essential and where it may be necessary
to depart from the silicon manufacturing
paradigm. Fortunately, there have been many
advances in the development of low-cost pat-
terning techniques for organic electronics
and in implementing systems with such
techniques. Such an all-organic four terminal
device has been recently demonstrated.[20]
The device described above is particu-
larly useful in understanding organic tran-
sistor sensor operation. Charges trapped
in the organic sensing layer are reflected as
shifts in the threshold voltage in the lower
(Si) channel. These shifts can be accurately
measured and the trapped charge density
deduced. The total charge density in the top
Figure 5. a) and b) Chemical memory mode of operation of a four-terminal sensor; c) CHEMFET (organic) channel can be measured by moni-
mode; d) OTFT sensor mode. Note that chemical memory mode is much more sensitive than toring the conductivity of the silicon channel.
CHEMFET mode. The schematic is also shown. This way, the effects of polar analytes which

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-10
1.4x10 Analyte delivery ends
-10
1.2x10
-10
1.0x10
-11
8.0x10
I (A)
-11
6.0x10
-11
4.0x10
-11
2.0x10
0.0
-11 analyte delivery begins
-2.0x10
-5 0 5 10 15 20 25 30 35
time (s)
Figure 6. Left: Organic channel current in a four-terminal sensor showing an increase during analyte delivery. Right: The channel current in the silicon
channel. The sharp increase in current following analyte delivery (to the organic channel) mirrors the increase in the organic channel. Unlike the organic
channel current, the Si channel current stays the same after analyte delivery is stopped.
can significantly alter the charge density in the organic channel,
can be measured. The electrostatically coupled channels will
also permit capacitance measurements offering an alternative
to conductometric sensing, providing yet another window into
the sensing process.
The various modes of operation of a four terminal sensor
are shown in Figure 5. The use of four-terminal devices in
understanding organic TFT sensor physics is illustrated in the
example discussed below. A four-terminal device in which the
organic channel had bad electrical contacts (Nickel) was evalu-
ated after exposure to an alcohol vapor. The organic channel
current increases sharply upon analyte delivery upon improve-
ment of the electrical contact by the vapor dipoles that facili-
tate charge injection, as shown in Figure 6. The filling of the
organic channel due to the improved contact is reflected in the
Si channel current (and hence conductivity) which goes up.
Monitoring the silicon current allows us to quantitatively assess
the charge concentration in both channels. Such experiments
will be very helpful in understanding sensor behavior.
2.5. Vertical Scaling and Heterostructures
Creation of effective OFET sensors requires simultaneous opti-
mization for several criteria. Total currents must be high enough
so that changes can be distinguished from noise. The responses
must be fast enough so that appropriate remedial action can be
taken in a timely way. Responses should be dominated by ana-
lytes of interest, or by specific interferents in the case of con-
trol devices in an array, so that useful chemical information is
derived. These requirements call for architectures in which the
responsive OSC layers are as thin as possible, so that analytes
will strongly and rapidly influence the channel properties, the
OSC surfaces are rich in analyte binding groups, so that ana-
lyte binding probability is high, and the interface between the
OSC film and the dielectric substrate is a well-ordered, high-
carrier-mobility layer.
Adv. Mater. 2010, 22, 3799–3811 © 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
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5
4
analyte delivery ends
3
I (mA)
2
1
analyte delivery begins
0
40 -5 0 5 10 15 20 25 30 35 40
time (s)
(s
The UCSD group compared the response of 4-monolayer
and 50-monolyer Co phthalocyanine films to various organic
vapors. In the particular case of nitrobenzene vapor, the
response was twenty times stronger and four times faster for
the thinner films relative to thicker ones.[9] However, the inter-
pretation of the thickness effect on all analytes studied was
complicated by the relatively different roles that surface impu-
rities and electronic states played in the interactions with dif-
ferent molecules.
The JHU group set out to separately minimize the thickness
required for a working OFET in the 6PTTP6 system, and then
to cap that minimal OSC film with a receptor layer in the form
of the hydroxylated blend discussed above.[21] The device struc-
ture is shown in Figure 7.
The field-effect mobility of this device was extracted to be
0.0072 cm2 V−1 s−1, slightly higher than that of the device with
only the 4 nm of 6PTTP6 but no blend film above it.
As shown in Figure 8, the device exhibited large and repro-
ducible response upon exposure to 5 ppm DMMP, largely due
to exposure-induced decrease in mobility. The utilization of
the ultra-thin semiconductor film significantly increased the
response speed (now less than one minute) and sensitivity of
the device when compared to the previous result we obtained
with the conventional bulk 6PTTP6 OFET, where similarly
large current differences were obtained only in the presence of
150 ppm DMMP vapors.
We expect to find further examples of the use of bilayer het-
erostructures in OFET sensors in the future, because of the
opportunity to retain electronic properties and tune receptor
action simultaneously. As one example already published, the
enantiomeric discrimination of alcohols reported by Torsi was
accomplished on a polymer bilayer, in which the bottom layer
had higher charge carrier mobility and the top layer supplied
the chiral receptor groups.[15] It is not likely that the top layer
alone, with its relatively bulky substituents, would have been
able to support enough lateral current to allow for strong sensor
signals.
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S
O O
HO S OH 0.0
HO6OPT
-1.0
(A) S D (A)

Id / μ A
4 nm 6PTTP6+HO6OPT -2.0
4 nm 6PTTP6 Vg=0 V
-3.0 Vg=-20V
300nm Dielectric Vg=-40V
-4.0 Vg=-60V
Gate Vg=-80V
Vg=-100V
-5.0
-100 -80 -60 -40 -20 0
Vd / V
4nm+4nm 6PTTP6-HO6OPT (B)

100

80
(B)

μFET/ μ0 / %
60

40

20 5ppm
Mobility DMMP
0
0 400 800 1200 1600 2000 2400
Time (s)

Vg=-20V Vg=-30V Vg=-40V

Vg=-50V Vg=-60V
0.0
Figure 7. A) Schematic illustration of ultra-thin OFET with receptor layer.
B) Tapping mode AFM images of 4nm blend of 6PTTP6 and HO6OPT on
top of a 4 nm 6PTTP6 layer.
-1.0
Id-sat (μA)

2.6. Lateral Scaling Effects and Nanostructures

The Texas group investigated the response of Ids, the drain-source
current, (operated in saturation region) upon exposure to the
saturation vapor of 1-pentanol, with a series of channel length
and varied grain sizes of pentacene. It was found that when the
grain size is small (80 nm), Ids exhibited a decreasing response at
channel lengths of 450 nm or more, whereas the response is in the
opposite direction (increasing Ids) at channel lengths of 150 nm
or less,[22] as shown in Figure 9a. In these figure, the shaded area
corresponds to the period when the analyte vapor was in pres-
ence, and Ids was normalized to the current measured just before
the analyte took effect. While the long channel length devices all
exhibited a decrease in current upon delivery of the analyte, the
small channel length devices showed an increase, sometimes by
a factor of > 5. There are two mechanisms influencing sensor
behavior: one causing a decrease in current (dominant in large
L devices) and one causing an increase (dominant in small L
devices). The crossover of response behavior depends on grain
size, occurring in the interval of channel length 150–450 nm for
≈80 nm grain size. When the average grain size of pentacene
is increased to 250 nm, the increasing Ids signal is enhanced
-2.0
-3.0
(C) 5ppm DMMP
0 4 8 12 16 20 24 28 32 36 40
Time (min )
Figure 8. A) The Id − Vd characteristics of the ultra-thin OFET with
receptor layer. B) Change of the mobility of this device upon exposure to
5 ppm DMMP; exposure times indicated in gray, recovery was induced by
flowing nitrogen, and could be accelerated by gentle heating. C) Change
of the current upon exposure to 5 ppm DMMP.(a)b)
under the same condition and the sensors exhibits the crossover
behaviors at larger channel lengths (from 450 nm to 1 um),
as shown in Figure 3b. Figure 3c shows the SEM image for a
150 nm channel with an average grain size of 250 nm, taken
after sensing measurements.

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COMMUNICATION
Figure 10 shows the sensing responses of long channel
(a) devices with pentacene grain size of 140 nm. For all devices
with channel lengths of 2 um or greater, Ids manifested
5
Normalized Drain Current

60 nm decreasing responses upon analyte delivery. The amplitudes of

150 nm decreasing signal for 2 um channels were smaller than those of
4 450 nm longer channels and this effect is stronger in the devices with
larger pentacene grains. These results are consistent with the
1 um reported work for sensing effects dependent on organic grain
3 grain ~ 80 nm
sizes and channel lengths in large scale.[19,23,24] The sensing
responses shown in Figure 9 and 10 are reproducible for dif-
2 ferent devices with the same channel lengths and grain sizes,
indicating that the response of pentacene transistors to the
1 1-pentanol vapor changes from decreasing Ids to increasing Ids,
when the channel lengths shrink from micrometer to 100 nm,
with a crossover happening in a transition interval of channel
0 length which is related to the grain sizes of pentacene.
0 10 20 30 40 50 60 In a unified picture, the chemical sensing effects at grain
Time (s)
boundaries and metal-organic semiconductor contacts both
(b) arise from the dipole nature of analyte molecules. No sensor
response is seen for non-polar analyte such as hexane. Due
to its polaronic nature, the charge transport in organic semi-
3.5 conductors is fairly sensitive to the local polar environment.
Changes in the local crystal structure nearby charge carriers
3.0 and thus changes to the polarizability of the lattice, could drasti-
Normalized Drain Current

cally affect the local distribution of energy states. This problem

2.5
was further exacerbated in the grain boundaries due to a large
2.0 amount of disorder. Organic semiconductors are especially
polarizable at grain boundaries. The predominant mechanism
1.5 which leads to a decrease in the magnitude of the current is
increased trapping of carriers in the grain boundaries due to a
1.0 modulation of the local electronic environment caused by the
presence of the polar organic vapors (an increase in the polar-
0.5
grain ~ 250 nm izability of the semiconductor in the grain boundaries). An
0.0 increased number of traps in the grain boundary would lead
0 10 20 30 40 50 60 to an increase in the activation energy for hopping through the
Time (s)
grain boundaries which was demonstrated by our group using
top contact pentacene transistors exposed to ethanol.[19] The
measured activation energy changed from 77 meV to 92 meV
when the analyte concentration was changed from pure nitrogen
to 100 ppm of ethanol.[19] This is illustrated in Figure 10b.
It has been experimentally shown that the analyte molecules of
stronger dipole moments trigger stronger responses from the
same OTFT chemical sensor.[25] Also results reported by Torsi
et al. already discussed above demonstrated the importance
of the analyte’s alkyl chain length in terms of its interaction with
the organic transistor.[26] The longer the carbon chain length,
the greater the interaction of that analyte molecule with the
semiconductor and the higher the mass uptake. The same
group also showed that increased mass uptake occurred when
the side chain of the polythiophene derivative was made to be
polar (by putting an ester in the side chain).[26] This enhance-
Figure 9. a) Sensing data of Ids (normalized to that measured just before ment of the mass uptake was even more pronounced than the
the analyte took effect) for 80 nm pentacene grain size and different increase produced by longer analyte carbon chains.[26]
nanoscale channel lengths (same W/L = 10), measured at Vg = Vds = Vside In the case of nanoscale OTFT sensors where the injection
= −2.5 V (two side guards were kept at the same potential as the drain). at contacts dominates charge transport, the increases in magni-
The channel lengths are indicated in (b). Sensing data of normalized
tude of the source to drain current upon exposure to the analyte
Ids for 250 nm pentacene grain size, measured at the same conditions as
(a). c) SEM image taken after sensing measurements of a 150 nm channel is due to changes in the nature of how charge is injected into
with an average pentacene grain size of 250 nm, scale bar = 400 nm. the channel. When carriers are injected into the semiconductor,
The semiconductor material is pentacene. they accumulate close to the contact interface and induce the

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(a)
(b) 92
90

Activation Energy (mev)

88
86
84
82
80
78
76
0 20 40 60 80 100
Concentration of Ethanol (ppm)
Time (s)

Figure 10. a) Sensing data of normalized Ids under the condition of Vg = Vds = −25 V for different microscale channel lengths, with average pentacene
grain size of 140 nm. b) Variation of activation energy with respect to the concentration of ethanol.

image charge in the metal electrode and thus form an inter- approximately two or three orders of magnitude less than that
face dipole.[27,28] The polarity of the analytes can work to shield of poly- and single-crystalline silicon, the slower speed is toler-
carriers in the semiconductor from the reverse electric field able for most applications of large-area sensors. In particular,
which results from the interface dipole. The larger the dipole for the fabrication of e-skins, the integration of pressure sen-
moment in the analyte, the greater the shielding effect and thus sors and organic peripheral electronics avoids the drawbacks of
the stronger the response in drain-current increase. Also the organic transistors, while taking advantage of their mechanical
smaller the channel length, the stronger this effect is due to flexibility, large area, low cost, and relative ease of fabrication.
more domination of the injection-limited charge transport. For Figure 11 shows a circuit diagram of an artificial skin system.
example, the injection barrier at contacts between Au and pen- A 16 × 16 active matrix of organic transistors, row decoder, and
tacene is attributed to the existence of interface dipoles. column selector are assembled by a physical cut-and-paste pro-
cedure to develop integrated circuits for data readout. Three
functional films – an interconnection layer, a pressure-sensitive
3. Detection of Energy and Physical Forces rubber sheet, and a top electrode for power supply – are then
laminated together with the organic ICs. Pressure images were
3.1. Introduction obtained by a flexible active matrix of organic transistors whose
mobility is as high as 1.4 cm2 V−1 s−1. These sensors can be
Besides applications to chemical sensors, OFETs play an impor-
tant role in realizing large-area flexible sensors of physical
phenomena.[29–32] In these sensors, two-dimensional arrays of
16x16 FET matrix
OFETs, which are referred to as active matrixes, are functioned
as two-dimensional arrays of electronic switches. Similar con-
figurations are used to drive liquid-crystal flat panel displays. In
large-area sensors, active matrixes are integrated with various
kinds of 2D array of detectors such as pressure detectors[29]
and photo-detectors.[30] In other words, the basic structure of
large-area sensors is a 2D array of sensor cells comprising
one detector and one access transistor. The sensor cells some-
times contain more sophisticated electronic functions such as
memories. The OFET-based large-area sensors are categorized
in two different functions. One is mechanical force detection
such as pressure,[29] and acoustic waves,[31] while the other is
electromagnetic energy detection such as light[30] and radiof-
requency.[32] In this section, the recent progress of the OFET- Row
based large-area sensors is reviewed. decoders

3.2. Mechanical Force Detection: Pressure, Acoustic Waves Column selectors

Figure 11. A circuit diagram of an artificial skin system. A 16 × 16 organic
The first example of large-area sensors is a pressure sensor, transistor active matrix, a row decoder and a column selector are manu-
which is often referred to as electronic artificial skins factured on plastic films separately and them assembled to make inte-
(e-skins).[29] Although the mobility of organic semiconductors is grated circuits for data readout.

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Figure 12. The stretchable active matrix did not exhibit any significant
change in electronic performance even when it was stretched up to 80%.
bent to a radius of 2 mm, which is sufficiently small for the
fabrication of human-sized robot fingers.
In order to realize stretchable e-skins, elastic conductors
have been developed[33] recently using single-walled carbon
nanotubes (SWNTs)[34,35] as a conducting dopant. SWNTs
were uniformly dispersed as chemically stable dopants in a
vinylidene fluoride-hexafluoropropylene copolymer matrix
by using an ionic liquid[36] of 1-butyl-3-methylimidazolium
bis(trifluoromethanesulfonyl)imide, and manufactured SWNT
composite films. The measured value of conductivity is as high
as 57 S cm−1. Such high conductivity is achieved because the con-
tent of SWNTs in the conductor can be increased up to 20 wt%
without sacrificing mechanical flexibility and softness. The
SWNT elastic conductor can be stretched to approximately 134%
of its original size without significant mechanical damage. The
elastic conductors are used as wirings in large-area stretchable
OFET ICs (Figure 12). These ICs, which have a high electronic
performance, can be stretched by up to 80% without any degra-
dation in their mechanical or electronic properties. This is an
important step in the development of ICs that can be used on
freely curved surfaces and in smart surfaces.
The second example is an ultrasonic sensor, which realizes
the three-dimensional (3D) sensing of the position of people and
objects in free space. Although position sensing in free space has
commonly been carried out using light, radio, and millimeter
waves, ultrasonic imaging can offer complimentary attractive
features such as a simple architecture and real-time nondestruc-
tive 3D imaging in free space at an ultralow cost.[37–41]
A large-area, flexible, ultrasonic 3D imaging system was pro-
duced by integrating an ultrasonic transducer array sheet with a
printed OFET active matrix.[31] The ultrasonic sensing cell com-
prises one organic transistor and one ultrasonic transducer. A
transistor active matrix sheet and an ultrasonic transducer array
sheet are manufactured separately and electrically connected to
each other. The system comprises 8 × 8 ultrasonic sensing cells
or others, with a printed area of 25 × 25 cm2. It is mechanically
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COMMUNICATION
flexible and can be wrapped around a cylindrical bar; this con-
figuration is suitable for obtaining a viewing angle of 360° for
a medium-length (≈ several meters) proximity robotic skin-like
sensor.
The OFETs are fabricated on a 75-μm-thick polyimide film.
The source, drain, and gate electrodes are deposited by inkjet
printing or vacuum evaporation. A 500-nm-thick polyimide gate
dielectric layer is formed by inkjet or spin coating, and a 50-nm-
thick pentacene channel layer is deposited by vacuum evapora-
tion by using a printed shadow mask. The mobility in the satu-
ration regime is 0.5 cm2 V−1 s−1, while an on/off ratio is 107
in DC measurements. The transistors operate efficiently in the
small signal regime of the ultrasonic transducers (≈1 mVp–p).
The transistors with the grounded gate can switch 40 kHz sig-
nals with an on/off ratio of greater than 104.
A 28-μm-thick piezoelectric polyvinylidene fluoride
(PVDF)[42,43] film, whose surfaces are covered by metal, is used
as a sheet-type ultrasonic transducer. The transducers are used
in the bending mode. To adjust the mechanical resonance fre-
quency to 40 kHz, the transducer is bent to improve the sen-
sitivity using a spacer sheet. The ultrasonic transducer has an
output voltage of ≈0.8 Vp–p and a narrow pulse width of ≈100 μs
after an amplification of 40 dB by the incidence of an ultrasonic
wave. The ultrasonic transducers can detect a stiff object that is
hidden inside a cloth, and also show broad directivity (> −5 dB
for ±60°).
The signal from the ultrasonic transducer is switched by
the organic FET at 40 kHz. The integrated sensing cells have
an on/off ratio of 104 at 40 kHz. 3D ultrasonic images can be
obtained for multiple target objects over this sheet. This system
can detect target objects behind a cloth and a paper.
3.3. Electromagnetic Energy Detection: Light, Radiofrequency
A large-area photodetector is another new development of
large-area sensors. Large-area, flexible, and lightweight photo-
detectors, which are referred to as sheet-type image scanners, are
fabricated on a plastic film with integrating OFETs and organic
photodiodes.[30] Recently, large-area near-infrared photodetec-
tors have been reported based on quantum dots.[44] Since active
matrixes of this sensor are made of silicon, we will focus on
image scanners using OFETs in this section.
The sheet scanner does not require any mechanical or optical
component such as focusing lenses. In conventional scanners,
a linear array of photodetectors is moved from the top to the
bottom of a page to capture images or characters. In the new
design, a two-dimensional array of organic photodiodes cou-
pled with organic transistors is used. Instead of a line-by-line
mechanical scanning procedure, the signal of the photodiodes is
read out by electrically probing the organic transistors, avoiding
the need to use any movable part. As a result, the device is thin,
lightweight, and mechanically flexible. The effective sensing
area is four square inches and the current resolution of 36 dots
per inch (dpi). The photodetectors can detect black and white
tones by sensing the difference in reflected light from the dark
and bright parts of an image.
OFET matrix and photodiode matrix have been manufactured
separately on different plastic films and then laminated with
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Au (gate) Au (source) In this way, the device distinguishes between black and white
in the reflection geometry. Indeed, one of the organic photode-
Gate dielectric
Pentacene Transistor tectors is positioned on a sheet of white paper that has a black
region printed by a laser printer and photocurrent ratio of 8:1 is
Au (drain) PEN obtained at voltage bias of −4V.
Laser via
The last example we discuss is sensing of magnetic fields.
Parylene
Using a 2D coil array that couples with OFETs, a contactless
Au (cathode)
Silver paste position system can be realized.[32] A contactless position-
PTCDI (N)
sensing sheet comprises sheets of the position-sensing coil
CuPc (P) Laser via
array and OFET active matrix. An OTFT active matrix is fabri-
Parylene cated on a polyimide film. Silver gate electrodes and polyimide
ITO PEN
gate dielectric layers are patterned by using inkjet printing. A
(anode) Photodiode pentacene channel layer and gold source/drain electrodes are
deposited in a vacuum. The channel length and width are 13 μm
and 48 mm, respectively. A position-sensing coil array is manu-
Parylene Cl
factured by screen printing. The inner diameter of the copper
CuPc
* CH2 CH2 n * coils is 10 mm and the outer diameter is 25 mm. Both the
N N N
width and spacing of the copper lines are 100 μm. The number
PTCDI
N Cu N of turns is 38. The inductance and resistance are 20 μH and
O O 17 Ω, respectively. A position-sensing coil array and an OFET
N N
N active matrix sheet are interconnected using Ag paste. The
H N N H
pentacene FETs exhibit mobility of 1 cm2 V−1 s−1 and an on/off
O O ratio of 105.
A position-sensing unit (Figure 14) contains a resistance
O Pentacene
* O C O component in the form of an OFET and an inductance com-
C O CH2CH2 n * ponent as position-sensing coils; therefore, it is similar to a
low pass-filter. The on/off ratio of the transistors at 2.95 MHz,
Figure 13. The cross-sectional illustration of one sensor cell of large-area which is the measurement frequency (fR) for position sensing
flexible image scanner. in this study, exceeds 103. Such an excellent on/off ratio even
at high frequency can be achieved because capacitance between
source and drain electrodes is decreased as much as possible.
each other with silver paste patterned by ultrafine printing tech- Low resistance of word- and bit-lines is crucial for reducing
nique. Organic transistors are manufactured by the methods
mentioned previously. The thin-film pentacene transistors have
an 18 micrometers channel length and a 0.7 cm2 V−1 s−1 hole
mobility. The base film of the photodiodes is an ITO-coated
PEN film with resistivity of 95 Ω/square. A 30-nm-thick p-type
semiconductor of copper phthalocyanine (CuPc) and a 50 nm
thick 3,4,9,10-perylene-tetracarboxylic-diimide (PTCDI) are
deposited in vacuum sublimation system and 150 nm thick
gold is deposited as cathode electrodes. The size of cathode
electrodes and periodicity of photodiodes used to integrate
with organic transistors are 450 × 450 μm2 and 700 × 700 μm2,
respectively, but smaller photodiodes are also fabricated for
comparison (Figure 13).
Both films with OFETs and photodiodes are transferred to
the vacuum chamber without exposing to air after manufac-
turing process and uniformly coated by 2 μm poly-monochloro-
para-xylylene (parylene) passivation layer. Spots of parylene on
electrodes are removed by a CO2 laser for electronic intercon-
nections. Then, those films are laminated with each other with
silver paste patterned by ultrafine printing technology.
If all incident light reaches the active layers, photodetectors
cannot distinguish black and white. Light-shielding layers are
prepared to prevent photodetectors from being exposed to direct
incident light. The direct light cannot reach the active layers.
Then the incident light passing though transparent regions
is reflected on the white part of the paper and reaches to the Figure 14. Structure of position-sensing system comprising spiral coils
active layers, while that on black doesn’t go to the active layers. and organic transistors.

3810 © 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Adv. Mater. 2010, 22, 3799–3811

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the fluctuation of gate voltage, leading to the decrease in indi-
rect capacitive coupling between source and drain electrodes
through gate electrodes.
As the receiver coil approaches to the position-sensing coil,
output voltage decreases due to electromagnetic coupling and
the change reaches 91% at the distance of 1 mm, demonstrating
the excellent functionality of the present contactless position-
sensing system. Sensitivity (reduction in output voltage as
receiver coil approaches) is determined by inductance of position-
sensing coil, which is increased with increasing inductance.
In this study, inductance of position-sensing coils is 20 μH,
which may be maximum value for the present structure.
4. Conclusion
This review has summarized device physics and demonstrations
of chemical and physical sensors that would be challenging
and/or much more expensive to fabricate with traditional
silicon circuitry. The applications presented are examples of
potentially fruitful applications of organic electronics, in which
qualitative and functional differences with silicon are achieved.
Rather than being developed in competition with silicon tech-
nology, organic, printable, and flexible active electronics are
thus finding unique technological spaces for which attributes of
organic and other alternative semiconductors are best suited.
Acknowledgements
A. D. thanks Daniel Fine, Liang Wang, Deepak Sharma, and Chenguan
Lee for helpful assistance, as well as the Welch Foundation, DARPA,
CONTACT and Sematech for financial support. H. E. K. is grateful to
J. Sun and B. J. Jung for experimental contributions, T. Dawidcyk for
experimental confirmations and editorial contributions, and NSF (Grants
0528472 and 0730926) and the Applied Physics Laboratory for funding.
This article is part of a Special Issue on Organic Electronics.
Received: August 12, 2009
Published online: July 5, 2010
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