Organic Electronics 14 (2013) 206–211

Contents lists available at SciVerse ScienceDirect

Organic Electronics
journal homepage: www.elsevier.com/locate/orgel

Continuous tuning of the mechanical sensitivity of Pentacene OTFTs

on flexible substrates: From strain sensors to deformable transistors
P. Cosseddu a,b,⇑, G. Tiddia a, S. Milita c, A. Bonfiglio a,b
a
Department of Electrical and Electronic Engineering, University of Cagliari, Piazza d’Armi, 09123 Cagliari, Italy
b
CNR – Institute of Nanoscience, Centre S3, Via Campi 213A, I-41100 Modena, Italy
c
Istituto per la Microelettronica e Microsistemi, CNR-IMM, Via Gobetti 101, 40129 Bologna, Italy

a r t i c l e i n f o a b s t r a c t

Article history: The aim of this work is to contribute to establish whether morphological properties prevail
Received 3 August 2012 over crystal lattice organization in determining the cause for the observed sensitivity of
Received in revised form 31 October 2012 organic semiconductors to mechanical deformations in Organic Thin Film Transistors
Accepted 31 October 2012
(OTFTs). To this aim, the morphology of the active layer (made by Pentacene) of OTFTs fab-
Available online 22 November 2012
ricated on flexible substrates was intentionally modified by properly changing the deposi-
tion rate. By comparing Atomic Force Microscopy (AFM), X-ray Diffraction (XRD)
Keywords:
investigations and the electrical characterization of the devices, we can conclude that sen-
Organic semiconductors
Plastic electronics
sitivity is clearly dominated by morphological rather than lattice effects. In addition, these
Sensors results suggest a simple method for obtaining, in devices based on evaporated small mol-
ecules, a fine tuning of the sensitivity to mechanical deformation that could be predictably
adjusted in a range that goes from a minimum, practically negligible, value, desirable for
applications in flexible electronic circuitry, to a maximum extent, useful for mechanical
sensing applications.
Ó 2012 Elsevier B.V. All rights reserved.

1. Introduction cations in which devices are continuously exposed to

Over the past few years, organic conjugated semicon-
ductors have attracted considerable attention since they
offer the opportunity to produce low cost and light
weighted devices on flexible plastic substrates, opening
an entirely new market segment. Amongst these devices,
Organic Thin Film Transistors (OTFTs) are recognized as
key tools/building blocks for the implementation of elec-
tronic logic circuits and have been intensively studied for
many applications such as displays, smart tags, and sensors
[1–4]. Flexibility, or, in other words, the possibility of
adapting the fabricated devices on different kinds of sub-
strates, is certainly one of the main advantages of this
new technology. For this reason, many efforts have been
recently made to develop flexible OTFT systems for appli-
⇑ Corresponding author at: Department of Electrical and Electronic
Engineering, University of Cagliari, Piazza d’Armi, 09123 Cagliari, Italy.
E-mail address: piero.cosseddu@diee.unica.it (P. Cosseddu).
mechanical stress, such as, for instance, in wearable
electronics [5–8]. As a matter of fact, organic semiconduc-
tor-based devices are severely affected by mechanical
deformation [9,10]. In particular, the surface strain induced
on the active layer usually gives rise to pronounced varia-
tions in the conductivity of the devices. As it was found
that sensitivity to surface strain is reproducible over a cer-
tain range of mechanical deformation [11–14], in some
cases, this feature was used for the fabrication of OTFT-
based mechanical sensors. On the other hand, there are
also many applications in which this mechanical sensitiv-
ity is undesired, because devices are required to operate
normally even during mechanical deformation. Therefore,
investigating the mechanical properties of organic semi-
conductors is of crucial importance for addressing the dif-
ferent requirements of these applications.
For all these reasons, several approaches have been pro-
posed so far for the fabrication of flexible OTFTs that can
sustain large deformations [15–18]. Sekitani et al. [19,6]

1566-1199/$ - see front matter Ó 2012 Elsevier B.V. All rights reserved.
http://dx.doi.org/10.1016/j.orgel.2012.10.033
 P. Cosseddu et al. / Organic Electronics 14 (2013) 206–211 207

proposed the fabrication of OTFTs on flexible substrates in ing the mechanical transduction for sensing applications
which the organic semiconductor film is embedded, in a on one hand, and, on the other hand, for strongly limiting
neutral strain position, within a multilayered structure. and eventually eliminating the OTFTs sensitivity to surface
In this way, by eliminating the surface strain on the organic strain in applications where this mechanical sensitivity is
film, they managed to obtain devices that are unaffected by considered detrimental.
bending until 1 mm of curvature radius. In our lab, we have
recently introduced a different approach that consisted in
the fabrication of organic transistors on very thin flexible 2. Materials and methods
substrates [12]. In fact, since the extent of surface strain in-
duced on the organic semiconductor mainly depends on OTFTs were fabricated on a flexible, 175 lm thick
the thickness of the substrate, by reducing this latter value poly(ethylene therephtalate) (PET). The first step consisted
to 400 nm, bending radii can be reduced to less than 1 mm of the deposition, through a shadow mask, of a gold film
with no effect of strain on the device electrical behavior. that acts as the gate electrode. Afterwards, a film of Paryl-
Another very interesting approach was recently introduced ene C (nominal thickness 1.5 lm) was deposited on the
by Graz et al. [20]. They fabricated OTFTs on elastomeric whole substrate in order to realize the gate dielectric. Gold
substrates and selectively modified the mechanical proper- Source and Drain electrodes were fabricated in bottom con-
ties of the elastomers in order to have highly deformable tact configuration by a standard photolithographic process,
areas, and very small stiffer islands on which the devices using for all devices the same geometry (width = 50 mm,
are located. Using this approach, they managed to apply length = 30 lm, gold layer thickness = 80 nm) and finally,
strain as large as 13% to the substrate surface without in all cases, a 45 nm thick Pentacene film (Sigma Aldrich)
damaging or anyhow affecting the device performances. was deposited by thermal evaporation at a pressure below
This was mainly due to the fact that most of the surface 1  106 mbar (see Fig. 1a).
deformation is accommodated by the highly deformable Drain-source current (Ids) measurements were carried
parts of the substrate, leaving unaffected the stiffer areas out at room temperature in air. A Keithley 2636A source-
where the devices are placed. meter, provided with gold tips for contacting the elec-
In order to shed some light on the mechanical sensitiv- trodes, was used for the electrical characterization.
ity of OTFTs, many efforts have been aimed towards the Atomic Force Microscopy measurements were obtained
investigation of the main causes that lead organic semicon- by means of a SPM SOLVER PRO by NT-MDT in semi-con-
ductors to be sensitive to mechanical stress [9,11,21–23]. tact mode using NT-MDT NSG01 tips.
In many cases, the current variation can be correlated to XRD measurements were collected in specular geome-
morphological changes taking place in the active layer, try by using a SmartLab diffractometer (Rigaku), equipped
thus modifying the hopping energy barrier for charge with a rotating anode (Cu Kak = 1.54180 Å) followed by a
transport [9,11,21]. Very recently, a correlation was ob- parabolic mirror, to collimate the incident beam.
served between the device electrical behavior and the The experimental set-up employed for the electrome-
modification of the structural properties of the organic ac- chanical characterization is reported in Fig. 1. The edges
tive film induced by the mechanical deformation [22]. of the plastic substrate are fixed on the armatures of a
Moreover, we have recently demonstrated, by comparing
OTFTs realized using two different classes of organic semi-
conductors [21], that the intrinsic morphological proper-
ties of the organic semiconductor film can dramatically
influence the sensitivity to mechanical deformation of
the devices.
In this paper we have further investigated this aspect,
focusing our attention on a single material (that is Penta-
cene, which is considered the benchmark for all organic
small molecules) with the aim of keeping constant the lat-
tice organization while varying only the morphology. As it
is well known that the morphology of films based on rod-
like molecules (such as Pentacene deposited by thermal
evaporation) may be intentionally modified by varying
the deposition parameters [24,25], and that the intrinsic
charge transport properties can be dramatically influenced
by the film morphology, we investigated the electrical re-
sponse to mechanical deformation of many identical de-
vices with a Pentacene active layer deposited with
different deposition rates, with the aim of revealing a pos-
sible correlation between morphological properties and
device sensitivity to mechanical deformation. The results
clearly show that such sensitivity can be predictably tuned Fig. 1. Schematic representation of the flexible OTFT structure (a), and
by properly modulating the grain dimensions of the active experimental set up employed for the electromechanical characterization
layer. These results indicate a possible method for optimiz- (b).
208 P. Cosseddu et al. / Organic Electronics 14 (2013) 206–211
bending machine. When one armature is moved towards
the other, the substrate is bent. Using this configuration,
a uniaxial deformation is applied on the OTFT surface;
the surface strain induced on the active layer (l) may be
evaluated using the following formula [26]:
 
worth mentioning that due to the high surface corrugation
dl þ ds 1 þ 2g þ vg2
Strain ¼
2R ð1 þ gÞð1 þ vgÞ
In which dl and ds are the thicknesses of the active layer
and of the substrate respectively, g is dl/ds, v is the ratio be-
tween the Young moduli of the active layer and of the sub-
strate (v = Yl/Ys) and R is the bending radius. Considering
that the substrate is more than two orders of magnitude
thicker than the active layer, the surface strain induced
on the active layer can be approximated by:
 
dl
Strain ¼
2R
Using this configuration, the whole structure can be bent at
different bending radii, allowing, at the same time, the
electrical characterization of the OTFTs. The bending radius
was estimated considering a homogeneous bending of the
PET foil. We have applied bending radii ranging from 4 cm
down to 2 mm, corresponding to an induced surface strain
from 0.22% to 4.4%. All the measurements have been per-
formed starting from the small deformation regime (large
bending radii), and the deformation was constantly in-
creased by reducing the bending radius. The reversibility
of the device behavior was checked by measuring the elec-
trical characteristics of the devices in the flat position after
each deformation step.
3. Results and discussion
Very recently we have demonstrated that Pentacene-
based OTFTs are very sensitive to mechanical deformation
[12,21]. Different experimental set-ups have been em-
ployed, and in all cases, a pronounced sensitivity to the
surface strain induced by mechanical deformation was ob-
served. Moreover, it was also demonstrated that such an
electrical response to mechanical deformation is dramati-
cally influenced by the intrinsic morphological properties
exhibited by different organic semiconductors (in particu-
lar, by small molecules and polymers) [21]. In this work we
have again employed Pentacene as organic semiconductor,
with the aim of intentionally inducing a modification of its
morphological properties without changing the lattice
structural arrangement. We have studied how the device
Fig. 2. AFM micrographs of Pentacene deposited using different deposition rates, indicated on each image.
electrical response to mechanical deformation is affected
by the different deposition rates. As previously introduced,
all devices have been fabricated on the same substrate and
with exactly the same geometry. In this case we have em-
ployed Parylene C as the gate dielectric. First of all, it is
of the Parylene C film, which was found to range around
ð1Þ
3 nm (expressed in terms of Root Mean Square Roughness,
RMSR), even employing a very slow deposition rate, usu-
ally a very granular film morphology, as shown in Fig. 2,
is obtained.
Nevertheless, it was also found that, by properly chang-
ing the deposition rate, it is still possible to predictably
modify the Pentacene morphology. In particular, as shown
in Fig. 2a–d, it was observed that an increase of the depo-
sition rate leads to a marked decrease of the average do-
main dimensions going from 250–300 nm to 80–100 nm
ð2Þ
for deposition rates of 0.08 Å/s and 11 Å/s respectively.
Moreover, the XRD patterns recorded in specular geometry
(h/2h scan), reported in Fig. 3, have revealed that all films
deposited on the PET + Parylene bilayer are polycrystalline
although with a degree of crystallinity much lower than
that observed in Pentacene films deposited on smoother
substrates such as SiO2 (shown as reference sample in
the Fig. 3). The Pentacene molecules arrange mainly in a
thin film phase structure and with the long molecular axis
almost perpendicular to the substrate. Furthermore, the
data recorded on different Pentacene films, fabricated
using very different deposition rates, namely 0.08 and
5 Å/s, do not show any significant difference in their crystal
properties detected along the surface normal, suggesting
that the molecular arrangement is the same despite the
very different morphology. This observation is essential
as it allows confirmation of our initial assumption, i.e. that
in this system, by varying the deposition rate, we only
modify the film morphology.
The average values of mobility and threshold voltage of
all the fabricated devices have been calculated and are re-
ported in Table 1. From these data, it can be noticed that a
slight but visible decrease of the average mobility is in-
duced by the reduction of the average grain dimensions,
passing from 5  102 cm2/V s to 2.5  102 cm2/V s when
the deposition rate is increased from 0.08 Å/s to11 Å/s.
First, the electromechanical characterization was per-
formed on devices fabricated using two different deposi-
tion rates, namely 0.08 and 5 Å/s, which, as shown in
Fig. 2a and c, give rise to very different average grain
dimensions. In Fig. 4, we report the data obtained by apply-
ing a tensile deformation to the organic semiconductor
 P. Cosseddu et al. / Organic Electronics 14 (2013) 206–211 209

able for surface strain ranging from 0% to 2%. For more

Fig. 3. XRD patterns of the films deposited at 0.08 and 5 Å/s together with
the reference pattern of the Parylene C substrate alone and a reference
Pentacene Film deposited on a ‘‘ideal’’ SiO2 substrate.
film. From the analysis of these results, several conclusions
can be drawn. First of all, in all sets of measured samples, a
clear, marked variation (i.e. a decrease) of the output cur-
rent was observed by increasing the surface strain induced
by bending the substrate. This behavior, as previously re-
ported [9,11,21] is linear, reproducible and fully recover-
pronounced deformations, the devices behavior starts to
be less reproducible, and, most importantly, the output
current measured after removing mechanical stress, does
not return to the value recorded before deformation. It is
worth underlying that all the measurements have been
performed in the same sequence: from lower (reversible)
to higher (irreversible) deformations. Therefore, all the
data reported within the reversible region refer to undam-
aged devices.
Moreover, a clear correlation between current and
mobility variations was also observed, as demonstrated
in Fig. 4b. On the contrary, there is no relation between
threshold voltage and strain (Fig. 4c). These results are in
accordance with what was already reported very recently
[21], and demonstrate that the current variation induced
by surface strain is mainly related to an alteration of the
charge carrier transport mechanisms. In fact, in the case
of Pentacene, the surface strain induced on the active layer
by a tensile deformation may lead to a possible increase of
spacing between molecules within the active layer, or,
most probably, to an increase in distance between adjacent
crystal domains. Thus, both mechanisms may be invoked
for justifying a decrease of the OTFT mobility. These obser-

Table 1
Average values of mobility and threshold voltage measured in all devices fabricated with different deposition
rates.

Rate (Å/s) 0.08 0.5 5 11

Mobility (cm2/V s) (5 ± 2)102 (3 ± 2)102 (2.5 ± 0.4)102 (2.5 ± 0.8)102
Vt (V) 22 ± 3 11 ± 2 26 ± 3 11 ± 1

Fig. 4. Electrical characterization of OFETs fabricated with Pentacene films deposited at two different rates: output current variation vs strain (a), mobility
variation vs strain (b), threshold voltage variation vs strain (c), conversion table indicating the employed bending radii and the correspondent induced
surface strain (d). In all devices a tensile deformation was applied.
210 P. Cosseddu et al. / Organic Electronics 14 (2013) 206–211

Fig. 5. Normalized transfer characteristics (ID/IDflat) for devices fabricated using 0.08 and 5 Å/s as Pentacene deposition rate (a and b respectively). IDflat was
recorded in the flat position at VG = 80 V. Measurements have been recorded both in tensile and in compression mode showing in the first case a decrease,
and in the second an increase of the output current. Mobility variation vs strain obtained by compression and tension experiments, for the two employed
deposition rates are summarized in (c).

vations are further confirmed by the measurements re-
ported in Fig. 5. In this case, we reported the normalized
(with respect to ID value recorded at VG = 80 V measured
in the flat position) transfer characteristics recorded both
for tensile and compressive deformations. Very interest-
ingly, it can be observed that, for both deposition rates, a
tensile deformation gives rise to a decrease of the output
current, whereas, a compressive deformation gives rise to
an increase. This feature can be ascribed to the fact that,
by applying a compressive deformation, the distance be-
tween adjacent domains can be reduced, thus decreasing
the hopping barrier, and, as a consequence, increasing
the mobility. Moreover, Fig. 5c, clearly shows that the
mobility variation trend is similar in both compression
and tension regimes.
The most intriguing feature in our results is that a
marked difference in the sensitivity was also observed in
the two sets of samples. In particular, the sensitivity of de-
vices fabricated using a faster deposition rate (character-
ized by average grain dimensions around 80–100 nm) is
much smaller than the one observed for devices fabricated
using a slower deposition rate, which usually gives rise to
average grain dimensions around 200–250 nm. The ob-
tained results seem to be in accordance to what we have
already observed in poly(3-hexylthiophene-2,5-diyl)
(P3HT)-based OTFTs [21]. In that particular case, we ob-
served a dramatic reduction of the sensitivity to strain that
was correlated to the very different morphological proper-
ties of the P3HT films in comparison with Pentacene.

Fig. 6. Current variation vs strain (tensile deformation) for different sets of devices fabricated using different deposition rates (a), correlation between
sensitivity slope DS and average grain diameter (b), showing a clear dependence of the device sensitivity to the morphological properties of the organic
semiconductor film.
 P. Cosseddu et al. / Organic Electronics 14 (2013) 206–211
To further investigate this phenomenon and to give a
broader validity to the presented results, devices with four
different deposition rates have been fabricated and charac-
terized. Their sensitivity to surface strain induced by bend-
ing is reported in Fig. 6a. For each curve, we have also
estimated the slope of the sensitivity curve (called DS, de-
fined as% Dl/% Dstrain) and have plotted it as a function
of the average domain diameter (Fig. 6b).
Interestingly enough, a clear dependence of devices
sensitivity on the deposition rate was observed. For a sur-
face strain of 1%, the sensitivity of devices fabricated using
the slowest deposition rate, 0.08 Å/s, is around 40%,
whereas for devices fabricated using the fastest deposition
rate, 11 Å/s, a much lower, almost negligible, sensitivity
was observed (3%). However, these results cannot be gen-
eralized, as they are strongly dependent on the particular
deposition chamber, and on the employed deposition
parameters. For these reasons, we have performed AFM
characterization of the devices, fabricated at different
deposition rates, and we have tried to correlate the DS fac-
tor with the average domain (assumed as round, these data
have been estimated by analyzing the AFM micrographs
with SPIP Software) diameter. As can be clearly observed
from the plots reported in Fig. 6b, there is a linear depen-
dence between DS and the domain diameter, at least in
the domain size range that we have investigated. We can-
not exclude that this trend may be different with different
domain sizes, but considering that no differences were ob-
served in the molecular arrangement, our results lead us to
conclude, once again, that the device mechanical sensitiv-
ity is correlated to the morphological rather than to the
crystal properties of the organic semiconductor film. These
results are particularly important because they also indi-
cate that by modifying, in a controlled way, the morpho-
logical properties of the active layer, it is possible to
finely tune the electrical response of OTFTs to surface
strain, going from a maximized effect suitable for sensing
applications (corresponding to large domains) to a mini-
mal, almost negligible, sensitivity, suitable for those appli-
cations in which the circuitry behavior must be insensitive
to the substrate deformation.
4. Conclusions
In conclusion, we have demonstrated that the influence
of mechanical deformation on the electrical behavior of
OTFTs based on Pentacene is strongly related to the mor-
phological, rather than to the lattice properties of the or-
ganic semiconductor film. Moreover it was also found
that by properly modulating the Pentacene morphology,
it is possible to tune the sensitivity to surface strain in a
predictable way; in particular, devices with a high sensitiv-
ity to strain can be fabricated for sensing applications by
211
using very low deposition rates, whereas, on the contrary,
for applications in which mechanical sensitivity must be
limited as much as possible, higher deposition rates can
be used allowing to decrease their sensitivity to strain by
more than one order of magnitude.
Acknowledgment
The authors acknowledge financial support by the Euro-
pean Commission, under the VII FP Project ‘‘Roboskin’’, #
231500.
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