Research Article

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Ultrasensitive Strain Sensor Produced by Direct Patterning of Liquid

Crystals of Graphene Oxide on a Flexible Substrate
M. Bulut Coskun,†,°,• Abozar Akbari,‡,• Daniel T. H. Lai,*,§ Adrian Neild,† Mainak Majumder,‡
and Tuncay Alan*,†
†
Laboratory for Micro Systems, Department of Mechanical and Aerospace Engineering, Monash University, Melbourne 3800,
Australia
‡
Nanoscale Science and Engineering Laboratory, Department of Mechanical and Aerospace Engineering, Monash University,
Melbourne 3800, Australia
§
See https://pubs.acs.org/sharingguidelines for options on how to legitimately share published articles.

College of Engineering and Science, Victoria University, Melbourne 3011, Australia

*
S Supporting Information

ABSTRACT: Ultrasensitive flexible strain sensors were developed

Downloaded via MONASH UNIV on May 4, 2023 at 22:55:40 (UTC).

through the combination of shear alignment of a high concentration

graphene oxide (GO) dispersion with fast and precise patterning of
multiple rectangular features on a flexible substrate. Resistive
changes in the reduced GO films were investigated under various
uniaxial strain cycles ranging from 0.025 to 2%, controlled with a
motorized nanopositioning stage. The devices uniquely combine a
very small detection limit (0.025%) and a high gauge factor with a
rapid fabrication process conducive to batch production.

KEYWORDS: strain gauge, rGO, direct GO patterning, shear alignment, high sensitivity, flexible substrate

1. INTRODUCTION graphite. GO sheets are essentially graphene layers decorated

Wearable, flexible strain sensors have attracted significant
attention in a myriad of applications ranging from biomedical
health monitoring1,2 to soft robotics.3,4 Thanks to their superior
mechanical and electrical properties and synergy with flexible
substrates, graphene-based devices offer improved measure-
ment sensitivities over conventional micromachined sensors,5−7
and there has been a considerable interest in their use for strain
sensing.8−22
The electrical resistance of pristine graphene changes when
subjected to strain.11 However, approaches based on structural
deformation of a single layer of graphene necessitate very high
strain inputs to open the band gap of the material,10 making
them unsuitable for detection of very low strains. A substantial
improvement in sensitivity can be obtained using multilayered
configurations9,12,13,23 in which the contacting graphene flakes
form an electrical network. The introduction of strain alters the
overlapping areas between flakes, significantly changing the
conductivity of the device.
Moreover, the use of pristine or chemical vapor deposited
graphene, while offering a very high quality, requires transfer
techniques or subsequent nanofabrication steps.24 Yet, to make
full use of the potential offered by miniaturized flexible devices
in practical applications, the devices should be produced
through rapid, cheap processes conducive to high-volume
production.25 This challenge can be addressed using a cheaper
alternative: reduced graphene oxide (rGO), produced in
dispersion17 through the oxidative chemical processing of
with oxygen-bearing functional groups26 which can be removed
to obtain reduced graphene oxide (rGO).
We developed a new class of highly flexible and ultrasensitive
rGO strain sensors based on our shear-alignment technique27
of liquid crystal nematic phase of GO dispersion which can
produce large-area films with controlled structural properties.
Here, we improved this technique to cast precisely defined rGO
layers on flexible polydimethylsiloxane (PDMS) substrates
which are selectively masked by a temporary vinyl layer (Figure
1). The direct casting on masked substrates takes place at room
temperature, is not sensitive to the substrates being used,27 and
can generate well-defined patterned structures without
subsequent transfer processes, resulting in improvements over
well-established techniques such as spin coating.28 Similarly, the
processing time is significantly shorter than that for vacuum
filtration8 methods. Finally, the geometric definition is better
controlled in comparison to that of spray coating.9 This
provides a rapid and scalable technique. However, it is known
that, during the drying of sprayed drops, nonuniform deposits
may compromise the uniformity of the films produced.29
Received: May 26, 2016
Accepted: August 4, 2016
Published: August 4, 2016

© 2016 American Chemical Society 22501 DOI: 10.1021/acsami.6b06290

ACS Appl. Mater. Interfaces 2016, 8, 22501−22505
ACS Applied Materials & Interfaces
Figure 1. Masked shear-alignment process. (a) The process starts with a blank substrate. (b) Then, a vinyl mask with the desired features is placed
on the substrate, (b) 0.5 mL of a GO dispersion is poured on the edge of the substrate, and (c) the dispersion is cast by moving a Doctor Blade. (d)
The mask is peeled off, and (e) remaining features on the substrate are reduced at 110 °C for 8 h and diced. (f) Photograph of the rGO film on the
substrate after the casting process. (g) FTIR spectra of the graphene-based sensor before and after reduction by thermal treatment. (h) XRD pattern
of the graphene-based sensor before and after reduction by thermal treatment.
2. EXPERIMENTAL SECTION
2.1. Preparation and Concentration of GO Dispersion. The
high concentration nematic liquid crystal phase of GO dispersion used
in the fabrication is a shear-thinning fluid which allows casting of a
uniform liquid thin film under high shear stress imposed by the motion
of a doctor blade, while a highly viscous phase in the absence of shear
stress ensures uniformity during the subsequent film drying step. A low
concentration GO (∼0.25 mg mL−1) was prepared by Hummers’
method30 followed by concentrating the dispersion by the dehydration
technique,27 where a cross-linked polyacrylate copolymer hydrogel was
used to absorb the water content until the desired concentration of 35
mg/mL was achieved. Polarized light microscopy using an LC-
PolScope imaging system (40× 0.75/0.85NA objective) was used to
confirm the nematic phase of the GO dispersion.31,32 With the LC-
Polscope technique, it is possible to detect the retardance along with
their dominant orientation simultaneously at all points of the image
without having to mechanically rotate the sample (Figure S1).
2.2. PDMS Substrate Preparation. A mixture of Sylgard 184
curing agent and base with a mass ratio of 1:10 was prepared. The
mixture was then poured in to a 6″ Petri dish and placed in a
desiccator for half an hour for degassing. Later, degassed PDMS was
thermoset for 6 h at 70 °C on a hot plate. Finally, the cured PDMS
substrate was plasma treated with 18 W power under 0.3 mbar
pressure for 5 min (Harrick Plasma PDC-32G) to introduce oxygen-
bearing functionalities to improve adhesion with the GO dispersion.
2.3. Masking Process. Rectangular patterns (35 × 10 mm) on the
vinyl tape were drawn using CutStudio and programmed to be cut by a
vinyl plotter (Roland SV-8). The plotter removes the rectangular
features from the vinyl tape (so that later the openings will be filled
with GO in the casting process). The desired sensor patterns were
attached onto a plasma-treated 800 μm-thick PDMS substrate,
effectively masking selected regions on the substrate
2.4. GO Film Casting. A simple lab-scale Doctor Blade (MTI
Corporation, United States) was used as a shear-alignment apparatus
to cast a continuous GO film. A 0.5 mL of nematic phase GO
dispersion (35 mg mL−1) was deposited at the edge of the mask
(Figure 1b). To create the thin film, the Doctor Blade was then moved
over the surface of the vinyl. This enabled spreading of the GO
dispersion into the patterned features shown in Figure 1c and crucially
provided the shear required for alignment of the graphene flakes.
Removal of the vinyl mask resulted in the desired GO patterns on the
substrate (Figure 1d), which was left overnight at room temperature to
dry. With the casting process complete, the final step was to remove
22502
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the oxygen functional groups from the GO sheets to obtain a
conductive rGO film. In this regard, a heat treatment technique was
used (at 110 °C for 8 h) to reduce the GO film (Figure 1e).
During the drying and heat treatment stages, the thickness of the
GO film decreased substantially. A photograph of the rGO sensor
resulting from this casting process is shown in Figure 1f.
2.5. Film Characterization. The GO film was characterized via X-
ray diffraction (XRD) and Fourier transform infrared (FTIR) methods
before and after reduction. The FTIR spectra were obtained using an
attenuated total reflectance Fourier transform infrared (ATR-FTIR)
instrument (PerkinElmer, United States) in the range of 600−4000
cm−1 at an average of 32 scans with a resolution of 4 cm−1. In the case
of GO, there was a strong and broad peak in the range of 3100−3700
cm−1 and a peak at 1650 cm−1 corresponding to the stretching of
hydroxyl groups, possibly from COOH groups in GO and/or the
presence of H2O in GO interlayers. Peaks at 1728, 1205, and 1070
cm−1 are attributed to stretching of the CO in carbonyl groups, C−
O−C in epoxide groups, and C−O in alkoxy groups, respectively.
Peaks at 1383 and 1400 cm−1 are attributed to the vibration of O−H
in C−OH groups. The XRD patterns of the GO and rGO films were
recorded using a Phillips 1140 diffractometer with a Cu Kα line
generated at 40 kV and 25 mA at a scan rate of 1°/min and a step size
of 0.02°.
3. RESULTS AND DISCUSSION
The FTIR spectra of the cast rGO film (Figure 1g) showed that
the oxygen functional groups experienced a reduction as
evidenced by a significant decrease in the intensity of the
relevant oxygen functional group peaks and a presence a new
peak at 1550 cm−1 which corresponds to a CC bond,
confirming reduction of the GO by the thermal treatment.
Similarly, the XRD spectrum (Figure 1h) revealed that the
interlayer distance of the rGO film decreased from ∼0.91 nm
(2θ = 9.68°) for the GO film to ∼0.39 nm (2θ = 22.8°),
confirming reduction of the GO sensor in agreement with the
observed FTIR spectra for these two samples. The end result
after casting was a uniform 6.4 μm-thick continuous film of
rGO on an 800 μm-thick flexible PDMS substrate, as shown in
Figures 2a and b. The reduction step19 resulted in a wrinkled
surface with a 928 nm root-mean-square (rms) surface
roughness (Figure 2c), as measured with an optical
DOI: 10.1021/acsami.6b06290
ACS Appl. Mater. Interfaces 2016, 8, 22501−22505
ACS Applied Materials & Interfaces
Figure 2. (a) Scanning electron micrograph of the deposited film. (b)
Optical micrograph showing the film cross section. (c) Surface
topography of the film resulting from the thermal reduction step. (d)
Line profiles in the direction parallel to the motion of the Doctor
Blade obtained with an optical profiler.
profilometer (Bruker Contour GT-I). The line profile in Figure
2d indicates a maximum step height of 3 μm along the direction
of the motion of the Doctor Blade, parallel to the axis in which
the strain measurements were made.
A typical strain gauge consists of a sensory conduction path
that generates a measurable electrical signal when subjected to
strain. For the present case, the dominant sensing mechanism is
the modification of the conduction path due to changes in the
overlapping area of, or the creation of gaps between, the
neighboring rGO sheets. As the thickness of the rGO film
(∼6.4 μm) is much smaller than that of the substrate (∼800
μm), it can be assumed that strain distribution across the
thickness is uniform9 and that the expansion response of the
system is dominated by the stiffness of the substrate.
To assemble the sensors, after making electrical connections
at both ends, the rGO-coated samples were clamped at both
ends with one end attached to a fixed block and the other end
connected to a linear XYZ actuator stage (Newport M562) as
shown in Figures 3a and b. The stage was driven by a
picomotor (Newport 8310CL motor and 8751CL closed loop
driver) programmed to produce a displacement range of up to
300 μm with a 63.5 nm step resolution. To measure the
resistance changes of the rGO sensor under the applied strains,
a read-out circuit based on an inverting op-amp configuration
was implemented. The circuit consisted of a fixed input resistor
and the rGO film which acted as the variable feedback resistor
(Figure 3c). The change in the rGO film’s resistance was
measured by means of voltage variations for the corresponding
strains as
⎛R ⎞ the percentage change in resistance at increasing deformations.
Vout = −Vin⎜ RGO ⎟
⎝ R SMD ⎠
where Vin is the input voltage and RRGO (base resistance ∼9.2
kΩ) and RSMD (fixed 10 kΩ) are the resistance of the rGO film
and surface mount resistor, respectively. Here, as Vin (−1 V)
and RSMD are fixed, the circuit provides a linear input-output
relation which would not be obtainable from a voltage divider
or Wheatstone bridge circuit. Hence, through the use of eq 1,
changes in RRGO can be determined. During the experiments,
Vout was monitored and recorded using a data acquisition card
(NI PCI 6251) and Labview with a 100 Hz sampling frequency.
The setup was placed under an optical microscope located on a
vibration isolation table to minimize environmental vibrations.
The rGO sensor was able to detect strains well below 0.1%,
which is rarely achieved in the literature for graphene-based
Research Article
Figure 3. (a) Schematic of the test setup. The rGO-coated PDMS
sample is clamped on a fixed block from one side and on moveable
XYZ stage actuated by a picomotor. (b) Schematic of the sample
showing the direction of the applied strain (εxx) that leads to a slight
contraction (εyy) in perpendicular direction driven by PDMS’s Poisson
ratio (0.5). (c) Readout circuit based on an op-amp (Texas
Instruments, LM324N) used in an inverted configuration to detect
the strain-induced changes in resistance.
sensors.13 Experiments were conducted for strain levels
increasing from 0.025 to 2%. Figure 4a shows the dynamic
response of the sensor under 4 different maximum strain levels
(i.e., 0.05, 0.4, 0.8, and 1.2%) and demonstrates a perfect match
in the initial inclination of the output voltage. Figure 4b shows
the change in resistance of the PDMS-based sensor for 50 strain
cycles of 0.6% maximum strain. The results indicate that the
response is repeatable and consistent. Figure 4c demonstrates
The data were acquired by averaging the results from 3 separate
(1)
experiments (each using different samples from a single batch)
and show a 5.8% standard deviation. These results indicate a
very high change in resistance, reaching over 400% at 2% strain
with two linear regimes below and above 0.8% strain.
We hypothesize that this is due to a transition in the effective
mechanism that modifies the conduction path. For lower strains
(below 0.8%), the resistance change is due to a change in the
overlapping areas of the neighboring rGO flakes. Whereas at
increasing strains up to 2%, the separation of larger rGO flake
groups or islands is responsible for the change in resistance.
Furthermore, above 2% strain, a permanent inclination in the
device’s voltage output under rest position was observed. This
is due to the increase in base resistance of the devices which
indicates formation of irreversible cracks in the rGO film at
22503 DOI: 10.1021/acsami.6b06290
ACS Appl. Mater. Interfaces 2016, 8, 22501−22505
ACS Applied Materials & Interfaces
Figure 4. (a) Response of rGO-coated PDMS to cyclic strain cycles
(0.05, 0.4, 0.8, and 1.2%) recorded with a 100 Hz sampling frequency.
(b) Response of the film after 50 cycles of strains under 0.6%. Voltage
output here is converted to the rate of change of resistance via eq 1.
(c) Percentage change in the resistance of rGO. The slope of the linear
fits defines the gauge factor as 137.2 ± 7.9 for strains below 0.8% and
261.2 ± 15.1 for strains above 0.8%.
higher strain inputs. Hence, the measurement range of the
present devices were set from 0 to 2% strain.
The common way to relate electrical changes to the
mechanical parameters for the strain sensors is the gauge
factor (GF). This is effectively a measure of the sensitivity of
the strain sensor and is acquired from the slope of the rate of
change of the resistance-strain curve23
ΔR
GF =
( R )
ε (2)
The GF was calculated by fitting a line to the data shown in
Figure 4c for the two regimes. Using the slope of these portions
of the response curve yields GF values of 137.3 and 261.2 for
strains below and above 0.8%, respectively. As the strain cycles
are still reversible above 0.8%, the sensor can easily be tuned to
have higher gauge factors at lower strains by prestraining. The
acquired gauge factors are comparable to or better than
previously reported values,8,9,12−24 (Table S1) while offering a
substantially simpler design and fabrication process. A similar
set of experiments was conducted for rGO casted on a
polyamide 66 substrate, and the results are demonstrated in
Figure S2.
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4. CONCLUSION
In summary, a new type of flexible and highly sensitive rGO-
based strain sensor was demonstrated. The device combines a
low cost and scalable deposition method and a simple detection
circuitry with a very high sensitivity (gauge factor up to 261).
The sensor can accurately detect strains as small as 0.025%
under cyclic loadings, hence providing significant advantages
for continuous real-time monitoring of minute deformations.
Direct pattern transfer through a masking process primarily
allows multiple copies of identical devices to be produced by a
single fabrication step. It also provides significant potential to
further improve the sensor size and performance through
geometric modifications.
■
*
ASSOCIATED CONTENT
S Supporting Information
The Supporting Information is available free of charge on the
ACS Publications website at DOI: 10.1021/acsami.6b06290.
Formation of liquid crystals of graphene oxide,
experimental results for rGO on the polyamide 66
substrate, and tabulated gauge factors of the previous
works from the literature (PDF)
■ AUTHOR INFORMATION
Corresponding Authors
*E-mail: Tuncay.Alan@monash.edu.au.
*E-mail: Daniel.Lai@vu.edu.au.
Present Address
°
M.B.C.: Department of Mechanical Engineering, University of
Texas at Dallas, Richardson, Texas 75080, United States.
Author Contributions
•
M.B.C. and A.A. contributed equally to the work. A.A.
prepared the rGO samples and characterized material proper-
ties. M.B.C. fabricated the flexible sensors, performed the
experiments and analyzed the data. D.L and T.A. oversaw the
research. The manuscript was written through contributions of
all authors. All authors have given approval to the final version
of the manuscript.
Notes
The authors declare no competing financial interest.
■
ACKNOWLEDGMENTS
Part of this work was performed at the Melbourne Centre for
Nanofabrication (MCN), the Victorian Node of the Australian
National Fabrication Facility (ANFF). The authors acknowl-
edge support received from the Monash University Post-
graduate Publications Award and Monash Centre for Atomi-
cally Thin Materials.
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22505 DOI: 10.1021/acsami.6b06290

ACS Appl. Mater. Interfaces 2016, 8, 22501−22505