Sensors and Actuators A 151 (2009) 154–158

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Sensors and Actuators A: Physical

journal homepage: www.elsevier.com/locate/sna

An invisible bend sensor based on porous crosslinked polyelectrolyte film

Q. Zhang a , L.V. Saraf b , J.R. Smith a , P. Jha a , F. Hua a,∗
a
Department of Electrical and Computer Engineering, Clarkson University, Potsdam, NY 13699, USA
b
Pacific Northwest National Laboratory, Richland, WA 99352, USA

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

Article history: This paper reports the fabrication and electromechanical characterization of a thin porous polyelectrolyte
Received 23 August 2008 film and its application in an invisible bending transducer. The porous film consists of 10 bilayers of
Received in revised form 29 January 2009 polycation and polyanion that are adsorbed using electrostatic self-assembly (ESA). Such porous film can
Accepted 19 February 2009
be thermally crosslinked. The size of the pores on top surface is adjustable and can be covered up by a
Available online 9 March 2009
type of Na+ -montmorillonite nanosheet whose size is comparable to those of the pores. As a result, the
sealed top surface can be coated by metal for an electrode. After such polymeric film is integrated into a
Keywords:
sandwich structure that was designed for a bend sensor, it can perform as an ultrathin piece of elastomer.
Electrostatic self-assembly
Porous polymeric film
It is found that the bending of the substrate resulted in the increasing of the current. It is hypothesized that
Ultrathin elastomer the tunneling current through the thin polymeric film changes when the film is compressed by bending.
Tunneling current Finite element simulation corroborates the existence of strain concentration especially near two ends of
Invisible sensor the polymer film and the shoulder of the bottom electrode.
© 2009 Elsevier B.V. All rights reserved.

1. Introduction
The bend sensor is used to detect the position and orientation
of an object, thus having wide applications in interactive com-
puter games, the automotive industry and manufacturing control
[1–5]. The commercial bend sensors are mainly dependent on a
conductive thin film whose resistivity changes with the curvature
[1,4–7]. In the usual case, such sensors have to occupy a consider-
able area in order to contain the long polymer resistive wire. At the
continuous monitoring mode, the resistive wire keeps consuming
electric power when the sensor is in an idle situation (flat position).
Capacitive type sensors detect the variation of the capacitance of a
dielectric layer between two parallel electrodes. The permittivity
variation of the dielectric layer as a response to flexion exhib-
ited limited sensitivity, thus requiring addition amplifying circuit
[8]. The change in dimension (thickness and area) of the dielec-
tric layer also results in the variation of the capacitance. However,
extra efforts are necessary to fabricate this type of sensor with high
nominal capacitance in order to reduce the loss due to parasitic
capacitance [2,9–11]. Moreover, the capacitive sensors may also
have current response to strain, resulting in power consumption.
This paper presents a bend sensor that possesses a capacitor-like
structure, which dramatically reduces the occupied area, thus mak-
ing pixel sensing feasible. The current between the two electrodes
∗ Corresponding author. Tel.: +1 315 2682126; fax: +1 315 2687600.
E-mail address: fhua@clarkson.edu (F. Hua).
vary with the flexion. When the sensor is in the flat position, it
hardly consumes power. Another unique feature is the sensor is
transparent in the visible light spectrum. This see-through structure
enables the sensors to fit special applications where the presence
of the hidden electronic surveillance is required not to be revealed.
They can be placed on large window panels or contact lens to detect
deformation. Installed outdoors, they have higher tolerance to sun-
shine and temperature variation because of reduced absorption. As
a result, less photo- and thermal-degradation are anticipated, lead-
ing to a longer field life and more stable operation [12]. They allow
an easy registration onto other objects because the features under-
neath are visible through the sensor. They not only sense the flexion
but also allow for diagnosis of other symptoms such as cracks devel-
oping on the surface under the sensor. Fig. 1a illustrates the visual
effect of the invisible bend sensors fabricated on a piece of plastic
transparency.
Such sensors have a vertical structure with two transparent
indium-tin-oxide (ITO) electrodes and a thin porous dielectric layer
(nanospring) in between as shown in Fig. 3h. In particular, the
top electrode is wider than the bottom one so that the dielectric
layer is confined between two electrodes. The dielectric layer is a
multilayer of polycation, poly(allylamine hydrochloride) (PAH), and
polyanion, poly(acrylic acid) (PAA), which are generated by electro-
static self-assembly (ESA). The porous structure is generated by a
process which was demonstrated by M. F. Rubner co-workers [13].
The self-assembled polyions are integrated mainly by electrostatic
interaction. The post-annealing turns the electrostatic interaction
into covalent bond [14]. It is speculated that the porous structure
makes the dielectric layer compressible and the covalent bonds

0924-4247/$ – see front matter © 2009 Elsevier B.V. All rights reserved.
doi:10.1016/j.sna.2009.02.034
 Q. Zhang et al. / Sensors and Actuators A 151 (2009) 154–158
Fig. 1. Visual effect of the invisible bend sensors fabricated on plastic transparency.
More than 10 sensors are allowed to be constructed on this area. The left is a typical
opaque commercial bend sensor.
enable it to respond quickly to cyclic flexion and relief. In other
words, the PAA/PAH multilayer performs like a thin piece of elas-
tomer. When the sensor is flat, there is hardly any conductive
electric current between two electrodes. When being bent, the soft
dielectric layer is compressed and the gap between the two elec-
trodes decreases. As a result, the flexion leads to the decreasing of
dielectric thickness and increasing of the current.
2. Finite element simulation
Simulation was performed using Abaqus software to visualize
strain among the multilayer. The dimensions are consistent with
the real device. Fig. 2 illustrates qualitatively the simulation of the
strain distribution in the sensor and most importantly the location
of the peak strain. The peak occurs at two ends of the dielec-
tric layer, as well as in the vicinity of the two shoulders of the
bottom electrode. It is found that the strain is increased as the
sensor is bent. The contours in this figure represent the minimal
in-plane principal strain field which reflects the deformation of
multilayers thin film. The seven vectors illustrated in the inset rep-
resent the magnitude and orientation of two points (illustrated
in the figure with two white dots) across the dielectric layer in
the shoulder region, which vary with the flexion of the sensor.
The top vector (the longest) corresponds to the distance between
the two points in the flat situation while the bottom vector (the
shortest) denotes the reduced distance in the most flexed situa-
tion.
3. Experimental details
3.1. Materials and equipment
The polyelectrolytes used for the self-assembly process were
PAH (aqueous solution, MW 70,000, 3 mg/mL) and PAA (aqueous
solution, MW 50,000, 3 mg/mL), both of which were obtained from
Aldrich–Sigma. The Na+ -montmorillonite nanosheet was obtained
from the clay minerals society. It was diluted to 7 mg/mL by DI
water. After sonification for 30 min, only the top layer of the clear
155
Fig. 2. The simulation result by Abaqus qualitatively illustrates the strain distribu-
tion in the dielectric layer. It shows that the dielectric layer which is sandwiched
between top and bottom electrodes is compressed when the sensor is bent. The
inset shows seven vectors rotating from top to bottom. The vectors represent both
magnitude and orientation of two points (illustrated by two white dots) across the
shoulder of the dielectric layer with the curvature of the sensor. The top vector is
the longest, representing the distance between two points in the flat position. The
bottom one is the shortest, representing the reduced dielectric thickness in the most
flexed situation.
solution was extracted for use. The plastic transparency was coated
with an ITO layer with a thickness of about 250 nm and sheet
resistivity of 8–12 /square and it was obtained from Delta Tech-
nologies. A transparent UV-curable polymer (NOA 73) used for
encapsulating the sensor was from Norland Products. The electri-
cal characterization was conducted by an HP 4156A semiconductor
parameter analyzer.
3.2. Fabrication of the sensor
The fabrication started from the ITO-coated plastic transparency
(Fig. 3a). The ITO layer was patterned to form the bottom electrode
(1 mm wide) using photolithography (Fig. 3b). The next lithogra-
phy step patterned out a 3 mm wide window on the photoresist
over the bottom electrode (Fig. 3b). Then 10 bilayers of polycation
and polyanion, PAH/PAA, were alternately adsorbed on the sur-
face using ESA assembly (Fig. 3c). In detail, the plastic substrate
was alternately dipped in each polyion solution for 10 min until 10
bilayers were achieved. Between every two dipping, an intermedi-
ate rinsing in DI water and drying by nitrogen were necessary in
order to remove weakly attached components, thus preparing the
surface for the subsequent adsorption [16]. After that, the result-
ing dense polyion film was dipped in an acidic solution (pH 2.4)
for 1 min to generate the porous structure (Fig. 3d). The sample
was further soaked in DI water for 10 h in order to shrink the
pores on the top electrode (Fig. 3e). Then, the pores were covered
by three layers of Na+ -montmorillonite nanosheet with compa-
rable size still using ESA assembly (Fig. 3f). Next, a 300 nm thick
ITO layer was sputter deposited for the top electrode (Fig. 3g).
The lift-off was implemented by dissolving photoresist, leaving
the transparent sensor structure on plastic substrate (Fig. 3h). The
sample was annealed at 180 ◦ C for 2 h to crosslink the PAH/PAA
polymer multilayer [14]. Finally, the sensor was encapsulated in
order to be isolated from the atmosphere by a thin transparent
film of polymer, NOA 73, which was cured by the irradiation of UV
light.
156 Q. Zhang et al. / Sensors and Actuators A 151 (2009) 154–158
Fig. 3. The schematic of the fabrication of the porous crosslinked film and its inte-
gration into a bend sensor. SEM images d shows porous structure of the film. Through
the holes on the top surface, polymeric fiber network in the multilayer is seen. SEM
image e shows a shrunk hole on the top surface after water treatment. Meanwhile,
the polymeric fiber network under the top surface still remains. SEM image f shows
a hole on the top surface is covered up by montmorillonite nanosheet.
3.3. Electrical characterization of the bend sensor
The electrodes were connected to a microprobe station. Two
volts was applied to the sensor and the current signals were col-
lected by a HP 4156A semiconductor parameter analyzer with a
current resolution of 1 pA. When measuring the current at a very
low level, the “long” measuring mode with the averaging function
was selected in an attempt to average out the noise.
4. Results and discussions
The simulation shows that the elastomeric dielectric layer is
compressed when the sample is bent. Moreover, the stress is not
uniformly distributed in the dielectric layer. The structural design
is a little different from a parallel plate capacitor in that the top
electrode is wider than the bottom one. Here, the top and bottom
electrodes have width of 3 and 1 mm, respectively. Therefore, the
bottom electrode is completely encapsulated by both the dielec-
tric and top electrode layer, which enables the formation of two
shoulder regions over the sidewalls of the bottom electrode. The
simulation illustrated that the highest strain occurs near two ends
of the dielectric layer and shoulders of the bottom electrode. For
example, the dielectric layer is ∼ 200 nm at the flat situation and
can be pressed down to tens of nanometers at the shoulders when
being bent. It may be these regions that are responsible for the main
reduction of the gap and the increasing of the current between two
electrodes.
The elastomeric dielectric layer is the core element of the sensor.
Its fabrication consists of five stages: (1) ESA of PAH/PAA to form
a dense polymer film, (2) porous structure (average pore diame-
ter is several to tens of microns) generation by acidic treatment,
(3) reduction of the hole size to less than 1 ␮m on the top elec-
trode, (4) seal up the top electrode by ESA of montmorillonite
nanosheet, and (5) crosslink of the polymer film by annealing. In
the first stage, a dense 10 bilayers of PAA/PAH film was deposited
by the ESA which made use of the alternate adsorption of oppositely
charged supramolecular species (Fig. 3c). Because PAA and PAH
carry different sign of charge, they were alternately adsorbed onto
the substrate by electrostatic attraction. At this point, the thickness
of the multilayer was ∼ 200 nm. In the second stage, the film was
dipped into a strong acidic solution, resulting in a porous structure.
SEM image of Fig. 3d shows typical holes that were open on the
surface film. Through the holes, a polymeric fiber network could be
seen. We speculate that the fiber network contributes to the com-
pressible property of the film. The film thickness was measured to
be ∼ 600 nm. The porous structure is a result of the acidic treatment
which may break the interaction among polymeric molecules and
be followed by a series of swelling and reorganization of the film
[17]. At this point, the holes on the top surface are several microns
to tens of microns wide. Obviously, this film is not suitable for the
electrode because ITO will drop into the holes and lead to short. The
solution is to use the montmorillonite nanosheet to cover up the
holes. The montmorillonite usually bears a natural negative charge
because of the isomorphous substitution of silicon in octahedral
sheets [18]. As a result, it can be alternately adsorbed with poly-
cation. Moreover, the high lateral aspect ratio renders it suitable
for construction of ultrathin ceramic films [18]. It is usually 1 nm
thick and several microns wide. However, it is not big enough to
cover the wide holes on the multilayer surface. Therefore, the sam-
ple was soaked in water for 10 h in the third stage during which the
holes were shrunk to less than 1 ␮m wide. Fig. 3e illustrates the SEM
image of a typical hole on the surface after water treatment. Mean-
while, the film thickness was reduced to ∼ 200 nm. It is important
to notice that the porous polymer fiber network still remains the
same after the water treatment. The fourth stage includes the ESA
of three bilayers of PAH/ montmorillonite nanosheet on the multi-
layer surface. At the end of this stage, the “leaking” film was sealed
up and became suitable for ITO deposition. Fig. 3f shows a hole on
the top electrode that was covered by the nanosheet. The thickness
increased by about 9 nm because of the nanosheet deposition. It
was found that the resulting film could respond to flexion with the
increasing of current owing to the porous structure. However, once
the flexed sensor returned to flat position, the current did not come
back to original value immediately. On the contrary, it usually took
at least 30 min to gradually come down. This slow cyclic response
may be attributed to the relatively weak electrostatic interaction
among the polymer molecules. Once the microscopic structure of
Fig. 4. The current between two electrodes as a function of the curvature of the
sensor. The testing voltage is 2 V.
 Q. Zhang et al. / Sensors and Actuators A 151 (2009) 154–158
Fig. 5. (a) IV curves under various flexion loads. (b) Three fitting parameters, R, D × E and P, derived from fitting the curves as a function of curvature. The fitting is based on
the model combining Fowler–Nordheim tunneling and ionic currents.
the multilayer was deformed, it took time to recover. The enhanced
cyclic response by crosslinking the film corroborated this hypothe-
sis to some degree. In the fifth stage, the film was annealed at 180 ◦ C
for 2 h to turn the electrostatic interaction into covalent bond [14].
The subsequent electrical characterization of the sensor showed a
fast current switch between the flat and most flexed position with
little time delay.
During the electrical characterization, two volts was found to be
an appropriate test voltage and applied across the two electrodes.
As shown in Fig. 4, the current increased as the sensor was bent. It
is noted that when the sensor was not bent, the current was close to
zero (at the pA level), indicating a low power-consuming device at
idle situation. The data shows that the current increasing becomes
sharp after certain curvature which is consistent with the simula-
tion result that the dielectric layer can be seriously deformed at the
shoulder of the bottom electrode if the flexion becomes large. Other
voltage levels had been tested and the similar IV trend was demon-
strated. However, the voltage level higher than 10 V was observed to
be detrimental to the structure and reduce the life time of effective
operation.
The conducting mechanism is not clear. Early reports point
out two possible mechanisms that govern the electric conduction
through the polyelectrolyte thin films produced by electrostatic
self-assembly and other approaches – the Fowler–Nordheim tun-
neling and ionic conduction [19–25]. We speculate that the charge
transport in this sensor is also a combination of tunneling and ionic
conduction. First, at such length scale, the Fowler–Nordheim tun-
neling current (I) is likely to play an important role, and is governed
by the dielectric thickness (D).
I(tunneling) = P exp(−D × E/v)
where P is proportional to v2 , E is the critical field for activated
tunneling, and v is the applied voltage [15]. Secondly, the ionic cur-
rent is a result of migration of mobile ions such as H+ , Na+ and
Cl− in the polyelectrolyte film [23–25]. They could be introduced
into the film from the salted bath solution or they remain in the
film because of a low ionization degree of polyelectrolytes in the
solution [26–28]. The resistivity is the function of mobile ion den-
sity and film thickness. Current resulted from short is not likely
because the sensor appears to be able to withstand a number of
flexion and relief cycles without degradation. In addition, the elec-
trical corrosion of the electrodes due to the high short current is not
observed. Three sets of current data as the function of voltage under
different flexion load are shown in Fig. 5a. After the turning point
at ∼1 V, the tunneling component with the exponential increase
becomes dominant over the ionic one with the linear increase. The
nonlinear IV curves are fit over the whole range of flexion load by
the model combining tunneling and ionic current. In Fig. 5b, three
157
fitting parameters, R (the ohmic resistance of ionic conduction),
D × E and P, show their consistency with the model as the flexion
load increases. R is derived from the slope of the straight line (not
shown) before the exponential increase of the IV curve. It decreases
with curvature, indicating the compression of the porous polyelec-
trolyte film when being bent. The estimated resistivity is at the
level of 0.5 × 108  m, which falls into the range of reported self-
assembled polyelectrolyte film at ambient humidity [19]. The value
of D × E from the fit also decreases with the flexion. This shows
the reduction of film thickness caused by bending, which is also
observed from the value of R. P is proportional to the density of the
charge carrier at fixed V. The value of P from the fit increases with
the bending, implying the increasing of available charge carriers
when the film is bent.
The multiple experiments demonstrated the function of the
montmorillonite nanosheets. Without them, the sensor was quite
likely to short between the two electrodes. After coating three
layers of nanosheet, the short was eliminated and this could with-
stand repetitive flexion. The experimental results, combined with
the SEM observation, make us believe that the montmorillonite
nanosheets can seal up the porous elastomeric dielectric layer. It
should be noted that such a bend sensor is somewhat like a unipolar
one, i.e., it can more effectively detect the deflection in the down-
ward direction that is shown in Fig. 2 than the other. If the sensor
is bent in other (upward) direction, the current variation is not as
obvious as the correct direction.
At last, the sensor was encapsulated by one thin layer of trans-
parent polymer film (NOA 73) which was cured by the UV light
illumination. The purpose is to isolate the sensor from the atmo-
sphere and prevent the gas influence to the sensor. Another function
of the encapsulation layer is to enhance the sensitivity of the sensor.
It was speculated that the NOA 73 with a higher modulus than the
dielectric layer enhances the push-up effect towards the dielectric
layer. The data shown in Fig. 4 was obtained with the encapsulation
on the sensor.
Such a sensor has an optical transparency of above 85%.
5. Conclusions
In conclusion, a porous polymer film is integrated into an invis-
ible bend sensor. The sensor occupies a relatively small area and
consumes little power at idle situation. The porous film sandwiched
between two electrodes undergoes deformation when being bent,
resulting in an increase of the current. Since the conductive current
of the film when the sensor is flat is negligibly small, the apparent
current increase is likely to be a result of tunneling effect. The film
can be thermally crosslinked and is capable of responding to cyclic
flexion. The montmorillonite nanosheet is a good material to seal
158 Q. Zhang et al. / Sensors and Actuators A 151 (2009) 154–158
up the porous film so that ITO electrode can be deposited on the
surface. The see-through structure adds beneficial features to the
sensor and allows for special applications.
Acknowledgements
A portion of the research described in this paper is performed
in the Environmental Molecular Sciences Laboratory, a national sci-
entific user facility sponsored by the Department of Energy’s Office
of Biological and Environmental Research and located at Pacific
Northwest National Laboratory.
The authors would like to thank the National Center for
Supercomputing Applications at the University of Illinois at Urbana-
Champaign for providing computational and software resources
and support.
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Biographies
Q. Zhang was born in China, on July 1977. She received her BS and MS in Elec-
trical Engineering from Harbin Institute of Technology, China, and University of
Twente, the Netherlands, in 1999 and 2005, respectively. Currently, she is pursu-
ing the PhD degree in the department of Electrical and Computer Engineering at
Clarkson University, New York, U.S.A. Her research effort is focused on the develop-
ment of invisible devices and circuits using different nanomanufacturing techniques
such as molecular self-assembly, nanomolding and transfer printing.
J.R. Smith was born in Vernon, Vermont on May 30, 1987. He is still attending
Clarkson University and will achieve his BS in Electrical Engineering in May 2009.
P. Jha was born in Bangalore, India on February 6th 1990. Currently he is pursuing a
BS in electrical engineering from Clarkson University.
F. Hua received the PhD degree in Engineering from Louisiana Tech University in
2003. He is currently an assistant professor of the department of Electrical & Com-
puter Engineering at Clarkson University in New York, U.S.A. His research interest
includes the design and fabrication of flexible and transparent electronic devices.