Sensors and Actuators B 117 (2006) 17–26

Hydrogel-based piezoresistive pH sensors: Design,

simulation and output characteristics
Quang Thong Trinh a , Gerald Gerlach a,∗ , Joerg Sorber a , Karl-Friedrich Arndt b
a Institute for Solid-State Electronics, Dresden University of Technology, Helmholtzstr. 18, 01062 Dresden, Germany
b Institute of Physical Chemistry and Electrochemistry, Dresden University of Technology, Helmholtzstr. 18, 01062 Dresden, Germany
Received 12 July 2005; accepted 28 October 2005
Available online 13 December 2005

Abstract
The paper summarizes a detailed design study of silicon piezoresistive pH sensors, whose operation relies on the pH sensitive swelling of a
polymer hydrogel. It is based on an analytical model of the hyperelastic–viscous behaviour of hydrogel. The pH sensor behaviour was investigated
by simulating and measuring the silicon membrane deflection and the stress inside the membrane. Simulation was performed using finite element
method (ANSYS). A technology to manufacture such hydrogel-based sensors was developed. We found satisfying agreement between simulation
and measured results for the sensor output characteristics.
© 2005 Elsevier B.V. All rights reserved.

Keywords: Piezoresistive sensor; pH sensitive hydrogel; pH sensor; FEM

1. Introduction influence of the hydrogel films’ preparation conditions on sensi-

Hydrogel-based pH sensors using mechano-electrical trans-
ducers have been developed for many years. The general sensor
principle is as follows: swelling due to pH value changes causes a
flexible plate bending. In case of capacitive transducers a change
in capacitance will be detected. For resistance bridge sensors,
due to membrane deflection, the corresponding membrane stress
will change the bridge resistance and consequently the output
voltage (Fig. 1).
Several studies of the development of such sensors have been
carried out. Han et al. [1] designed and fabricated a miniature
biosensor for glucose concentration measurement in blood using
the combination of a pressure transducer and a pH glucose gel.
Herber et al. [2,3] also developed a hydrogel biosensor for mon-
itoring carbon dioxide pressure in the stomach of the human
body connecting it to a silicon piezoresistive pressure transducer.
However, these studies have just focused on the use of pH sensi-
tive gels for concrete applications but not delved into the aspects
of material modelling techniques needed for the design and opti-
mization of devices. Our previous research was focused on the
∗ Corresponding author. Tel.: +49 351 463 32077; fax: +49 351 463 32320.
E-mail address: gerlach@ife.et.tu-dresden.de (G. Gerlach).
tivity and response time of such chemical and pH sensors [4–6].
However, a detailed investigation of the polymer gel behaviour
is crucial to establish reliable models for predicting the device
characteristics.
In this paper, a hyperelastic material model based on
Mooney–Rivlin’s approach has been applied for polymer hydro-
gels to simulate the pH sensor behaviour by finite element
method using ANSYS. An appropriate FE model was devel-
oped to predict and optimize the sensor design. In order to
affirm this material model, uniaxial tension tests of PVA–PAA
hydrogel have been performed. The sensor output characteris-
tics, such as sensor membrane deflections, output voltage and
sensor response time, were measured and compared to simula-
tion results.
2. Mechanical behaviour of polymer hydrogels
2.1. Material characterization
Polymer gels include a polymer network and interstitial solu-
tions. The network of polymer molecules holds the liquid in
place and so gives the gel its rigidity. Gels are wet and soft
and look like a solid material, but are capable of undergo-
ing large deformations. This is in contrast with most industrial

0925-4005/$ – see front matter © 2005 Elsevier B.V. All rights reserved.
doi:10.1016/j.snb.2005.10.041
18 Q. Thong Trinh et al. / Sensors and Actuators B 117 (2006) 17–26

Fig. 1. General operational principle of hydrogel-based piezoresistive pH sensors:
V volume change, σ silicon membrane stress,
R/R relative resistance change,
Uout output voltage.

materials, such as metals, ceramics and plastics, which are dry
and hard. To describe the polymer gels’ elastic behaviour, free
swelling experiments were performed to determine gel swelling
and deswelling, respectively, in the pH range of 1–12. The mea-
sured hydrogel strain is a function of pH value and varying from
some percentages at low pH levels to 34% at pH 11 [7]. The
results of this investigation showed that hydogel strains are large
and recoverable. The hydrogel strain versus pH value relation
was used for simulating the sensor properties.
Furthermore, the stress–strain characteristic of gels resulting
from a uniaxial extension test was determined by applying step-
wise increasing forces and by detecting the related strains, up to
a strain of 250%. The gel samples were prepared by deposition of
PVA/PAA solution. Then the dry film was peeled-off and cut into
strips. Since the experiment is not intended to fail the specimen,
there is no need to use dogbone- or dumbbell-shaped specimen.
The strip-shaped dry gel samples were isothermally annealed in
an oven at 130 ◦ C for 20 min before being soaked in deionized
water and then preserved in pH 1 solution. The undeformed gel
sample geometry was set to a ratio between length and width of
10:1 in order to ensure uniaxial stress conditions. The relation-
ship between stresses (force per unit unstrained cross-section)
and strains (percentage variation in the sample length) is shown
in Fig. 2. It presents the typical non-linear behaviour of rubber-
like materials [8].
often adequate for predicting its mechanical response. For hyper-
elasticity, mechanical properties are characterized by a strain
energy function, which is a scalar function of either a strain or
a deformation tensor [8]. The strain energy describes the work
stored in the body:
W = W(λ1 , λ2 , λ3 ), (1)
where λ1 ,λ2 ,λ3 are principal stretch ratios, λi = Li /L0i (i = 1, 2,
3), where Li and L0i are actual and initial lengths, respectively.
The energy function is determined by the thermodynamics
theory as follows [8]:
1
W= NkT (λ21 + λ22 + λ23 − 3) (2)
2
where N is the number of chains per unit volume in the network,
k the Boltzmann constant and T is the absolute temperature. The
quantity NkT is equivalent to the shear modulus of the hydorgel
material.
In case of large strains, the thermodynamic equation of state is
less satisfactory and a phenomenological approach is used. This
treatment does not consider the gel’s molecular structure but
uses the observed macroscopic behaviour of the system [9,10].
Using the theory of continuum mechanics, the strain energy
function for an isotropic material is in the following form [11]:

2.2. Material model of polymer hydrogel
The development of an appropriate material model of poly-
mer hydrogel materials has been an active research area for many
years. Very recently, a number of constitutive models have been
developed addressing different experimental observations. Tak-
ing the large volume change in account, hyperelastic models are
W = C1 (I1 − 3) + C2 (I2 − 3)
= C1 (λ21 + λ22 + λ23 − 3) + C2 (λ21 λ22 + λ21 λ23 + λ22 λ23 − 3)
(3)
where I1 and I2 are the first and second strain invariants. C1 and
C2 are the material constants having dimensions of MPa.
If the material is assumed incompressible, I2 can be rewritten
as:

I2 = λ21 λ22 + λ21 λ23 + λ22 λ23 = λ−2 −2 −2

1 + λ2 + λ3 .

In case of uniaxial deformation, the stretch ratios can be

expressed as:

λ1 = λ and λ2 = λ3 = λ−1/2 .

Then, the derivative of strain energy function with respect to

a strain component determines Cauchy stress (force per unit
unstrained area):



1 1
T1 = 2 λ − 2 C1 + C2 . (4)
λ λ
Eq. (4) is called the Mooney–Rivlin’s equation.
For polymer hydrogels, when combining the uniaxial
Fig. 2. Stress vs. strain characteristic of PVA–PAA hydrogel in pH 1 solution. mechanical extension with volume change due to actuation by
 Q. Thong Trinh et al. / Sensors and Actuators B 117 (2006) 17–26 19

chemical stimuli, the Cauchy stress can be expressed as [12]:



1 1
T1 = 2 λ − 2 Λ−1 C1 + ΛC2 , (5)
λ λ
where Λ is the swelling ratio of polymer hydrogel, i.e., the size
ratio between swollen and fully contracted states. Eq. (5) is
called the modified Mooney–Rivlin’s equation.
For an acidic gel like poly(vinyl alcohol)–poly(acrylic acid)
(PVA–PAA), it will fully contract in acidic solutions, i.e., at low
pH values like pH 1, and fully expand in base solutions, i.e., at
high pH values [13]. In this work, the starting state of polymer
gels used for pH sensors is in the fully contracted state since the
gel is preserved in pH 1 solution. Therefore, Λ = 1, and Eq. (5)
again becomes Eq. (4).

3. Sensor model and finite element simulation Fig. 4. Finite element model of the pH sensor: (1) silicon chip, (2) hydrogel
layer, (3) silicon rigid mesh and (4) channel for solution entering.
3.1. pH sensor design
swelling acts only on the silicon diaphragm. This makes the gel
In this work, a novel pH sensor design was used (Fig. 3). A
deformations similar to the uniaxial extension test.
thin layer of PVA–PAA hydrogel is placed in the cavity of a
The Cauchy stress following Eq. (5) developed due to gel
piezoresistive transducer (silicon chip) between the upper sil-
swelling is similar to the pressure acting on the plate of silicon
icon diaphragm and a lower silicon rigid mesh as shown in
piezoresistive pressure sensor chips leading to their bend and
Fig. 3. The solution itself enters the gel through the mesh chan-
causing the stresses inside. The output voltage can be determined
nels without means of a pump like in our previous designs
[4–6].
Since kinetics of gel swelling is a function of both gel dimen-
sion and diffusion coefficient, the response time is proportional
to the square of its dimension [14]. Therefore, in order to
decrease the reaction time constant, the gel dimension was cho-
sen to be smaller than that of the silicon diaphragm. Because of
the gel is fixed in the hard square frame, the force exerted by gel

Fig. 3. pH sensor design: (1) silicon chip, (2) piezoresistors, (3) silicon mem-
brane, (4) hydrogel layer and (5) silicon rigid mesh. Fig. 5. Process scheme for fabricating silicon rigid mesh.
20 Q. Thong Trinh et al. / Sensors and Actuators B 117 (2006) 17–26
as [15]:
1 1
Uout = − Ucc (πl − πt )(σl − σt ) = − Ucc (πl − πt )σSi,Res
2 2
(6)
where Ucc is the applied voltage, σ l and σ t the longitudinal and
transverse stress, respectively, and πl and πt are the piezoresis-
tive coefficients. In case of (1 0 0) silicon having resistors aligned
along the 1 1 0 directions, the piezoresistive term amounts to
(πl − πt ) = 138.1 × 10−11 Pa−1 .
3.2. Finite element simulation
Finite element modelling and simulation was performed
using the commercial software package ANSYS, which offers
a built-in hyperelastic material and geometric modelling capa-
Fig. 6. Photo of the fabricated silicon mesh: (a) bottom view (unpolished side),
(b) top view (polished side).
bility [11]. Only a quarter of the model is considered due to
sensor symmetry. The SOLID45 element is used to model the
silicon chip and the silicon rigid mesh, the HYPER58 one is used
for the hydrogel piece. The CONTACT49 element is applied to
maintain the model continuity and presents the force caused by
hydrogel swelling to the silicon diaphragm.
In order to model the chemically caused hydrogel swelling,
we have used its analogy to thermal extension. Equivalent strain
due to swelling is determined by free swelling experiments as
described above [7]. According to this assumption, we easily
use the thermal expansion term offered by ANSYS to simulate
the swelling phenomenon. The viscous behaviour of polymer
gels was neglected in this study since the focus was brought to
the static behaviour. The FE sensor model used for simulation
is shown in Fig. 4.
4. Sensor fabrication
4.1. Gel preparation
Gel has been produced by deposition of PVA/PAA polymer
solution. Dry polymer films were peeled off and cut into small
Fig. 7. Photo of the assembled piezoresistive pH sensor.
Fig. 8. Cross-section of a completed hydrogel-based pH sensor: (1) silicon chip,
(2) hydogel layer, (3) silicon rigid mesh, (4) channels, (5) socket, (6) bonded
wires and (7) socket pins.
 Q. Thong Trinh et al. / Sensors and Actuators B 117 (2006) 17–26 21

Fig. 9. Hyperelastic material curve fitted by ANSYS.

square slabs before being baked in an oven at 130 ◦ C for 20 min.

The thermally treated PVA/PAA slabs were soaked in deionized
water to get initial equilibrium swelling state and subsequently
in buffered pH 1 solution to reach the least swollen state.

4.2. Rigid mesh fabrication

In this work, the rigid meshes have been made by micro-

machining technique. They were fabricated using a 3 in. n-type
1 0 0-oriented and 320 ␮m thick single-polished silicon wafer.
First, the wafer was wet oxidized for 8 h to grow a 1.5 ␮m thick
SiO2 layer. The oxide was patterned on both sides of the wafer by
photolithography to create etch-masks for holes. Subsequently,
the wafer was immersed in 30% KOH solution for etching chan-
nels from both sides. The last step was dicing of the wafer
resulting in the rigid meshes with outer dimensions correspond-
ing to those of the silicon chip cavity. The fabrication sequence
of silicon meshes is shown in Fig. 5, and a photograph of the
manufactured mesh in Fig. 6.

4.3. Sensor assembly

In this process, the 40 ␮m thick gel was placed inside

the cavity of a commercial pressure sensor chip (AE series,
AktivSensor, Stahnsdorf, Germany). Membrane dimensions are
3 mm × 3 mm with a thickness of 20 ␮m. In order to complete
the sensor, the rigid mesh made by silicon micromachining tech-
nique was bonded to the chip using two-component epoxy. A
photograph of the assembled sensor is shown in Fig. 7 and the
cross-section of the completed device is illustrated in Fig. 8.

4.4. Experimental model validation

First, the sensor diaphragm deflection was measured using Fig. 10. Finite element simulation: (a) membrane deformation and (b) contour
nanofocus microscan method (NMS). For this measurement, pH plot of membrane stress.
22 Q. Thong Trinh et al. / Sensors and Actuators B 117 (2006) 17–26

solutions were poured into and drawn out of the sensor succes-
sively.
For the measurement of the sensor output voltage, which is
the main parameter of such piezoresistive pH sensors, a supply
voltage of 5 V is applied to the sensor. The output voltage is
displayed on a multimeter and the measurement data is acquired
by computer. These measurements have been described in details
in Ref. [16].
presented in Fig. 9 shows that the mechanical behaviour of
PVA–PAA gels was corresponding to hyperelastic material prop-
erties. Hence, the physical values of the constants C1 and C2
in Eqs. (3)–(5) were automatically determined. For the fully
contracted gel (preserved in pH 1 solution), the calculated
parameters are C1 = 0.15 MPa and C2 = 0.06 MPa. The mate-
rial parameters C1 and C2 are related to the shear modulus,
G:

5. Results and discussion
5.1. Material parameter determination
The results of uniaxial extensional test were used to verify
the material model characterizing the mechanical behaviour of
PVA–PAA hydrogels. Using available ANSYS codes (TBFT
command), a fitting program was performed. The fitting result
G = 2(C1 + C2 )
In our work, G gets the value of 0.42 MPa, which is in relatively
good agreement with reported results in Ref. [12]. Calculations
performed with these values for C1 and C2 delivered the same
results. The comparison with Marra et al. [12] shows that our
gels are a slightly softer because the hydrogels here were not pro-
cessed in the same way regarding polymerization temperature
and time.

Fig. 11. Results of finite element analysis: (a) membrane deflection profile and (b) membrane longitudinal and transverse stress profile.
 Q. Thong Trinh et al. / Sensors and Actuators B 117 (2006) 17–26 23

5.2. Simulation results
Determination of deformation and stress distribution inside
the bending plate are main objectives for the static structural
analysis by FEM. Fig. 10 shows the contour plots for membrane
deformation and stress. The maximum strain case amounts to
34%, which is given for pH 11. The in-plane stresses in the two
main directions within the silicon plate were found to be exactly
equal to each other due to the symmetry involved in the problem.
Concretized calculations are presented by profiles shown in
Fig. 11. The maximal deflection was calculated as 15.1 ␮m at
the membrane center (Fig. 10a). Fig. 10b shows the membrane’s
longitudinal and transverse stresses. It can be seen that the lon-
gitudinal stress gradient is higher than the transverse one. The
maximum stresses, corresponding to the hydrogel’s maximum
strain, are two orders of magnitude less than the maximum ten-
sile strength of silicon (σ yield = 7 GPa) [17]. Thus, it gives proof
that the pH sensor can operate safely in the pH range 1–11. Based
on the membrane stress calcualtions, the sensor output voltage
can be predicted using Eq. (6).
5.3. Measurement results
Nanofocus microscan measurements were used to determine
membrane deformations profiles (Fig. 12). These results demon-
strate that the sensor, namely the silicon membrane, exhibits

Fig. 12. Nanofocus microscan measurement: (a) 3D image of membrane bending and (b) membrane deflection profile.
24 Q. Thong Trinh et al. / Sensors and Actuators B 117 (2006) 17–26

Fig. 13. Long-term sensor output voltage behaviour.

good response due to PVA–PAA gel swelling. For the case of sociation constant pKa of PAA. The sensitivity value of this novel
pH 11, the measured value was about 14.3 ␮m. pH sensor is twice of those in our previous studies [4–6].
Due to the plate bending and hence stresses developed in it, The sensor response time is illustrated in Fig. 15a for pH 5.5
the changes in the sensor output voltage in accordance with pH and 11 solutions (measurements started at pH 1). It is probable
were detected. The measured long-term behaviour of the sen- that the much larger amount of hydroxyl groups at high pH
sor output voltages in pH range from 1 to 12 and vice versa values leads to the stronger and faster ionization process and
is shown in Fig. 13. In this measurement, the pH 1 solution results in the faster response time at pH 11.
was used as reference. The sensor output voltage shows a repro-
ducible response to pH value changes. Increase and following
decrease of pH causes a slight hysteresis. With increasing pH,
the ionization degree is going up and hence the output voltage
increases. However, as the pH further increases, the gel swelling
tends to decrease due to the osmotic pressure difference of free
ions inside and outside decreases. As a result, when the pH value
exceeds 11, the effect of ionic strength surpassed the effect of
the electrostatic repulsion between the polycarboxylate groups
making the gel deswelling and consequently leading to the lower
output voltage at pH 12 [13].

5.4. Comparison between simulation and measurement

Fig. 14 shows the comparison between calculated and mea-

sured results for membrane deflection and output voltage in the
range of pH value from 4 to 11. As can be seen from this figure,
the measured results appeared to be well-suited for the calcula-
tions. There is a leap between pH 4 and 5 in these graphs because
transition occurs here when pH value rises above the dissociation
constant pKa of PAA (pKa = 4.7). That means that the ionization
process of polycarboxylic groups within the polymer network
happens and creates the electrostatic repulsion force leading to a
significant increase of swelling. In our case, the polycarboxylic
groups were fully ionized at pH 11. That means that the gel gets
the maximum expansion here.

5.5. Sensor sensitivity and response time

Sensitivity and response time are main criteria of a sensor.

As can be seen from the long-term output voltage, the sensor Fig. 14. Comparison of calculated and measured results: (a) membrane deflec-
sensitivity was about 30 mV/pH in the pH range above the dis- tions vs. pH value and (b) sensor output voltage vs. pH value.
 Q. Thong Trinh et al. / Sensors and Actuators B 117 (2006) 17–26
Fig. 15. Time dependent sensor output voltage: (a) measurement and (b) finite
element calculation.
Because of the rate-limiting of diffusion processes, the
mechanical readjustments of gel depend on the pH range. As
a result, the response time at pH 5.5 is longer than at pH
11.
The calculated results are compared with the measured data
in Fig. 15b. The deformation time history measured by free
swelling experiments represents the input of finite element
analysis and the output voltage needed to realize this deforma-
tion history is output of the calculation. It can be seen that for
both cases the measured response time is evaluated about four
times longer than the calculated one. Possibly, this difference is
caused by the fact that the time constants used for calculations
were determined using free-swelling experiments. It should
be reminded that in these experiments the gel was immersed
alone into the solution. Hence, both the diffusion process and
the response could take place more quickly. In addition, the gel
extension was assumed happening instantaneously. However,
when placed in the silicon chip cavity, the penetration of
solution ions into the polymer network is much more difficult,
therefore resulting in the longer response time. Due to the
reasons mentioned in Section 3.1, the sensor response time can
be improved by using thinner hydrogel layers. However, it must
correlate to the silicon membrane thickness for sufficiently good
sensitivity.
25
6. Conclusions
The output characteristics of the silicon piezoresistive pH
sensors has been evaluated. The sensor operational prin-
ciple relies on the pH sensitive swelling of poly(vinyl
alcohol)–poly(acrylic acid) hydrogel. The sensor behaviour was
simulated by finite element method (ANSYS). Free swelling
experiments and mechanical tests of PVA–PAA hydrogel have
been carried out in order to prove the simulation results. It
was shown that the hydrogel exhibits hyperelastic property.
A fabrication technology for such pH sensors was proposed
using micromachining technology. The main sensor character-
istics, such as silicon membrane deflection, output voltage and
response time have been computed and measured. A relatively
good agreement was found in comparing static simulations and
experimental results.
Acknowledgements
This work was supported by German Research Council
(DFG) as project C11 of SFB 287. The authors also would like
to thank Dipl.-Ing. Marco Luniak of the Electronics Packag-
ing Laboratory (IAVT) for performing the nanofocus microscan
measurements and Dr.-Ing. Thomas Pusch and Ms. Marion Stohr
of the Textile and Clothing Institute (ITB) for performing the
uniaxial extension measurements.
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Biographies
Quang Thong Trinh received the BS degree in physics from Hanoi Uni-
versity in 1984 and the MSc degree in materials science from International
Trainning Institute for Materials Science (ITIMS) in 1999. He is currently
working towards the PhD degree in electronics engineering at the Institute
for Solid-State Electronics, Dresden University of Technology. His current
interests include technology development for applications of piezoresistive
sensors, design development by simulation and modelling of MEMS.
Gerald Gerlach received MSc and PhD degrees in electrical engineering
from Dresden University of Technology in 1983 and 1987, respectively. He
worked in research and development in the field of sensors and measuring
devices and sensors at several companies. In 1993, he became a profes-
sor at the Department of Electrical Engineering at Dresden University of
Technology. Since 1996 he has been the head of the Institute for Solid-State
Electronics. His research is focused on sensor and semiconductor technology,
simulation and modelling of micromechanical devices and the development
of solid-state sensors, especially pyroelectric infrared sensors and piezore-
sistive humidity and gas sensors. From 1994 to 2000 Prof. Gerlach served
as Deputy Dean and Dean of the Electrical Engineering Department at TU
Dresden, respectively. Since 2000 he has been vice president of the German
Society for Measurement and Automation Technology (GMA) and since 2002
member of the Presidency of the VDE (German Association of Engineers in
Electrical Engineering, Electronics, Information Technology).
Joerg Sorber received his PhD degree in electrical engineering from Dres-
den University of Technology, Germany, in 1983. From 1978 to 1995 he
worked in the field of advanced driving systems at the Institute for Preci-
sion Engineering at TUD. Since 1996 he has been Senior Scientist at the
Institute for Solid-State Electronics at TUD. His current research interests is
focused on the design of sensors and sensor systems including the simulation
of their components as well as of complex systems, applications of sensitive
hydrogels in chemical and pH sensors.
Karl-Friedrich Arndt studied physics at Dresden University of Technology.
In 1975, he got the PhD and in 1982 the Dr.rer.nat.habil degree at Technische
Hocschule Merseburg. In 1990, he became full professor of physical chem-
istry of polymers at TU Dresden. The main focus of his work is synthesis
and characterization of soluble polymers and polymer networks with sensor
and actuator properties.