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J. Phys. D: Appl. Phys. 33 (2000) 12391243.

Printed in the UK

PII: S0022-3727(00)07200-4

Experimental study of dielectric


constant influence on
electrorheological effect
Y C Lan, S Q Men, X Y Xu and K Q Lu
Institute of Physics and Centre for Condensed Matter Physics, Chinese Academy of Sciences,
Beijing 100080, Peoples Republic of China
E-mail: yclan@aphy.iphy.ac.cn
Received 26 August 1999, in final form 28 January 2000
Abstract. A TGS ((NH2 CH2 COOH)3 H2 SO4 )/silicone oil suspension, which is the
simplest system, is employed to investigate the complex permittivity dependence of the
electrorheological (ER) effect under ac electric fields. By measuring the temperature
dependence of the shear stress across the Curie temperature of TGS particles, the dependence
of the ER effect on dielectric constant has been reliably obtained under ac fields. Under
high-frequency fields in which range the dielectric mismatch dominates, the shear stress
increases with the particle dielectric constant. The experimental data are in agreement
qualitatively with the previous mismatch models although deviation appears. The shear stress
of the ER fluid was also measured at intermediate frequencies.

liquid, respectively. Equation (2) can be reduced to [6, 9]

1. Introduction

An electrorheological (ER) fluid consists of finite-conductive


dielectric particles in a relative insulating liquid. When an
electric field is applied, the viscosity and the shear stress of
the ER fluid increase dramatically [1, 2]. The phenomena
and the physical mechanism have attracted considerable
attention. Up until now, theoretical studies have predicted
that the field-induced polarization, either originating from the
dielectric mismatch between the particles and the suspending
fluid under high-frequency electric fields or coming from the
conductivity mismatch under dc or low-frequency electric
fields, is responsible for the abrupt increase of the shear stress
of ER fluids [35]. The induced shear stress is usually
proportional to the square of the induced dipole moment pm
of the particles [68].
2
= |40 f R 3 Eloc |2
pm

(1)

where R is the radius of the particles and Eloc the local electric
field. | |2 can usually be expressed as follows:


 p () f () 2
2


| | = 
p () + 2f () 
=

(p f )2 + 0 2 (p f )2
.
(p + 2f )2 + 0 2 (p + 2f )2

(2)

Here is the mismatch factor, () = 0 i/ is the


complex permittivity, is the relative dielectric constant,
is the conductivity, = 2f is the annular frequency of the
applied electric field (f is the frequency of the electric field)
and the subscript p and f refer to the particles and insulating
0022-3727/00/101239+05$30.00

2000 IOP Publishing Ltd

|h | =
|l | =

p f
p + 2f

p f
1
=
p + 2f
+2

(high frequency)

(3)

(dc or low frequency)

(4)
where  = p /f is the ratio of particle-to-fluid
conductivity.
From experiments, it has been proved that the induced
shear stress of ER fluids is related to the size of the particles
[6, 10], the frequency of the applied electric fields [2, 11],
the electric strength E, as well as to the dielectric constant
and conductivity of the particles and insulating oil [12, 13],
as represented by equations (1) and (2). Additionally,
the interface properties between the particles and the oil
also influence the ER effects [14, 15]. In real ER fluids,
the above-mentioned factors are always interactional. For
example, dielectric constant of particles always changes with
electric strength and frequency in ferroelectrics [16], and the
conductivity of silicone oil increases nonlinearly with electric
field strength [17]. Thus, to investigate the particle dielectric
constant effect is very difficult because of the complexity
of these factors and the lack of a simple system. Up until
now, the reported permittivity dependence of ER effects are
inconsistent because many factors influence the ER effect
simultaneously.
In this paper, a simple system is constructed, which can
be used to investigate the influence of the particle dielectric
constant on the ER effect under high-frequency fields. In
the system and under certain conditions, all the parameters
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Y C Lan et al

except the dielectric constant of particles can be ignored or


cancelled. Therefore, the influence of the dielectric constant
on the ER effect can be obtained reliably.
2. Experimental details

The ER fluid studied is composed of ferroelectric singlecrystal TGS ((NH2 CH2 COOH)3 H2 SO4 ) particles (30 m
in diameter) dispersed in silicone oil with a volume fraction
of 25%. TGS single crystal was ground, meshed between
25 m and 35 m sieves and then heated to remove water.
The shape of the particles was irregular. The silicone oil was
boiled at about 300 C before being mixed with particles in
order to remove moisture.
A modified rheometer with an oil bath was employed
to perform the measurement of rheological properties under
electric fields at different temperatures. The precision
of temperature was controlled to better than 0.2 C. The
shear stress of the ER fluid was measured under different
equilibrium conditions.
The dielectric constants of TGS and silicone oil were
measured with a HP4192A impedance analyser at different
frequencies in the temperature range 2080 0.2 C.
In the experiments only one kind of solid particle,
TGS single crystal particles, and one kind of suspending
fluid, silicone oil, were employed. Under the controlled
experimental conditions, the system is the simplest one to
investigate the permittivity effect of particles from which
reliable data with better resolution can be obtained. The
detailed reasons are given below.

Figure 1. Dielectric constant of TGS versus temperature at


different frequencies.

, 100 Hz; , 1000 Hz; , 4000 Hz. The


full curve is the fitting curve of the dielectric constant along the
b-axis, the dashed and dotted lines those along the a-axis and
c-axis respectively.

3. Results and discussions

3.1. Permittivity properties of TGS and silicone oil


Figure 1 shows the dielectric constants of TGS single
crystal versus temperature (T ) at different frequencies with
1 V mm1 . The dielectric constant of TGS along the
ferroelectric direction (b-axis) shows a dramatic change and
those along other directions are relatively independent of
temperature in the tested range. The average dielectric
constant of TGS, calculated by [18]
p = b + (1 )

a + b + c
3

(5)

is plotted in figure 2 after taking the orientation of particles


into account, where p is the average dielectric constant
of particles, is the preferred orientation degree, a, b,
c refer to three crystal axes of the particles and b is the
polarization axis (direction of the particle chains). The
average dielectric constant of TGS, p , varies continuously
with increase of temperature and is peaked at the Curie
temperature (Tc = 50 C) where the dielectric constant is
more than an order of magnitude larger than that in the other
temperature regions. Additionally, the dielectric constant of
TGS is nearly independent of frequency in the range 100
4000 Hz.
Although the dielectric constants were measured at a low
electric field while the ER effect appeared at high fields, the
measured dielectric constant data were also used to study
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Figure 2. Variation of the shear stress with temperature at


1500 Hz ac fields. The dashed curve represents the average
dielectric constant of particles at 1500 Hz.

the dielectric constant influence on ER effects, because the


electric strength influences the TGS dielectric constant very
slightly beyond the Curie point [19].

Dielectric constant influence on electrorheological effect

are independent of frequency in the tested range (see


figure 1).
Therefore, only one parameter, the dielectric constant of
particles, influences the ER effect in our experiments; all the
other parameters such as the applied electric field frequency
and the dielectric constant of oil f , are constants;
temperature, viscosity of oil etc, can be ignored. Thus the
system is the best and the simplest one to investigate the
influence of the dielectric constant of particles. The measured
permittivity dependence of the shear stress should be more
reliable than other experiments.
4. High-frequency electric field

Figure 3. Dielectric constant of silicone oil versus temperature at

1000 Hz.

The effect of temperature on the dielectric constant of


the silicone oil, f , is shown in figure 3, which is almost
independent of temperature in the tested temperature range.
It is also found that f is independent of frequency in the
range 1004000 Hz. Therefore, f can be regarded as a
constant in our experiments, f (, T ) 2.75.
From the above experimental data, we can learn that
some parameters can be ignored in the ER fluid if the shear
stress of ER fluid is measured with increasing temperature
under high frequency electric fields.
(1) The conductivity effect can be cancelled under highfrequency fields (see the introduction and equation (3)).
(2) The dielectric constant of silicon oil is almost a constant
in the experiments.
(3) The temperature changes the viscosity of silicone oil
and the van der Waals force as well as the dielectric
constant of particles. The viscosity of the medium has no
influence on the ER effect [14]. The van der Waals force
exponentially changes with temperature ( eU/kT , k
is the Boltzmann constant and U is energy), resulting
in only a very small variation from 20 C to 80 C.
Therefore, the temperature effect can be ignored.
(4) From the experimental process, it is learned that the
effect of particle size R can be ignored as only one type
of solid particle is used in our experiments.
(5) It is also learned that the interfacial properties between
particles and oil are the same during the experiments
because only one type of particle and one type of oil
were used to prepare the ER fluid.
(6) The frequency of the applied electric fields is kept
constant in the experiments and dielectric constants

Under ac fields, the static conductivity effect can be neglected


only if = 2f  /0 for both fluid and particles [4, 9].
In the system, the conductivity of silicone oil (f 1013
1012 S m1 ) and the conductivity of TGS (p 1010
109 S m1 ) requires f to exceed 100 Hz to be in a dielectric
regime. Therefore, only dielectric mismatch should be
considered at 1500 Hz, and the dielectric constant mismatch
can be investigated at the frequency.
Figure 2 shows the shear stress , which is normalized
by subtracting zero-field shear stress, as a function of
temperature for various external ac field strengths E0 . The
dashed curve in figure 2 illustrates the relation of the average
dielectric constant p of TGS, for which the values were
merged by considering the orientation of the particles in
electric fields (see equation (5)), to the temperature. It is
obvious that the shape of is similar to that of p . Both and
p first increase with temperature, go through a maximum at
50 C (Tc ), and then decrease when the temperature is raised
further. The results were reproducible under the given set of
conditions.
As the temperature only affects the dielectric constant p ,
which changes the shear stress under the present conditions,
a certain relationship must exist between and p . Figure 4
illustrates the effect of dielectric constant of the particles,
p , on the shear stress at different field strengths, in which
the data for each curve were extracted from figure 2 over
the whole temperature. A large increase in shear stress
occurs for the dielectric constant up to about 250. Beyond
this value, the rate of change in the shear stress diminishes
and tends to a saturated value when the dielectric constant
of the particles is further increased. So further increase in
the dielectric constant of particles produces only a marginal
increase in the shear stress. This is in agreement qualitatively
with equations (1)(3) and the dielectric mismatch model.
On the basis of a point dipole model [16], would be
proportional to the mismatch factor
2 = (p f )2 /(p + 2f )2 .
However, in the case of a real ER fluid the point dipole
approximation is no longer valid because the multipole
interaction would be important when the particles are nearly
touching in the chains. Instead of the point dipole model,
many authors have performed theoretical calculations by
using various approaches and tried to give an analytical
expression to the relation of shear stress to permittivity
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Y C Lan et al

Figure 4. The shear stress versus p at different fields. Full


symbols, T > Tc ; open symbols, T  Tc .

Figure 6. Variation of the shear stress with temperature at


100 Hz electric fields.

results by assuming that the shear stress is proportional to


the interaction force of the particles in chains. Figure 5
presents a comparison of the measured /(E0 )2 versus 2
curve and the calculated ones according to Tao et al [22],
Conrad et al [21] and the point dipole approximation [16].
In the comparison we normalized the data at the highest value
of /(E0 )2 to 1 by adjusting the proportional parameter.
It is obvious that the point dipole approximation is far from
the measured result, while some improvements have been
achieved in other approaches. The measured shear stress
is more sensitive to the variation of permittivity mismatch
factor 2 than that predicted by the calculations in the lower
2 region. Recently, Li and Ma [23] calculated the shear
stress of ER fluid under high-frequency electric fields using
a first-principles method and compared their results with our
experimental data. Excellent agreement was obtained.
Figure 6 shows the shear stress versus temperature at
100 Hz. The tendencies are similar to those at 1500 Hz,
indicating that the dielectric mismatch also dominates the
ER effect for the 100 Hz field in the system.
5. Conclusions
Figure 5. Normalized shear stress versus 2 at 1500 Hz,

1700 V mm1 . Symbols represent experimental data, lines


represent results calculated according to (a) the point dipole
approximation, (b) Conrad et al [21], (c) Tao et al [22].

mismatch factor [4, 2022]. Although only the results about


the interaction force of the particles in the chains were given in
these calculations, we can compare them with our measured
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In summary, the shear stress of ferroelectric TGS


particle/silicone oil fluid has been measured under ac electric
fields in a simple system. The relationship between the
particle permittivity and shear stress has been obtained
directly. The experimental data are more reliable due to
the same conditions in ER fluids. The comparison of the
measured results with the available calculations has been
made and agreements are obtained although deviation is
observed.

Dielectric constant influence on electrorheological effect

Acknowledgments

This work was supported by the Chinese Natural Science


Foundation and a grant for a Key Research Project in the
Climbing Program from the State Science and Technology
Commission of China.
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