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471

Effect of External Magnetic Field on Ultrasonic


Propagation Velocity in Magnetic Fluids∗

Masaaki MOTOZAWA∗∗ , Yoshiyuki MATSUMOTO∗∗ and Tatsuo SAWADA∗∗

Experimental results for the properties of ultrasonic propagation velocity in kerosene-


based and water-based magnetic fluids are reported. Ultrasonic wave frequencies of 1 MHz,
2 MHz and 4 MHz are used and the measurement scheme is based on the pulse method. The
external magnetic field intensity is varied from 0 mT to 550 mT and the angle between the
magnetic field direction and the direction of ultrasonic wave propagation is varied from 0◦
to 90◦ . The ultrasonic propagation velocity in magnetic fluids is dependent on temperature,
elapsed time of applying the magnetic field, and magnetic field intensity. Hysteresis and
anisotropy of ultrasonic propagation velocity are observed. These interesting results seem to
be related to chain-like cluster formation in the magnetic fluids and the characteristic period
of Brownian motion of the magnetic particles.

Key Words: Magnetic Fluid, Sound Velocity, Ultrasonic Propagation Velocity, Anisotropy,
Chain-Like Cluster, Hysteresis

A technique called the Ultrasound Velocity Profile


1. Introduction
(UVP) method, which was developed by Takeda(2), (3) , is
A magnetic fluid is a stable colloidal suspension of a method of measuring a velocity profile along a line with
many surfactant-coated ferromagnetic particles in a liq- respect to the velocity component along the ultrasonic
uid carrier such as water or kerosene. The particles are beam. This technique has two main advantages in com-
about 10 nm in size. The preparation of a stable mag- parison with methods like LDV or PIV. First, it can be
netic fluid involves a delicate balance between the attrac- applied to an opaque fluid. Second, flow mapping is prac-
tive and repulsive forces on each particle. Under no ex- tical because a linear measurement is used. As such, it
ternal magnetic field, the particles are in Brownian motion is a useful method for measurement of a velocity compo-
and remain suspended(1) . When a magnetic field is ap- nent of a magnetic fluid, and recently it has been applied
plied to a magnetic fluid, several interesting flow phenom- to flow measurements of a magnetic fluid(4), (5) .
ena, which are not seen in a Newtonian fluid, have been When applying the UVP to velocity profile mea-
observed because of the combination of magnetism and surement of magnetic fluid flow, it is important to have
liquidity. These flow behaviors of a magnetic fluid seem an accurate measure of ultrasonic velocity in a magnetic
to be caused by the formation of chain-like clusters. How- fluid. However, the ultrasonic velocity in a magnetic fluid
ever, there have been few studies to clarify the influence changes depending on the application of an external mag-
of these clusters on magnetic fluid flow behavior. netic field in addition to depending on the temperature
When magnetic fluids are used in a fluid mechanical of the magnetic fluid. It is believed that when an exter-
system such as a magnetic fluid damper, a magnetic fluid nal magnetic field is applied to a magnetic fluid, some of
actuator, etc., it is necessary to have detailed measurement the colloidal particles coagulate and form chain-like clus-
of internal velocity profiles. However, because a magnetic ters(6) . It seems that the Brownian motion of magnetic par-
fluid is opaque, we cannot use optical methods such as ticles as well as this chain-like cluster formation have an
Laser Doppler Velocimetry (LDV) and flow visualization influence on ultrasonic velocity in a magnetic fluid. There-
techniques such as Particle Image Velocimetry (PIV). fore, it is very difficult to measure the ultrasonic velocity

Received 16th May, 2005 (No. 05-4003)
in a magnetic fluid precisely.
∗∗
Department of Mechanical Engineering, Keio Univer- Several studies have been performed to investigate the
sity, 3–14–1 Hiyoshi, Kohoku-ku, Yokohama 223–8522, properties of ultrasonic propagation velocity in a magnetic
Japan. E-mail: sawada@mech.keio.ac.jp fluid. Parsons(7) proposed a linear hydrodynamical theory

JSME International Journal Series B, Vol. 48, No. 3, 2005


472

of a magnetic fluid under a magnetic field. He derived


the expression of the sound attenuation coefficient. Chung
and Isler(8) measured attenuation coefficient and ultrasonic
propagation velocity in a magnetic fluid experimentally.
They found anisotropy of ultrasonic propagation. Interest-
ingly, there is some difference between Parsons’ theoreti-
cal results and the experimental data obtained by Chung
and Isler. Gotoh and Chung(9) attempted to derive ex-
pressions of the attenuation coefficient from the ferrohy-
drodynamical theory which took no account of internal
freedoms of the fluid. Taketomi(10) calculated the atten-
uation coefficient expression while considering the chain-
like cluster formation. He considered both rotational and
translational motions of the magnetic particles. Recently,
Skumiel and Hornowski(11) and Jozefezak(12) measured ul-
trasonic propagation velocity and attenuation coefficient in
a magnetic fluid by changing the magnetic field intensity
and the sweep rate. In our previous study(13) , we measured
ultrasonic propagation velocity of a 1 MHz wave and at-
tenuation coefficient in a water-based magnetic fluid. Hys-
teresis and anisotropy of ultrasonic propagation were dis-
cussed. Fig. 1 Experimental apparatus
As mentioned above, some theoretical and experi-
mental studies have been carried out to clarify the proper-
ties of ultrasonic propagation in magnetic fluids. However, ultrasonic pulse is generated simultaneously by the ce-
the ultrasonic propagation mechanism is still not clear. In ramic oscillator and propagates through the magnetic fluid
the present paper, we have carried out precise measure- in the test cell. The ultrasonic pulse is then received at a
ments of ultrasonic propagation velocity in two different second ceramic oscillator on the opposite side of the test
magnetic fluids while changing the external magnetic field cell. The received signal is sent to the oscilloscope. The
intensity and the angle between the direction of the mag- ultrasonic propagation velocity in the magnetic fluid can
netic field and the direction of ultrasonic propagation. We be calculated based on the traveling time of the ultrasonic
use 1 MHz, 2 MHz and 4 MHz ultrasonic waves in the ex- pulse. The temperature of the magnetic fluid is controlled
periment. The test fluids are kerosene-based and water- by the temperature control unit and is measured by a ther-
based magnetic fluids. The influence of chain-like clus- mister. A magnetic field can be applied to the magnetic
ters on ultrasonic propagation velocity and the effects of fluid by an electromagnet. The angle between the direc-
anisotropy, hysteresis and frequency dependence on ultra- tion of magnetic field and the direction of ultrasonic prop-
sonic propagation are presented. agation is freely adjustable.
Figure 2 shows the details of the test cell, which has a
2. Experimental Apparatus and Magnetic Fluids
concentric structure. Two ceramic oscillators are equipped
A kerosene-based (HC-50) and a water-based (W-40) on the inner rectangular vessel as an emitter and a receiver,
magnetic fluid are used. The HC-50 has 50% weight con- respectively. The inner vessel is filled with a magnetic
centration of fine magnetic particles (Fe3 O4 ) in a kerosene fluid and the ultrasonic wave propagates through 32 mm.
and is produced by Taiho Industries Co., Ltd., Japan. Its The outer cylindrical container is filled with circulating
viscosity and density at 25◦ C are 15 mPa·s and 1.39 × water. The temperature of the magnetic fluid is kept at
103 kg/m3 , respectively. The W-40 has 40% weight con- 25◦ C by this circulating water, which is supplied by a tem-
centration of fine magnetic particles and is produced by perature control unit. Three test cells are available. Each
the same company. Its viscosity and density at 25◦ C are test cell has different ceramic oscillators, which have ul-
25 mPa·s and 1.40 × 103 kg/m3 , respectively. trasonic frequencies of 1 MHz, 2 MHz and 4 MHz, respec-
Figure 1 shows a block diagram of the experimental tively.
apparatus. The ultrasonic measurement scheme is based External magnetic flux density can be changed from
on the pulse method. A burst wave and trigger signal are 0 mT to 550 mT. The angle φ between the direction of
generated synchronously by the pulse generator. The trig- ultrasonic propagation and the direction of magnetic field
ger signal is sent to the oscilloscope and the burst wave is can be adjusted freely from 0◦ to 180◦ . The distribution of
transmitted to the ceramic oscillator in the test cell. The the magnetic field along the field axis x is shown in Fig. 3.

Series B, Vol. 48, No. 3, 2005 JSME International Journal


473

Fig. 4 Temperature dependence of the ultrasonic propagation


velocity

Fig. 2 Test cell

Fig. 5 Temperature dependence of the ultrasonic velocity with


ultrasonic frequencies

Fig. 3 Magnetic field distribution


This seems to be because the Brownian motion of the mag-
netic particles increases with the increase in temperature.
The measurement area of the test cell is from 15 mm to Figure 5 shows the temperature dependence of ul-
−15 mm. We considered the external magnetic field to trasonic velocity in W-40 at various pulse frequencies
be uniform in the measurement area because there is lit- (1 MHz, 2 MHz and 4 MHz). As can be seen, ultrasonic
tle variation in the field. velocity does not vary significantly with frequency. There-
fore, pulse frequency has little influence on ultrasonic
3. Results and Discussions
propagation velocity in the absence of a magnetic field.
3. 1 Temperature dependence Similar results were obtained for HC-50.
Figure 4 shows the temperature dependence of ultra- 3. 2 Time dependence
sonic velocity in various fluids when no magnetic field is Figure 6 shows the relative change of ultrasonic prop-
applied. Ultrasonic velocities in the magnetic fluids, W- agation velocity versus elapsed time from applying the
40 and HC-50, are shown by open circles and triangles, magnetic field using a 1 MHz ultrasonic wave. The rela-
respectively. Ultrasonic velocities in the carrier liquids, tive change of ultrasonic propagation velocity is expressed
pure water and kerosene, are indicated by closed circles by ∆V/Vo, where ∆V is defined by ∆V = V − Vo, and
and triangles, respectively. The solid line represents the V and Vo are ultrasonic propagation velocities with and
ultrasonic velocity in pure water obtained by Del Grosso without an external magnetic field, respectively. In this
and Mader(14) . It can be seen that the ultrasonic velocity experiment, the magnetic field intensity is held at 100 mT,
in both magnetic fluids is smaller than that in the carriers and the angle φ is 0◦ . The ultrasonic propagation veloc-
because the magnetic particles have an influence on the ity increases over the time the magnetic field is applied
ultrasonic velocity. As the temperature increases, the ul- to a magnetic fluid. This increase seems to be caused by
trasonic velocity in the magnetic fluids slightly decreases. chain-like cluster formation. The external magnetic field

JSME International Journal Series B, Vol. 48, No. 3, 2005


474

Fig. 6 Time dependence of ultrasonic propagation velocity Fig. 7 Anisotropy of ultrasonic propagation velocity with
magnetic field intensity in W-40

causes the inner magnetic particles to coagulate and form


chain-like clusters and these clusters then have an influ-
ence on ultrasonic propagation. Figure 5 indicates that the
ultrasonic propagation velocity in both types of magnetic
fluids increases with the elapsed time from applying the
magnetic field. The clusters seem to grow to a maximum
level for about 1.5 hours in W-40, and 2 hours in HC-50
because following this time, ∆V/Vo is almost constant.
The change in ultrasonic propagation velocity in HC-50
is smaller than that in W-40. This seems to be caused by
differences in chain-like cluster formation between W-40
and HC-50. It is suggested that the chain-like clusters in
HC-50 are smaller, shorter and thinner than those in W-40
because of differences in the structure of surfactants. Fig. 8 Anisotropy of ultrasonic propagation velocity with
3. 3 Anisotropy of ultrasonic propagation velocity magnetic field intensity in HC-50
Anisotropy of ultrasonic propagation velocities in W-
40 and HC-50 are shown in Figs. 7 and 8, respectively.
Figure 9 shows the anisotropy of ultrasonic propagation
velocity in HC-50 in a 3D format. Before each experi-
ment, the magnetic field is applied for a few hours to ob-
tain sufficient chain-like cluster formation. The ultrasonic
propagation velocity is then measured every 3◦ for a dura-
tion of 1 minute. Both in W-40 and HC-50, it can be seen
that the minimum ultrasonic propagation velocity is ob-
tained near φ = 90◦ , and the maximum velocity is obtained
at φ = 0◦ . The chain-like clusters form along the direction
of the magnetic field. Thus, at φ = 0◦ , the chain-like clus-
ters do not interfere strongly with ultrasonic propagation
because the direction of ultrasonic propagation and the
chain-like clusters is parallel. Conversely, at φ = 90◦ , as
the direction of ultrasonic propagation and chain-like clus-
ters are perpendicular, the effect of the chain-like clusters
becomes stronger and the minimum velocity is obtained at
φ = 90◦ . As the magnetic field intensity increases, the rel- Fig. 9 Anisotropy of ultrasonic propagation velocity in HC-50
(Fig. 8) in 3D form
ative change in ultrasonic propagation velocity also gen-
erally increases because the chain-like clusters grow with
magnetic field intensity. differences in properties between W-40 and HC-50. Mag-
In Fig. 7, ∆V/Vo shows a somewhat irregular distri- netic particles in a water-based magnetic fluid are coated
bution. It is supposed that this irregularity relates to the with two layers of absorbed dispersant molecules. On the

Series B, Vol. 48, No. 3, 2005 JSME International Journal


475

other hand, magnetic particles in a kerosene-based mag- change in the ultrasonic propagation velocity is smaller
netic fluid are coated with a single layer. In addition, in and a larger step allows for a reduced measurement time.
our previous measurements(13) using W-40 for a 1 MHz As seen in Fig. 10, there is clear hysteresis in relation to
ultrasonic wave, we did not obtain similar results. From the applied external magnetic field for φ = 0◦ . When the
these results, the water-based magnetic fluid shows signif- external magnetic field intensity increases, the ultrasonic
icant irregular phenomena which we believe is related to propagation velocity also increases. Conversely, in the de-
the two layer structure of the surfactant. crease process, the ultrasonic propagation velocity first in-
3. 4 Hysteresis of ultrasonic propagation velocity creases and then decreases slightly. The peculiar results
Figures 10 and 11 show hysteresis of ultrasonic prop- appear to be the result of anisotropy as well as chain-
agation velocity in W-40 versus external magnetic field in- like cluster formation. In the process of increasing mag-
tensity for φ = 0◦ and φ = 90◦ , respectively. In these exper- netic field, the chain-like clusters form and grow along the
iments, the magnetic field is applied using the following direction of magnetic field in proportion to its intensity.
process: increase the magnetic field intensity 12 mT every When the magnetic field decreases, the chain-like clus-
2 minutes until reaching 550 mT (closed circles). There- ters do not break instantly and may even continue to grow
after, decrease the magnetic field intensity by 24 mT every slightly. On the contrary, as seen in Fig. 11, at φ = 90◦ ,
2 minutes (open circles). In our previous measurement, there is no remarkable hysteresis. Because the chain-like
there was little difference on the ultrasonic propagation ve- cluster formation strongly interferes with ultrasonic prop-
locity in the change process of magnetic field intensity by agation in a magnetic fluid, the ultrasonic propagation ve-
12 mT and 24 mT every 2 minutes. In the increase proc- locity is generally smaller than that without external mag-
ess, we used 12 mT every 2 minutes because the change netic field. These complicated and interesting phenomena
in ultrasonic propagation velocity is larger. On the other are believed to be derived from the change of bulk mod-
hand, we chose 24 mT in the decrease process because the ulus according to the chain-like cluster formation. How-
ever, the detailed mechanism is not yet clear.
Figure 12 shows similar results for ultrasonic propa-
gation velocity at φ = 0◦ in HC-50. The ultrasonic prop-
agation velocity in HC-50 also increases in proportion to
the magnetic field intensity as the magnetic field intensity
increases. When the magnetic field decreases, however,
the ultrasonic propagation velocity remains at almost the
same level. Against, this seems to indicate that the chain-
like clusters do not break easily when the magnetic field
decreases. In other experiments using 2 MHz and 4 MHz
ultrasonic waves, we observed similar tendencies. In order
to understand these interesting phenomena, it is necessary
to further investigate the structure of magnetic particles
and the process of chain-like cluster formation.
Fig. 10 Hysteresis of ultrasonic propagation velocity in W-40 3. 5 Frequency dependence
for φ = 0◦ Figure 13 shows anisotropy of the ultrasonic propa-

Fig. 11 Hysteresis of ultrasonic propagation velocity in W-40 Fig. 12 Hysteresis of ultrasonic propagation velocity in HC-50
for φ = 90◦ for φ = 0◦

JSME International Journal Series B, Vol. 48, No. 3, 2005


476

the change of ultrasonic propagation velocity is smaller


than that in W-40. It seems that the chain-like clusters in
HC-50 are smaller than those in W-40. These interesting
results are believed to be dependent on the concentration
of magnetic particles, the ultrasonic wavelength and
relaxation time connected with magnetization. The water-
based magnetic fluid (W-40) shows significant unstable
rheological properties, possibly caused by the two layer
structure of the surfactants. The ultrasonic propagation
velocity also varies according to the ultrasonic frequency,
which appears to be related to the characteristic time of
Brownian motion of the magnetic particles.
Fig. 13 Comparison of anisotropy of ultrasonic propagation We obtained several interesting experimental results
velocity for W-40 and HC-50 related to ultrasonic propagation velocities. These results
have not been clarified by previous theoretical approaches.
At the present stage, it is necessary to carry out more vari-
gation velocities in W-40 (left figure) and HC-50 (right ous and detailed experiments to clarify the mechanisms of
figure). In both figures, the magnetic field intensity is the ultrasonic propagation properties in magnetic fluids.
300 mT. The ultrasonic propagation velocity changes as
Acknowledgements
the frequency varies. Even though ∆V/Vo did not change
significantly for different frequencies in both W-40 and We would like to thank Mr. K. Kobayashi of Honda
HC-50, there exists a slight frequency dependence. This Electronics Co., Ltd. for his collaboration in experiments.
may be related to the fact that the magnetization of mag- This work has been partially supported by a Grant-in-Aid
netic fluid is known to be affected by both the Néel re- for Scientific Research (C) of Japan Society for Promotion
laxation and the Brownian relaxation. Néel relaxation is of Science.
caused by the reorientation of the magnetization vector,
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JSME International Journal Series B, Vol. 48, No. 3, 2005

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