Permeability and electromagnetic-interference characteristics of FeSiAl alloy

flakespolymer composite
Shigeyoshi Yoshida, Mitsuharu Sato, Eishu Sugawara, and Yutaka Shimada
Citation: Journal of Applied Physics 85, 4636 (1999); doi: 10.1063/1.370432
View online: http://dx.doi.org/10.1063/1.370432
View Table of Contents: http://scitation.aip.org/content/aip/journal/jap/85/8?ver=pdfcov
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JOURNAL OF APPLIED PHYSICS

VOLUME 85, NUMBER 8

15 APRIL 1999

Permeability and electromagnetic-interference characteristics

of FeSiAl alloy flakespolymer composite
Shigeyoshi Yoshida,a) Mitsuharu Sato, Eishu Sugawara, and Yutaka Shimadab)
Tokin Corporation, R & D Center, 298 Shibokuchi, Takatsu-ku, Kawasaki, Kanagawa 213-0023, Japan

A magnetic sheet made of FeSiAl flakes was found to have excellent permeability and
electromagnetic-interferences characteristics in a quasimicrowave band. The flakes prepared by
attrition were embedded in a polymer with their planes lying parallel to the sheet plane. This sheet
exhibits a peculiar dual dispersion in permeability. The Curie temperature of the flakes increases
with increasing specific surface area of the flakes. This suggests the composition of the flakes
changes to excess Fe by oxidation of Si and Al. This deviation from the Sendust composition brings
an increase of a magnetoelastic effect and the dual frequency dispersion seems to be associated with
stress caused by attrition. On the basis of these results, flakes with more desirable permeability
characteristics were produced from raw powder with less Fe content. Consequently, we could
fabricate a magnetic composite that possesses superior noise suppressing effect in a
quasi-microwave band. 1999 American Institute of Physics. @S0021-8979~99!42308-4#

I. INTRODUCTION

In the high frequency bands, where wavelengths of electrical signals are comparable with dimensions of electric circuits, connections of circuit elements have to be looked upon
as distributed constant circuits. This tends to cause impedance mismatching in electrical junctions resulting in circuit
oscillation and microwave radiation. To suppress radiation
from these distributed circuits, a material with a large highfrequency loss placed in the vicinity of the lines is effective.
That is expected to damp the oscillation by inductive coupling with the lines, or by absorbing radiation.1
The excellent high frequency permeability characteristics of sputtered multilayer magnetic films patterned into narrow stripes have been studied.2 In our experiments, the flakes
are thinner than the skin depth and a large aspect ratio and
electrical isolation with dielectric matrix such as polymer,
are expected to give rise to analogous high frequency characteristics.
This article describes the permeability characteristics of
FeSiAl alloy flakespolymer composites and its noise
suppression effect in a near field mode.
II. EXPERIMENTAL PROCEDURE

The FeSiAl flakes that have a thickness close to the

skin depth and a large aspect ratio, can be produced by mechanical attrition of FeSiAl powder. Attrition of water
atomized FeSiAl alloy powder ~9.7 wt % Si5.4 wt %
Albal Fe! comprising teardrop particle shapes of 14 mm
mean diameter was carried out in a hydrocarbon solvent by
using an attritor. Magnetic slurry containing the flakes and
polymer was coated repeatedly by using doctor-blade, and
the flakes were oriented with their planes parallel to that of
the layer by shearing stress generated in coating.
a!

Electronic mail: yosida-s@po.iijnet.or.jp

Also with: Tohaku University, Res. Inst. for Sci. Measurements, Aoba-ku,
Sendai, Miyagi 980-0812, Japan.

b!

Permeability measurements were carried out for toroidal

samples of F83F333 mmt by 1 turn coil method using an
impedance-material analyzer (HP-4291A116454A). Curie
temperatures were estimated by extrapolation of the decreasing temperature curve of saturation magnetization measured
with a magnetic balance. Noise suppressing effects of 100
mm square sheet samples were measured by a near field
mode measurement system1 that assumes use of the sheets in
small size electric devices.
III. RESULTS AND DISCUSSION

Permeability characteristics of FeSiAl flakes

polymer composites are shown in Fig. 1~a! as a function of
frequency. As shown in Fig. 1~b!, permeability ( m 8 max) of
the composite made of FeSiAl flakes is obviously superior to that of a rubber-ferrite or composite made of asatomized FeSiAl powder. The composite made of flakes
attrited for 7.5 h shows maximum m 8 of about 16, thereafter,
it decreases with increasing attrition time. Mechanical distortion associated with the attrition process or change of the
crystalline phase in FeSiAl are the subjects to be studied
here.
The ultimate products of a polymer composite exhibit
magnetic resonance in a few 10 MHz range, and moreover,
decrease of permeability in 100 MHz range which seems
also to be caused by a magnetic resonance. As a result,
imaginary part of permeability ( m 9 ) shows twin peak dispersion and m 9 is high over a wide frequency range. As a
result, the material has a remarkable feature of noise suppressing in high frequency electromagnetic-interferences
~EMI! countermeasures.
Mechanisms for this peculiar frequency characteristics
may be any of: ~1! appearance of a new crystalline phase
with different magnetic anisotropy, ~2! resonance by local
magnetic anisotropy caused by local mechanical distortion,3
~3! L C resonance due to the metallic/dielectric multilayer
structure,4 or ~4! domain wall resonance. Validity of ~1! can
be studied by measuring the temperature dependence of the

0021-8979/99/85(8)/4636/3/$15.00
4636
1999 American Institute of Physics
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Yoshida et al.

J. Appl. Phys., Vol. 85, No. 8, 15 April 1999

4637

FIG. 3. Curie temperature T c of FeSiAl alloy flakes as a function of

attrition time.

FIG. 1. Frequency dependence of permeability of the composite materials.

~a! Change of the permeability with the attrition time. ~b! Example of a
rubber-ferrite.

saturation magnetization (M s ). Examples of temperature dependence of M s are shown in Fig. 2. In Fig. 2~a!, as-attrited
flakes exhibit an irreversible change on temperature dependence of M s . But as shown in Fig. 2~b!, no remarkable
change was observed between the increasing and decreasing
run for as-atomized powder and after annealing of flakes.
This suggests that the irreversible change for flakes by longer
attrition is due to relaxation of residual distortion. The monotonous temperature dependence of M s suggests that the
flakes after annealing are single phase. However, we notice
that the Curie temperature T c of the flakes attrited 20 h becomes higher by 80 centigrade in comparison with T c of the
as atomized powder. Attrition time dependency of T c is
shown in Fig. 3, where T c increases proportionally with increasing attrition time. This suggests that the composition of
FeSiAl flakes tends to acquire excess Fe by attrition.
From the fact that specific surface area of the alloy powder is
also proportional to the attrition time, the increase of T c
seems to occur by selective oxidation of Si and/or Al at the
surface of the flakes.
This suggests that a magneto-elastic effect plays a role in
determining the resonance frequency and the frequency characteristics of FeSiAl flakes, because the magnetostriction
constant l s changes sensitively as the composition of original FeSiAl alloy changes.
To verify the composition change in the flakes after attrition, scanning Auger electron microscope ~SAM! analysis
and x-ray photoelectron spectroscopy ~XPS! were performed
for the bulk FeSiAl alloy samples which were heat treated
for 50 C324 h. From the depth profiles of the bulk Fe
SiAl alloy obtained by SAM, the oxidation depth is estimated to be 30 . Considering this result, semiquantitative
analysis by XPS was carried out for the surface sputtered to
50 depth. Table I shows the results. For the surface at the
depth of 20 s sputtering, a large quantity of oxygen close to
TABLE I. Contents of C, O, Si, Al, and Fe of FeSiAl ~9.89 wt % Si
5.59 wt % Albal Fe! alloy surface.
Etching time ~s!

Si

Al

Fe ~at. %!

0
35
43
6
6
10
FIG. 2. Increasing and decreasing temperature runs of normalized saturation
20

49
13
14
24
magnetization M s (T)/M s (25 C) of FeSiAl alloy powder. ~a! As-attrited
60
1
11
8
14
66
flakes ~20 h attrition!. ~b! As-atomized powder and after annealed flakes ~20
h attrition!.
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4638

Yoshida et al.

J. Appl. Phys., Vol. 85, No. 8, 15 April 1999

TABLE II. Contents of Si, Al, and Fe of FeSiAl ~9.89 wt % Si5.59

wt % Albal Fe! alloy surface.
Etching time ~s!

Si

Al

Fe ~at. %!

0
20
60

27
25
9

27
27
16

45
47
75

50 at. % exists. Table II shows normalized quantities for the

three elements that constitute the original alloy. Si and Al are
condensed at the surface of bulk alloy by about 3 and 5
times, respectively, of the original alloy composition.
Moreover, from the bonding-state analysis by XPS, at
the depth of 2060 s sputtering, most of Si and Al are in
oxidized state. Therefore, in the surface layer of FeSiAl
bulk alloy, Si and Al seem to be relatively condensed in
comparison with composition of original alloy, and they exist as oxides.
To get more quantitative information on the composition
change of original alloy accompanying surface oxidation,
nine kinds of FeSiAl alloy samples that have different
compositions were prepared, and quantitative analysis by inductively coupled plasma ~ICP! and T c measurement were
performed. As a result, T c of FeSiAl alloys with compositions near that of Sendust are sensitively dependent on Fe
contents, and it is estimated that T c increases by 4050 C
with an increase of 1% of Fe.
Thus, we conclude that the increase of T c of flakes accompanying progress of attrition is due to a shift of the composition to excess Fe.
Therefore, one of the dominant factors that determine
the permeability characteristics of the attrited FeSiAl
flakes is a magnetoelastic effect caused by composition
change of the alloy powder. Further quantitative study on the
relation between these factors and frequency characteristics
of permeability is in progress.
By speculation of the composition change caused by increase of the powder surface area, we can fabricate a composite with lower l s and consequently a large magnetic loss
in a lower frequency range. Raw powder with composition

FIG. 5. Near field noise suppression effect. Sheet thickness: 0.5 mm. ~1!
Flakes with less Fe content. ~2! Flakes with Sendust composition. ~3!
Rubber-ferrite.

of poorer Fe ~9.8 wt % Si6 wt % Albal Fe! than that of

Sendust was prepared. The permeability characteristics of the
composite made of poorer Fe flakes is shown in Fig. 4, superior permeability in a quasi-microwave band was obtained
as expected.
Noise suppressing effects in near field were investigated.
A result is shown in Fig. 5 for the sample made of flakes
attrited 7.5 h and the sample made of poor Fe flakes and a
rubber-ferrite. In the comparison of transmission attenuation
shown in Fig. 5~a!, the composite with poor Fe flakes shows
large attenuation over the whole measurement band. Furthermore, the poor Fe sample exhibits obvious superiority in
coupling attenuation normalized to air @Fig. 5~b!#.
IV. CONCLUSION

The FeSiAl polymer composite exhibits superior permeability characteristics at high frequencies. A T c increase
of the flakes with progress of attrition suggests excess Fe
within the flakes and, consequently, a magnetoelastic effect
seems to give a large influence to permeability. By preparing
raw compositions with poorer Fe than that of Sendust, a
sheet with excellent permeability characteristics and EMI
suppressing effect in a quasimicrowave band is available.
1

FIG. 4. Frequency dependence of permeability of the composite sheet made

of poor Fe raw material.

S. Yoshida, M. Sato, and Y. Sato, Abstract of 97 EMC Symposium, 4-1-1

~1997!.
2
S. Tanabe, H. Ohji, K. Inoue, and T. Ozeki, Proc. Perp. Mag. Rec., 91,
197 ~1991!.
3
Y. Shimada, M. Shimoda, and O. Kitakami, Jpn. J. Appl. Phys., Part 1 34,
4786 ~1995!.
4
B. C. Webb, M. E. Re, M. A. Russak, and C. V. Jahnes, J. Appl. Phys. 68,
4290 ~1990!.

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