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Journal of Non-Crystalline Solids 287 (2001) 428431

www.elsevier.com/locate/jnoncrysol

The magnetoelastic properties of as-quenched and annealed


Fe73:5 x Alx Si13:5B9Cu1Mo3 x 0; 2; 4; 6 alloys
P. Mnguez a,*, H.A. Davies b, I. Todd b, M.R.J. Gibbs c,
A. Garca-Arribas a, J. Gutierrez a
a

Dpto. Electricidad y Electr


onica, Fac. Ciencias, Univ. Pas Vasco/EHU, Apartado 644, 48080 Bilbao, Spain
b
Department of Engineering Materials, University of Sheeld, Sheeld S13JD, UK
c
Department of Physics and Astronomy, University of Sheeld, Sheeld S37RH, UK

Abstract
The eects of substitution of Fe by Al on the magnetoelastic properties of the Fe73:5 Si13:5 B9 Cu1 Mo3 composition
have been measured on amorphous as-quenched and nanocrystalline annealed samples. This substitution of Fe by Al
decreases the saturation polarization, JS , and the eective anisotropy, hKi, and increases the saturation Young's
modulus, ES , in the as-quenched samples. The magnetic eld dependence of Young's modulus, EH , measured by the
magnetoelastic resonance method and analyzed by the moment rotation model, has been used to estimate saturation
magnetostriction, kS , in the as-quenched and annealed samples. Results show that, for the as-quenched samples, there is
no correlation between the estimated saturation magnetostrictions and the percentage of Al. For the 4% atomic Al
samples, annealed between 500C and 560C, the estimated kS decreased with the annealing temperature to
2 ppm. 2001 Elsevier Science B.V. All rights reserved.

1. Introduction
Iron-based composite soft magnetic alloys
with nanometer-sized crystallites based on the
Fe73:5 Si13:5 B9 Cu1 Nb3 composition are of scientic
and technological interest and have been studied
since their discovery, a decade ago [1]. Cu and
Nb act, respectively, to maximize the density of
crystal nuclei and to retard grain growth, thus
promoting the formation of a ner grain struc*
Corresponding author. Tel.: +34-94 601 53 71; fax: +34-94
601 30 71.
E-mail addresses: pmg@we.lc.ehu.es (P. Mnguez), h.a.
davies@sheeld.ac.uk (H.A. Davies), i.todd@tnw.tudeift.nl
(I. Todd), m.r.gibbs@sheeld.ac.uk (M.R.J. Gibbs), alf@we.
lc.ehu.es (A. Garca-Arribas), jon@we.lc.ehu.es (J. Gutierrez).

ture. These types of alloys, that have soft magnetic properties, are suitable for many types of
magnetic components such as saturable reactors,
choke coils and transformers [2]. Also, from the
fundamental viewpoint, the dependence of the
soft magnetic properties of Al-substituted alloys
on the Al content and subsequent annealing
processes has been studied recently [3,4]. The
main eect of Al on these alloys is to change
their soft magnetic properties. Moreover, in
other works the eects of substitution of Nb by
Mo were investigated [5]. In this work we have
studied the eect of Al addition and of the
thermal treatment on the magnetoelastic properties of Fe73:5 x Alx Si13:5 B9 Cu1 Mo3 x 0; 2; 4; 6
alloys, in which Mo has eects similar to those
of Nb.

0022-3093/01/$ - see front matter 2001 Elsevier Science B.V. All rights reserved.
PII: S 0 0 2 2 - 3 0 9 3 ( 0 1 ) 0 0 5 8 7 - 7

P. Mnguez et al. / Journal of Non-Crystalline Solids 287 (2001) 428431

429

2. Experimental details

3. Results and discussion

Fe73:5 x Alx Si13:5 B9 Cu1 Mo3 alloys 0 6 x 6 6


were fabricated in the form of ribbons (cross-sections were typically of 20 lm  2 mm) by melt
spinning in a He atmosphere. Samples of the ascast ribbons, approximately 22 mm in length, were
sealed in a silica ampoule into which high purity
Ar had been introduced at 1/3 atm. pressure. These
were then heat treated in a conventional tube
furnace for 1 h. During these heat treatments,
which were designed to produce partial devitrication of the ribbons, the temperature was monitored using a calibrated K-type thermocouple
which recorded the annealing temperature with an
accuracy of <1 K. The thermal prole of the furnace, having already been ascertained, the samples
were then positioned within the stable hot zone of
the furnace approximately 150 mm in length) using
ceramic supports such that the sample and the
furnace bore were concentric. The silica ampoules
were removed after 1 h at temperature and the
samples allowed to cool, by air convection, in their
protective Ar atmosphere to room temperature.
The saturation polarization, JS , and the coercivity,
HC , were measured using a hysteresis loop tracer.
The eld dependence of Young's modulus, EH ,
was measured by the magnetoelastic resonance
method MR [6]. All magnetoelastic measurements
were performed, around the rst vibration mode,
with the samples having both ends free. This
conguration gave resonant frequencies at magnetic saturation between 90 and 110 kHz in the
rst vibration mode for the as-quenched samples
and of approximately 130 kHz for the annealed
samples. Young's modulus, E, is obtained from the
following expression [6]:
s
n E
frn
;
1
2L q

Fig. 1 shows the dependence of the saturation


polarization JS as a function of the Al content. The
linear decrease in JS from 1:23  0:01 T for the
base composition to 1:11  0:01 T at x 6 (at a
rate of 0.02 T/at.%Al) is as we expected for replacement of Fe by a non-ferromagnetic element
such as Al [3].
Fig. 2 shows the dependence of Young's modulus with the applied eld on the as-quenched
samples. The maximum DE magnitude occurs for
the 4% atomic Al content sample. This fact indicates that there is no correlation between Al content and magnetoelastic properties. The eective
anisotropy constant is given by

where L is the length of the sample, q the density


and n is the mode of the vibration. All DE curves,
which represent the change of Young's modulus,
E, with the applied eld, H , are shown normalized
to the saturation Young's modulus, ES . Errors
were calculated using standard procedures from
experimental data.

JS HK
;
2
2
where, in our case, the average anisotropy eld,
HK , was taken as the eld at which the minimum of
hKi

Fig. 1. Variation in saturation polarization, JS , as a function of


the Al content for the as-quenched samples. Line is tted by the
least squares method.

Fig. 2. Normalized Young's modulus against applied eld for


the as-quenched samples. Lines are drawn as a guide to the eye.

430

P. Mnguez et al. / Journal of Non-Crystalline Solids 287 (2001) 428431

Table 1
Obtained values of JS ; hKi; ES and kS for the as-quenched
samples
Al (%)

hKi J=m3

ES (GPa)

kS (ppm)

0
2
4
6

503  25
285  10
334  10
268  10

137  14
146  15
159  16
167  17

7  0:4
4  0:2
7  0:4
4  0:2

DE occurs. The results obtained (Table 1) show


that hKi is less in the Al-substituted samples. On
the basis of the moment rotation model [6], the
maximum change in Young's modulus occurs at
H HK and is determined by the expression [7]
ES

Emin
Emin

9k2S ES
;
2hKi

where kS is the saturation magnetostriction, and


Emin and ES are Young's moduli at the minimum of
the curves and at saturation, respectively. These
moduli can be calculated from (1) and the saturation Young's modulus ES increases with the Al
content, as can be seen in Table 1.
With these considerations in mind, we estimate
the saturation magnetostriction values for our
samples. Table 1 shows the estimated kS s for the
samples in the as-quenched state. No correlation
was found between the estimated saturation magnetostriction, kS , and the Al content.
All the DE curves have a minimum. According
to Squire's model [8] this minimum implies that the
average domain angle in all the samples is between
45 and 90. Dierent anisotropies are developed
during the fabrication process of the samples and,
since the sample containing 4 at.% Al has the
larger DE eect, the largest average angle should
occur in this composition.
Therefore, the 4 at.% Al sample is the one that,
in principle, is the better approximation to the
moment rotation model. For this reason we studied the dependence on annealing temperature of
the magnetoelastic properties for the 4% at. Al
containing samples after annealing at 500C,
520C, 540C and 560C. The coercivity was found
to decrease from 35  1 A/m in the as-quenched
sample to 6  1 A/m in the sample annealed at
500C, remaining almost constant in the rest of the

annealed samples. The magnitude of the DE eect


for this set of samples is represented in Fig. 3.
From these curves we have determined that the
saturation Young's modulus increased from approximately 159 to 200 GPa, due to an increasing
fraction of nanocrystallites of FeSiAl that appear
as a rst consequence of the thermal treatments
[9]. Following the same model as for the as-quenched samples the saturation magnetostrictions, kS ,
are estimated again and are given in Fig. 4. We
note that the estimated kS s decrease as the annealing temperature increases as a result of the
increasing volume fraction of nanocrystalline
grains of FeSiAl having a negative magnetostriction [9]. In the same way, the calculated eective
3
anisotropy decreases from 80  5 J=m in the
3
sample annealed at 500C to 55  3 J=m in the
sample annealed at 560C. This fact indicates that

Fig. 3. Normalized Young's modulus against applied eld for


the annealed samples, for the x 4 composition. Lines are
drawn as a guide to the eye.

Fig. 4. Variation in saturation magnetostriction kS as a function of the annealing temperature for the annealed samples.
Lines are drawn as a guide to the eye.

P. Mnguez et al. / Journal of Non-Crystalline Solids 287 (2001) 428431

431

the size of the crystalline grains decreases [10] even


if the total volume of the crystalline phase increases in the samples. These anisotropies are
within the range reported by other authors [11].

research on nanophase soft magnetic alloys at the


University of Sheeld is supported by the Engineering and Physical Sciences research Council
under the Advanced Magnetic Programme.

4. Conclusions

References

The addition of Al decreased the eective anisotropy, hKi, and increased the saturation
Young's modulus, ES . There is no correlation between the saturation magnetostriction, kS , and the
Al content. This independence is inuenced by
dierent induced anisotropies on the samples
during the fabrication process more than by the Al
content in the samples. The estimated saturation
magnetostriction decreased over the range of annealing temperatures studied.

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Hernando (Eds.), Nanostructured and Non-Crystalline
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[10] A. Hernando, J. Phys. 11 (1999) 9455.
[11] L.K. Varga, L. Novak, F. Mazaleyrat, J. Magn. Mater. 210
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Acknowledgements
We gratefully acknowledge the contribution of
Professor Jean-Marc Greneche for M
ossbauer
measurements on the as-quenched samples. The

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