Impacts of amorphous and crystalline cobalt ferrite layers on the giant magnetoimpedance response of a soft ferromagnetic amorphous ribbon

D. Mukherjee, J. Devkota, A. Ruiz, M. Hordagoda, R. Hyde, S. Witanachchi, P. Mukherjee, H. Srikanth, and M.

H. Phan
Citation: Journal of Applied Physics 116, 123912 (2014); doi: 10.1063/1.4896583
View online: http://dx.doi.org/10.1063/1.4896583
View Table of Contents: http://scitation.aip.org/content/aip/journal/jap/116/12?ver=pdfcov
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JOURNAL OF APPLIED PHYSICS 116, 123912 (2014)

Impacts of amorphous and crystalline cobalt ferrite layers on the giant

magneto-impedance response of a soft ferromagnetic amorphous ribbon
D. Mukherjee, J. Devkota, A. Ruiz, M. Hordagoda, R. Hyde, S. Witanachchi, P. Mukherjee,
H. Srikanth, and M. H. Phana)
Center for Integrated Functional Materials, Department of Physics, University of South Florida, Tampa,
Florida 33620, USA

(Received 5 May 2014; accepted 16 September 2014; published online 26 September 2014)
A systematic study of the effect of depositing CoFe2O4 (CFO) films of various thicknesses
(d 0600 nm) on the giant magneto-impedance (GMI) response of a soft ferromagnetic amorphous ribbon Co65Fe4Ni2Si15B14 has been performed. The CFO films were grown on the amorphous ribbons by the pulsed laser deposition technique. X-ray diffraction and transmission electron
microscopy revealed a structural variation of the CFO film from amorphous to polycrystalline as
the thickness of the CFO film exceeded a critical value of 300 nm. Atomic force microscopy evidenced the increase in surface roughness of the CFO film as the thickness of the CFO film was
increased. These changes in the crystallinity and morphology of the CFO film were found to have a
distinct impact on the GMI response of the ribbon. Relative to the bare ribbon, coating of amorphous CFO films significantly enhanced the GMI response of the ribbon, while polycrystalline
CFO films decreased it considerably. The maximum GMI response was achieved near the onset of
the structural transition of the CFO film. These findings are of practical importance in developing
C 2014 AIP Publishing LLC.
high-sensitivity magnetic sensors. V
[http://dx.doi.org/10.1063/1.4896583]
I. INTRODUCTION

The giant magneto-impedance (GMI) effect of a soft ferromagnetic material is of growing research interest for its
potential applications to the fabrication of highly sensitive
and cryogen-free magnetic sensors.13 GMI is a large change
in the ac impedance of a ferromagnetic conductor subject to
an external dc magnetic field.4 The effect has been mostly
observed in rectangular and cylindrical geometries, such as
ribbons,46 films,2,7 and micro-wires2,8 of different soft ferromagnetic materials. Among them, Co-based amorphous ribbons with nearly vanishing magnetostriction (k  0) have
been reported to exhibit GMI effects with a high degree of
field sensitivity and are therefore promising candidate materials for making advanced magnetic sensors.911 For a given
ribbon of thickness 2t, the complex impedance Z R jX
(where R and X are resistance and reactance, respectively; j
is the imaginary unit) is given by Z R jX
Z Rdc jktcothjkt;

(1)

where Rdc is the dc resistance and k (1 j)/dm is related to

q
the skin depth dm plq f of the ribbon. Here, q and lT are
T

the resistivity and transverse permeability of the ribbon,

respectively, and f is the frequency of an ac current. At low
frequencies (f  kHz) where the skin effect is weak, the primary contribution to lT and hence to the magnetoimpedance (MI) comes from inductive voltage. However, at
moderate frequencies (f  1 MHz), the skin effect is strong
and both R and X contribute to the MI.8,11 At higher frequencies, the ac current is confined to the sheath of the ribbons
a)

Author to whom correspondence should be addressed. Electronic mail:

phanm@usf.edu

0021-8979/2014/116(12)/123912/8/$30.00

surface so that the skin effect is very strong. In this frequency range, dc resistance dominates the GMI and the surface of the ribbon is very sensitive to its electric and
magnetic environment.3 A small modification of physical
properties on or near the surface of the ribbon could thus
lead to a large alteration in its GMI response.
A controlled engineering of the surface of a soft ferromagnetic ribbon has proved useful in enhancing the GMI
effect and its field sensitivity (g).1217 For example,
Taysioglu et al.,12,13 Peksoz et al.,14 Laurita et al.,16 and
Chaturvedi et al.17 reported the enhanced GMI response of
an amorphous Co-based ribbon when coated with copper and
zinc oxide, diamagnetic organic thin film, cobalt, and carbon
nanotubes, respectively. Recently, we have achieved a large
enhancement in the GMI response of a Co-based amorphous
ribbon coated with a 50 nm thick CoFe2O4 (CFO) film using
the pulsed laser deposition (PLD) technique.18 The improved
effect was attributed to the reduction of the surface roughness of the ribbon and the closure of magnetic flux paths due
to the CFO layer. On the other hand, it has been noted that
the crystallinity and magnetic properties of a CFO film
grown on an amorphous substrate (e.g., SiO2/Si) varied significantly with film thickness.1921 The structure of the CFO
film varied from amorphous to polycrystalline as the film
thickness exceeded a critical value.21 Since GMI is a
surface-related phenomenon, this structural transformation
of a CFO film grown on a Co-based amorphous ribbon upon
variation in CFO film thickness is expected to have distinct
impacts on the GMI response of the ribbon.
To elucidate the influence of the coating layer crystallinity on magneto-impedance, we have performed a thorough
study of the structure, magnetic properties, and GMI
effect of a commercial Co65Fe4Ni2Si15B14 amorphous

116, 123912-1

C 2014 AIP Publishing LLC

V

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ribbon coated with CFO films of various thicknesses

(d 0600 nm) by PLD. A careful analysis revealed that the
structure of the CFO film changed from amorphous to polycrystalline as the film thickness exceeded 300 nm. This crystallization of the CFO film was shown to coincide with a
change in the trend of maximum GMI ratio with film thickness. The CFO coating enhanced the GMI response of the
ribbon for d  300 nm while reducing it for d > 300 nm.
Since both coating and annealing effects occurred simultaneously during PLD, our study demonstrates the usefulness of
an in-situ annealing and coating method based on PLD for
improving the GMI response of soft ferromagnetic amorphous ribbons for high-performance sensor applications.
II. EXPERIMENT
A. Growth of CFO films on amorphous magnetic
ribbons

Co65Fe4Ni2Si15B14 ribbons with a thickness of 15 lm

(MetglasV 2714 A) were prepared by a rapid quenching
method. Cobalt ferrite (CFO) coatings with nominal thicknesses of 50 nm, 100 nm, 200 nm, 300 nm, 400 nm, and
600 nm were deposited on the ribbon pieces of width 2 mm
via PLD. The CFO films were deposited at 450  C and the
increase in the film thickness (50 nm 600 nm) corresponded
to that of the annealing time (8.33100 min). A compressed
powder target of CFO was ablated using an excimer (KrF)
laser of wavelength 248 nm and operating at 10 Hz while
providing an energy density of 2 J/cm2 at the target surface.
The distance between the heater element or substrate holder
and the target was 4 cm. Under these conditions, the growth
/pulse. In a typical deprate was measured to be around 0.1 A
osition process, first two ribbons were attached to the heater
element with one of the ribbons covered completely with a
shadow mask to provide a control sample. Once a base pressure of 1.0  106 Torr was reached, the heater element was
raised to 450  C. It was critical to attain high vacuum in the
deposition chamber before heating the ribbons, in order to
prevent their surface oxidation. If oxidized, the ribbons
became brittle and crumpled on touching. After the deposition, the chamber was kept under vacuum as the heater block
was very slowly cooled to room temperature (2 h). To understand the growth mechanism of CFO film on an amorphous
substrate, the CFO coatings were also deposited on amorphous SiO2/Si (100) substrates (dimensions: 1 cm  1 cm 
0.5 mm) under the same conditions as those on the ribbons.
R

B. Sample characterization

The interfacial microstructure in the PLD-deposited

CFO/SiO2/Si layered structures was analyzed using a highresolution transmission electron microscope (HRTEM) (FEI
Tecnai F 20 S-Twin TEM). The sample for cross-sectional
HRTEM analyses was prepared by milling a 5 lm  10 lm
rectangular strip with 100 nm thickness from the sample surface using a focused ion beam (FIB) (JEOL 4500 FIB/SEM)
and Pt welding it to a Cu TEM grid. The phase formation and
crystallographic orientation of the films on the ribbons were
analyzed using X-ray diffraction (XRD) with Cu Ka radiation

J. Appl. Phys. 116, 123912 (2014)

(Bruker D8 Focus Diffractometer with Lynx Eye position

sensitive detector). Peak shifts due to sample misalignment
were accounted for while performing the XRD scans. The
surface morphologies were observed using an atomic force
microscope (AFM) (Digital Instruments III). The chemical
composition analysis was performed using energy dispersive
spectroscopy (EDS) (Oxford Instruments, INCA x-sight). The
magnetic properties of uncoated and CFO-coated ribbons
were measured by a vibrating sample magnetometer (VSM).
C. Magneto-impedance measurements

MI measurements of all uncoated and CFO-coated ribbon samples were performed by the four-point measurement
technique using an HP4192A analyzer with a constant ac
current of 5 mA along the ribbon length of 5 mm over a frequency range of 0.113 MHz and in the presence of axial dc
fields up to 6120 Oe. The details of the measurement system
can be found elsewhere.22 The GMI ratio (DZ/Z) and its field
sensitivity (g) in the samples were calculated as according to
DZ
ZH  ZHmax
 100;
%
Z
ZHmax
 
DZ
2
Z max
g
;
DH

(2)

(3)

where Z(H) is the impedance of the samples in the presence of

an axial dc field H and Hmax (120 Oe) is the magnetic field
that saturates the Z. DH is the full width at half maximum
(FWHM) of a field dependent GMI curve at a given frequency.
III. RESULTS AND DISCUSSION

In order to understand the growth mechanism of CFO

films on Co65Fe4Ni2Si15B14 amorphous ribbons, we first
examined the growth of the CFO layer on the widely used
amorphous substrate SiO2/Si (100) under identical conditions, the results of which are shown in Fig. 1. In contrast to
the thin and readily deformed amorphous ribbons, the
0.5 mm silicon-based substrates provided the necessary mechanical strength for the ion-beam milling process required
for the HRTEM sample preparation. Consequently, microstructural analysis was performed on CFO/SiO2/Si, which
can be assumed to exhibit a similar morphology to the CFO
deposited on the Co-based ribbons subject to the same
growth parameters. Unlike the deposition of CFO on singlecrystal substrates, such as Si (100),19 Al2O3 (0001),19 SrTiO3
(100),23 and MgO (100),23 using PLD, for which the crystal
lattice of the substrate surface assisted the nucleation of polycrystalline CFO nano-islands during the initial growth
phase,20 the use of an amorphous substrate prevents their formation. This is evident in the cross-sectional HRTEM
images shown in Figs. 1(a) and 1(b) for the 50 nm thick CFO
film grown on amorphous SiO2/Si. From this figure, it can be
seen that although the CFO layer makes a sharp interface
with the substrate, the presence of a thin (3 4 nm) layer of
SiO2 (observed in all images as a result of surface oxidation
of single crystal Si (100) substrates) prevented a direct interface between CFO and the underlying Si (100) surface,

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J. Appl. Phys. 116, 123912 (2014)

FIG. 1. (a) and (b) Cross-sectional

HRTEM images captured at different
locations along the interface of 50 nm
thick CFO coating deposited on amorphous SiO2/Si (100) substrates under
the same conditions as CFO coated ribbons using PLD; (c) typical SAED pattern obtained near the interface of the
CFO coating on SiO2/Si substrate; (d)
representative EDS spectrum obtained
from the amorphous CFO layer showing stoichiometric composition within
error limit of 0.01 atomic percent.

eliminating a preferred direction for the formation of CFO.

As a result, the initial CFO layers did not exhibit any longrange polycrystalline structure and were mostly amorphous
in nature. However, as more and more flux of ablated species
arrived at the heated substrate, the adequate substrate temperature possibly resulted in the crystallization of the subsequent layers. In Figs. 1(a) and 1(b), a well-defined crystal
structure with continuous sharp lattice fringe spacings is
observed far from the substrate, consistent with the facecentered cubic CFO crystal structure. The crystal planes of
CFO as marked in this figure were identified from the lattice
spacings. Also within each grain boundary (marked by white
dashed lines in Figs. 1(a) and 1(b)), the grains exhibited
single-crystalline nature with a size distribution of
1030 nm, suggesting that the CFO coatings were composed
of single-crystal nano-grains.24 The overall polycrystalline
nature of the CFO coatings is evidenced from the selected
area electron diffraction (SAED) pattern in Fig. 1(c) obtained
near the interface. EDS spectra collected from different
zones of the amorphous CFO layer (Fig. 1(d)) revealed a
stoichiometric composition with the atomic % Co:Fe ratio of
1:2 (within an error limit of 0.01 atomic %). Similar characteristics within the CFO layer grown on amorphous
Co65Fe4Ni2Si15B14 ribbons are inferred from the above
analysis.
Figure 2 shows the XRD patterns of CFO-coated magnetic ribbons for various thicknesses of the CFO layer starting from 0 nm (uncoated) up to 600 nm (denoted as
CFO-0 nm, CFO-50 nm, CFO-200 nm, CFO-300 nm, CFO400 nm, and CFO-600 nm, respectively). For CFO-coated
ribbons with d 0200 nm, the XRD patterns showed a typical amorphous behavior with a broad hump peak at low
angles from 20 to 30 . No crystalline peaks were detected
in the scans within the resolution limit of the XRD.

However, staring from CFO-300 nm, one can observe the

appearance of CFO peaks along with the amorphous background of the ribbon. We define dc 300 nm as a critical
thickness at and beyond which the CFO film is of detectable

FIG. 2. XRD patterns of CFO coated amorphous ribbons grown for various
thicknesses of the CFO layer staring from 0 nm (uncoated), 50 nm, 200 nm,
300 nm, 400 nm, and 600 nm, denoted as CFO-0 nm, CFO-50 nm, CFO-100 nm,
CFO-200 nm, CFO-300 nm, CFO-400 nm, and CFO-600 nm, respectively.

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FIG. 3. AFM 3-D images of (a)

uncoated ribbon, (b) 50 nm thick CFO
coated ribbon, (c) 300 nm thick CFO
coated ribbon, and (d) 600 nm thick
CFO coated ribbon, respectively. The
scan areas are 5 lm  5 lm. The zheights are (a) 25 nm, (b) 50 nm, (c)
50 nm, and (d) 250 nm, respectively.

polycrystalline phase. The peaks that appeared match with

the CFO face-centered cubic lattice with a space group Fd3 m (227). The XRD peak intensities increased as the thickness of the CFO layer was increased. This implied that after
a critical thickness (dc  300 nm), crystallization of CFO
occurred on the amorphous ribbons. On the other hand, XRD
scans for the just annealed ribbons (with no CFO coating)
exhibited an amorphous like behavior irrespective of the
annealing time. These results indicated that while the ribbons
remained amorphous in nature, the structure of the CFO film
transformed from amorphous to polycrystalline with an
increase in the film thickness from 0 to 600 nm.
Figure 3 shows the AFM 3-D images of the (a) uncoated
ribbon, (b) CFO-50 nm coated ribbon, (c) CFO-300 nm coated
ribbon, and (d) CFO-600 nm coated ribbon with the z-heights
of 25 nm, 50 nm, 50 nm, and 250 nm, respectively. The scan
areas for all samples were 5 lm  5 lm. From Figs. 3(a) and
3(b), it is evident that there is an increase in the surface roughness with a 50 nm thick CFO layer on the ribbon as compared
with the surface of the uncoated ribbon. As the CFO layer
thickness is increased, the increase in the surface roughness is
observed in Fig. 2. Due to the large surface features for CFO600 nm, a z-height of 250 nm was required for imaging. We
had earlier reported a similar trend in surface roughness for
CFO thin films grown on Si substrates using PLD.19
In order to visualize the enhanced surface roughness
with thicker CFO layers, representative AFM images
acquired under similar magnifications are compared in Fig.
4. The comparison of these images clearly suggests that the
thicker the CFO film, the rougher the surface. The root mean
square surface roughness (Rrms) values increased from
5.2 nm for CFO-50 nm (Fig. 4(a)) to 10.4 nm for CFO600 nm (Fig. 4(b)). Such structural and morphological variations are shown below to have significant impacts on the
magnetic properties and GMI response of the ribbon.

To assess the effect of CFO coating on the magnetic

properties of the ribbon, the magnetic hysteresis M(H) loops
of the uncoated and CFO-coated ribbons were recorded at
300 K. Figure 5 shows the normalized M(H) curves of these
samples. It can be seen that the magnetic hysteresis of all the
samples was minimal and the magnetization reached saturation at small applied fields, indicating their soft

FIG. 4. AFM 3-D images of (a) 50 nm thick CFO coated ribbon and (b)
600 nm thick CFO coated ribbon, respectively, shown on the same scan area
of 2 lm  2 lm and z-height of 100 nm.

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FIG. 5. Magnetic hysteresis loops of uncoated and CFO-coated ribbons.

ferromagnetic characteristics. Relative to their uncoated

counterparts, the CFO-coated samples exhibited slightly
larger susceptibility (see Fig. 5(a), for example, for the
uncoated and CFO-300 nm coated ribbons). As the thickness
of the CFO film was increased from 50 nm to 600 nm, the
shape of the M(H) curves remained almost unchanged (Fig.
5(b)) while the change in coercive field (HC) with the CFO
film thickness was noticeable (Fig. 5(c)). As one can see in
Fig. 5(c), the HC had the smallest value for the CFO-50 nm
sample and it increased with increasing the thickness of the
CFO film. A considerable increase in HC observed for CFO-

J. Appl. Phys. 116, 123912 (2014)

coated ribbons with d  300 nm was likely associated with

the transition from the amorphous to polycrystalline structure of the CFO film.21
In order to understand the impact of CFO coating on the
GMI response of the ribbon, magnetic field and frequency
dependences of GMI ratio (DZ/Z) of the uncoated and CFOcoated ribbon samples were studied systematically. Figure 6
shows, for example, the magnetic field and frequency dependence of DZ/Z for the uncoated ribbon and CFO-coated
ribbons with film thicknesses of 50 nm, 200 nm, and 400 nm.
It can be observed that low frequency MI curves of the samples exhibited a single-peak behavior, whereas high frequency MI curves possessed a double-peak behavior. The
observed single- and double-peak behaviors are associated
with the longitudinal and transverse alignment of magnetic
anisotropy with reference to the external field direction.1,25
It is also noted in Fig. 6 that for all samples investigated,
with increasing frequency, the maximum MI ratio (i.e., [DZ/
Z]max) first increased, reached a maximum at a particular frequency f0 (often defined as a characteristic frequency), and
then decreased for higher frequencies (f > f0). This trend can
be interpreted by considering the relative contributions of
domain wall motion and magnetization rotation to the transverse permeability and hence to the MI.2 At very low frequencies f < 1 MHz (t < dm), [DZ/Z]max was relatively small
due to the dominant contribution of the induced magnetoinductive voltage to the measured magnetoimpedance. In the
range 1 MHz  f  f0 MHz (t  dm), the skin effect was dominant, hence a higher [DZ/Z]max was observed. Above f0,
[DZ/Z]max decreased with increasing frequency. This is
because, in this frequency region, the domain wall displacements were strongly damped owing to eddy currents, thus
contributing less to the transverse permeability and hence
less [DZ/Z]max. A similar explanation can also be applied to
the frequency dependence of g shown later in Fig. 8.
It has been reported that heat treatment26,27 and laser
annealing28 of a soft ferromagnetic amorphous ribbon could
have a significant impact on the MI response of the ribbon.
The MI effect and g are highly sensitive to the annealing
temperature and time. As we noted above, the PLD technique allowed a simultaneous variation in the thickness of
the CFO film and the annealing time. Since the CFO films of
different thicknesses were grown on the amorphous ribbons
at a fixed temperature of 450  C with the same rate of
0.1 nm/s, thicker CFO films took longer time to grow. In
addition to the effect of CFO coating, the annealing effect
(e.g., annealed at 450  C for various times) should also
impact the MI response of the CFO-coated ribbon samples.
Therefore, to isolate the effects of CFO coating, the MI
effect of each coated ribbon was compared with its corresponding control samplethe ribbon annealed simultaneously but completely masked during deposition. Figure 7
shows the frequency dependence of [DZ/Z]max for selected
samples of uncoated (control) and CFO-coated ribbons. As
one can see in this figure, the [DZ/Z]max reached peak values
of 33.3%, 47.7%, and 20.7% for 50 nm, 300 nm, and 600 nm
thick CFO-coated ribbons, respectively, as compared with
17.3%, 48.6%, and 28.9% for their corresponding controls.
These observations are of particular interest. In the case of

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FIG. 6. Field and frequency dependences of the GMI ratio for (a) an uncoated annealed ribbon and coated ribbons with CFO layer thicknesses of (b) 50 nm, (c)
200 nm, and (d) 400 nm.

the control samples, it appears that with increasing the

annealing time, [DZ/Z]max first increased (Fig. 7(a)), reached
a maximum at a certain time (Fig. 7(b)), and then decreased
for longer annealing time (Fig. 7(c)). Since the control samples were annealed at 450  C, well below their crystallization
temperature of 550  C (as provided by MetglasV), heat treatment could not affect their crystallinity. However, annealing
in vacuum could cause relaxation of domain structure to first
increase lT and hence [DZ/Z]max up to its maximum value
for short annealing time and then negate the effects for further annealing. A similar trend has been reported previously
for annealed Co-based28 and Fe-based27 amorphous ribbons.
It is also interesting to note that relative to their control counterparts, the coating of a 50 nm CFO film (Fig. 7(a)) showed
the greatest increase in the MI response among the CFOcoated ribbons. The positive effect of the CFO coating on
MI response became weaker as the CFO thickness was
increased from 50 nm to 300 nm, and was actually negative
for thicker CFO thicknesses (d > 300 nm). These results can
be explained by considering the magnetic flux closure and
surface irregularities due to the deposition of a thin CFO
R

layer.18 Since the CFO film was amorphous in the CFO50 nm/ribbon bilayer (as seen in the XRD), the presence of
the CFO film could allow the magnetic field to penetrate
through the ribbon better than in its control (uncoated) counterpart, thus enhancing lT and [DZ/Z]max. In the case of the
CFO-300 nm/ribbon bilayer, however, the control was
observed to have the maximum lT and the CFO film was
partially crystallized, the flux closure was not sufficient to
further increase lT and hence [DZ/Z]max. The CFO-600 nm/
ribbon bilayer showed presence of polycrystalline CFO
phases that resulted in the formation of rigid and random
magnetic domains (as evidenced by the increase in Hc in Fig.
6(c)). This possibly resulted in the decrease in lT and consequently the [DZ/Z]max.
To better illustrate the effect of CFO coating, we plotted
in Fig. 8 the frequency dependence of [DZ/Z]max (Fig. 8(a))
and g (Fig. 8(b)) for various CFO-coated ribbon samples.
The highest (47.7%) and lowest (20.7%) values of [DZ/Z]max
were observed at f 0.9 MHz and 2 MHz for CFO/ribbon
bilayers with the CFO thicknesses of 300 nm and 600 nm,
respectively. [DZ/Z]max values 33.3%, 42.8%, and 25.3%

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FIG. 8. Frequency dependence of (a) [DZ/Z]max and (b) field sensitivity for
CFO-coated ribbons with varying CFO thickness.

FIG. 7. Frequency dependence of MImax for CFO-coated ribbons and their

control (uncoated) ribbons for CFO layer thicknesses of (a) 50 nm, (b)
300 nm, and (c) 600 nm.

were obtained at f 1.5 MHz for the bilayers with the CFO
thickness of 50 nm, 200 nm, and 400 nm, respectively. The
values of g calculated for 50 nm, 100 nm, 200 nm, 300 nm,
400 nm, and 600 nm CFO-ribbon bilayers at 1 MHz were
determined to be 0.84, 0.98, 2.54, 2.31, 1.08, and 0.85%/Oe,
respectively. It can be seen that although the highest value of
[DZ/Z]max was achieved for the CFO-300 nm sample, the
CFO-200 nm sample showed the largest g among the CFOcoated samples. The reason for this was that the crystallization of CFO in CFO-coated ribbons with d  300 nm broadened the FWHM of GMI curves and consequently reduced g.
Since the CFO-300 nm ribbon and its control had similar values of [DZ/Z]max in the frequency range of 0.113 MHz (Fig.
7(b)), the highest peak of [DZ/Z]max observed in Fig. 8(a) for
this sample could be attributed to the annealing effect, rather
than the CFO coating. We recall that the surface roughness
of the CFO film increased gradually with increasing the film
thickness, and the crystal structure of the CFO film changed

from amorphous to polycrystalline at dc  300 nm. In connection with the GMI analyses, it appears that the largest
GMI ratio and field sensitivity of CFO-coated ribbon samples were achieved near the onset of the structural phase
transition of the CFO film. A similar trend was also reported
by Coisson et al.,29 but for the structural phase transition of a
Co-based ribbon itself. We note that we used the commercial
Co65Fe4Ni2Si15B14 amorphous ribbons to fabricate the CFO/
Co65Fe4Ni2Si15B14 bilayer structures for demonstrating our
concept, so the GMI ratios obtained for the present CFOcoated ribbon samples are smaller than those previously
reported for some Co-based amorphous ribbons.1 If the optimized Co-based ribbons are used, however, one should
expect to achieve higher values of GMI ratio for their CFOcoated ribbons. An important consequence that emerges
from the present study is that we demonstrate the possibility
of using an additional coating layer of CFO to tune and optimize the GMI response of a soft ferromagnetic amorphous
ribbon through controlling the crystallinity and thickness of
this magnetic coating layer, and that PLD is an excellent
technique for this purpose.
IV. CONCLUSIONS

We have systematically investigated the effect of depositing CoFe2O4 films of various thicknesses (d 0600 nm) on
GMI response of an amorphous Co65Fe4Ni2Si15B14 ribbon.
We have observed a structural transformation of the CFO film

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123912-8

Mukherjee et al.

J. Appl. Phys. 116, 123912 (2014)

from amorphous to polycrystalline phases as the thickness of

the CFO film exceeded a critical value of 300 nm. Relative to
the uncoated ribbons, the ribbons coated with amorphous
CFO films showed significantly the enhanced GMI response.
On the contrary, those coated with polycrystalline CFO films
showed the reduced GMI response. The maximum GMI
response was achieved near the onset of the structural transition of the CFO film. The work highlights the PLD as an insitu annealing and coating method for improving the GMI
response of soft ferromagnetic amorphous ribbons for highperformance sensor applications.
ACKNOWLEDGMENTS

The research was supported by Florida Cluster for

Advanced Smart Sensor Technologies (FCASST) and by
USAMRMC through Grant Nos. W81XWH-07-1-0708 and
W81XWH1020101/3349. Metglas/Hitachi Metals America
was acknowledged for providing Cobalt based METGLASV
2714A ribbons.
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