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Article history: We report magnetic and magnetoimpedance (MI) properties of cobalt-rich amorphous alloys to investi-
Received 26 August 2017 gate the role of small quantities of 3d or 4d transition-metal elements in Co-rich alloys. The microstruc-
Received in revised form 17 October 2017 ture, thermal stability, AC soft magnetic properties and magnetoimpedance of the ribbons are
Accepted 18 October 2017
investigated by substituting Nb in place of Ni and Mn. Present study shows an improvement in glass
Available online 23 October 2017
forming ability and reduction in electrical conductivity of the ribbon with Nb substitution. Higher Nb
containing alloy shows minimum core loss compared to other compositions over a range of frequencies.
Keywords:
Ribbon with higher core loss exhibited higher MI ratio (100% at 3 MHz), but decreased rapidly at higher
Magnetic permeability
Core loss
frequencies due to its larger electrical conductivity. The ribbon with lower electrical conductivity showed
AC hysteresis loop a steady MI ratio and field sensitivity with frequency. These results indicate that MI and core losses at
Magnetic anisotropy medium range of frequencies can be tuned by adding Nb that provides most favourable electrical conduc-
Coercivity tivity and magnetic permeability values, which result in optimum skin depth and MI. The effect of elec-
Magnetoimpedance trical conductivity on MI is also validated through numerical simulations using standard electrodynamics
models.
Ó 2017 Elsevier B.V. All rights reserved.
https://doi.org/10.1016/j.jmmm.2017.10.071
0304-8853/Ó 2017 Elsevier B.V. All rights reserved.
468 S.K. Manna, V. Srinivas / Journal of Magnetism and Magnetic Materials 449 (2018) 467–474
saturation magnetization and lower electrical conductivity. It was Alfa Aesar. Subsequently, long amorphous ribbons having 1–2 mm
suggested that Cu increases the nucleation rate of Fe–Si crystallites width and 40–45 lm thickness were obtained by single roller
and favors homogeneous nanocrystallization, whereas Nb inhibits quenching technique. As-quenched ribbons with compositions
the grain growth [10]. Herzer [11] suggested that if grain sizes are Co73Fe4.5(Ni0.5Mn0.5Nb0.5)Si4.2B16.8, Co73Fe4.5(Mn0.5Nb1.0)Si4.2B16.8
below the ferromagnetic exchange length, then as per random ani- and Co73Fe4.5(Nb1.5)Si4.2B16.8 are referred as Rib-I, Rib-II and Rib-
sotropy model, one can achieve soft magnetic character. In addition, III respectively in the following text. The amorphous state of as-
this composite structure leads to the compensation of the kS value quenched ribbons was confirmed by X-ray diffraction study. Ther-
between the amorphous and nanocrystalline phases with opposite mal stability of all the ribbons was investigated by differential
signs of kS values, thus decreasing the magnetoelastic energy [12]. scanning calorimeter (DSC) with a scanning rate of 20 °C/min.
The DC and low frequency AC magnetic measurements on Molybde- Surface and bulk microstructure has been investigated by scan-
num doped (Mo) FINEMET didn’t show significant changes though ning and transmission electron microscopy (TEM). A Philips
the heat treatment resulted in improvement of magnetic parame- CM20 TEM was used for the study of bulk structure of amor-
ters. This is attributed to variations in Fe-Fe inter atomic distances phous/nanocrystalline ribbons. The ribbons were initially polished
due to the change in Mo and Nb atomic diameters [13]. On the other and then a dimple was made at the center of the ribbons by using
hand, it is suggested that amorphous alloys are good candidates for the GATAN Ion milling source. These samples were then loaded
low field magnetic sensor applications, i.e. giant magne- on to a Copper grid to investigate the microstructure. The AC
toimpedance (GMI) effect [14]. These properties are closely related magnetic measurements were performed on ring shaped samples
to specific magnetic domain structure of amorphous ribbon, i.e. under magnetic field (1000 A/m or 12.6 Oe) and frequencies
with single axial domain typical for Fe-rich or high transverse mag- (20 kHz) with a commercial B-H loop tracer setup (Model:
netic domain for Co-rich amorphous ribbons. The GMI effect is a AMH-20 K-S). Impedance measurements on 5 cm long ribbons
classical electromagnetic phenomenon observed when impedance were carried out with an impedance analyser (Model: HP
(Z) of a magnetic element changes on application of magnetic field. 4192A) in the frequency range 500 kHz–13 MHz by passing 10
This change in Z occurs mainly due to the change in transverse per- mA alternating current. A magnetic field up to ±100 Oe was
meability (mt) or skin depth (dm), on application of external mag- applied along the length of the ribbons, using a Helmhotlz coil.
netic field [15]. The dm is related to the transverse magnetic The MI ratio and magnetic field sensitivity (g) were evaluated
permeability, mt, electrical conductivity, r and given by [14]: using an expression – MI(%) = (DZ/Z)% = [(Z(H) Z(Hmax))/Z
1=2 (Hmax)] 100 and g = (d/dH)(DZ/Z), where Z(H) and Z(Hmax) are
2 impedance under applied field H and maximum field Hmax (100
dm ¼ ð4Þ
lt rf Oe) respectively.
Fig. 1. (a) XRD patterns and (b) DSC thermographs of as-quenched (AQ) ribbons (c) ribbon wound in ring shape for AC magnetic measurements (d) TEM image and (e)
corresponding SAED pattern of Rib-I.
Table 1
Experimentally obtained thermal, electrical and magnetic parameters.
Sample Tx1 (°C) Tx2 (°C) DT = (Tx1 Tx2) (°C) r (/ohm-m) Hc at DC (Oe) l (DC) DC hyst. losss (erg/g-s) P (at 50 Hz) (erg/g-s) P (at 500 Hz) (erg/g-s)
Rib-I 470 578 108 6.3 105 0.036 13,530 3.7 1.33 104 83 104
Rib-II 473 583 110 4.8 105 0.114 7126 4.9 0.21 104 19 104
Rib-III 480 608 128 4.5 105 0.064 18,177 6.6 0.04 104 5 104
3.2. Static magnetization bons. The coercivity of the ribbons was also measured precisely
using coercimeter [Model: CR-02] and the values are recorded as
The saturation magnetization values of Rib-I, Rib-II and Rib-III 0.06, 0.34 and 0.15 (±0.01) Oe for Rib-I, Rib-II and Rib-III respec-
are observed to be 128, 127 and 114 emu/g respectively (Fig. 2). tively. The differential susceptibility, vdiff (dM/dH) increases to a
Significant decrease in MS of Rib-III could be due to variations in maximum value at low applied fields and then sharply decreases
elemental moment and exchange coupling strengths between as the field increased (see inset (b) of Fig. 2). The maximum value
matrix and transition elements Ni, Mn and Nb. Nevertheless, the of vdiff was observed for Rib-III, whereas it is almost equal for Rib-I
MS values of presently studied alloys are higher than the values and Rib-II.
reported in the literature on Co-Fe-B-Si alloy system [27,28]. From
Fig. 2 it can be seen that the coercivity of all samples is fraction of
an Oersted, which indicates ultra-soft magnetic nature of the rib- 3.3. AC magnetic properties and core loss
The hysteresis loops were recorded in the frequency range DC in the core loss with frequency could be attributed to eddy current
to 20 kHz with a maximum magnetic field (Hmax) of 12.6 Oe loss at higher frequencies.
(1000 A/m) and depicted in Fig. 3(a–c) at some selective frequen- A remarkable improvement in core loss of Rib-III can be seen at
cies. The magnetic parameters, such as, Bm, Coercivity (BHC), core higher frequencies compared to that of Rib-I and Rib-II. Further the
loss (P) were obtained from the room temperature hysteresis data maximum magnetic induction value (Bm) and lower BHC value
measured at different frequencies. As the frequency of the excita- remain essentially constant with frequency for Rib-III up to 20 kHz.
tion field is raised, the area under the loop increased due to Fig. 4(a) describes the total core loss (Pt) variation with fre-
increase of eddy current loss with frequency [29]. A contrasting quency at constant flux density, Bm = 1 kG. This figure shows Pt
frequency response of hysteresis loops is observed in three cases. varies very rapidly in Rib-I compared to Rib-II and Rib-III and sug-
For Rib-I the loop area changed rapidly with sharp increase in coer- gests that Rib-I suffers maximum loss, due to its large eddy current
civity, core loss and decrease in Bm with increasing frequency of the loss associated with higher electrical conductivity. Fig. 4(b) shows
AC magnetic field. However, increased Nb content in sample Rib-II the corresponding trend in the variation of coercivity (BHC) with
restricts the rapid changes in hysteresis parameters with frequency frequency. The BHC values for all ribbons initially increased linearly
and interestingly these parameters are least affected in the case of with frequency and then decreased slightly above a characteristic
Rib-III as listed in Table 1. It can be seen that the hysteresis loss frequency. This occurs when the magnetization due to the driving
increases with increasing Nb content in the sample. The increase field is low enough, and the value of H(t) needed to make M(t)
equal to zero is reduced [30]. It is interesting to note from the fig-
ure that maximum Nb containing ribbon (Rib-III) shows lowest
coercivity as compared to other two compositions in the whole fre-
DC (a) Rib-I quency range (DC to 20 kHz).
0.2 KHz Variation of lr with field for different frequencies is shown in
0.5 KHz the inset of Fig. 4(c) for Rib-I. It can be observed from the figure
2 0.7 KHz that lr goes through a maximum at certain H for a particular fre-
quency. The initial increase in lr is due to domain wall motion in
magnetization process and the decrease at higher fields is because
B(kG)
20.0 KHz
0 Z Z Z
dM irr
l0 M an dHe ¼ l0 MdH þ l0 kdð1 cÞ dHe ð5Þ
dHe
-2
where, the first term on the right-hand side represents the magne-
tostatic energy, and the second term is dissipation loss due to pin-
-4 ning of magnetization vector. In this equation He = H + aM, the
coefficients k and d are the pinning parameter and directional
-12 -8 -4 0 4 8 12 parameter respectively. dH/dt is positive for d = +1 and negative
H (Oe) for d = 1. The amount of reversible change in magnetization is
given by constant c. When hysteresis is recorded under time vary-
Fig. 3. B–H loops of (a) Rib-I, (b) Rib-II and (c) Rib-III at different frequencies. ing fields the energy losses appear due to changes in the irreversible
S.K. Manna, V. Srinivas / Journal of Magnetism and Magnetic Materials 449 (2018) 467–474 471
Fig. 4. Variation of (a) total core loss, Pt (Bm = 1 kG), (b) coercivity, BHC (Hm = 12.6 Oe), (c) maximum relative permeability (max. lr) and (d) maximum flux density (BS) with
frequency for all ribbons. Inset of (c): lr variation with H for Rib-I.
magnetization Mirr. In addition the eddy current losses arise in elec- ability. When Hext exceeds HK, the transverse permeability is
trically conducting media, which has to be added to the right-hand decreased due to the longitudinal field Hext which tries to rotate
side of Eq. (5) and gives the expression for hysteresis loops with AC magnetization in the direction of external field. As a consequence
magnetic field. When both excess and classical losses are added in with increasing Hext, skin depth increases and result in decrease
the energy equation features like increase in coercivity, energy loss of MI(%). The double peak behavior of all AQ ribbons in the fre-
per cycle, the invariance of remanence with frequency were repro- quency range of present study (0.5 MHz to 13 MHz) indicates the
duced [32]. presence of transverse magnetic anisotropy [15]. On close observa-
tion of MI curves, one can see the HK value for a particular sample
3.4. Magnetoimpedance properties increased with increasing frequency. For example, HK of Rib-I
increased from 3 Oe to 7 Oe when frequency changed from 0.5
The impedance, Z of the ribbons was measured as a function of MHz to 13 MHz. The shift in HK with increasing frequency of all
external DC magnetic field, H at various frequencies up to 13 MHz. ribbons is depicted in Fig. 6(a).
Fig. 5(a–c) shows the variation of MI(%) as a function of external DC The shift of HK towards a higher value of Hext is probably due to
magnetic field, H for Rib-I, Rib-II and Rib-III at some representative large eddy current effect with increasing frequency (f 5 MHz). At
frequencies – 0.5, 3, 7 and 13 MHz. For all ribbons at a particular higher frequency the domain wall displacements were strongly
frequency, the MI(%) is seen to increase up to a certain switching damped by eddy current pinning and give larger HK value. Another
field, known as the anisotropy field, HK and thereafter it gradually interesting aspect of MI% vs H curves is that the dip between the
decreases with the field. two peaks at origin is largest for Rib-II, and lowest for Rib-III. This
This type of MI profile is termed as double peak MI profile, and depth profile suggests large number of transverse domains present
the origin of double peak behavior can be explained by the facts: in Rib-I and Rib-II, compare to Rib-III. The maximum MI ratios for
There are two kinds of magnetic anisotropy acting on the ribbons, Rib-I, II and III are 100%, 86% and 92% respectively have been
one corresponds to transverse anisotropy and other is DC axial observed at 3 MHz. As the skin depth depends on frequency of
magnetic field. In the low field region, close to origin, the external AC field, these above observations can be interpreted by the com-
magnetic field (Hext) tries to overcome the transverse anisotropy bination of inductive and resistive parameters such as, permeabil-
and permeability increases. On further increase in Hext, the magne- ity (lr) and electrical conductivity (r) of the ribbons. Rib-I has
tization vector overcomes the existing transverse anisotropy, when larger r (6.3 105/ohm-m) and moderate lr value (13,500)
it reaches HK. At this point the magnetization responds quickly to and exhibits highest MI(%). This is consistent with most magneti-
external magnetic field and gives rise to a large transverse perme- cally lossy character (see Table 1). Rib-III higher lr (18,500) and
472 S.K. Manna, V. Srinivas / Journal of Magnetism and Magnetic Materials 449 (2018) 467–474
-100 -80 -60 -40 -20 0 20 40 60 80 100 important factors that should be satisfied by material [20]. A com-
petition between lr and r to results in optimum skin depth, dm
100 0.5 MHz
(a) Rib-I according to Eq. (4). It may be speculated that magnetically lossy
3.0 MHz materials with reasonable lr can generate higher MI values as
80 7.0 MHz shown in the case of Rib-I. Chaturvedi et al. [22] reported surface
13.0 MHz smoothness of Co69Fe4.5X1.5Si10B15 ribbon improved when X was
60 replaced by Ni, which indeed enhanced the MI(%). This might be
also a reason behind the largest MI(%) in Rib-I. Fig. 6(b) shows
40 the magnetic field dependence of sensitivity, g at different fre-
quencies for Rib-I. The maximum g value (gmax) was observed at
20 very low field (H < HK) due to sharp change in MI(%). The variation
tendency of g in low fields is consistent with that in MI variation
0 as shown in Fig. 5. Same trend in g variation with H was also
observed for other two ribbons. Fig. 7 displays the frequency
80 dependent maximum MI ratio (MI(%)max) and its maximum field
(b) Rib-II sensitivity (gmax) respectively for all ribbons. It can be observed
that at lower frequency (f 1 MHz) (i.e. dm > a, ribbon thickness)
60 the value of MI(%)max was relatively low due to the contribution
of magneto inductive part to the magnetoimpedance. At moderate
MI(%)
Fig. 6. Variation of (a) anisotropy field (HK) with frequency for all ribbons and (b) field sensitivity (g) with H at different frequencies for Rib-I.
S.K. Manna, V. Srinivas / Journal of Magnetism and Magnetic Materials 449 (2018) 467–474 473
Fig. 7. MI(%)max and gmax variations with frequency for all ribbons.
Fig. 8. Calculated GMI curve with different electrical conductivity (ranging from 2 105 to 15 105/ohm-m) of the FeCo(NiMnSb)SiB ribbons. Side panel: Calculated
variation of MI(%)max with frequency for different electrical conductivity values.
474 S.K. Manna, V. Srinivas / Journal of Magnetism and Magnetic Materials 449 (2018) 467–474
shows the simulated MI curves for different r values, at 5 MHz fre- Acknowledgements
quency. With increasing r, the MI(%) enhanced sharply.
All the simulated curves show double peak nature, indicating The authors acknowledge Prof. K. Balasubramanian, Dept. of
that the parameters used here are suitable for Co based ribbons Mechanical Engineering, Indian Institute of Technology Madras,
(Transverse alignment of magnetic anisotropy). The calculated MI Chennai for allowing us to use some experimental facilities.
(%) value is an order magnitude larger than the experimentally
obtained value. This discrepancy is due to the over simplification Appendix A. Supplementary data
of domain dynamics with the usage ideal parameters in theoretical
modelling. Although the magnitude of MI differs, the trend of MI Supplementary data associated with this article can be found, in
variation with magnetic field and frequency are similar in simu- the online version, at https://doi.org/10.1016/j.jmmm.2017.10.071.
lated data and experiments.
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