3. Theoretical analysis and Measurement
The equivalent input loss factor (
ξ) has been defined as the inverse of the product of
k2 and
Q. It quantifies the ratio between the power conversion and the power loss in the magnetic-to-mechanical energy conversion. Following the previous investigations [
4,
8,
35,
37,
47],
ξ can be written as
where
ce is the loss coefficient for the eddy current,
χ is the magnetic susceptibility of the ribbons,
Q0 is the quality factor under magnetostriction-free conditions. From the right-hand side of Eq. (1), the first term with
ce represents the energy loss for dynamic magnetization procedure, which is affected by the magnetic properties of the ribbon, the second part represents the loss not related to the eddy current. In single ribbons, the eddy current loss dominates after the heat treatment under the annealing temperature far below the crystallization temperature. Following Herzer
et al. [
48], the formula of
ce is expressed as
where
t is the ribbon thickness,
ρel is the electric resistivity,
β is the angle between the average magnetic anisotropy and the ribbon direction.
is the averaged longitudinal magnetization (
JH) normalized to the saturation magnetization (
JS).
w is the magnetic domain width, the formula is given as [
48]
where
is the magnetic exchange length.
A is defined as the exchange stiffness and
K is the anisotropy constant.
Nzz and
Nyy are demagnetization factors along the longitudinal and width direction of the ribbon, respectively. With the help of Eq. (2) and (3), the contribution of the eddy current in Eq. (1) can be rewritten as
Taking into account that the average anisotropy angle
β is close to zero for the ribbons annealed at low temperatures, Eq. (4) is rewritten as
When the magnetic domain width is usually much larger than the ribbon thickness in low-temperature annealed samples, the assumption
w >>
t can be considered in the calculation. Thus, Eq. (5) can be rewritten as
The equivalent loss factor induced by the eddy current loss for the ribbons annealed at low temperature depends only on the variation of χ and fr for the ribbons.
b) Magnetic and magnetomechancial properties
The hysteresis loops of magnetic materials could provide important information on the magnetic properties of materials.
Figure 2(a) shows the dc magnetic hysteresis loops of the samples annealed in air at different annealing temperatures (
TAN) for 20 minutes. The loops show small values of remnant magnetization and
Hc for all the samples, suggesting that the samples remain good soft magnetic properties after the heat treatment in air. As shown in the inset in
Figure 2(a), the values of
Hc basically stay close to 0.1 Oe in the region of
TAN from 370 °C to 450 °C. However,
Hc begins to grow sharply with the increase of
TAN when
TAN exceeds 450 °C. In this case, the change of the chemical concentration causing the ordered clusters, the subsequent topological and chemical long-range orderings on the surface of the ribbons results in the variations in the values of
Hc [
31,
33,
34,
36,
47,
49]. When
TAN is above 500 °C,
Hc shows a burst increase which suggests further deterioration in the soft magnetic properties. This is due to (1) the increasing fraction of the surface crystallization at high
TAN; (2) a film of boron oxides formed with excessive boron atoms which are separated from the α-Fe crystallites, since the α-Fe crystallites have much lower solubility of B than that of amorphous Fe [
4,
22,
28,
31,
33,
36]. Consequently, the magnetic domains in the amorphous remainders are thinned and turned to the out-of-plan direction by the compress stress that are induced by the surface crystallization and surface oxidation films [
4,
22,
28,
31,
33,
36], leading to the increasing of
Hc.
In our previous work, we have reported the
TAN dependency of
k and
Q for single FeSiB ribbons, the value of
k reaches its maximum around
TAN of 430 °C, while
Q shows a minimal value around
TAN of 410 °C [
4]. The
k2 and
Q-1 evolution after annealed at various temperature
TAN are shown in
Figure 2(b). In low
TAN region below 400 °C, with increasing
TAN,
k2 increases while
Q-1 decreases at almost the same pace, indicating
k2 and
Q-1 are correlated in low annealing temperature region. For higher
TAN from 400 °C to 500 °C, the variation of
k2 and
Q-1 become non-synchronous, indicating the correlation level of these parameters drops significantly. As a result of synchronous change of
k2 and
Q-1 for low
TAN below 400 °C, the equivalent input loss
ξ stays almost invariable for low
TAN below 400 °C, as reported by our earlier investigations [
4].
c) Softening of magnetic and elastic properties
Figure 3 shows the measured values of the inductance (
L) at 10 kHz after isothermal annealing at various temperature
TAN, it can be observed that
L increases with
TAN in the region from 350 °C to 410 °C, then decreases for
TAN from 420 °C to 490 °C. According to the formula
, the values of
L are proportional to the magnetic permeability (
μr) of the ribbon. Similar behavior of
μr can also be observed from the magnetic hysteresis loops in
Figure 1(a).
Figure 4 shows the
TAN dependence of resonant
fr and anti-resonant
fa. It can be observed that in low
TAN region, both
fr and
fa decrease with the increase of
TAN and reach a minimal value at 410 °C. Then they rise as
TAN continues to increase. Following the formula of
, the values of
fa is related to
E of the ribbon [
8]. Besides, it can be observed in
Figure 4 that
fr-curve and
fa-curve has almost the same pattern and the similar amplitudes, which indicates that
fr also reflects the change of
E. By comparing the behavior of
L and
fa (
fr) versus
TAN, it can be noticed that the two parameters exhibit a respective extreme value as the function of
TAN. However, the curves of
L and
fa show a lag of 20 °C versus
TAN to reach their max/min values.
By comparing the
TAN-dependence of
L with
TAN-dependence of
Q-1 factors, it can be observed that the variations of
L and
Q-1 with the increase of
TAN are almost the same below 400 °C, the
fa (
fr) has similar profile with
k factor. According to Eq. (6), the trend of
k and
Q are recognized as the competition of the magnetic and mechanical properties,
χ and
fa (
fr). Since the
L-curve and
Q-1-curve shares the same trend and same extreme value point of
TAN below 410 °C, while
fa (
fr)-curve and
k-curve show the inverse trend and same extreme value point of
TAN below 430 °C, it is probable that
L or
μr is dominant on the values of
Q-1 factors while
fa (
fr) or
E has the dominative effect on
k factor for the low
TAN below 410 °C (for
L and
Q) or 430 °C (for
fa and
k). Moreover, because
k and
E are related to each other, the annealing experience though
α-relaxation has an important influence on the softening in elasticity below 430 °C [
4]. For higher
TAN, because of the emerging of the surface crystallization and the long-range chemical orderings with B oxidation during the annealing procedure, the competition of magnetism and elasticity becomes much more complex, leading to the divorce between
k2-curve and
Q-curves as well as between
fa (
fr)-curve and
L-curve versus
TAN [
4,
31,
33,
34,
36,
38,
47].
Below 410 C-
TAN, the
β-relaxation in Fe-lack zones was dominant and lead to the chemical short-range ordering (CSRO) in Fe-rich zones with the doped B atoms by diffusion[
4]. In addition, the topological short-range ordering (TSRO) also occurs at this low
TAN region as another result of
β-relaxation, leading to the releasing of internal stress, both of which alleviate the pinning effect of the magnetic domain by defects in the sample [
4], the expanding speed of magnetic domain increase therefor, i.e.
L (
μr) increases. For
TAN from 450 °C to 500 °C, the sharp decrease of
L (
μr) may be due to the emerging of surface crystallization together with more severe surface oxidation that leads to the apparency of the grain boundary as well as magnetic anisotropy deviating from the long axis direction, both of which inhibit the movement or rotation of the magnetic moment of the magnetic domain, resulting in the smaller variation rate of the magnetic moment. The increase of
Hc above 450 °C also coincides with the decrease of
L (
μr), suggesting the deterioration of the soft magnetic properties in high
TAN region.
The decrease of
E in the low
TAN region suggests that the deformation quantity of the ribbon becomes smaller with the increasing
TAN. According to previous studies [
4,
38], as a result of
β-relaxation for low
TAN, besides of the increasing of Fe-Fe bond caused by the CSRO, the TSRO could also be triggered by
β-relaxation close to the cluster-matrix boundaries. The TSRO brings a decrease in the ductility of the sample, thus the sample becomes “more flexible” to be stretched. Consequently,
E (
fa and
fr) becomes smaller after annealed at relatively low temperature and reaches minimum at 430 °C, as shown in
Figure 4. The
E (
fa and
fr) vs.
TAN curve switches to an increasing trend when
TAN exceeds 430 °C. This can be attributed to the apparency of
α-relaxation, which is more intensive and usually occurs at high
TAN. This
α-relaxation further enhances the diffusion of the atoms, affecting the atomic orderings in a larger scale and usually reshaping the clusters. Fe or metalloid atoms experiencing a long-term relaxation in the B-rich area leads to the generation of some clusters with high elasticity that increase the values of
E. In addition, because the annealing procedure in this article is taken in air, the oxidation is more strongly and penetrates deeper in the ribbons at high
TAN, this also has a strong influence on the rigidity of the ribbon [
4,
20].
From
Figure 3 and
Figure 4, it can be obtained that the variation trends of magnetic susceptibility
χ (
χ is also proportional to
L in
Figure 3) and resonant (anti-resonant) frequency
fr (
fa) are synchronous but opposite for low
TAN from 350 °C to 400 °C, the product of
χ and
fr (
fa) remains close to a constant. Besides, the measured
h, relating to
k2Q, is nearly a constant value in this region of
TAN following our previous investigations[
4,
25]. Therefore, according to Eq. (1), it could be inferenced that the loss factor
ce which represents the eddy current loss should be basically unchanged for low
TAN from 350 °C to 400 °C for the single FeSiB ribbons. This is consistent with our analysis in the theoretical section as well.
When
TAN approaches to the crystallization temperature (
Tx) of the FeSiB glassy metals, the size of the magnetic domain decreases due to the change of surface stress [
4,
34,
36]. According to Herzer
et al. [
4,
8,
35,
37,
47,
49], the loss factor
ce is related to the width of magnetic domain
w, following the Eq. (2). Therefore, the synchronously changing behavior of
k2 and
Q-1 suggest that the improvement of the soft magnetic properties may derive from the increase of the numbers of the activated magnetic units rather than the variation of the width of magnetic domains in low
TAN region. Thus, the values of
ξ for the ribbons annealed at low
TAN remaining constant is more due to the increase of the quantity of magnetic units, rather than the change in the domain size.
d) Time-Temperature equivalence for the annealing
Figure 5 (a) and (b) displays the variation of
k,
k2Q and
Q factor for different annealing times
tAN at
TAN from 470 °C to 490 °C, respectively. A significant decrease of
k factor with the increase of
Q factor occurs with the increase of
tAN for
TAN of 470 °C and 490 °C. The curve of
k and
Q show a cross profile at
tAN = 40 minute and 15 minutes, respectively. After the ribbons are annealed for 40 minutes at
TAN = 470 °C and 15 minutes at
TAN = 490 °C,
k decreases approximately from 60% to 40%, while the values of
Q increase close to 200. The equivalent input loss factors
ξ show a max value when
tAN is 20 minutes for both samples, which suggests the optimal annealing time for the annealing at 470 °C and 490 °C. Based on the data mentioned above, it is implied that the decrease in
k is caused by the surface oxidation and surface crystallization that induces the increase of the coercivity by the out-of-plane magnetic anisotropy. The increase of
Q factors might be due to the long range-orderings that take place in the surface regions of the ribbons.
The
Q factor represents the quality of mechanical performance in our FeSiB ribbons, a high value in
Q factor indicates a high ratio between the storage power to the power loss. From
Figure 5(a) and (b), it can be observed that the overall trend of
k,
k2Q and
Q curves at 470 °C
TAN are similar to that at 490 °C
TAN, separately. Besides, the increase of
TAN from 470 °C to 490 °C narrows the
TAN window before the magnetomechancial properties deteriorate obviously. In terms of the
h factors, it is similar to increase
TAN for a constant
tAN or to increase
tAN at a fixed
TAN, which suggests that
TAN and
tAN have equal effect on the
h factor in the heat treatment procedure for the FeSiB ribbons to some extent. However, the equivalence of
tAN and
TAN in terms of the magnetomechanical power conversion efficiency seems to exist only at relative higher
TAN, we do not observe this equivalence with
TAN below 400 °C.
e) Magnetomechancial properties in epoxy-ribbon composites
A schematic diagram of a laminated composite consisting of magnetostrictive amorphous FeSiB ribbons bonded by epoxy resin is given in
Figure 6(a). Several FeSiB foils are fabricated by using hot-pressing techniques and an A-B part epoxy. The should-be ratio between the epoxy (A part) and the curing agent (B part) is 3:1.
Figure 6(b) is a photo of the laminated FeSiB composites, we apply a dc magnetic field along the laminated composite, as shown in the upper part of
Figure 6(b). The ratio between the quantity of magnetostrictive layers and the quantity of epoxy resin is varied to investigate the change of
k,
Q, and
k2Q in FeSiB laminated composites with different foil numbers. The results are given in
Figure 7(a). It is found that as the number of FeSiB layers increases, the
k factors increase slightly and then decrease rapidly, while the
Q factors show an overall increase trend to a maximum close to 400, corresponding to a foil number from 18 to 21 in the FeSiB laminates. The efficiency factor
k2Q firstly increases for more FeSiB ribbons layers, and then reaches a relatively stable value around 25 corresponding to the FeSiB foil number from 12 to 21.
Figure 7(b) shows the trend of the -3 dB bandwidth (
Δf) and
E for the FeSiB laminated composites with different foil numbers.
In
Figure 7(a), it is observed that when the foil number is small, there is no obvious similarity or correlation between the
k and
Q factors as FeSiB layer numbers varies. The
k and
Q in the laminated composites with 9-layers, 6-layers, and 3-layers of FeSiB ribbons are examples. But for the laminated composites with more foil number of 12-layers, 15-layers, 18-layers and 21-layers, the data suggest that there is a mutually exclusive relationship between the
k and
Q factors. This causes the
k2Q factors reaching a relatively stable state and that the
k2Q factors does not continue increasing with the increase of the FeSiB layer number. For the record, it is needed to particularly emphasize that the ratio between epoxy and curing agents is
not 3:1. The amount of the curing agent is reduced, giving a ratio less than 3:1 between the epoxy and the curing agent, so the epoxy resin was not fully solidified for the laminated samples. Thus, the mechanical loss due to the inter-friction is increased comparing to the samples with fully cured epoxy. Unlike the eddy current loss in the single-foil ribbons, the dominant loss in the FeSiB laminates is ascribed to the mechanical loss that triggers the temperature rising when the laminated composites are driven under high power conditions.
According to previous research, as
TAN approaches to
Tx, the size of the magnetic domain decreases due to the change of surface stress [
4,
34]. As mentioned above, the efficiency of a single-foil ribbon experienced a low
TAN remains constant, and this is more due to the increasing of the number of the magnetic units, rather than the change in the magnetic domain size. In contrast, the increase of the
k2Q factors at
TAN above 450 °C is due to the reduction of magnetic domains size. Following the Eq. (1), because the
k2Q factors of the laminated FeSiB composites is approximately a constant for high layer number laminates, and because the variation trend of
E (associated to
fr and
fa) and the bandwidth (associated with χ) of the laminated FeSiB composites remains consistent with each other for all the foil numbers,
ce of the laminated composites should remain constant, too. As the foil number of the FeSiB laminates decreases, the volume proportion of magnetostrictive materials (FeSiB) in laminated composite gradually increases. Using similar analyzing principle to
Figure 7(a), the reason for the constant values in
k2Q factors for the ribbons with the foil number from 12 to 21 is probably due to the increase in the number of ribbons, rather than the change in the relative fraction of the ribbons. The reason for the change in the
k2Q factors for the laminates with the foil number from 3 to 12 is due to the variation of the relative volume fraction of FeSiB ribbons, but rather than the variation in the ribbon number. That is to say, the change in
k2Q factors between the laminates with the ribbon number from 3 to 12 derives from the relative size of the magnetic units, which corresponds to the relative volume fraction of FeSiB ribbons in the laminates; while the constant
k2Q factors between the 12-layers and 21-layers laminates come from the change in the number of magnetic units, rather than the change in relative volume of magnetic units.