This article focuses on the modeling of the hysteresis loop featured by Fe-Cu-Nb-Si-B nanocrystalline alloys with transverse induced anisotropy. The magnetization reversal process of a magnetic correlated volume (CV), characterized by the induced anisotropy Ku, and a deviation of the local easy magnetization direction featuring the effect of a local incoherent anisotropy Ki, is analyzed, taking account of magnetostatic interactions. Solving the equations shows that considering a unique typical kind of CV does not enable accounting for both the domain pattern and the coercivity. Actually, the classical majority CVs obeying the random anisotropy model explains well the domain pattern but considering another kind of CVs, minority, mingled with classical ones, featuring a magnitude of Ki comparable to Ku, is necessary to account for coercivity. The model has been successfully compared with experimental data.

The nanocrystalline Fe-Cu-Nb-Si-B Finemet type alloys are characterized by a very low coercivity (Hc<0.5A/m), comparable to the one featured by NiFe permalloys type crystalline alloys, or Cobalt based amorphous alloys (Hc0.3A/m), while exhibiting far greater spontaneous magnetization Js1.2T compared to 0.55T for Co based amorphous or 0.75T for Permalloys.1 In addition, the low thickness (around 20μm) of nanocrystalline ribbons, combined with a relatively high resistivity, dealing with metallic alloys, (ρ115μΩcm1), allow to obtain wound cores with low eddy current losses. As a result, this family is now widely used in middle frequency applications.

The remarkable magnetic specificity of those alloys, compared with classical crystalline ones, is that the thickness of a domain-wall (DW) is greater than the typical size D of a nanograin. As a result, the randomly distributed easy magnetization directions (EDs) featured by nanograins lead, at the scale of the DW, to an averaged effective anisotropy of amplitude KeK1, K1 denoting the magneto-crystalline constant relative to the nanocrystalline SiFe phase. More accurately, as explained by the random anisotropy model (RAM),2 the magnetic correlation length obeys LcoA/K1, with A the exchange stiffness and K1 the mean fluctuation of the magneto-crystalline anisotropy averaged on a magnetic correlated volume (CV) Lco3. With D classically around 12nm, vanishing K1 is obtained. In this limit, Keff is controlled by additional contributions, as the magnetoelastic anisotropy, explaining that the optimized alloys correspond to a resulting magnetostriction λs0, obtained when the magnetostriction of the residual amorphous phase balances the magnetostriction of the crystalline phase. The almost perfectly flat energetic landscape fulfilled by optimized ribbons allows developing coherent induced anisotropy, with magnitude denoted Ku in the following. Ku is obtained by means of dedicated annealing treatments, i.e. applying during annealing a magnetic field Han,2 a high magnetic field3 (i.e. μ0Han>1T, usually provided by a superconducting magnet), or a tensile stress.4–6 From an applicative point of view, the case of transverse Ku, i.e. ED perpendicular to the direction of the applied field Ha, is of great interest, leading to a practically linear behavior Jm(Ha), Jm denoting the macroscopic polarization, with a slope adjusted by the parameters (magnitude of the field or stress) applied during the annealing treatment. This case is illustrated on Fig. 1.

FIG. 1.

(a): Schematic representation of the field annealing process and the induced strip domain structure obtained after annealing. The resulting coherent rotation magnetization mechanism is illustrated on a plane ribbon. (b): Half-loop obtained after transverse field annealing applied on a Nanophy® core. The anisotropy constant Ku is obtained measuring the dashed surface.

FIG. 1.

(a): Schematic representation of the field annealing process and the induced strip domain structure obtained after annealing. The resulting coherent rotation magnetization mechanism is illustrated on a plane ribbon. (b): Half-loop obtained after transverse field annealing applied on a Nanophy® core. The anisotropy constant Ku is obtained measuring the dashed surface.

Close modal

According to the RAM, the macroscopic magnetic properties featured by nanocrystalline ribbons result from the statistical behavior of CVs, but most of the attention of the dedicated literature is centered on the modeling of the coercivity. The aim of this paper is to extend the analysis to the description of the hysteretic loop, through an analytical formalism. We’ll focus on cores featuring transverse Ku, especially interesting regarding applications, as written above. From the modeling point of view, another positive point is that with Ku great enough, DWs displacements, with their inherent complexity, are negligible, compared to coherent rotation magnetization mechanism contribution.

This article develops previous results,7 with a revised rigorous modeling of magnetostatic interactions (Sec. II B), a much more detailed study of the contribution of hard Correlated Volumes to the magnetization, with an accurate description of the different scales involved (Sec. III, introduction), completing analytic formulations (Sec. III B), illustrating the role of magnetostatics in the asymmetry featured by local loops (Sec. III C). The discretization of the continuous distribution of hard Correlated Volumes was improved, leading to much more satisfactory simulated macroscopic contribution (Sec. III D). At least, the approach leading to the analytic estimation of the mean deviation of the local easy axis is detailed in  Appendix.

Wounded Nanophy® cores featuring typical composition Fe73Cu1Nb3Si16B7 were provided by Aperam Alloys Amilly Company for experiments. Dimensions of the cores were outer diameter Dext=3cm, inner diameter Din=2.5cm and height h=1cm. Those cores were annealed under transverse field, as pictured on Fig. 1a, with typical duration one hour and annealing temperature 550 °C, under hydrogen atmosphere in the G2Elab furnace. After annealing, cores were characterized by fluxmetric measurements. Loops were performed at frequency f=0.5Hz, i.e. in the quasi-static regime, a typical one being plotted on Fig. 1b. Ku=16.2J/m3 was determined measuring the dashed area delimited by the decreasing branch of the loop. This value will be used in the following for numeric evaluations.

As explained in the introduction, the anisotropy experienced by CVs is mainly due to the coherent transverse anisotropy Ku. It is worth noting that if Ku was acting alone, the macroscopic law Jm(Ha) would be perfectly linear, until saturation, with a reference susceptibility μ0χref=Js2/2Ku. As shown on the experimental loop illustrated on Fig. 1b, the coercivity is non null, and usually attributed to a residual uncoherent anisotropy. For analytical convenience, this anisotropy is assumed to exhibit the same symmetry that the coherent one, i.e. uniaxial, Ki (subscript i as intrinsic) denoting its typical magnitude.

The coexistence of those two anisotropies was extensively treated by Herzer et al.2,6,8–10 According to Ref. 8, the effective anisotropy constant Ke obeys

(1)

Following Herzer, we consider that the residual magneto-crystalline anisotropy, averaged over the scale of CVs, is the main origin for Ki for most of the CVs. Those CVs are thus considered "typical" and, obeying the RAM formalism, will be denoted CVRs in the following, devoted parameters being labelled with superscript R. According to Ref. 6, KiR verifies

(2)

with x the crystalline volume fraction, β=0.4 a factor reflecting the cubic symmetry of the crystals, L040nm the basic exchange length related to K1=8kJ/m3. This value corresponds to the composition of the nanocrystalline phase after crystallization, i.e. Fe80Si20 atomic [Ref. 11, fig. 2.10], the dependence of K1 with composition being obtained from Ref. 12. Typical values corresponding to the anneals are x0.7, D=13nm [Ref. 11 Fig. 2.9], Ref. 13. With Ku=16J/m3, (2) leads to KiR=0.17Ku. With (1) (replacing Ke and Ki by KeR and KiR), one obtains KeR=1.014Ku. As a result, KeR is approximated to Ku.

Dealing with the ED resulting from the superposition of Ku and KiR, ones have to take in mind that, due to magnetostatic energy, the magnetization vector, at the scale of the magnetic domains, lies in the plane of the ribbon. As a result, we simplify the description, not considering the absolute easiest direction featured by a CV, but the easiest direction in the ribbon plane. The direction of this one can be described by a single variable, θED, referenced to the direction of Ha. Noting εR the mean deviation of the local ED, two kinds of CVs are thus considered, noted by subscript + or , with θED+=π/2εR and θED=π/2+εR (cf. Fig. 2), the polarizations being associated to angles θ+ and θ (cf. Fig. 2). The energy featured by a CV is made up of the anisotropic contribution, with uniaxial symmetry, the Zeeman contribution (= applied field energy), and the magnetostatic one (long range interaction with surrounding CVs). Normalizing by Ku, the resulting reduced energy densities are thus written:

(3)
(4)

where ha=0.5JsHa/Ku denotes the reduced applied field, keR=KeR/Ku the reduced anisotropy, (=1), u+ and u referring to the magnetostatic energies.

FIG. 2.

Representation of each kind of typical CV (in white) interacting with the surrounding medium in a Weiss Domain (the EDs are dashed). (a): Configuration Ca; (b) and (c): Configuration Cb in two consecutive Weiss Domains D1 and D2. Dealing with Cb, the differences between polarizations j+ and j belonging to the same domain are strongly exaggerated for clarity.

FIG. 2.

Representation of each kind of typical CV (in white) interacting with the surrounding medium in a Weiss Domain (the EDs are dashed). (a): Configuration Ca; (b) and (c): Configuration Cb in two consecutive Weiss Domains D1 and D2. Dealing with Cb, the differences between polarizations j+ and j belonging to the same domain are strongly exaggerated for clarity.

Close modal

The magnetostatic energy is a key point in the description of soft granular systems, but is often neglected dealing with continuous media, as in Refs. 14–17. As pointed out by the pioneer work of Néel,18,19 this should not be the case. We so present here a way to account for it.

It is worth noting that the CV must be considered immersed in a tridimensional environment. Indeed, even if for a magnetic domain, the magnetization vector is kept in the ribbon by the dipolar field, the characteristic length of a CV LcoA/KeRA/Ku 1μm, with A1.51011J/m20 is far small than the ribbon thickness, around 20 μm.

The modeling of interactions of a peculiar CV with the surrounding CVs is a very difficult challenge because of the great number of variables. A classical way to simplify the problem is to work in the frame of a mean field theory, as it will be done here. This kind of approach consists in replacing the surroundings CVs by an equivalent homogeneous medium (HM in the following), featuring a mean polarization JD=JCVD, i.e.

(5)

the subscript D indicating the magnetic domain the peculiar CV belongs to. j+()=cosθ+()ux+sinθ+()uy denotes the polarization of each kind of CV (the reference system is indicated on Fig. 2), and jaD the mean polarization of the amorphous phase, at the scale of the considered domain. The problem is further simplified, noticing that the SiFe phase is the most representative one (x0.7), and thus considering x=1 in (5).

In addition, the HM features an effective susceptibility χ, assumed isotropic and uniform for analytical convenience. This means that the HM locally adapts to a local fluctuation of magnetization induced by a fluctuation of the ED at the scale of the given CV, with a resulting non uniform polarization JDJD. As a result, the vicinity of a peculiar CV acts as a shielding shell, reducing drastically the magnetostatic energies, compared to the situation featured by a HM with uniform polarization.

To quantify this effect, one starts from the reference state pictured on Fig. 3a where the polarization is uniform everywhere, i.e. JCV (thin arrow) =JD (bold arrows), noticing that the directions of Ha and JD are considered different because JD is the average polarization at the scale of a magnetic domain, different from the macroscopic polarization Jm=JD , where the external brackets indicate an average of JD on a significant number of domains.

FIG. 3.

(a): reference state: JCV=JD ; (b): Due to local fluctuation of ED, the direction of JCV differs from the averaged polarization. As a result, magnetic charges appear at the interface, leading to a dipolar field outside the CV.

FIG. 3.

(a): reference state: JCV=JD ; (b): Due to local fluctuation of ED, the direction of JCV differs from the averaged polarization. As a result, magnetic charges appear at the interface, leading to a dipolar field outside the CV.

Close modal

As shown on Fig. 3b, because of local deviation of the ED, JCV differs from JD. Magnetostatic charges appear thus at the interface, inducing a dipolar field (thin lines on Fig. 3b), resulting in a variation (not pictured) of polarization in the HM.

Noticing that the fields associated to the equilibrium resulting from the magnetic charges are variations with respect to the field Ha corresponding to the reference state (a), they will be denoted with prefix Δ in the following.

Following the general way indicated in Ref. 12, we obtain ΔHCV=ΔHCVCA+ΔHCVr where ΔHCVCA and ΔHCVr denote respectively the cavity and the reaction field contributions, according to the terminology popularized by Onsager.21 In the present case, ΔHCVCA and ΔHCVr obey

(6)

As expected, ΔHCV is null if JCV=JD

The torque exerted on the macrodipole associated to the central CV by the reaction field being null, the magnetostatic energy density U coupling the CV to the charges is reduced to

(7)

where θDθCV denotes the angle between JD and JCV. Eq. (7) provides a more rigorous evaluation of the magnetostatic energy than the one simply postulated in Ref. 7 by analogy with Ref. 13.

The determination of the effective susceptibility associated to the HM is of course a tricky task, the field induced by magnetic charges in the vicinity of the central CV being variable in amplitude and direction, and the intrinsic behavior featured by the surrounding CVs shaping the HM being hysteretic! Obviously, only numerical investigations are relevant to face this challenge accurately. In the frame of this first approach, analytical, we’ll simply consider that the susceptibility χref introduced above is a reasonable good order of magnitude, i.e. χ=Js2/2μ0Ku. One obtains χ360001. As a result, 3+2χ can be approximated by 2χ in (7), leading to the reduced magnetostatic energy

(8)

In our context, jCV equals j+ or j and JD=(j++j)/2. After some elementary manipulations, (8) yields, neglecting constant terms, to the reduced magnetostatic energy featured by a CVR

(9)

Inserting the magnetostatic contribution (9) in (3) and (4), and remembering that keR=1, leads to the reduced energies

(10)
(11)

Equilibrium angles θ+()e are roots of equations w+()/θ+()=0. Differentiating (10) and (11) and introducing the new equilibrium variables θav=θ+e+θe/2, θd=θ+eθe/2, one obtains the equilibrium equations:

(12)
(13)

Adding (12) and (13) leads to

(14)

Two configurations solutions Ci=θavi,θdi start to emerge, verifying

(15a)
(15b)

It is noticeable that Cb entails no coercivity. From this point of view, configuration Ca seems to be more convenient to model the experimental macroscopic behavior. But another crucial point is that the y transverse component jtriD of the mean polarization in a Weiss domain associated to configuration i=aorb obeys

(16)

From (16) and (15a) jtraD=0 is obtained, as illustrated on Fig. 2a. This means that, at the scale of a Weiss Domain, there is no magnetostatic energy. The cost associated to domain walls in the strip structure classically observed by Kerr effect (see for instance Ref. 9, Fig. 5), schematically pictured on Fig. 1a, is thus not justified in this case. In other words, Ca cannot account for the strip structure. We underline that those deductions are very strong, being independent of the procedure used to model the magnetostatic interactions, the magnetostatic term being cancelled when adding (12) and (13) to obtain (14).

One completes the description of configurations Ca and Cb subtracting (13) to (12). This leads, besides relations (15a) and (15b), to

(17a)
(17b)

From (17a), one deduces the coercivity featured by configuration Ca, i.e.

(18)

Fig. 4a shows the simulated loops associated to configurations Ca (Eq. 15a, 17a) (bold) and Cb (Eq. 15b, 17b) (dashed). We simulated with εR=π/125, for matching the experimental value hcex=0.025 and hca. Apart from the disagreement already pointed out about the domain structure, the configuration Ca fails to reproduce the experimental mean slope and exhibits a crossing of the branches followed by the instability at point Q clearly unrealistic in regard to the experimental loop.

FIG. 4.

(a): Simulated loops for configurations Ca (bold) and Cb (dashed), compared to the experimental loop (thin red). εR=π/125 was chosen for matching experimental value of hc and the simulated one hca. (b) Transverse polarization for configuration Cb.

FIG. 4.

(a): Simulated loops for configurations Ca (bold) and Cb (dashed), compared to the experimental loop (thin red). εR=π/125 was chosen for matching experimental value of hc and the simulated one hca. (b) Transverse polarization for configuration Cb.

Close modal

At the opposite, Cb exhibits a non null transverse polarization, as schematized on Fig. 2b and 2c. Moreover, as shown on Fig. 4b, jtrbD decreases when ha increases, agreeing well with the evolution of the magneto-optical contrast shown in Ref. 2, Fig. 2b. Lastly, Fig. 5a shows that θdb is nearly null, leading with (9) to the cancellation of the local dipolar energy. As a result, Cb is more favorable, as Fig. 5b shows, comparing the mean equilibrium energies wei=w+e+wei/2.

FIG. 5.

(a). Evolution of differential angle θd for the two configurations (b). Comparison of energies for Ca and Cb.

FIG. 5.

(a). Evolution of differential angle θd for the two configurations (b). Comparison of energies for Ca and Cb.

Close modal

Looking to typical CVs featuring residual incoherent anisotropy attributed to RAM, it is thus concluded thatCbis the only eligible configuration, which does not account forhc.

It is noticeable that the existence of the configuration solution Cb is due to the coupling of θ+ and θ through the magnetostatic term (see Eqs. 10 and 11). Without this term, a unique configuration would emerge, equilibrium angles θ+e and θe obeying the classical Stoner-Wolfarth formalism,22 leading to a macroscopic behavior very comparable to the one featured by configuration Ca. This reinforces our initial statement, that is, independently of the way to model it, to take into account the magnetostatic term is of crucial importance.

According to previous conclusions, CVRs are considered obeying the anhysteretic Cb behavior. To account for hc, some minority CVs (noted CVHs, as harder) have so to be involved, featuring a reduced uncoherent anisotropy keH>keR. Parameters characteristic of this new population will be labelled with superscript H. We’ll describe at first how CVHs interact with CVRs and finally the impact of this cohabitation at the macroscopic scale. Between those extremes, different intermediate scales will appear. To facilitate the comprehension, we propose on Fig. 6 a global view of those different scales and corresponding polarisations notations, thick double arrows indicating the magnetostatic coupling.

FIG. 6.

Global synoptic of the different scales at which the magnetic behavior can be apprehended, with corresponding notations, starting from the local individual CVH until the macroscopic level. z denotes the hard CVs volumic fraction. In this symbolic scheme, keH and keH represent the actual continuous distribution of hardnesses. The distribution will in fact be approximated by 3 hardnesses (Sec. III D).

FIG. 6.

Global synoptic of the different scales at which the magnetic behavior can be apprehended, with corresponding notations, starting from the local individual CVH until the macroscopic level. z denotes the hard CVs volumic fraction. In this symbolic scheme, keH and keH represent the actual continuous distribution of hardnesses. The distribution will in fact be approximated by 3 hardnesses (Sec. III D).

Close modal

To study the behavior of CVHs, the frame of the mean field theory introduced above is still followed. The major difference, compared with the case of CVRs, is about the link between the environment and the peculiar CV considered: Indeed, the CVHs volumetric part is expected to be only some % of the totality. The environment of a CVH can thus be nearly considered entirely made of CVRs, the mean properties of the corresponding HM being so disconnected from the central CVH considered now.

CVRs feature configuration Cb and for simplicity the corresponding differential angle is assumed to be null, according to Fig. 5a. As a result, all the CVRs belonging to a Weiss Domain exhibit the same polarization, described by a single angular variable and denoted jR=cosθRux+sinθRuy. It is obtained with (15b) cosθR=ha/cos2εR, that is, neglecting cos2εR:

(19)

For analytical convenience, in the frame of the description of the surrounding medium of a peculiar CVH, jR will be assimilate with jD, neglecting the influence of the minority CVHs contribution. It is thus obtained jD=1 and θD=θR, yielding with (8) to the magnetostatic energy associated to a CVH

(20)

Equations (19) and (20) are inserted in (3), (4), replacing keR=1 by keH and εR by εH, yielding to:

(21)
(22)

This leads, after differentiation, to the equilibrium equations

(23)
(24)

A key point is to evaluate the typical hardness required to allow irreversibility, this point conditioning the possibility to account for dissipation and thus for coercivity. We’ll denote θ+j a critical angle (subscript j as jump). θ+j verifies (23), being a peculiar equilibrium angle, and the additional relation 2w+θ+2θ+j=0. Denoting θRj the peculiar value of θR at which the jump occurs, it is thus obtained

(25)
(26)

Similar expressions are obtained for θj, replacing εH by εH.

θRj given, to determine the corresponding expression of keH, one can express the combined equation (25)2+(26)2. This leads to the second order equation

(27)

Where =cos2θ+j ; V=3sin2θRj9cos2θRj; U=1+35cos2θRj; W=40.5sin22θRj.

The minimum value keHlim to obtain a jump for a given θRj corresponds to the cancellation of the discriminant of Eq. (27), that is

(28)

Injecting (28) in (27), one obtains the corresponding critical angle

(29)

The corresponding deviation εHlim is obtained injecting (28) and (29) in (26), and obeys finally

(30)

The curve εHlimkeHlim is plotted on Fig. 7 (continuous black). As expected, this curve is decreasing, a little value of keH requiring a great deviation of the ED to maintain the anisotropy energy at a sufficient level to allow irreversibility.

FIG. 7.

Graphical determination of the representative minimum hardness to allow irreversibility determined as the intersect of the curve describing the intrinsic relation εHlimkeHlim and the curve εHkeH associated to representative CVHs.

FIG. 7.

Graphical determination of the representative minimum hardness to allow irreversibility determined as the intersect of the curve describing the intrinsic relation εHlimkeHlim and the curve εHkeH associated to representative CVHs.

Close modal

Nevertheless, the question of the representability of a couple keHlim,εHlim has now to be asked. Indeed, from a general point of view, the effect of a given hardness keH should ideally be rendered averaging the contributions considering all deviations εH, according with the distribution εHkeH. Regarding the complexity of the task, we simplify, considering that the couple keH,εHkeH is representative of the actual average. In the present context, this means that among all couples keHlim,εHlim, the one featuring εHlim=εHkeHlim is relevant, others playing a role of curiosities weightless. It is thus necessary to complete the study looking to mean properties of deviation to provide a comprehensive overview of the representative minimum value   eHklimre to obtain a jump. This is done in the  Appendix. Particularizing notations to the present context, the mean deviation εH for a given intrinsic hardness kiH obeys

(31)

Inserting (1) (replacing Ke by KeH and Ki by KiH) in (32), one obtains

(32)

The corresponding curve is plotted on Fig. 7 (dashed red). In the context of irreversibility, the representative minimum hardness   eHklimre to obtain a jump is so determined by the intersect of εHlimkeHlim and εHkeH curves, as shown on Fig. 7. One obtains   eHklimre1.234. With (1), this leads to an intrinsic anisotropy   iHklimre0.72Ku. In the peculiar case featured by the experimental loop pictured on Fig. 1, one obtains   iHklimre4.3KiR. As expected, the population of minority CVs considered has to be harder that the majority CVRs studied at first, to account for coercivity. This is consistent with our scheme.

Dealing with representative CVHs, we’ll consider in the next only coupleskeH,εHfeaturingεH=εHkeHgiven by (32).

The magnetic behavior featured by CVHs immersed in CVRs is deduced from Eqs. (23) and (24). Dealing with CVHs+, we consider (23)2, obtaining the second order equation

(33)

Where y=cosθRA=1+8sin2θ+eB=3keHsinθ+esin2θ+e+εHC=keH2sin22θ+e+εHcos2θ+eθ+e given, two roots are obtained, verifying

(34)

Ones has to take in mind that, according to the strip structure, θR0,π or θRπ,2π, depending on the Weiss Domain the CVH belongs to. We’ll arbitrary consider θR0,π. cosθRa and cosθRb been known, θRa and θRb are so entirely determined. Considering the input variable θ+e0,2π, one obtains the relevant solution θR checking what root θRa or θRb verifies (24). Remembering that ha=cosθR (Eq. 20), one obtains the local loop featured by CVHs+ plotting the points ha,cosθ+e. The same approach will apply to CVHs, replacing θ+e by θe and εH by εH in parameters A, B and C.

keH given, the corresponding averaged loop is obtained plotting the points ha,j+=cosθ+e+cosθe/2. At this stage, ha is the entrance variable. This means that it is necessary to interpolate corresponding values of cosθ+e and cosθe. This will impact the strategy we’ll adopt looking to macroscopic scale (Sec. III D).

1. keHkeHlim

Fig. 8a and 8b illustrate the case keH=1.23  eHklimre. The loops associated to each kind of CVH are plotted on Fig. 8a. They are anhysteretic, as expected, the double arrows indicating that the same route is travelled increasing or decreasing the field. Logically, the averaged loop is anhysteretic too. Nevertheless, the thin arrows point the approach of instability which will lead to irreversibility for an infinitesimal increase of keH.

FIG. 8.

(a). Local anhysteretic loops characteristics of CVHs featuring keH=1.23 (b). Corresponding averaged anhysteretic loop.

FIG. 8.

(a). Local anhysteretic loops characteristics of CVHs featuring keH=1.23 (b). Corresponding averaged anhysteretic loop.

Close modal

A non-trivial characteristic is the negative slopes observed towards saturation (ha>0.81), looking to individual behaviours (Fig. 8a). It is explained noticing that the natural tendency of the local polarization is to proximate the ED. But the magnetostatic cost being related to θDθCVH (see Eq 20), the local Polarization has to proximate jD too. As a consequence, different stages occur, i.e., considering CVH+ for illustrating (see Fig. 9):Stage I: j+ is late with respect to jD, looking towards the easy angle θED=π/2ε;Stages II, III, IV: j+ is in advance, looking towards the approaching easy angle θED=3π/2ε;We now focus on stages II and III. The situation can be explained considering for simplicity that the evolution of ha is small enough in these stages to neglect the variation of the Zeeman contribution in regard of the magnetostatic and anisotropic energy variations (note that the evolution of ha is anyway partially accounted trough the evolution of θD, impacting the magnetostatic term). As a result, optimizing the energetic compromise between anisotropic contribution and magnetostatic one leads to the increase of θ+e with θD, that isStage II: θ+e increasing with θD (and so with ha=cosθD), jx+=cosθ+e increases too, so long as θ+e<π;Stage III: θ+e being greater than π, the increase of θ+e with θD leads to a decrease of jx+ with ha;Stage IV: The energetic compromise is here essentially driven by the anisotropic term and the Zeeman one, the sharp increasing values of ha due to the asymptotic approach to saturation leading to a Zeeman contribution more significant than the magnetostatic one. As a result, jx+ increases with ha until saturation.

FIG. 9.

Qualitative explanation of the negative slope observed for ha > 0.81 on the loops illustrated on Fig. 8a: illustration of the evolution of j+ towards negative saturation, ha increasing from I to IV. The differences of orientations are amplified for visibility.

FIG. 9.

Qualitative explanation of the negative slope observed for ha > 0.81 on the loops illustrated on Fig. 8a: illustration of the evolution of j+ towards negative saturation, ha increasing from I to IV. The differences of orientations are amplified for visibility.

Close modal

In the frame of our modeling, the stage IV is not observed, the asymptotic approach to saturation being not rendered, due to the crude simplifications characteristic of our analytic approach, leading to jxD=ha and thus a saturating field equal to 1. For this reason, we restrict our simulations to the arbitrary interval ha<0.95.

2. Coercive case

A coercive behavior, corresponding to kiH=2, is pictured on Fig. 10 for comparison with the anhysteretic preceding case. An interesting characteristic of local loops is the asymmetry featured by increasing and decreasing branches, as evidenced looking to the different values of remanences or critical fields, i.e., considering for instance the loop associated to CVH : hj=h2a=0.72hj=h2b=0.84jr=0.655jr=0.44where arrows refer to the increasing and decreasing branches.

FIG. 10.

Local coercive loops characteristics of CVHs featuring kiH=2 (b). Corresponding averaged coercive loop.

FIG. 10.

Local coercive loops characteristics of CVHs featuring kiH=2 (b). Corresponding averaged coercive loop.

Close modal

This is explained looking again to magnetostatic interactions, controlled by jD. Figure 11 illustrates this question, dealing with a CVH+, looking to the peculiar situation of points P (decreasing branch) and P (increasing branch) corresponding to ha=±h0 indicated on Fig. 10a. As illustrated on Fig. 11 by bold vectors, the local polarization j+(P) would be symmetrical of j+(P) if the polarization of the environment was fulfilling this property too, according to Curie’s principle, i.e. θD(P)=θD(P)+π. This is not the case, θD(P) equaling =πθD(P). As a result, the absolute value of the x component of j+(P) is much greater than the one of j+(P). The symmetry is of course restored looking to the averaged loop, as shown on Fig. 9b, the asymmetry featured by CVHs compensating the one of CVHs+, but even at this scale, the memory of the local asymmetry is present, revealed by the two levels of irreversibility h2a and h2b.

FIG. 11.

Illustration of the interplay of the local polarization and the polarization of the surrounding domain explaining the asymmetry featured by local loops. Letters P and P refer to points P and P indicated on the local loop featured by a CVH+, as illustrated on Fig. 10a.

FIG. 11.

Illustration of the interplay of the local polarization and the polarization of the surrounding domain explaining the asymmetry featured by local loops. Letters P and P refer to points P and P indicated on the local loop featured by a CVH+, as illustrated on Fig. 10a.

Close modal

According to this explanatory framework, the asymmetry will be stronger the relative pound of magnetostatic interactions stronger is. This is illustrated on Fig. 12a, simulating the case kiH=1, the local loop corresponding to CVHs being not pictured to preserve clarity. Compared to Fig. 10a, the strengthening of the asymmetric character is spectacular, illustrating the sensitivity of the resulting loop to values of parameters when the energetic compromise involves contributions of comparable magnitudes.

FIG. 12.

(a): Illustration of the interplay between magnetostatic interactions and local anisotropy on the resulting asymmetry featured by ascending and descending branches of a local loop. The relatively small value kiH=1 yields to an asymmetry much more pronounced than in the case kiH=2 pictured on Fig. 10a. (b) Compensation of asymmetries looking to the averaged polarization (= considering the contribution of CVH together with the one of CVH+).

FIG. 12.

(a): Illustration of the interplay between magnetostatic interactions and local anisotropy on the resulting asymmetry featured by ascending and descending branches of a local loop. The relatively small value kiH=1 yields to an asymmetry much more pronounced than in the case kiH=2 pictured on Fig. 10a. (b) Compensation of asymmetries looking to the averaged polarization (= considering the contribution of CVH together with the one of CVH+).

Close modal

To simulate the impact of CVHs on the macroscopic loop, the continuous distribution of kiH should be rendered. We simplify, choosing arbitrary 3 CVHs type of same pound for discretizing the distribution of hardnesses, i.e.   αkiH=2,   βkiH=1.5 and   γkiH=1. The resulting averaged loop (= mixing those 3 contributions) is plotted on Fig. 13a.

FIG. 13.

(a): Averaged loop relative to the distribution of CVHs, i.e.   αkiH=2,   βkiH=1.5 and   γkiH=1 with equal pounds. (b): resulting macroscopic hysteretic component of the polarization (magenta), compared with experimental curves (Ku=16.2J/m3,Ku=12.1J/m3).

FIG. 13.

(a): Averaged loop relative to the distribution of CVHs, i.e.   αkiH=2,   βkiH=1.5 and   γkiH=1 with equal pounds. (b): resulting macroscopic hysteretic component of the polarization (magenta), compared with experimental curves (Ku=16.2J/m3,Ku=12.1J/m3).

Close modal

Denoting z the CVHs volumetric part, the macroscopic polarization jm obeys:

(35)

z is determined matching the experimental remanence jrex with the simulated one jHavr=0.46 (indicated on Fig. 13a). In the case of the sample pictured on Fig. 1, jrex=0.0265. This leads to z16=5,76%, the subscript referring to the corresponding experimental value of Ku. The CVHs are clearly minority, in accordance with our hypothesis.

As mentioned at the beginning of Sec. III, CVHs were introduced for accounting coercivity or equivalently hysteretical character of the macroscopic loop. It is obvious that the narrow elongated look featured by the experimental loop pictured on Fig. 1b does not allow an easy characterization of this specific aspect, retaining the conventional graphical representation jm(ha). It is so preferable to get rid of the anhysteretic skeleton. Facing this problem, it is considered in Ref. 7 the hysteretic component of the field hhy(jm)=ha(jm)ha(jm)/2. The entrance variable being the polarization, this involves interpolating excitation fields. Remembering that data were at first interpolated with respect to polarizations (cf. Sec. III C), a loss of accuracy may occur due to successive interpolating operations, especially in regions associated to fronts. To avoid this problem, we propose here an equivalent alternative, retaining, as for local investigations, ha as entrance variable: following Ref. 23, we so focus on the hysteretic component jhy of the macroscopic polarization, jhy obeying

(36)

With (35), this simply yields to

(37)

The resulting jhy curve is plotted (bold red) on Fig. 13b, and compared to two experimental curves: the hysteretic polarization jhy16 obtained from the sample illustrated on Fig. 1, featuring Ku=16.2J/m3 (black continuous), and jhy12 obtained from the sample illustrated on Fig. 1,7 featuring Ku=12.1J/m3 (black dashed). In this last case, the reduce remanence equals 0.0285. This impacts the volumic part of CVHs, leading to z12=6,2% instead of z16=5,76% (considering the same distribution of CVHs, indexed on the value of Ku). To facilitate the comparison, jhy12 has been renormalized, actual values being multiplied by jr16/jr12 for equaling the amplitude of the corresponding curve (black dashed) with others. From this, it is concluded that the postulated distribution of CVHs used for simulating is in qualitative agreement with experimental results.

The simulations reported concern nanocrystalline soft ribbons featuring transverse loops. They are based on an analytical minimization of the total energy, made of Zeeman, anisotropic, and magnetostatic contributions, evaluated at the scale of individual CVs. Particular care is brought to the description of the magnetostatic interactions, modelled in the frame of a mean field theory.

The solving of equations show that majority CVs obeying the RAM explain well the domain pattern but one has to consider another kind of CVs, minority, featuring a magnitude of local uncoherent anisotropy Ki comparable to Ku, to account for the hysteretic character.

These investigations are very general and not addressed to the specific loops chosen for illustrating.

Hc reflecting the contribution of minority CVs, its use, in the context of transverse loops, as an experimental parameter reflecting the RAM, seems to be somewhat questionable.

The origin of the "hard" CVs is an opened question. In the case of transverse field annealing, a residual uncoherent magnetoelastic anisotropy could result from external stress applied during annealing.7 Our own experimental investigations concerning field annealing, dealing with stress induced anisotropy, the evolution of coercivity with Ku reported in Ref. 6 should allow fruitful complementary experimental confrontation for modeling.

Numerous simplifications, inherent to the analytic approach, have been applied, dealing for instance with the uniaxial character of the uncoherent anisotropy or its 2D treatment, or the absence of hard CVs in the description of the environment of a given CV. The toughest problem is probably the assumption of an isotropic susceptibility χ for describing the equivalent homogeneous medium surrounding a peculiar CV, and the subsequent magnetostatic interactions. This crude simplification is probably responsible for the impossibility to simulate the asymptotic approach to saturation. This interpretation is reinforced by preliminary advanced modeling, simulations restoring the asymptotic behavior when the anisotropic character of χ is taken into account. This will be the subject of a future publication.

This work was supported in part by the "Association Nationale de la Recherche et de la Technologie" (convention CIFRE 2015/1098).

We consider a population of CVHs featuring an intrinsic uniaxial anisotropy of amplitude Ki with randomly distributed intrinsic Easy Directions in a plane, superimposed on a coherent uniaxial anisotropy of amplitude Ku and easy direction EDKu in the same plane. The objective of this appendix is to provide an analytic estimation of the mean deviation ε of the ED featured by the resulting effective anisotropy with respect to EDKu as a function of Ki/Ku, starting from the 3D simulations reported by Flohrer et al.9 

In Ref. 9, Ki was attributed to the RAM, however simulations do not require any hypothesis about the origin of Ki. The results can so be reused in a more general context. We’ll do it focusing on the asymptotic values featured by ε in the limit KiKu: the mean deviation is thus entirely determined by the random distribution of intrinsic Easy Directions, εlim obeying

(A1)
(A2)

We’ll so adapt the 3D simulations of Flohrer et al to the 2D context by a simple linear correction carried out for matching the simulated asymptotic value εlim to the 2D situation, multiplying thus by εlim2D/εlim3D=π/4 the values ε taken from Ref. 9, Fig. 3, uniaxial curve. The resulting sampled points are plotted on Fig. 14 and fitted by the law

(A3)
FIG. 14.

Evolution of the average orientation of the ED for randomly oriented individual EDs with uniaxial anisotropy constant Ki and a superimposed uniform uniaxial anisotropy Ku.

FIG. 14.

Evolution of the average orientation of the ED for randomly oriented individual EDs with uniaxial anisotropy constant Ki and a superimposed uniform uniaxial anisotropy Ku.

Close modal
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