We propose an exact expression to describe the hysteresis loops of an ensemble of Stoner–Wohlfarth particles undergoing an alternating quasi-static magnetic field. A statistical approach, which treats the quantities characterizing each particle as random variables, is adopted to get the orientation distribution of the local polarizations with respect to the applied field direction and the constitutive equation of the whole particle assembly. The hysteresis loop area gives the energy loss figure, but we have also obtained a straightforward integral expression for this quantity. The analytical relationships for the symmetric loops and the losses are successfully tested against numerical results, and the mathematical method adopted also displayed the ability to reproduce the “elemental loop” associated with any given particle of the system. While having a fundamental character, the proposed approach bears applicative interest, representing a versatile tool as the core of codes that simulate the behavior of devices employing magnetic components.
I. INTRODUCTION
Magnetic materials exhibit a broad variety of compositions and microstructures and a wide spectrum of responses to a varying magnetizing field .1–3
Although such behavior is the result of three-dimensional (3D) magnetization process, a two-dimensional theoretical approach is often regarded as appropriate, in addition to being perfectly adequate for a large class of materials, such as steel sheets, amorphous and nanocrystalline alloys, and thin films. It is also possible, in many cases, to consider a given material as an ensemble of mesoscopic regions (“particles”), either interacting or independent, each characterized by the local polarization and a magnetic anisotropy {uniaxial [see Fig. 1(a)], biaxial, cubic, etc.}, and even single-domain, if sufficiently small.
Panel (a) shows, for a particle of the system, the relative orientation of the local anisotropy and the local polarization with respect to the reference direction determined by the applied field . In the (H‖, H⊥) plane, the corresponding astroid representation, with vertices ±HK, is displayed in (b), with uH being the associated Gibbs free energy. (c) Branches of a general hysteresis loop, drawn starting from the demagnetized state (DEM). (d) Correspondence between the Q quadrants and the values of the γ angle.
Panel (a) shows, for a particle of the system, the relative orientation of the local anisotropy and the local polarization with respect to the reference direction determined by the applied field . In the (H‖, H⊥) plane, the corresponding astroid representation, with vertices ±HK, is displayed in (b), with uH being the associated Gibbs free energy. (c) Branches of a general hysteresis loop, drawn starting from the demagnetized state (DEM). (d) Correspondence between the Q quadrants and the values of the γ angle.
The Stoner–Wohlfarth (SW) theory,4–8 in its native formulation (which considers single-domain particles as independent, endowed with uniaxial anisotropy, and at T = 0 K), fits the simplifications mentioned above and is, thus, widely exploited in modeling. The main fields where the SW approach (often with some modifications) plays an important role are (1) magnetic nanoparticles,9–12 notably for magnetic hyperthermia;13,14 (2) ferromagnetic thin films15–17 and magnetic random access memories;18–20 (3) amorphous and nanocrystalline materials;21–25 (4) soft magnetic composites;26,27 (5) permanent magnets;28 and (6) study of the effect of spin-polarized currents.29,30
In the SW model, the response to an applied field of a particle characterized by the local uniaxial anisotropy is described by a vector hysteresis transducer providing the constitutive law for the reversible coherent rotations and the irreversible jumps of the local polarization . In other words, one gets the equilibrium orientation γ of each as a function of the anisotropy constant K, its orientation φ, and [see Fig. 1(a)]. With being the polarization of the whole particle assembly, the constitutive equation of the system comes out after integration over the probability density functions (pdfs) of K and φ. The design of magnetic components needs to implement in numeric modeling codes: a step with high computational cost, scaling up with the device size. Indeed, an explicit γ = γH(K, φ) solution for the orientation is not available so far, being the equilibrium angle obtained either following numeric procedures25,31 or using analytic approximations.
In the first case, the problem is commonly faced by adopting the astroid representation for the SW transducer [see Fig. 1(b)] and exploiting the so-called “tangent method,”7 as well as searching for the minimum of the Gibbs free energy of each particle utilizing, e.g., the Newton–Raphson method. These are time-consuming approaches, not efficient when implemented in codes used to design magnetic devices.
Researchers following the second way tried, for example, to recover the SW loop branches with ad hoc analytic functions,32 or proposed an H = H(J) “inverse” constitutive law,12 or limited the analytic solution to the low-field regime.33 Alternatively, an SW-like hysteron with different kinds of approximations for the anisotropy energy term,34,35 or with an equivalent field playing the role of the anisotropy,36 has been also adopted.
This work is not focused on the search of the γ = γH(K, φ) single particle solution [see Fig. 1(a)], afterward integrated over the whole system, but it deals at the start from the entire particle assembly by handling each quantity as a random variable (rv) with associated pdf. Statistical methods37,38 are then utilized to retrieve pH(γ): the equilibrium angle pdf, ending with an exact expression for the hysteresis loops (and consequently for the energy losses) of the whole system. The single particle behavior comes out as a particular case. Apart from its importance from the basic viewpoint, this result turns out to be useful for applications (chiefly in the magnetic loss prediction39), shortening the cumbersome and slow procedure needed for the design of devices.
In this paper, after a review of the SW model features essential for our purposes (Sec. II A), and some hints about the numerical approach and the adopted statistics (Sec. II B), the core of the work is discussed in Sec. III. Here, the statistical approach is outlined, and the pdfs controlling the equilibrium orientation of the local polarization vs a quasi-static are worked out, separately accounting for the irreversible (Sec. III A) and reversible (Sec. III B) phenomena. In both these subsections, the pdf evolution is described starting from the demagnetized state and following the system magnetization along the branches of the hysteresis loop driven by an alternating field [Fig. 1(c)], separately for the four Q quadrants shown in Fig. 1(d). Eventually, the obtained constitutive equation (and thus the hysteresis loop and loss) is successfully tested against the numerical procedure, both for the entire assembly (Sec. III B 5) and for the case of a single particle (Sec. III B 6). An approximate analytic expression for the energy loss, not involving the knowledge of the hysteresis loop, is worked out and effectively checked (Sec. IV), and finally, in Sec. V, some possible advancements of the proposed approach are listed.
II. THE CLASSICAL SW MODEL AND ITS NUMERICAL IMPLEMENTATION
A. The Stoner–Wohlfarth model
The introduction reports the strategies followed in the literature to find the γ equilibrium angle for each particle. In the following, the statistics of the system is described by the ψ(K, φ) joint probability density function, with K > 0 and φ limited to the [0;π/2] range for symmetry reasons.
B. Numerical implementation
III. THE ANALYTIC-STATISTICAL APPROACH FOR AN ENSEMBLE OF SW PARTICLES
In this work, we have abandoned the problem of finding the exact analytical solution for the local equilibrium orientation γ of a single SW particle in favor of a statistical approach that considers the whole assembly of SW particles from the beginning. Accordingly, the quantities K, φ, and γ (−π to +π) are treated as random variables, along with their ψ(K, φ) and pdfs (the first normalized to 1 for each φ angle). In the latter, “b” indicates the loop branch considered [see Fig. 1(c)], “Q” is the quadrant to which γ pertains [see Fig. 1(d)], and H plays the role of a parameter. All along the paper, the evolution of the γ values, which are bound to increase from −π to π [see Fig. 1(d)], dictates the sequence adopted to discuss the Q quadrants (III → IV → I → II).
Along each loop branch, the applied field triggers the irreversible rotations (IRs) and drives any local of the whole particle ensemble to its equilibrium angle (reversible rotations) at the same time. Despite the ensuing complex interplay between reversible and irreversible processes, the technique developed here treats them separately, and the γ pdf is consequently worked out in two steps: before finding , i.e., the pdf determined by the IRs only, which bring the local to their absolute minimum (Sec. III A), and subsequently accounting for the coherent reversible rotations (by means of the relaxation to the equilibrium orientation), ending with (Sec. III B). This approach is sketched in Fig. 2.
Evolution of the probability density function, from the K and φ statistics to the γ statistics. The two steps describing the irreversible and reversible processes in sequence are put in evidence. The superscripts (b, Q) of the pdfs are understood for the sake of simplicity. Note the dependence on (K, φ) of pDEM and pH,IRR, and on γ of the final pH pdf.
Evolution of the probability density function, from the K and φ statistics to the γ statistics. The two steps describing the irreversible and reversible processes in sequence are put in evidence. The superscripts (b, Q) of the pdfs are understood for the sake of simplicity. Note the dependence on (K, φ) of pDEM and pH,IRR, and on γ of the final pH pdf.
A. Step 1: Irreversible rotations (IRs)
At this stage, we assume to drive the irreversible processes only, again leaving the local to point along one of the two sides of the φ easy axis directions of the particle to which it pertains. For this reason, the magnetization distribution among the quadrants, rearranged by the occurrence of the IRs, is again described by a pdf stated in terms of K and φ instead of γ: , for the three loop branches of Fig. 1(c), as listed in Sections III A 1 -III A 4, and illustrated in Fig. 3 for a given φ = φ1.
For a given φ = φ1, and with a postulated ψ(K, φ1), the evolution of the pdfs (see the left part of Fig. 2) is described for the four Q quadrants [see Fig. 1(d)]. As H drives the system along the branch sequence of Fig. 1(c), the [Eq. (6)] describing the demagnetized state (DEM) transforms into the , , and as a response to the irreversible rotations (IRs) displayed by the gray arrows.
For a given φ = φ1, and with a postulated ψ(K, φ1), the evolution of the pdfs (see the left part of Fig. 2) is described for the four Q quadrants [see Fig. 1(d)]. As H drives the system along the branch sequence of Fig. 1(c), the [Eq. (6)] describing the demagnetized state (DEM) transforms into the , , and as a response to the irreversible rotations (IRs) displayed by the gray arrows.
1. First magnetization curve (FMC)
For H increasing from DEM [Fig. 1(c)], Eqs. (1b) and (1c) state that the in quadrant III smoothly (i.e., without IRs) crosses the γ = −π/2 threshold and move to quadrant IV when φ > π/4 and H > HIII→IV = (K/Js)sin 2φ [a value always lower or equal to Hc,K(φ): the threshold for IRs]. As stated above, we are not interested at this stage in the equilibrium position of , so we account for these reversible rotations by assigning the same pdfs to these quadrants: . Note that this “doubling” of the does not affect the normalization because each does not pertain to Q = III and Q = IV for the same field, the Step 2 (Sec. III B) taking charge of finding the actual orientation vs H. As H increases from zero [where Kc,0 = 0, see Eq. (4)] to the peak value Hp, the in quadrant III or IV switch to quadrant I if K < Kc,H(φ), and the corresponding is reported in Fig. 3(b). Note that = 0 because the system geometry [Fig. 1(a)] does not allow irreversible rotations to the second quadrant, a fact in agreement with the detailed discussion reported in the Appendix, which shows that no energy minima of uH [Eq. (1a)] can appear in Q = II.
2. Recoil curve (REC)
When the field is reduced from Hp to zero, the polarization decreases from its peak value Jp = J(Hp) to the remanence Jr. Along this branch, no IRs occur, and thus, is frozen to the value reached along FMC at H = Hp: [see Fig. 3(c)]. Here, again, we have = because the “doubling” of the pdfs, pointed out in FMC persists, but, as above, it does not affect the normalization.
3. Negative descending branch (NDB)
Eventually, the system is brought from the remanence to the negative tip of the hysteresis loop, lowering H from 0 to −Hp, with the magnetization evolving as described by [Fig. 3(d)]. For what concern the IRs and the smooth transitions discussed in Sec. III A 1, a “symmetrical” reasoning applies here, with the quadrants I, II, and IV correspondingly playing the role of Q = III, IV, and I in FMC, and the γ = π/2 crossing occurring at the threshold HI→II = −HIII→IV [≤Hc,K(φ)], when φ > π/4.
4. Thresholds of the functions
The quantities Kc,H(φ1) and Kc,Hp(φ1) of Fig. 3, signaling a variation of the values for a given φ = φ1, become the Kc,H(φ) and Kc,Hp(φ) threshold functions when considering the entire 0 ≤ φ ≤ π/2 range. As H, starting from the demagnetized state (DEM), oscillates between the ±Hp peak values of the hysteresis loop, the Kc,H(φ) threshold follows it, swinging between Kc,0 = 0 and Kc,Hp(φ), with the function that accordingly changes. An example for Q = I across NDB is depicted in the (φ, K) plane of Fig. 4.
An example of the “irreversible” pdf (on the right) selected by the Kc,H(φ) and Kc,Hp(φ) thresholds (on the left). See Fig. 3 for other cases.
An example of the “irreversible” pdf (on the right) selected by the Kc,H(φ) and Kc,Hp(φ) thresholds (on the left). See Fig. 3 for other cases.
B. Step 2: Coherent reversible rotations and constitutive equation
Given H and γ, and considering the scheme of Fig. 2, for the three branches of the hysteresis loop indicated in Fig. 1(c), the pdf, which accounts for irreversible and reversible processes, is obtained through standard statistical methods.37,38
The magenta regions represent the DH(γ) integration domains of the cumulative distribution functions [Eq. (13a)], for the three “b” branches (FMC, REC, and NDB) reported in Fig. 1(c), and the four Q quadrants. Note that when Q = II in FMC and REC, and Q = IV in NDB, no DH domain appears, according to the fact that, in these conditions, the local cannot find any stable equilibrium orientation. In Q = IV of FMC and REC, and in Q = II of NDB, the top-left DH border is correspondingly given by the function = |H|Js/sin(2φ) [Eq. (8) with γ′ = ∓π/2], with asymptotes φ = π/2 in both cases. Observe the thin white curves , whose evolution from to γ (thick black curves) devises the DH(γ) regions.
The magenta regions represent the DH(γ) integration domains of the cumulative distribution functions [Eq. (13a)], for the three “b” branches (FMC, REC, and NDB) reported in Fig. 1(c), and the four Q quadrants. Note that when Q = II in FMC and REC, and Q = IV in NDB, no DH domain appears, according to the fact that, in these conditions, the local cannot find any stable equilibrium orientation. In Q = IV of FMC and REC, and in Q = II of NDB, the top-left DH border is correspondingly given by the function = |H|Js/sin(2φ) [Eq. (8) with γ′ = ∓π/2], with asymptotes φ = π/2 in both cases. Observe the thin white curves , whose evolution from to γ (thick black curves) devises the DH(γ) regions.
1. First magnetization curve (FMC)
According to Sec. III A 4 and Fig. 3(b), along this branch, the Kc,Hp(φ) curves do not play any role (and thus are not depicted in Fig. 5), whereas the Kc,H(φ) ones not only signal the K thresholds where the pdfs [retrieved from Fig. 3(b)] change but also represent a portion of the DH integration domains (magenta regions in Fig. 5, for Q = III and Q = IV) border.
a)
b)
c)
d)
2. Recoil curve (REC)
3. Negative descending branch (NDB)
4. Compact expression for the pdfs
Limits of the integral appearing in Eq. (26), for the FMC, REC, and NDB branches of the hysteresis loop [see Fig. 1(c)], and the Q quadrants. The threshold is given by Eq. (10), with γ′ = γ.
5. Constitutive law and hysteresis loop
Figure 7 shows, for the whole −π ≤ γ ≤ π range, an example of vs H evolution, calculated with Eq. (26), and the corresponding hysteresis loop [Eq. (28)] with Js = 1.61 T. We have assumed ψ(K, φ) =f(K)g(φ), with the marginal pdfs supplied by Eqs. (5a) and (5b) and = 3000 J/m3.
When a quasi-static alternating field is applied, the evolution of pH(γ) [Eqs. (26) and (27)] is displayed for the FMC, REC, and NDB branches [Eq. (28)] of the hysteresis loop drawn on the top, where the fields in correspondence of which the pH(γ) are calculated are marked with open dots of the same color. The dashed black lines represent the demagnetized state (H = J = 0) realized when Eq. (6) is satisfied. On the other extreme, pH(γ) becomes the Dirac delta function δD(γ) or δD(γ + π) when H → ±∞, respectively. Observe the symmetry of the pH(γ) corresponding to the ±Hp peak fields.
When a quasi-static alternating field is applied, the evolution of pH(γ) [Eqs. (26) and (27)] is displayed for the FMC, REC, and NDB branches [Eq. (28)] of the hysteresis loop drawn on the top, where the fields in correspondence of which the pH(γ) are calculated are marked with open dots of the same color. The dashed black lines represent the demagnetized state (H = J = 0) realized when Eq. (6) is satisfied. On the other extreme, pH(γ) becomes the Dirac delta function δD(γ) or δD(γ + π) when H → ±∞, respectively. Observe the symmetry of the pH(γ) corresponding to the ±Hp peak fields.
The effectiveness of the statistical method is apparent in Fig. 8, where the quasi-static hysteresis loops, computed at different peak polarization Jp using Eq. (28) and the corresponding loss figures (inset), perfectly recover the ones obtained via the numerical procedure presented in Sec. II B [again it is assumed ψ(K, φ) = f(K)g(φ), with the marginal pdfs furnished by Eqs. (5a) and (5b)].
Alternating quasi-static magnetizing field. The excellent agreement between the First Magnetization Curve (open dots and dashed lines) and the hysteresis loops numerically found, and the ones obtained via the statistical method, are displayed ( = /Js; Js = ). The inset shows the behavior of losses, with the red curve representing both the values given by the loop areas and the empirical ones of Eq. (33), this last plotted in correspondence with the Jp(Hp) peak polarizations of Eq. (34). One cannot appreciate significant differences between the two loss figures.
Alternating quasi-static magnetizing field. The excellent agreement between the First Magnetization Curve (open dots and dashed lines) and the hysteresis loops numerically found, and the ones obtained via the statistical method, are displayed ( = /Js; Js = ). The inset shows the behavior of losses, with the red curve representing both the values given by the loop areas and the empirical ones of Eq. (33), this last plotted in correspondence with the Jp(Hp) peak polarizations of Eq. (34). One cannot appreciate significant differences between the two loss figures.
6. Elemental hysteresis loops
The ability of the analytic procedure to reproduce the elemental loops obtained when H oscillates with peak values |Hp| = Hc,K(φ1) [Eq. (3)] and J = Js cos γ measured along the direction is apparent in Fig. 9, from the comparison with the cycles numerically computed.
Alternating quasi-static magnetizing field. For different φ1 angles between the local easy axis and the applied field direction ( = 2K1/Js; Js = ), it is apparent the capacity of the statistical approach to perfectly cover the elemental hysteresis loops obtained through the numerical procedure outlined in Sec. II B.
Alternating quasi-static magnetizing field. For different φ1 angles between the local easy axis and the applied field direction ( = 2K1/Js; Js = ), it is apparent the capacity of the statistical approach to perfectly cover the elemental hysteresis loops obtained through the numerical procedure outlined in Sec. II B.
IV. ENERGY LOSS: AN APPROXIMATE INTEGRAL EXPRESSION
(a) The continuous green line describing the elemental hysteresis loop transforms into the dashed orange rectangle when only irreversible rotations are accounted for (Js = 1 T, K = 1 J/m3, φ = 35°, Hc,K(φ) = 1.02 A/m, Jc = 0.243 T, Jr = 0.819 T, Jp = 0.92 T). The difference between the loop areas is put in evidence by the gray pseudo-triangles. (b) Behavior vs φ of the loss W, and its irreversible component WIRR (both independent of Js), of the corresponding elemental loops. For φ = 0, the absence of irreversible processes entails W = WIRR = 8K [Eq. (31)]. (c) Interpolation of the K independent quantity W/WIRR vs φ, obtained (see inset) through the least squares linear fit of such a ratio vs .
(a) The continuous green line describing the elemental hysteresis loop transforms into the dashed orange rectangle when only irreversible rotations are accounted for (Js = 1 T, K = 1 J/m3, φ = 35°, Hc,K(φ) = 1.02 A/m, Jc = 0.243 T, Jr = 0.819 T, Jp = 0.92 T). The difference between the loop areas is put in evidence by the gray pseudo-triangles. (b) Behavior vs φ of the loss W, and its irreversible component WIRR (both independent of Js), of the corresponding elemental loops. For φ = 0, the absence of irreversible processes entails W = WIRR = 8K [Eq. (31)]. (c) Interpolation of the K independent quantity W/WIRR vs φ, obtained (see inset) through the least squares linear fit of such a ratio vs .
V. CONCLUSIONS
The developed mathematical tool analytically predicts the response of an assembly of non-interacting SW particles driven by a quasi-static alternating magnetic field. The exact integral relationships for the hysteresis loops and losses allow one to bypass the computationally slow numeric procedure necessary to implement the SW model in software used to predict the behavior of devices containing magnetic components.
The versatility of this approach lies in its skills listed below.
It works with any anisotropy distribution, permitting one to easily predict the role played by the sample texture (e.g., the effect of a macroscopic easy axis induced either by annealing or by applied stress).
The same analytic-statistical procedure, although more complicated, can be exploited with any field history (e.g., rotating fields,31,34 loops with bias, and asymmetrical minor loops).
Marginal modifications of the approach allow it to account for the presence of domain walls inside the particles, following the idea suggested in Ref. 22.
The whole mathematical structure is prone to a generalization for systems of particles endowed with biaxial anisotropy.
Under whatever field history and accounting for interactions, in Ref. 40, a mathematical technique capable to track the irreversible switches in a particle assembly described by the SW model has been worked out (so preserving the non-local memory of the system), together with a graphic representation that turns out to be an extension of the one operating in the Preisach model. One can then envisage a coupling between such a tool and the one developed here, with the aim to assess a more general analytical approach to the particle systems description.
ACKNOWLEDGMENTS
This research work was carried out in the framework of the Grant No. 19ENG06 HEFMAG project, which was funded by the EMPIR program, and co-financed by the Participating States and the European Union’s Horizon 2020 research and innovation program.
AUTHOR DECLARATIONS
Conflict of Interest
The author has no conflicts to disclose.
Author Contributions
C. Appino: Conceptualization (lead); Data curation (lead); Formal analysis (lead); Investigation (lead); Methodology (lead); Software (lead); Supervision (lead); Validation (lead); Visualization (lead); Writing – original draft (lead); Writing – review & editing (lead).
DATA AVAILABILITY
The data that support the findings of this study are available within the article.
APPENDIX: MINIMA OF THE GIBBS FREE ENERGY DENSITY uH VS THE ANISOTROPY AXIS ORIENTATION φ
For a general γ′ equilibrium orientation of , with (where γ depends on the Q quadrant considered, and is its lower limit), the range, corresponding to a minimum of the particle Gibbs energy uH(K, φ; γ′) [Eq. (1a)], is determined by the overlap between two φ regions: the first one, where [Eq. (8)] is positive, and the second one satisfying Eq. (9), 0, as illustrated in Fig. 11 (remember that φ is limited between 0 and π/2 for symmetry reasons).
The intervals, where the Gibbs free energy uH(K, φ; γ′) of a “particle” displays a minimum, are shown for each branch and quadrant (note that no exists for Q = II in FMC or REC, and for Q = IV in NDB). The values of and of the asymptotes of and are given by Eqs. (10) and (11), respectively. In the case Q = I for FMC and REC, the picture displays the situation occurring when γ ≤ π/4, corresponding to the of and crossing. A similar situation is found in the case Q = III for NDB, when γ ≤ −3π/4.
The intervals, where the Gibbs free energy uH(K, φ; γ′) of a “particle” displays a minimum, are shown for each branch and quadrant (note that no exists for Q = II in FMC or REC, and for Q = IV in NDB). The values of and of the asymptotes of and are given by Eqs. (10) and (11), respectively. In the case Q = I for FMC and REC, the picture displays the situation occurring when γ ≤ π/4, corresponding to the of and crossing. A similar situation is found in the case Q = III for NDB, when γ ≤ −3π/4.
The interval is found before for the field values 0 ≤ H ≤ Hp, i.e., when the First Magnetization Curve (FMC) and the RECoil curve (REC) are covered (upper strip of Fig. 11). In this case, for Q = III and Q = IV, the two regions partially overlap, and the limits are [; = γ′ + π] and [; π/2], respectively [see Eqs. (10) and (11)]. In Q = I, the entire region where 0 falls in the range where 0; , which drops outside, does not play any role, and the limits are [; π/2]. Eventually, in Q = II, the two regions do not overlap, signaling the fact that, in this quadrant, no stable equilibrium position for exists. This fact agrees with the result = 0, which is reported at the end of Sec. III A, and is derived simply by observing the system geometry [Fig. 1(a)].
When H < 0 (lower strip of Fig. 11), i.e., along the Negative Descending Branch (NDB), a very similar and, to some extent, specular scenario appears—the situations in Q = III, IV, I, and II now recovering the ones found along FMC and REC in Q = I, II, III, and IV, respectively.