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Some recent developments in magnetism in Czechoslovakia

Luboš Valenta

To cite this version:

Luboš Valenta. Some recent developments in magnetism in Czechoslovakia. J. Phys. Radium, 1959,

20 (2-3), pp.414-420. �10.1051/jphysrad:01959002002-3041400�. �jpa-00236060�

(2)

SOME RECENT DEVELOPMENTS IN MAGNETISM IN CZECHOSLOVAKIA

By LUBO0160 VALENTA,

Faculty of Technical and Nuclear Physics, Prague, Czechoslovakia.

Résumé. 2014 On présente

un

résumé de quelques-uns des derniers résultats obtenus

en

magné-

tisme

en

Tchécoslovaquie. Il

concerne

les questions suivantes : 1. Relaxations magnétiques dans MnFe2O4. 2. Variations de la largeur de la raie de la résonance

en

fonction de l’aimantation spontanée de ferrites polycristallins de manganèse et de manganèse et de zinc et la vérification

expérimentale de la théorie de Clogston et al. 3. Une nouvelle possibilité d’interprétation des dévia-

tions de la loi pour la perméabilité initiale dans le

cas

du mécanisme de rotation du vecteur d’aiman- tation. 4. L’approche à la saturation. 5. Une nouvelle méthode de

mesure

de l’effet magnétocalorique

des ferrites. 6. L’introduction conséquente de l’idée de L. Néel des sous-réseaux magnétiques dans

la théorie de Heisenberg et

sa

généralisation pour le

cas

de ferrimagnétisme et antiferromagnétisme

et des lames minces de spin arbitraire. 7. L’influence de l’inhomogénéité- du champ démagnétisant

sur

la résonance ferromagnétique. 8. La théorie de la structure des domaines élémentaires

aux

lames minces de MnBi. 9. L’interprétation de l’hystérésis du coefficient démagnétisant balistique.

10. Sur la définition du paramètre p caractérisant les dimensions des échantillons nonellipsoïdaux.

11. La désaimantation des matériaux ferromagnétiques par

un

champ alternatif magnétique.

Abstract. 2014 Some

new

results obtained recently in magnetism in Czechoslovakia

are

briefly

summarized : 1. Magnetic relaxation in MnFe2O4. 2. Dependence of the line breadth of the

resonance line

on

the spontaneous magnetization in polycrystalline manganese and manganese

zinc ferrites and the question of the experimental verification of the theory of Clogston and al.

3. A

new

possibility of explaining the deviations from the initial permeability law for the

case

of rotation of the vector of the spontaneous magnetization. 4. Concerning the spontaneous magne- tization

near

saturation. 5. A

new

method for measuring of the magnetocaloric effect in ferrites.

6. About the consequent introduction of the Néel’s idea of the magnetic sublattices in Heisenberg’s theory and its generalization for ferrimagnetics, antiferromagnetics and thin films with

an

arbi- trary spin. 7. Influence of the inhomogenity of the demagnetizing field

on

the ferromagnetic

resonance.

8. The theory of the domain structure in thin films of MnBi. 9. The explanation

of the hysteresis of the ballistic demagnetizing factor. 10. Concerning the definition of the para- meter p characterizing the non-ellipsoidal specimens. 11. Demagnetization of ferromagnetic

materials by

an

alternating magnetic field.

JOURNAL DE

PHYSIQUE 20, 1959,

1. Introduction.

-

In this paper

a

brief sum-

mary is given of some new results obtained recently

in magnetism in Czechoslovakia. Most of them

are as yet unpublished, some are preliminary

results or concern

a

part of à wider programme. -

In addition some papers are mentioned which were

published in Czech or Slovak only.

2. Ferrimagnetism and antiferromagnetism.

-

a) EXPERIMENTAL PART.

-

1. Krupicka and

Vilim [1] have recently found well pronounced

relaxations of the Richter type in manganese fer- rites with the general formula

MnFe204.xMn3O4-YO (0 x 0,37).

The activation energies obtained from their experi-

ments are in good agreement with those obtained from acoustical relaxation effects [2], [3]. Measu-

rements of the temperature dependence of the

electrical conductivity, made recently by Zâvéta [4]

also show similar results with one exception in the

stoichiometric ferrite MnFe204, where the acti-

vation energy measured was about 0,08 eV while

that obtained from magnetic relaxation is approxi- mately 0,3 eV. It seems to be reasonable to con-

clude from this that there exist some divalent ions

of Fe in MnFe2O4 and hence some manganese ions with higher valence than two.

From the preliminary results it seems probable

that the presence of divalent iron ions causes some new relaxations. Hence the relaxation spectrum consists, at least, of two bands corresponding to

the changes of valence of iron resp. manganese ions. In the range of frequencies used up to now, the corresponding maxima are superposed, and

their existence may be inferred from the asymetry

of the temperature dependence of tg 8, where 8

denotes the loss angle.

Because of the rather lower activation energy in the relaxation caused by iron ions,

a

superposition

of iron and manganese maxima appears with increas-

ing frequency. A lowering of the effective acti- vation energy follows in consequence. In this way the decrease of the activation energy in manganese ferrite with the decreasing oxygen content may also be explained (see table I).

It should be mentioned, that relaxations of the

same type have been found by Krupicka in manga-

nese zinc ferrites and in manganese magnesium

ferrites also.

2. Reinvestigating his recent results [5], [6]

Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphysrad:01959002002-3041400

(3)

415 TABLE 1

obtained on polycrystalline manganese and man- ganese zinc ferrites, Krupicka bas found

a

well-

defined linear dependence of v’M: (Ma is the spon- taneous magnetization)

on

AH (line breadth of the

resonance line) in the region of temperatures

-180 °C-0 °C (see fit. 1). The examined speci-

FIG. 1.

-

Dependence of the line breadth

on

spontaneous magnetization.

niens differ in the content of the oxygen which

implies

a

différence in Curie temperature (81 OC

resp. 111 OC). Nevertheless the curves for the

spontaneous.magnetization plotted against reduced temperature T/Tg were the same.

These results are in good agreement with the theory proposed for monocrystals by Clogston et

al. [7] where a linear increase of AH with VE,

and for the same materials with the différent Curie

temperatures the decrease with increasing T, is to

be expected. For the comparison of the theory

with experiment it is supposed that, due to the low

value of the crystal anisotropy, the AH in poly- crystals is mainly determined by the size of the individual crystals. Furthermore the slope of the

curves in fig. 1 should, according to [7], be pro-

portional to the mean square deviation of the effective exchange field which really seems to be greater in specimens with the higher content of

oxygen and hence of the vacancies in the lattice.

3. An interesting observation concerning the

initial permeability in sintered -ferrites has been made by Sternberk. It concerns the deviations from the usually used law

where uo is the initial permeability, K the first anisotropy constant and k

a

constant more closely

defined by the nature of the crystal anisotropy.

As is known, (1) has been derived for the process of the rotation of the vector of magnetization and

the deviations are interpreted as caused by the

mechanism of the motion of Bloch walls. Stern-

berk’s idea is the following : One may suppose the ferrite in the first approximation to be com- posed of crystal grains situated in the hollows of the surrounding medium. The effective internal field is then the sum of the external field He plus

the Lorentz’ field 4 M. Sternberk has shown the Lorentz’ field u 3 7rM. Sternberk has shown

(see also [8], [9]) that for the relative volume occu- pied by the ferrite grains lying in the limits

0,75 V 1 and for £ > 10 where uo is the

initial permeability of the tested material Ma J[K[

should normally lie between 1-2. In table II there are compared different values taken from many papers. The agreement with the rather crude model is quite satisfactory.

4. Let us remark, that Sternberk has been led [9]

to similar conclusions also from the investigation

of the behaviour near saturation of some

nickel, manganese and manganese zinc ferrites.

5. The low heat conductivity in ferrites makes the measurement of the magnetocaloric effect in

these materials very difficult. This has been studied classically (see e.g. the papers [10, 11, 12, 13]) using thermo-electrical éléments. Zâveta [14]

has therefore proposed the use of the adiabatic

change of the electrical resistance connected with the change of the magnetic field.

His idea is the following : First of all the depen-

dence of the electrical resistance

on

the tempe-

rature R(T)H-O and R(T)H=Hm is found. Then the

adiabatic change of the resistance (AR)s with

H

=

Hmis measured. Nowthe difference between

(dR)s and (OR)T for the isothermic change (see

(4)

416

TABLE II

(1) Calculated from the

data

on

effective field of the crystal anisotropy 2Kl/Ms resp. 0,2 KIM..

(2) ) Precise composition unknown.

(8) Measured

on

the powdered material (see Birks [38]).

(4) Calculated

on

the basis of Guillaud’s [47] and Pauthenet’s [46] data using for the density p the value p::: 5 g’/cn13

FiG. 2.

-

To the derivation of the Eq. (3).

(fin. 2) enables us to find the required (LlT)B. This

is because

where e is practically the same for R(T)H-o

and R(T)H"’Hm (k is the Boltzmann’s constant).

From the geometry one may see that

If elk is found graphically from (2) then we may find (A T)s from (3).

The applicability of the method has been tested

by Zàvéta

on

the manganese ferrite

MnOFe2O3 + 0,08 Mn3o4 + 0,055 0 (fig.3).

FIG. 3.

-

Temperature dependence

of the magnetocaloric effect.

A typical anomaly is seen at the Curie point.

Thus the usefulness of the proposed method is

quite evident.

(5)

417

b) THEORY. - 6. The great progress made in the last years in the theory of ferrimagnetism and antiferromagnetism is intimately connected with the use of the idea of the magnetic sublattices as introduced by Néel (see first of all his fundamental papers [15, 16]). The thorough investigation of

the applicatibility of this idea in the theory thus

seems désirable.

The author [17] tried to find what the results

would be if this idea were introduced into Hei-

senberg’s theory when using the modification given by Van Vleck [18]. The hamiltonian used had the usual form for the exchange interaction. The

crystal lattice is supposed to be composed of Néel’s

lattices. Similarly to [19], [20] the existence of the sublattices is characterised quantum-mecha- nically by the supposition that the spins of the particular sublattices have the definite eigenvalues simultaneously. The hamiltonian of this system is formulated in terms of the " rot’ated " spin operators

as

used by Oguchi [21]. Using the approximations equivalent to those of Van Vleck [18] one obtains the dependence of the spon- taneous magnetization on the temperature and the intensity of the magnetic field.

The theory includes for this model the theory of

the ferrimagnetism, antiferromagnetism and the theory of thin films proposed recently by the

author [20]. The results obtained are analogous

to those obtained from the molecular field theory

as

given by Néel [16], Yafet and Kittel [22] etc...

and to those obtained by Van Vleck [23] using the

method of Stoner [24]. For the special case

S =1/2 the theory agrees with the theory of

Vlasov and lshmukhametov [19] and with that of the author [20]. The angle between the directions of the magnetization in the sublattices may be

expressed in terms of the exchange integrals.

Hence the principal possibility follows for the

experimental determination of the exchange inte- grals.

The corresponding situation in the region of

low temperatures is

now

being investigated.

3. Concerning the influence of the inhomogenity

of the demagnetizing field on ferromagnetic

résonance.

-

7. It is interesting to know how the departures from the homogeneity of the magnetics

field within the specimens change the results obtain- ned in the case of the homogenous magnetization.

The first qualitative study has been given by Pilscikov [25] and Frait [26]. Moreover Frait has

now

shown [27] how to treat the problem quanti- tatively in the case when we are able to calculate

the internal magnetic field in the ferromagnetic body. It is tben possible to calculate the permea-

bility as

a

function of the coordinates. The mean

value of some function of u, say f(u) >, e,g, of

the components of the complex permeability, may

be then obtained from

where ha(x, y, z) is the intensity of the high fre-

quency magnetic field and the integration is

extended over the whole volume of the specimen.

Calculating f({J..) > in dependence on the inten- sity of the static external field, one obtains the

resonance curves, which can be compared with experiment.

FIG. 4.

-

Résonance

curve

for the absorption in plane parallel rectangular FeNi plate (78 % Ni).

theoretical curve,-.-.-... experi-

mental

curve.

fi- external magnetic field, frequency

9 000 MHz.

In fig. 4

a

comparison is made of the theoretical

curve with the experimental one obtained from the

measurement on

a

Fe-Ni alloy with 78 % Ni for a specimen in the form of a plane parallel rectangular plate. The agreement is quite satisfactory.

4. Thin films.

-

8. As shown by Màlek and Kambersky [28] an explanation may be given for

the domain structure found recently by Williams

et al. [29] on thin films of MnBi. An explanation

may also be given, based

on

Kittel’arefined theory ([30], § 3,lb). The différence lies in the f act, that in

Màlek’s and Kambersky’s Itreatment the magnetics

interaction of both surfaces is incittded. They

obtained the density of the demagnetizing energy per square centimeter

where T is the thickness of the film and D is thé

domain size. The surface density y of thé Blocli

(6)

wall has been estimated at 15 erg cm-2. The energy of the Bloch walls is therefore

From the minimum condition for the sum of both

énergies they obtained the dependence of tbe size

FIG. 5.

-

Dependence of the domain size

on

the thickness in MnBi films.

of the domains on the thickness T of the thin film (see fig. 5). ForT--10-5emitisD2-3.10-5em.

For T 10-g cm the domain structure practically disappears. For T > 10- 5

cm

D increases

as

Tl/2

similarly to the theory of Kittel. Williams et al.

have found D ~ 3-6.10-5

cm

for T ss 10- 5 cm.

It has been shown that neither

a

more precise

calculation of the Bloch wall energy, nor

a

change

in the form of domain patterns (e.q. chess-board

pattern) essentially change the results. As

a

con-

sequence of the great anisotropy there is

no

possi- bility for domains magnetized parallel to the sur-

face.

At the end it follows that for thin films of MnBi used

as

the storage elements, their resolution

power is limited to 109 informations/cm2.

5. Magnetostatics. - 9. In 1950 Janus et al. [31]

have discovered the hysteresis of the ballistic demagnetizing factor NB (see Fig. 6). Hajko and

Daniel-Szabô [32] have found

a

simple expla-

nation : The infiniteness of NB is inferred from the fact that in the centre of

a

rod where M == 0 we

fin d that there is

a

demagnetizing field Hdem 0

which is formally expressed

as

Hdem

= -

NB M.

Thus the origin of the demagnetizing field must be

in the other parts of the specimen. Hence the

traditional suppositions usually made about the magnetization in rods must be abandoned and

replaced by some new one which respects the real

situation. These conclusions have been confirmed

experimentally by Hajko and Daniel-Szabô as

shown in fig. 7. There the ratio of the magne- tization at the place studied to the absolute value

of the simultaneous one in the centre of the rod is plotted against the distance from the centre.

The sequence of the curves from 1 to 6 corresponds

Fie. 6.

-

Ilysteresis of tbe ballistic deinagnetization factor (measured by V. Ilajko and J. Daniel-Szabô).

FIG. 7.

-

Dependence of thé rémanent magne fixation li

rods

on

the distance froin the centre of thé rod measured

on

the descendent part of thé hysteresis loop.

to the motion along the decreasing part of the hysteresis loop from the upper top to the lower one.

10. Hajko [33] has proved that for uniformly

magnetized rectangular rods the ballistic dema-

gnetizing factor is formally the same

as

in the case

(7)

419 of the ellipsoidal and cylindrical specimens when

the parameter p is defined after Schneider [34J

as

where 1 is the length of the rod and a, b its trans-

versal dimensions. It may be easily shown that Hajko’s arguments may be generalized for rods

with any cross section which have a centre of sym-

metry. Then A’B

=

Q where Q is the angle in

which both basic planes perpendicular to the axis

of the rod, are seen from the centre. For long rods

we have again approximately.

if we de fine

where Fis the surface of the cross-section.

6. On the demagnetization of ferromagnetic

materials by alternating magnetic field. -11. Star- ceva and Shur [35] observed that in some cases thé

application of a decreasing alternating magnetic

field results in

an

increase of the remanent magne- tization and may be accompanied by the change of

its sign. Hajko and Daniel-Szab6 investigated

this effect

on

toroidal specimens made from magne-

tically soft metallic and ferritic materials. The initial magnetic state has been obtained in the way

seen in fig. 8. The results of their experiments

Fie. 8.

--

To the préparation of the initiai magne tic states.

(fig. 9), show thé variation of the i-eiiiaiienu

magnetization Jr after

an

application of an alter- nating magnetic field with

a

maximum ampli-

tude Il.. In their experiments the amplitude

decreased continuously to zero. Similarly to [35]

all these results may again be qualitatively explained by the Kondorsky’s hypothesis of

domains in the crystal with different critical fields.

Similar curves have been found by Hajko and

Daniel-Szabô for the dependence of the apparent

remanent induction in ferromagnetic rods and ellipsoids.

.Fie. 9.

-

Dependence of the remanent magnetization Jr

on

the maximum amplitude of the alternating magnetic

field.

7. Acknowledgements.

-

The author would like

to express his hearty tbanks to his friends and colleagues Dr. S. Krupicka, Dr. J. Sternberk,

K. Zâvéta, Dipl. phys., Z. Frait, CSc., Z. 8/làlek, CSc.

V. Kambersky, Dipl. phys., Doc. Dr. V. Hajko

and Doc. J. Daniel-Szabô for the aid in preparation

of this report.

REFERENCES

[1] KRUPI010CKA (S.), VILÍM (F.), Czechosl. J. Phys., 1957, 7, 723.

[2] FINE (M. E.), CHION (C.), Phys. Rev., 1957, 105, 121.

[3] GIBBONS (D. F.), J. Appl. Physics, 1957, 28, 810.

[4] ZÁV011ATA (K.), Czechosl. J. Phys., in print.

[5] KRUPI010CKA (S.), Czechosl. J. Phys., 1956, 6, 458.

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[7] CLOGSTON (A. M.), SUHL (H.), WALKER (L. R.),

ANDERSON (P. W.), J. Phys. Chem. Solids, 1956, 1,

129.

[8] STERNBERK (J.), Czechosl. J. Phys., 1957, 7, 372.

[9] STERNBERK (J.), Dissertation. Czechosl. Acad. Sc., Prague, 1958 (in Czech.)

[10] WEISS (P.), PICCARD (A.), C. R. Acad. Sc., Paris, 1918, 166, 352.

[11] WEISS (P.), FORRER (R.), Ann. Physique, 1926, 5, 153.

[12] POTTER (H. H.), Proc. Roy. Soc., 1934, 146, 362.

[13] CLARK (C. A.), SUCKSMITH (W.), Proc. Roy. Soc., 1954,

A 225, 147.

[14] ZÁV011ATA (K.), To be published in Czechosl. J. Phys.

[15] NÉEL (L.), Ann. Physique, 1932, 17, 61 ; 1936, 5, 232.

[16] NÉEL (L.), Ann. Physique, 1948, 3, 137.

[17] VALENTA (L.), Czechosl. J. Phys., to be published.

[18] VAN VLECK (J. H.), The Theory of Electric and

Magnetic Susceptibilities, Oxford, 1932.

(8)

420

[19] VLASOV (K. B.), ISHMUKHAMETOV (B. Kh.), J. Exp.

Theor. Phys., U. S. S. R., 1954, 27, 75.

[20] VALENTA (L.), IAN USSR, 1957, 21, 879 ; Czechosl.

J. Phys., 1957, 7,127 ; 1957, 7,136.

[21] OGUCHI (T.), Progr. Theor. Phys., 1953, 9, 7.

[22] YAFET (Y.), KITTEL (Ch.), Phys. Rev., 1952, 87, 290.

[23] VAN VLECK (J. H.), J. Chem. Phys., 1941, 9, 85.

[24] STONER (E. C.), Proc. Leeds Phil. Soc., 1930, 2, 56.

[25] PILS010CIKOV (A. I.), IAN USSR, 1956, 20, 1286.

[26] FRAIT (Z.), Report

on

the Czechoslovak-Polish Confe-

rence on

Solid State Physics, Sopoty, 1956.

[27] FRAIT (Z.), Dissertation. Czechosl. Acad. Sc., Prague,

1958 (in Czech).

[28] MÁLEK (Z.), KAMBERSKÝ (V.), to be published in

Czechosl. J. Phys.

[29] WILLIAMS (H. J.), SHERWOOD (R. C.), FOSTER (F. C.),

KELLBY (E. M.), J. Appl. Phys., 1957, 28, 1181.

[30] KITTEL (Ch.), Phys. Rev., 1946, 70, 965.

[31] JANUS (R. J.), DRO017D017DINA (V. J.), 0160ABALINA (E. F.),

Sbornik posvja0161010Dennyj semidesatiletiju akademika

A. J. Joffe, Moscow, 1950, 402.

[32] HAJKO (V.), DANIEL-SZABO (J.), 010Cs. 010Cas. Fys., 1956, 6, 352 (in Slovak).

[33] HAJKO (V.), Mat. Fys. 010Cas., SAV, 1957, 7, 46, (in Slovak).

[34] SCHNEIDER (W.), Z. Physik, 1927, 42, 883.

[35] STAR010DEVA (I. E.), SHUR (J. S.), Fizika metallov i metal-

lovedenie, 1956, 3,1,190.

[36] BICKFORD (L. R.), Phys. Rev., 1950, 78, 449.

[37] BOZORTH (R. M.), TILDEN (E. F.), WILLIAMS (A. J.),

Phys. Rev., 1955, 99,1788.

[38] BIRKS (J. B.), Proc. Phys. Soc., London, B 63,1950, 65.

[39] GALT (J. K.), MATTHIAS (B. T.), REMEIKA (J. P.), Phys. Rev., 1950, 79, 391.

[40] YAGER (W. A.), GALT (J. K.), MERRITT (F. R.), Phys.

Rev., 1955, 99, 1203.

[41] OKAMURA (T.), KOJIMA (Y.), Phys. Rev., 1952, 86,

1040.

[42] BOZORTH (R. M.), CETLIN (B. B.), GALT (J. K.),

MERRITT (F. R.), YAGER (W. A.), Phys. Rev., 1955, 99,1898.

[43] OKAMURA (T.), KOJIMA (Y.), Phys. Rev., 1952, 85, 690.

OKAMURA (T.), KOJIMA (Y.), TORIZUKA (Y.), Sc.

Rep. Res. Inst. Tôh. Univ., 1952, A 4, 72.

[44] GALT (J. K.), YAGER (W. A.), REMEIKA (J. P.),

MERRITT (F. R.), Phys. Rev., 1951, 81, 470.

[45] MILES (P. A.), Nature, 1954, 174, 177.

[46] PAUTHENET (R.), Ann. Physique, 1952, 7, 710.

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[48] NÉEL (L.), J. Physique Rad., 1948, 9, 193.

DISCUSSION

Mr. Schlômann (Comments).

-

I would like to point out that the upper one of the curves shown in fig. 1, if extrapolated back to Ms === 0, goes ïnto the region of negative line breadth. This

indicates, 1 believe, that other line broadening

mechanisms are also important in the present case.

Mr. Kurti.

-

What was the value of Hm used in the measurements of the magnetocaloric effect ?

How do the values of Ts compare with those calcu- lated from magnetization curves ?

Mr. Valenta.

--

The value of the field

was

5 500 Oe. The comparison was to my knowledge

not carried out.

Mr. Wohlfarth.

-

The curves giving the rema-

nence after A. C. demagnetization are analogous

to those reported in my communication for magne-

tically hard powder materials, where the underly- ing theory is perhaps a bit more realistic than for

the magnetically soft materials described here.

Mr. Valenta.

-

Yes, I agree.

Mr. Dates.

-

1) How was Hdem measured ? 2) How did t,he measurements agree with those of Düssler ?

Mr. Valenta. - 1) The induction Bis determined

in the well known fashion by the ballistic method and the field HB

was

also found ballistically with

a

flat coil which

was

placed close to the surface of

the sample.

2) 1 am not well enough acquainted with

Düssler’s paper to answer satisfactorily.

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