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Random anisotropy effects on the phase transition of amorphous Dy xGd1-xNi

B. Dieny, B. Barbara

To cite this version:

B. Dieny, B. Barbara. Random anisotropy effects on the phase transition of amorphous Dy xGd1-xNi.

Journal de Physique, 1985, 46 (2), pp.293-302. �10.1051/jphys:01985004602029300�. �jpa-00209968�

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293

Random anisotropy effects on the phase transition

of amorphous DyxGd1-xNi

B. Dieny and B. Barbara

Laboratoire Louis Néel CNRS-USMG, 166X, 38042 Grenoble Cedex, France (Reçu le 3 mai 1984, révisé le 11 octobre, accepté le 23 octobre 1984)

Résumé. 2014 Nous avons étudié, par des mesures d’aimantation en champs faibles, le rôle d’une anisotropie aléatoire

sur les propriétés critiques des amorphes DyxGd1-xNi.

A l’équilibre, les exposants critiques sont donnés, discutés, et comparés à ceux précédemment obtenus pour d’autres systèmes.

Des effets hors d’équilibre ont été examinés et montrent l’existence de lignes d’irréversibilité dans les plans H-T, T-(D/J) et (D/J)-H.

Abstract. 2014 The influence of the magnitude of a random anisotropy on the critical properties of amorphous DyxGd1-xNi has been studied by means of low field magnetization experiments.

At equilibrium, critical exponents are given, discussed and compared to those previously obtained on other systems.

Non equilibrium effects have been investigated showing the existence of irreversibility lines in the planes H-T, T-(D/J) and (D/J)-H.

J. Physique 46 (1985) 293-302 FÉVRIER 1985,

Classification

Physics Abstracts

75.SOK

1. Introduction.

Topological disorder in amorphous alloys leads to

distributions of random fields at the atomic scale.

Two extreme cases are usually considered :

-

« spin glasses » in which random fields result from a wide distribution of positive and negative exchange interactions with an average around zero;

-

« amorphous magnets » with essentially posi-

tive exchange interactions at the atomic scale and a

distribution of local anisotropy directions.

This paper deals with such « amorphous magnets » and particularly with the nature of the phase transition they undergo at a temperature Tf between the parama-

gnetic and the low temperature phases. This study has

been stimulated by the theoretical work of Aharony

and Pytte who pointed out that random anisotropy systems should have qualitatively different characte- ristics from those of ferromagnets [1 ]. Von Molnar

et al. have shown [2] that amorphous GdAg (case of a

low anisotropy to exchange ratio D/J) presents an apparent divergence of the susceptibility at T f but only an extremely small spontaneous magnetization

below this temperature; on the opposite, amorphous DyCu (case of a large D/J ratio) exhibits a finite initial

susceptibility xo, at any temperature. Some comple-

mentary studies have been done by O’shea et al. [3].

More recently, it has been theoretically demons-

trated that xo may not diverge if D/J is not too small;

in such a case xo - (J/D)4 in three dimensions [4, 5].

In order to study the influence of the anisotropy

to exchange ratio D/J on the nature of the phase

transition at Tf, we have prepared five amorphous samples of DYxGd1-xNi for the following nominal compositions x

=

0, 0.25, 0.5, 0.75, 1. In all these samples, Ni is not magnetic. When x varies from 0 to

1, the anisotropy to exchange ratio increases by about

one or two orders of magnitude. An accurate determi-

nation of this ratio will be published later together

with a quantitative study of the evolution of the phase

transition of DYxGdl-xNi as a function of D/J. This

determination of D/J is carried out by fitting isother-

mal magnetization curves in the high field region

where the HPZ model [6] is valid.

In this paper, we will give only a general qualitative

outline of our study. In a first part (section 3) we refer to

the properties at the thermal equilibrium. The second part (section 4) is devoted to the non equilibrium pro- perties in connection with the onset of irreversibility

in spin glasses.

Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphys:01985004602029300

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2. Experimental methods.

Our samples were prepared by sputtering from alloy targets onto liquid nitrogen cooled Al substrates.

The resulting film thickness, of the order of 20-50 Jlm, allowed us to perform magnetic studies in absence of any substrate.

The amorphous character was checked by X-ray scattering; we find an upper limit of microcrystal size of 15 Á.

The chemical composition of our films was checked by an atomic absorption method; these compositions

are the following : GdNi1.27’ Gdo.77Dyo.23Nil.19, Gdo.48DYo.52Nil.35’ Gdo.27DYo.73Nii.18, DyNil.32-

D.C. magnetization measurements have been per- formed by two methods : a classical induction one for intermediate and high fields and a method based on

SQUID detection in low fields (SHE SQUID Magne- tometer). The magnetic field was always applied in the plane of our films leading to extremely low demagne- tizing effects.

3. Reversible magnetization measurements.

Except for GdNi which exhibits few irreversible

effects, magnetization measurements were performed

at constant field and by decreasing the temperature from T = 100 K down to 4.2 K. The Arrott plots for

three samples GdNi, ÐYo.5Gdo.5Ni and DyNi (nomi-

nal compositions) are given in the figure 1, 2 and 3.

3.1 GdNi. CASE OF A LOW ANISOTROPY.

-

The

general features of our results for GdNi (Fig. 1) are

very similar to those predicted theoretically by Aharony and Pytte in their earlier article in which D J [1]. These authors propose the following equation of state in 3D :

T f is the ordering temperature, s = 4 - d where d is the dimensionality of the system, and y

=

1, if the thermal fluctuations are not taken into account

The last term AM2(H/M)-e/2 results from an expansion to the leading term in DIJ : A - (D/J)2.

On the theoretical Arrott plot, this term induces a change of sign of the curvature at the temperature Tf

and leads to the absence of finite intercept with the M2

axis below Tf. On the other hand, a divergence of the

initial susceptibility is reminiscent from the non

random case.

On the Arrott plots of a-GdNi, we observe similar properties :

-

The change of sign of the curvature of the iso- thermal lines indicates that the phase transition tem- perature Tf is between 61.4 and 62.4 K.

-

The susceptibility seems to diverge at this temperature (see also Ref. [5]).

-

The important curvature near the origin without

any finite intercept (within our error bars) with the line of zero internal field traducts an absence of sponta-

neous magnetization at Tf and until some degrees

below Tf. However, at lower temperature, a second

regime appears characterized by the arise of a sponta-

neous magnetization. This can be clearily seen on the M(H) curves where a linear part (demagnetizing

field line) is observed at lower temperature (Fig. 4) and disappears above ~ 55 K. This spontaneous magneti-

zation (magnetization in zero internal field) grows up to a value of 25 % of the satured magnetization Msat at 4.2 K.

At low temperature, the spontaneous magnetiza-

tion is Ms - Msat for a collinear ferromagnet and Ms ~ 0.5 Msat for an asperomagnet Thus, the long

range magnetic order of a-GdNi characterized by

the existence of a small spontaneous magnetization

at low temperature cannot simply be of collinear

ferromagnetic or of asperomagnetic type.

Fig. 1.

-

Arrott plots for amorphous GdNi. N is the demagnetizing factor. M is given in JIB/formula, H in Oe.

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295

Fig. 2.

-

Arrott plots for amorphous DyNi.

From a practical point of view, the existence of a

spontaneous magnetization at low temperature in GdNi allowed us to measure the demagnetizing field

factors of our in-plane field film : N

=

24.0 Oe. for-

mula/,uB (Fig. 4), this value is very close to the one

estimated by assuming that the sample is an oblate ellipsoid. This demagnetizing field factor has been used in the determination of critical exponents in GdNi.

Before studying the critical behaviour of this system, it is useful to stress possible origins for the observed small but finite spontaneous magnetization at T Tf.

Such an observation is in contradiction with the macro-

scopic isotropy of ideal amorphous alloys. The point

here is that our system and more generally any soft

amorphous system cannot be considered as ideally

disordered from the point of view of their magnetism.

Sample inhomogeneities such as tensile or compressive stresses, thermal strains, anisotropic microstructures...,

lead to non random anisotropy components. Aharony

and Pytte [1 ] pointed out that the effect of a non

random anisotropy, for instance a cubic anisotropy

term - Do(S: + S4y + S4z) would be drastic even if

Do D. Chudnovsky and Serota [5] have recently

studied the effect of the superposition of an uniaxial

coherent anisotropy onto the local random aniso- tropy. This superposition gives rise to a divergency

of xo and to a spontaneous magnetization given by :

Our preliminary study of the anisotropy of DyxGd1 -xNi alloys gives D/J ~ 10-2 for GdNi and

therefore if Ms ~ 0.25 Msat then D0 ~ 10-g D which

is extremely small. Although we have to be very careful in using quantitatively theoretical expressions, this

result clearly indicates that even very small uniform

anisotropy components can explain the spontaneous

magnetization observed in a-GdNi. This result is also

Fig. 3.

-

Arrott plots for amorphous DYo.sGdo.sNi.

Fig. 4.

-

Low field magnetization curve of a-GdNi. The

departure from the straight line occurs for M

=

Mr and

H

=

NMS where N is the demagnetizing field factor.

valid for other Gd-based alloys in which D/J is always

of the order of 10- 2 and more generally for soft amorphous materials. Therefore the observation of a

divergence of the initial suscpptibility in these mate-

rials is also, at least for a part, due to sample inhomo-

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geneities. In these circumstances, it seems presently hopeless to find any experimental proof in favour or against an intrinsic divergence of the susceptibility in

these materials. In the opposite limit of large aniso- tropies, it is rather easy to show that the susceptibility

does not diverge [2]. Our results on DyNi and DYxGdl-xNi (see below) confirm strikingly this

observation. Therefore, there must be a transition

versus D/J above which Xo does not diverge and below

which it does diverge. From the theoretical point of

view of Aharony and Pytte [4], this transition takes

place at D

=

0. If this was really the case, it would be

extremely difficult to show it experimentally. The

best would be to increase progressively D/J and to

observe when the breakdown of the divergence of xo

occurs. The study of some alloys with 0 x 0.25

will be useful in order to get some insight into the understanding of this « ferromagnetic » to « spin glass » transition versus D/J.

Whatever the origin of the divergence [5] ] of Xo in a-GdNi, it is interesting to know the value of the critical exponent y. Assuming the usual x - (1 - T/Tf)-Y form, we have plotted X/(dX/d7) versus

T (see Fig. 5). If the susceptibility diverges at T f, one

must observe a linear dependence in temperature for T > T f with the slope 1 / y. This is what we get and the value y

=

1.40 ± 0.06 is close to what is generally

observed with ferromagnets or extremely soft amor- phous magnets [7, 8] y

=

1.33. The deviation from the linear dependence for T f T 1.05 T f is probably

due to our measurement field, still too large (10 One).

However, a breakdown of the divergence of xo near

Tf in a-GdNi cannot be totally excluded.

The field exponents 6 and 62 defined by M - Hl/ðl

at T f and M - H1/u2 below T f have also been extract- ed from our low field experiments simply by plotting log M versus log Hint at different temperatures (Hint

=

H - NM). This procedure which does not take into

account higher order terms in the field expansion is

rather tricky except at T f and below Tf. Around this temperature, Ms M(H) even for fields of the order of some tens of Oe.

Fig. 5.

-

Determination of y and Tf from x/(dx/dT) =

-1(T - Tf) in a-GdNi. The measurement field is equal to

y 10 Oe.

The result given in figure 6 shows that 61

=

2.25 ±

0.10 and £52

=

6.0 + 0.1. These values may be compar- ed to the predicted mean field exponents [1] : 61

=

7/3

and b2

=

5. The agreement is amazingly good, espe-

cially if we consider the role of sample inhomogeneities

mentioned above. Furthermore, von Molnar et al. [2]

got nearly the same 61 exponent in a-GdAg. Therefore,

it seems probable that the extremely weak sponta-

neous magnetization observed at T ~ Tf does not

affect seriously the value of the field exponent b1 at Tf.

In conclusion of this part, our low field measure-

ments in a-GdNi allow to check qualitatively the two

limits of the equation of state of Aharony and Pytte :

the limit T

=

T f where M

=

H1/ð1 and the limit T _ y B’y

T > Tf f where X - x T Tf Tf y. . The measured expo-

Tf ) p

nents 61 and b2 are not very different from those pre- dicted within a mean field hypothesis : ð1

=

2.25 compared to 7/3, b2

=

6 compared to 5. The value

y

=

1.4, compared to the mean field one : y

=

1, shows that critical fluctuations must be taken into account in a-GdNi.

Fig. 6.

-

Thermal variation of 6 defined by H - M,3. Only the values 6 at T f, and 6, below Tf are significant.

a : GdNi ; b : DyNi.

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297

It would be of interest to know the theoretical exponents 61 and 62 within the framework of the second scaling hypothesis of Aharony and Pytte [4]

in which xo does not diverge.

Table I shows the critical exponents determined from low field experiments on soft amorphous alloys.

The values of 61 are definitely different from those

expected for ferromagnets. However this difference becomes smaller with YFeo3, a weak ferromagnet

The very existence of 62 shows a qualitative diffe-

rence with ferromagnets for which this exponent has no meaning due to finite M..

These results contradict the conclusions drawn from large field experiments such as in a-GdAu [7]

or from low field experiments in extremely soft met- glas [8] where D/J -> 0 (a hopeless case for determin-

ing intrinsic characteristic of disorder, although this

material constitutes one of the most important appli-

cations of amorphous alloys in magnetism). In both

cases, too large applied fields and/or uniaxial parasitic anisotropy components break up the spherical sym- metry and therefore induce a spontaneous magnetiza-

tion.

Before ending with soft amorphous systems, let us mention a possibility of crossover between the random

anisotropy regime and a ferromagnetic like regime

induced by dipolar energy effects [9]. Following the simple argument of competition between exchange

and random field (Imry and Ma [10]), it is shown that

a random anisotropy system breaks up into domains of size lc/a ~ (J/D)1/(2-d/2) in which the spins are nearly aligned (M - MJ.

But the magnetization being non uniform from one

domain to another, it induces local dipolar effects. The

dipolar energy of order N(I/a)d Ms (N effective demagnetizing factor of a domain, a interatomic

distance) must compete with the anisotropy energy

D(I/a)d/2.

Two cases can be considered :

i) low dipolar effects :

The domain size is unchanged

ii) large dipolar effects

The domain size is modified /’

-

J and is The domain size is modified l’c a

=

- 1 NM2 and is

independent of the dimensionality. Within this hypo-

thesis l’c is always smaller than Ic. Such a reduction of the domains size can be important in soft amorphous

materials and may be understood in terms of a break-

ing up of Imry and Ma domains into Weiss domains.

In the case of a-GdNi, D/J ~ 10-2 , HA

=

D/Ms ~ 103 Oe and HD

=

NMS N 102 Oe. A breaking up of

Imry and Ma domains implying HD/HA >> (D/J)3

for d

=

3 could occur in this system at low tempera-

ture. A crossover from Weiss-type domains to Imry

and Ma domains may occur at To when M. decreases

i.e. when the temperature approaches Tf. Such an

intrinsic effect may explain the rapid increase of the

Table I.

-

Critical exponents 6 determined on amorphous alloys from low field experiments (H/M

=

Xo 1(D/J) +

X 1 (DIJ) M" - 1).

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measured spontaneous magnetization for T $ To Tf.

3.2 DyNi. CASE OF A LARGE ANISOTROPY.

-

The

general features of the Arrott plot for this system

(Fig. 2) where D/J = 1 are quite different from those of GdNi (low D/J case). On the other hand, these

features are similar to those obtained in spin glas-

ses [2, 12].

As in spin glasses and contrarily to the low aniso-

tropy case, it is difficult to see on these plots at which

temperature the transition occurs. However, we know from field measurements of M(T) or of XO(T) (Fig. 8. 2a) that, if there is a transition, it should occur

around 13-14 K. At this temperature Xo ’(7)

570 Oe/ JlB/form is clearly far from the demagnetizing

factor limit N = 6.5 Oe/,uB/form demonstrating that

there is no divergency of the susceptibility in a-DyNi.

The field exponents of DyNi, 61 and 62 are determin-

ed using an Arrott-like plot :

in which the susceptibility is assumed finite : a(T) - 1/xo(T) ~ function of D/J. The exponent 6 is obtained from a log-log plot of 1/xo - H/M vs. M. Such a procedure is not necessary in a-GdNi and more

generally in soft systems where X0-1 ~ 0. As indicated

before only the exponents 6

=

61 at T f and 6 = ð2

below T f are relevant. We got ðl

=

62

=

2.40 ± 0.05 (Fig. 6b). This result is in agreement with that obtained for DyCu [2] and seems to indicate a general behaviour

of amorphous magnets with large D/J. This result could also be valid for the low D/J case if the field exponent below Tf, 62 was, to some extent, changed by the parasitic uniform anisotropy components, a

plausible hypothesis.

3.3 Dyo.5Gdo.5Ni. INTERMEDIATE CASES.

-

In this system with an intermediate value of D/J, the Arrott plot (Fig. 3) shows a behaviour very similar to that

predicted by Aharony and Pytte [1]. However, the measuring fields are too large to provide good enough

information. As an example, it is not possible to know

with certainty whether xo diverges or not from figure 3. Low field experiments on this system and with other compositions are in progress. We have already

measured the xo in very low fields. They are compared

to the demagnetizing field susceptibilities in figure 7.

It is clear that xo does not diverge whatever is the value of x i.e. of D/J, except perhaps with GdNi

which has been discussed above. In a coming paper, xo will be plotted vs. D/J, in order to see whether

the recent prediction, Xo - (D/J)4, is right or not.

4. Onset of irreversibility.

The onset of irreversibility in random anisotropy systems has not been really studied. We give here a

first approach based on an analogy with spin-glasses

Fig. 7.

-

Low field initial susceptibility measured at Tf in DYxGd1-xNi. The demagnetizing field limit is given in

dashed line. The ratio D/J varies by at least one order of magnitude between x

=

0.25 and x

=

1.

for which this problem has been crucial for many years. It is now starting to be understood in terms of a crossover between weak and strong irreversibi-

lity [I I along the line H2 ~ (Tf - T)cP where p ~ 3

is the usual crossover exponent [12] associated with the Edwards-Anderson order parameter [13]. However

this point is still controversial and one may also think that the exponent 2/3 of H vs. (Tf - T) characterizes

a true transition in the Heisenberg model [14] or is

related to a breaking of the replica symmetry in Heisenberg [15] or in Ising [16] models.

The line above which irreversible effects vanish

can be obtained from the M(T) curves measured by increasing and then by decreasing the temperature, the sample having previously been zero field cooled.

Some of these curves are given in figure 8a for mode-

rate fields. The temperature above which M(T) is reversible, for a given field, gives a point of the irre-

versibility line. In these materials, this temperature is

slightly above M(T) peak. Such a line has been plotted figure 9 for DYo.sGdo.sNi. We have used 12 different

fields between 13 and 2 000 Oe. The H(T) function

decreases and vanishes at Tf, a result normally expect- ed. More interesting is the linear plot obtained for

log H vs. log (Tf - T). Furthermore, the temperature exponent is found equal to 1.57 ± 0.02, which is very close to the one observed in Heisenberg spin glasses,

and the coefficient is equal to 5.5 Oe/(K’-5’).

This result shows a striking analogy between ran-

dom anisotropy magnets and spin-glasses, which is already suggested by the general behaviour of the

magnetization curves (see Fig. 8a, b). A detailed study

of this question will be published soon. Another very

interesting point to look at is the possibility of an

extension of the study of the onset of irreversibility

on the (D/J)-T and (D/J)-H planes. In spin glasses,

it is extremely difficult to modify continuously the

frustration and therefore there are no studies of

irreversibility, except on the H-T plane.

As we have not yet determined accurately D/J vs. x

we will just give here some results versus x.

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299

Fig. 8.

-

(a) zero field cooled ( ) and field cooled (....) magnetization versus temperature in a-Dy xGd1-xNi (b) Hysteresis loops measured at 4.2 K in a-Dy,,Gd, - _,Ni.

1) For 0 K x 0.5. 2) For 0.75 - x - 1.

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Fig. 9.

-

Irreversibility line in the random anisotropy system a-DYo.sGdo.sNi.

Insert : Log-log plot of H(Oe) vs. T(K) giving H

=

5.5 x (Tf - T)1.S7. f

.

Let us consider for example the (D/J)-T plane

for which H

=

0 or any parallel plane defined by

H

=

constant. Irreversibility lines for the limit T Tf, analagous to the H2 ~ (T f - T)J> line of the H-T plane, can be deduced from the magnetization curves

measured in a constant field H; these irreversibility

lines will be given elsewhere.

For T T f, one expects another type of crossover between a non equilibrium state dominated by ther-

mal activation (kT D/J) and a state at equilibrium (kT » D/J ; D/J represents here the average height

of energy barriers). In this case, the crossover line should be given by (D/J) - TI". Several criteria may be used to determine such a line : we have chosen to

plot the ratio T;/T f versus x where Ti is the tempera-

ture of the inflexion point of the zero field cooled

M(T) curve. Figure 10 shows that this ratio decreases

abruptly between x

=

0.5 and x

=

0.25. The same

feature is also observed on the coercive field (Fig. 8b)

but some more experiments are needed to show this

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301

Fig. 10.

-

Inflexion point of the zero field cooled M(T)

curve versus the content of dysprosium. This curve can be

considered as an irreversibility line in the (D/J)-T plane.

clearly. This abrupt decreasing around x

=

0.25 may be due to the functional dependence of x vs. D/J ; it

may also indicate a very rapid drop of irreversible effects near the weak anisotropy regimes.

Many interesting questions arise from this first

study on the onset of irreversibility in random aniso- tropy systems which we will try to answer in the future.

5. Conclusions.

This paper summarizes some recent magnetization

measurements performed at low and moderate fields

on the model system a-DYxGdl-xNi where Ni is non

magnetic and the anisotropy to exchange ratio D/J changes continuously with x.

We have confirmed some previous equilibrium

results on a-GdAg and a-DyCu [2] and we have shown

that both low and large anisotropy systems obey a

field power law M - H1/b at T f and just below Tf.

At Tf, 61 = 2.3, whatever the value of D/J is. Below T f large anisotropy systems give b2

=

61 - 2.3 ± 0.1

and for low anisotropy systems ð2 ~ 5-6. This last result may simply not be relevant due to the effect of

sample inhomogeneities in soft amorphous materials.

In the low field limit, the alloys of formula

Dy,,Gd, -.,Ni (except x

=

0), in which D/J changes by

at least one order of magnitude, do not show any divergency of xo at Tf. The particular behaviour of

GdNi has been discussed in details :

Because of the weakness of the ratio D/J, coherent anisotropy components due to internal stresses lead

to an apparent divergency of xo at Tc; but a slight

increase of the random anisotropy suppresses this effect. Similarly, one could expect that chemical disorder can destroy the divergency of xo at Tc in crystalline magnets.

Such a possibility has been proposed among others

by Mukamel and Grinstein [18].

Finally, we have studied the onset of irreversibility

in these amorphous alloys showing the existence of a

line very similar to the so-called « de Almeida-Thouless line » [16] of spin glasses. Furthermore, we have given preliminary results of a study of the irreversibility

versus D/J.

The global behaviour of our model system

DyxGdl _xNi shows an evolution from a « spin-glass

like » to a « ferromagnetic like » behaviour which can

be interpreted roughly in terms of (D/J)

-

dependent

intrinsic domains introduced by Imry and Ma [10].

This point as well as others mentioned in this paper will now be developed

Acknowledgments.

We gratefully acknowledge A. Lienard and G. Fillion for their help during the preparation of amorphous samples and SQUID measurements and S. von

Molnar, T. McGuire and D. Gambino for their association in the early stage of this work.

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