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Experimental arguments for a non-zero transition temperature in RKKY Heisenberg spin glasses without

anisotropy

A. Fert, N. de Courtenay, H. Bouchiat

To cite this version:

A. Fert, N. de Courtenay, H. Bouchiat. Experimental arguments for a non-zero transition temperature in RKKY Heisenberg spin glasses without anisotropy. Journal de Physique, 1988, 49 (7), pp.1173-1178.

�10.1051/jphys:019880049070117300�. �jpa-00210799�

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Experimental arguments for a non-zero transition temperature in RKKY Heisenberg spin glasses without anisotropy

A. Fert, N. de Courtenay and H. Bouchiat

Laboratoire de Physique des Solides, Université de Paris Sud, 91405 Orsay, France (Reçu le 17 novembre 1987, accepté sous forme définitive le 23 fivrier 1988)

Résumé.

2014

Alors que l’existence d’une transition de phase à température non nulle est bien admise pour les

verres de spin de type Ising à 3 dimensions, des travaux théoriques récents suggèrent que Tc est nul pour des

verres de spin Heisenberg sans anisotropie et que le Tc non nul des systèmes réels est dû à l’anisotropie. Pour

éclaircir ce problème, nous analysons l’influence de l’anisotropie

sur

le comportement critique et la température de transition de phase d’alliages CuMn et AgMn dopés avec des impuretés d’or ou de platine.

Cette analyse suggère plutôt un Tc fini pour les verres de spin Heisenberg RKKY dans la limite d’anisotropie

nulle.

Abstract.

2014

While the existence of

a

phase transition at finite Tc is well admitted for Ising spin glasses in 3- dimensions, recent theoretical studies have proposed that Tc is zero in Heisenberg spin glasses and that the finite Tc of real systems is induced by the anisotropy. To clear up this question,

we

analyse the influence of the

anisotropy

on

the critical behaviour and the transition temperature of CuMn and AgMn alloys doped with Au

or

Pt. This analysis rather suggests

a

finite Tc for RKKY Heisenberg spin glasses in the limit of

zero

anisotropy.

Classification

Physics Abstracts

75.30 - 75.30G - 75.30H - 75.40

1. Introduction.

There is now a strong experimental evidence for a

phase transition at finite T, in spin glass alloys [1].

On the theoretical side, it seems well admitted that, in three-dimensional systems, a phase transition

takes place in Ising spin glasses [2] but not in short

range Heisenberg spin glasses [3]. The case of

RKKY Heisenberg spin glasses is not completely

clear. On the basis of scaling arguments, Bray et al.

[4] have proposed that a RKKY spin glass in 3d is at

its lower critical dimension, so that the transition at finite Tc observed in metallic spin glasses should be

due to the existence of anisotropy. Bray et al. [4]

predict for the variation of 7c with the anisotropy in

a RKKY vector spin glass with Dzyaloshinsky- Moriya (DM) or dipolar anisotropy:

which gives :

J and dJ =- D are the exchange and anisotropy strengths respectively (A is a constant of order unity

and yD = 3/2 for 3-dimensional systems). As d tends

to zero, Tc tends to zero but the logarithmic depen-

dence of equations (1) can explain that T, does not change very much in the experimental range of d.

Computer simulations on RKKY Heisenberg sys- tems have been recently published [5]. They are compatible with the predictions of Bray et al. [4] but

cannot rule out completely the possibility of a non-

zero Tc. In this paper we present some arguments for

a non-zero Tc in RKKY Heisenberg spin glasses.

These arguments are derived from experimental

data on CuMn and AgMn alloys in which the DM anisotropy is made to vary by adding Au or Pt impurities [6]. More precisely our arguments are based on :

(a) our previously published analysis of the influ-

ence of anisotropy on the critical behaviour [7] ; (b) an analysis of experimental data for Tc(d) [8],

with T, (d) extrapolated in the limit d --+ O.

We discuss the two preceding points in sections 2 and 3 respectively.

2. Influence of anisotropy on the critical behaviour.

de Courtenay et al. [7] have studied the critical

behaviour of the non-linear susceptibility for series

Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphys:019880049070117300

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1174

of CuMn and AgMn alloys doped with Au impuri-

ties. We show in figure la an example of the

influence of the DM anisotropy strength (fixed by

the concentration of Au) on the non-linear suscepti- bility KNL at T = T,, : two different regimes, corre- sponding to exponents 8 I = 3.1 ± 0.2 and 8 H =

4.5 ± 0.2, are observed in the low and high field

limits and the field of the cross-over between the two

regimes increases with the concentration of Au, i.e.

with the DM anisotropy strength (1). A similar anisotropy dependent cross-over between two differ- ent values, y I and y H, of the exponent y is also

Fig. 1.2013(a) Non-linear susceptibility KNL

versus

H at r==7e for CuMnO.2 at% alloys doped with Au [7].

KNL is defined by M

=

XH(1 - KNL). With KNL ~ H2/6,

the slopes at low and high fields correspond to 5j

=

3.1 ± 0.2 and 8 H

=

4.5 ± 0.2. Similar results have been found in AgMnAu alloys [7] ; (b) K NL/ a * (d)

versus

H/H*(d) for series of CuMnAu and AgMnAu alloys at T - Tc, with a * (d ) and H* (d ) varying

as

d1.7 and dO.9 respectively [7]. This scaling expresses equation (2b).

(I) Notation : KNL

=

(X - M/H)/X with X

=

(M/ H)H -+0’ KNL - h2/s for T h2, KNL - h2/T y for

h2 Tlp, with

T =

r/7, - 1, h

=

gJ-LB H/kB Tc, CPA

=

anisotropy cross-over exponent, cp H

=

ï’ H s H/ ( s H -1 ).

observed in the temperature dependence of the non-

linear susceptibility at low fields above Tc (see Ref.

[7] for a detailed report).

These experimental results, which show an ani- sotropy induced cross-over between two critical

regimes [9], are accounted for in reference [7] by using a three-parameter scaling function (1) :

with values of the reduced anisotropy d calculated as a function of the concentration of gold [7]. For example, we show in figure Ib how all the data at

Tc for series of CuMnAu and AgMnAu can be gathered on a unique curve by plotting KNL/ a * (d ) (with a * - d0.9 versus H/H* (d ) (with H* - dl-1),

in agreement with the limit of equation (2a) foi

T - 0 :

with

This analysis has given the exponent of the

anisotropy induced cross-over, (P A =z 0. 8 -t 0. 1 for

both the CuMn and AgMn systems, and two sets of exponents (cp I, 8I, yI) and (cp H, 03B4H, yH) characteriz-

ing the scalin function in the

two limits, d >

T I’P A, d> , (PA ’OH and d « T, d .r. h’,"PA qH re-

spectively [7]. We note that one value Of 0 A

accounts for the dependence of both a* and

H* on d, which checks the selfconsistency of the picture.

Obviously, if a scaling function in the form of

equations (2) exists and if its low anisotropy limit for

d much smaller than T 1/’PA and h 1/’OA ’OH is well

established, this means that, in the limit of zero

anisotropy, RKKY Heisenberg spin glasses present

a transition at Tc =F 0 with the set of exponents 03B4H, YH9 ’PH’ etc. The experiments of reference [7]

have convincingly shown the existence of an ani- sotropy dependent scaling and the d ---> 0 limit of the critical behaviour appears to be clearly observed, see

e.g., the right side of figure 1. However, even for the sample with the lowest anisotropy, CuMn without

Au (d

=

0.036), the Heisenberg regime is observed only for h > 2 x 10- 2, 7 > 0.1. This range of

T

corresponds to a correlation length smaller than

100 A. In this length range deviations from the

RKKY behaviour (R - 2 instead of R - 3) 4re-expected

[10] and this could be a plausible explanation for a

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critical behaviour different from that expected by Bray Moore and Young [4] for RKKY Heisenberg spin glasses. Whence we infer that the analysis of the

influence of the anisotropy on the critical behaviour suggests the existence of a transition at finite

Tc for zero anisotropy Heisenberg systems but

cannot be absolutely conclusive (of course, the

existence of an Heisenberg regime would be proved

more strongly if there would exist a spin glass with a

lower anisotropy and Heisenberg regime extending

to smaller values of h and T).

3. Shift of the transition temperature induced by the anisotropy.

The most direct way to see if Tc (d = 0 ) has a zero or

non-zero value is to analyse the variation Tc(d) and

to extrapolate to d

=

0. A difficulty arises from the additional variation of Tc due to the reduction of the

isotropic exchange by mean free path effects. Fortu- nately Vier and Schultz [8] (VS) have studied the variation of Tc in very extensive series of CuNin and

AgM alloys doped with several types of impurity,

Au and Pt giving rise to anisotropy-induced positive shifts, and In, Sn, Sb giving rise to negative mean free-path effects. Moreover VS have used their data

on alloys doped with In, Sn or Sb to derive an empirical law describing accurately the variation of

Tc due to mean free path (MFP) effects [11] :

where p is the resistivity of the alloy at low tempera-

tures and

This empirical law can be used to correct the data of VS on CuMn and AgMn doped with Au or Pt for the

mean free path effects.

In figure 2 we show the variation of Tc measured by VS in CuMn4 at% and AgMn5.5 at% alloys doped with Au or Pt. From equation (3) the shift of T, due only to the reduction of the mean free path by

the Au or Pt impurities can be written :

We have calculated A Trp by using the values of po and [Tc(p

=

0 ) - Tc (p

=

oo )] quoted above and

Fig. 2. - Tc versus y for C_uMn4 at%Pty%, CuMn4 at%Auy% and AgMn5.5 at%Auy% alloys : (0 ) experimental Tc found by Vier and Schultz [8] ; (.) Tc corrected for mean free path effects (see text).

p (CuMn4%Auy% ) =10.8 + 0.49 y [14] ,

p ( AgMn5.5% )

=

8.63 03BC03A9cm [8] ,

p (AgMn5.5%Auy% )

=

8. b3 + 0.38 y [13] .

The data of VS corrected for the mean free path

effects are represented by black symbols in figure 2.

For the CuMnPt and AgMnAu series the corrections for mean free path effects are relatively small, whereas, for CuMnAu, the experimental shift and

the correction have approximately the same magni-

tude. We will therefore limit our analysis to the

CuMnPt and AgMnAu systems for which the exper- imental data cannot be significantly affected by an

error in the calculation of the mean free path

contribution [14].

We now calculate the anisotropy d as a function of

the concentration of Au or Pt. For, say CuMnPt, we write [15, 7] :

where Vrn and Vr are the DM coefficients associat- ed with Mn-Mn-Mn and Mn-Mn-Pt triangles respect-

ively, Vo is the RKKY coefficient, yAu and xmn are the concentrations of Au and Mn and Rc = 42 A,

ro

=

2.55 A (in AgMn, Rc

=

39 A, ro

=

2.89 A) [15, 7]. The values of the ratios V1/Vo have been derived

in previous works by combining ab initio calculations and experimental data [6, 7, 16, 17] and are listed in

table I. One can rely on this set of values which

appeared to account consistently for several spin-

orbit induced properties, from ESR shifts to changes

in the critical behaviour. The corresponding values

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1176

Table I. - Relative strengths of the DM and RKKY

interactions in CuMn or AgMn alloys doped with Au

or Pt : (a) from ab initio calculations of the spin-orbit scattering by Pt, see reference [6] : (b) obtained from

( v 1 N by comparing the macroscopic ani-

( 0 CuMn

sotropy energy of CuMnPt with that of CuMn, see reference [16], or that of CuMnAu, see reference [13] ; (c) obtained from ( ( v0 v 1 Mn by cumn comparing

the ESR shift of CuMn and AgMn alloys, see reference [7].

-

of d derived from equation (5) range from 0.0036

(CuMn) to 0.33 (AgMn5.5%Au5%), see table II.

We now compare the variation of Tc induced by

Au or Pt impurities in CuMn or AgMn with the

variation expected in several models :

.

(a) the variation expected by Bray, Moore and Young [4] (BMY) for RKKY vector spin glasses can

be derived from equation (1a). We have calculated

Tc for the CuMnPt and AgMnAu series of VS [8] by using the values of d

=

DIJ calculated above, A =1, YD

=

3/2 and by choosing J to obtain Tc = 24 K for CuMn4 at% (d

=

0.036) and T, =

18.5 K for AgMn5.5 at% (d

=

0.095). The values of

Tc calculated for the series CuMn,Pty are shown in figure 3, see curve BMY, and can be compared with the corrected experimental Tc (i.e. the experimental Tc of VS corrected for the mean free path effects, as explained above). It turns out that equation (1)

Fig. 3.

-

T,

versus

y for CuMn4 at%Pty% alloys. VS : experimental values of Viers and Schultz [8] corrected for

mean

free path effects. BMY : T,, calculated from equation (1). MCMB : Tc calculated from equation (6). KS : Tc calculated from equation (7).

predicts too large shifts of Tc. We can lower the

calculated shifts by lowering the values of d uni- formly. When we lower the factors of d by about an

order of magnitude, the calculated Tc come closer to

the experimental Tc but it is hard to obtain a good fit throughout the whole concentration range. This can be clearly understood from figure 4 where j2 ITC’ 2 is

Fig. 4. - J2/ T;

versus

In (dJ / Tc). The straight line is the variation predicted by equation (1). The experimental T,

are

those obtained by Vier and Schultz [8] corrected for

mean free path effects. In order to fit the experimental

curve with the calculated line in the left side of the figure,

we

have taken values of d lowered by

a

factor of 8 (with respect to their values of Tab. II), and J

=

63 K for

CuMn4 at% or J

=

44.6 K for AgMn5.5 at%.

Table II.

-

The transition temperature Tc measured by VS, reference [8], the transition temperature corrected

for mean free path effects, T§", and the anisotropy parameter d calculated from equation (5) with the

parameters V1/Vo of table I for series of CuMnPt and AgMnAu alloys.

°

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plotted as a function of In (dY/Tc). Whereas equation (1) gives a straight line in such a plot, the experimental variation departs definitely from a straight line (in Fig. 4 we used A/yD

=

4/3, values of

d lowered by a factor of 8 [18] and J

=

63 K for

CuMn4 at% or J

=

44.6 K for AgMn5.5 at%, which

allows us to obtain an approximate agreement between the calculated and experimental data in the

left side of the figure). Alternatively, by lowering

the value of A and keeping the values of d of table II, the calculated and experimental data can be brought closer but again, as expected from figure 4,

the form of the calculated and experimental curves

are different. We can however remark that, if the data of figure 4 for CuMn and AgMn respectively

are considered independently, they are approxi- mately consistent with two straight lines (excepted

for the most Pt-doped CuMn alloys, Cm = 1 % and 1,96 %). This means that an approximate agreement

can be obtained only by introducing in equations (1)

different values of A (by a factor of about two) for

the CuMn and AgMn systems ;

(b) the variation of T,*expected for short range vector spin glasses in 3 dimensions is written [3] :

The values of 7c calculated in this way for the series

CuMn.,Pty (with a value of J fixed to obtain

Tc

=

24 K for the value d

=

0.036 of CuMn4 at%)

are shown in figure 3, see curve MCMB. The calculated shifts are much larger than the exper- imental ones ;

(c) the variation of Tc predicted in the mean field

model of Kotliar and Sompolinsky [19] is written:

This gives the curve KS in figure 3. The predicted

values of the shifts induced by Pt are much too small.

(d) The scaling function, equation (2), can be

written :

which implies for the variation of Tc with d :

As discussed in section 2, the analysis of the ani- sotropy induc d cross-over between two critical

regimes in CuM u and AgMnAu has given [7] :

We have plotted the experimental Tc of VS [8]

(corrected for mean free path effects) as function of

do.8, see figure 5. It appears that all the Tc gather on

two straight lines. These straight lines intercept the

vertical axis at Tc (d

=

0 )

=

22.4 K for CuMn4 at%

Fig. 5.

-

T,, versus d0.8 for the CuMnPt and AgMnAu

series (T, from VS, Ref. [8], after correction of the mean

free path effects ; d calculated as described in the text).

and T,(d

=

0) = 15.8 K for AgMn5.5 at%.

Moreover, when Tc/Tc(d

=

0) is plotted as a func-

tion of dO.s, see figure 6, all the experimental data of

the two series gather on a unique straight line corresponding to the equation :

with

a

=1.13 ± 0.1. One could wonder whether the

non-zero limit of T,, obtained by extrapolating to

zero DM anisotropy cannot be accounted for by a

residual non-DM anisotropy. Actually it would be necessary to assume that the residual non-DM

anisotropy has the order of magnitude of the DM anisotropy of CuMn, which is ruled out by the

definite DM character (unidirectional) of the macro- scopic anisotropy of CuMn.

Fig. 6.

-

Tc/Tc(d

=

0) versus do.8 for the CuMnPt and

AgMnAu series. Tc (d = 0) is derived from figure 5 : Tc(d

=

0)

=

22.3 K for CuMn4 at%, T,,(d

=

0)

=

15.7 K

for AgMn5.5 at%.

4. Conclusions.

We have analysed experimental data on the effect of

the DM anisotropy on the critical behaviour and the

transition temperature of AgMn and CuMn alloys

doped with Pt or Au impurities. Our aim was to

clarify the role of anisotropy in Heisenberg spin

glasses : is there a transition at finite temperature in

three dimensional RKKY spin glasses ?

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1178

The experimental data for our series of CuMnPt and AgMnAu alloys fit with the following picture :

(i) the effect of anisotropy on the critical behavior of the non-linear susceptibility can be described by a scaling function of the 3 parameters T, h and d. We

obtain cfJ A === 0.8 for the exponent describing the

cross-over between the low and high anisotropy regimes ;

(ii) a good fit is obtained with Tc(d

=

0) =1= 0 and Tc(d)

=

Tc(d

=

0)(1 + 1.13 d0.8 for both the CuMn

and AgMn systems. An approximate fit can also be

obtained with the picture of Bray, Moore and Young [4], T - [1 + 2 A IYD In (Tc/dJ)]-1I2, but only when

different values of A (by a factor of about two) are

taken for the CuMn and AgMn series.

In conclusion, our analysis of the experimental

data cannot rule the picture of Bray, Moore and Young [4] but a better agreement is obtained with

Tc (d = 0 ) =A 0 and A Tc - d . It thus brings new

arguments in favour of a transition at finite tempera-

ture in RKKY Heisenberg spin glasses without anisotropy. We hope these new data will lead to further theoretical and experimental arguments.

Acknowledgments.

We acknowledge fruitful discussions with M. A.

Moore and P. Young who suggested the plot of figure 4.

References

[1] For

a

general review, see e.g. BINDER, K. and

YOUNG, A. P., Rev. Mod. Phys. 58 (1986) 801.

[2] BRAY, A. J. and MOORE, M. A., J. Phys. C 17 (1984) L 463 ;

MCMILLAN, W. L., Phys. Rev. B 30 (1984) 476 ; BHATT, R. N. and YOUNG, A. P., Phys. Rev. Lett. 54

(1985) 924 ;

OGIELSKI, A. T. and MORGENSTERN, I., Phys. Rev.

Lett. 54 (1985) 928 ;

SINGH, R. R. P. and CHAKRAVARTY, S., Phys. Rev.

Lett. 578 (1986) 245 ;

REGER, J. D. and ZIPPELIUS, A., Phys. Rev. Lett. 57

(1986) 3225.

[3] MORRIS, B. W., COLBORNE, S. G., MOORE, M. A., BRAY, A. J. and CANISIUS, J., J. Phys. C 19 (1986) 1157 ;

OLIVE, J. A., YOUNG, A. P. and SHERRINGTON, D., Phys. Rev. B 34 (1986) 6344.

[4] BRAY, A. J., MOORE, M. A. and YOUNG, A. P., Phys. Rev. Lett. 56 (1986) 2641 ;

BRAY, A. J. and MooRE, M. A., Phys. Rev. B 34 (1986) 6561.

[5] REGER, J. D. and YOUNG, A. P., to be published.

[6] FERT, A. and LEVY, P. M., Phys. Rev. Lett. 44

(1980) 1538.

[7] DE COURTENAY, N. , BOUCHIAT, H., HURDEQUINT, H. and FERT, A., J. Phys. France 47 (1986) 1507 ; J. Appl. Phys. 61 (1987) 4097.

[8] VIER, D. C. and SCHULTZ, S., Phys. Rev. Lett. 54

(1985) 150.

[9] The existence of

an

anisotropy induced cross-over has been discussed by BRAY, A. J. and MOORE,

M. A., J. Phys. C 15 (1982) 3897 ;

FISCHER, D. S. and SOMPOLINSKY, H., Phys. Rev.

Lett. 54 (1985) 1083 ;

YESHURUN, Y. and SOMPOLINSKY, H., Phys. Rev.

Lett. 56 (1986) 984 ;

KOTLIAR, G., Phys. Rev. B 16 (1987) 8646.

[10] LEVY, P. M. and ZHANG, Q., Phys. Rev. B 33 (1986)

665.

[11] The following theoretical articles have

now

justified

the non-zero limit of Tc for 03C1 ~ ~ which charac- terizes equation (3): JAGANNATHAN, A.,

ABRAHAMS, E. and STEPHEN, M. J., Phys. Rev.

B 37 (1987) 436 ;

ZYVZIN, A. Y. and SPIVAK, B. Z., JETP Lett. 43

(1986) 234 ;

BERGMANN, G., Phys. Rev. B 36 (1987) 2469.

[12] SCHMITT, R. W. and JACOBS, I. S., J. Phys. Chem.

Solids 3 (1957) 324.

[13] GOLDBERG, S. M., LEVY, P. M. and FERT, A., Phys.

Rev. B 31 (1985) 3106 and references therein.

[14] As

a

matter of fact, there is some discrepancy

between the variation of Tc

as

a function of the DM strength in CuMnAu on one hand and

CuMnPt

or

AgMnAu

on

the other hand. We suppose this is due to an error in the correction of the significant

mean

free path effects of CuMnAu.

[15] LEVY, P. M., MORGAN-POND, C. and RAGHAVAN, R., Phys. Rev. B 30 (1984) 2358.

[16] LEVY, P. M., MORGAN-POND, C. and FERT, A., J.

Appl. Phys. 53 (1982) 2168.

[17] DE COURTENAY, N., FERT, A. and CAMPBELL, I. A., Phys. Rev. B 30 (1984) 6791.

[18] An error by

a

uniform factor of 8 in the calculated values of d cannot be ruled out absolutely.

Whereas the relative values of d for series of

doped CuMn and AgMn alloys has been verified by

a

number of experiments (ESR, transverse susceptibility, anisotropy dependence of the criti- cal exponents), their absolute value is fixed by only the ab initio calculations of Levy and

coworkers [6,16] expressing the DM interactions induced by non magnetic transition metal impuri-

ties (e.g. Pt, Pd...)

as a

function of the number of d electrons and their spin-orbit constant 03BBd. For

our

series

we

have used the calculation for Pt impurities to fix the absolute values of d.

However there is some possible

error on

the

number of d electrons of Pt and also

on

the

prefactor of equation (5). Finally,

an

error by

a

factor of 8

on

the absolute values, although

unlikely, cannot be ruled out completely.

[19] KOTLIAR, G. and SOMPOLINSKY, H., Phys. Rev. Lett.

54 (1985) 1063.

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