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Submitted on 1 Jan 1978
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MAGNETIC FIELD DEPENDENCE OF THE
SUSCEPTIBILITY AND SPECIFIC HEAT IN A (La,
Gd) Al2 SPIN GLASS
C. Bredl, F. Steglich, H. Löhneysen, K. Matho
To cite this version:
JOURNAL DE PHYSIQUE
Colloque C6, supplément au n° 8, Tome 39, août 1978, page C6-925
MAGNETIC FIELD DEPENDENCE OF THE SUSCEPTIBILITY AND SPECIFIC HEAT IN A ( L a , G d ) A l2 SPIN GLASSX
C D . Bredl, F. S t e g l i c h , H.V. Lohneysen and K. Matho
II. Physikalisches Institut der Univers-tt&t Win, Ziilpicher Str. 77, D-5000 Win, W. Germany
xx Centre de Reeherehes sur les Tr§s Basses Temperatures, CNBS, B.P. 166 X, 38042 Grenoble, France
Résumé.- La chaleur spécifique magnétioue linéaire, Cm = yT, de <Laog2Gd008)Al2est réduite par un
champ magnétique H. Pour H £ 1 tesla, y(H) est expliqué à l'aide dû* modèle RKKÏ. La forte diminution de Y observée dans des champs faibles (H ^ 0,1 tesla) est comparée à la forte réduction de la
suscep-tibilité et attribuée au blocage de nuages superparamagnétiques.
Abstract.- The linear magnetic specific heat, C^ = yT, of (Lao.92Gdo.b8)A12 is reduced in a magnetic
field H. For H £ 1 tesla, y(H) is explained within the RKKY model. The steep decrease of y already in small fields (H < 0.1 tesla) is compared to the strong depression of the susceptibility and in-terpreted as being due to the blocking of superparamagnetic clouds.
The predominant features of spin glasses, the "cusp" in the low field susceptibility x a n d
onset of remanence below a temperature T, show up in magnetic measurements. A phenomenological des-cription l\l invokes the existence of superparama-gnetic clouds which are blocked below T- : the bloc-king of a few clouds with large moments can account for the magnetic effects. Calorimetric investiga-tions have not revealed any 'incident' in the tem-perature variation of the zero field magnetic spe-cific heat C . They show a rather large contribu-tion already well above T_ as well as a characte-ristic law C = Y T near T,_ and down to lowest
tem-m f
peratures. This suggests that only a few degrees of freedom can be connected with the blocking me-chanism, the majority being related to the internal formation of clouds.
The (La, Gd )Alg system has been shown to be a spin glass through previous investigations of x>
111 and C , /3/. Here we present a comparative stu-m
dy for a c = 8 % single crystal in fields up to 5 tesla with particular emphasis on the low field region.
The main results on x a re reported in figure 1 : (i) the susceptibility maximum x is
decrea-max sed by 85 % in a field of 0.1 tesla and (ii) Tf
is displaced from 2.3 K to 1 K. In the model of su-X work performed within the research program of
Sonderforschungsbereich 125 Aachen-Jillich-Koln
perparamagnetic clouds /!/, we interpret this as the clouds being progressively locked in as H is increased, most of the clouds are blocked in a field of 0.1 tesla, i.e. their relaxation times be-come larger than the measuring time of x (^10 1s ) .
5 |\ (La0.92Gd0.08)A,2 |
2 V * x 9
Vv *
Q\ 1 1 1 1—lo
0 0 0 5 H (Tesla) 0J
Fig. 1 : Susceptibility maximum x a an<i
temperatu-re Tf of Xmax v s- H- Lines are intended as
visual guide
The magnetic specific heat C per impurity spin, obtained by subtraction of the matrix contri-bution, varies linearly with T, as found previously for this system /3/. This holds from the lowest accessible temperature 0.4 K up to ^ 4 K, well above T, = 2.3 K. The two important results we wish to report are : (i) in the presence of a ma-gnetic field, the linear C dependence on T is not altered up to H = 5 T (ii) y decreases with H, hence all data can be described by the equation
Cm(H,T) = y(H) . T ~ where a = 1 .OO
+
0.05 as determi- ned from log-log plots. The experimental y(H) va- lues divided by k are shown in figure 2. In aB
field of 5 tesla, y is reduced by 50 %. However, a strong initial decrease in as low as 9.1 tesla affects approximately 10% of y.
Fig. 2 : Coefficient y of the linear magnetic spe- cific heat in units of kg
E.
magnetic field H. In- sert shows low field date on expanded vertical sca- le (horizontal scale unchanged !). Solid and dot- ted lines are fits to data as explained in the textWe can compare the experimental y(H) curve with the coefficient yRKKy of Cm at low temperatu- res which was calculated from the contribution of small clusters to the free energy in the scaling limit of the dilute R K model /4/ : ~
Here J, is the digamma function, S the spin value 4
and W1 =
-
V /v an energy proportional to the RKKY 3 0amplitude Vo divided by the atomic volume v. We first note that from eq. (I) the area under the y(H) curve should depend only on S and g :
a, r2kB2s
tesla K-$2)
jo
yRm(H) dH =-
= 2.46-
'6 % ~ ~ g
-
The area under the measured Y(H)/kg curve, inclu- ding a long tail as suggested by the upward curva- ture of the last points, cf. figure 2, is estima- ted roughly as 2.4 tesla K - ~ against 4.3 obtained from eq.(2) with S = 7 1 2 and g = 2. The order of magnitude agreement supports that the magnetic spe- cific heat is indeed dominated by the freezing of degrees of freedom within small RKKY clusters.
We can now try a fit to our data simply by scaling yRKKY(H), eq.(l), with a reduction factor 0.55 to account for the numerical discrepancy in the aeras. The solid curve in figure 2 represents yb(H) = 0.55 y-(H) for Wl/kB = 13.4 K. For H 0.5 tesla, Y (H) describes the experimental
b
points quite well. At high fields, i.e.
gl.iBH ?, r(2S + I) c W1, yb(H) shows a long tail with a H - ~ decay. This tail is due to the Lorent- zian wings in the RKKY energy spectrum. The quan- titative disagreement in the areas as well as the values for W1 determined from different experiments
(Vo as obtained by high field magnetization /2/ yields Wl/kB = 3.5 K) is probably due to three fac- tors : (i) the Gd concentration is rather high (8%) (ii) for the calculation of V from M only the se- cond virial approximation was used 151 (iii) high energy cutroffsare present in the spectrum 161. We estimate H
*
0.5 tesla and Hlf* 12 tesla for the1 a
antiferromagnetic and ferromagnetic cut-offs, res- pectively. The asyumetry is caused by a ferromagne- tic first and second neighbor RKKY interaction in this system 121. Qualitatively, the presence of cut-offs leads to a rapid decay of y(H) in the ran- ge of corresponding external fields.
At low fields, H
4
0.5 tesla, yb varies s m o o t h l y s ~ ~ and cannot account for the strong ini- tial variation of the experimental y(H) curve. One can empirically describe the "excess" above the RKKY "background" by Ay (H) /k = (Y (H)-
yb (H) ) /kgS~
= 0.033 KK1(l
-
(HI1 tesla) ) for H2
1 tesla (see dotted line in figure 2). This anomalous field de- pendence with a half width of 0.1 tesla suggests that Ay(H) is related to the same irreversible properties of spin glasses which also govern thex
(H) behavior discussed above.the remanent magnetization of spin glasses /I/. Multiplying the density of these "superparamagnetic
excitations", n(E) = ~ A ~ ( O ) / I T ~ ~ ~ ~ , by the half width of 0.1 tesla, we estimate a corresponding
fraction of ~ l o - ~ d e ~ r e e s of freedom of the total magnetic entropy. Since each Gd spin has 8 degrees of freedom this corresponds to
*lo2
spins in a su- perparamagnetic cloud.In conclusion, our estimate of the small fraction of degrees of freedom associated with the blocking of superparamagnetic clouds is based on the observation of two distinct characteristic field scales in the coefficient y(H). This estima- te should be valid quite independently of the de- tailed physical picture for the blocking.
References
/I/ Tholence, J.L., and Tournier, R., J. Physique 5 (1974) C4-229
-
/2/ v. ~Ehneysen, H., Tholence, J.L. and Steglich, F., 2. Physik B. in print
/3/ Trainor, R.J. and Mc Collum, D.C., Phys. Rev. B9. (1 974) 2145 ; ( 1 975) 3581
-
/4/ Matho, K., these conference Proceedings /5/ Larkin, A.I. and KmeltNitskii, D.E., Soviet
Physics JETP