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High-pressure magnetization of the heavy-Fermion system CeRu2Si 2 .
J. Voiron, J.-M. Mignot, P. Lejay, P. Haen, J. Flouquet
To cite this version:
J. Voiron, J.-M. Mignot, P. Lejay, P. Haen, J. Flouquet. High-pressure magnetization of the heavy-Fermion system CeRu2Si 2 .. Journal de Physique, 1988, 49 (9), pp.1555-1560.
�10.1051/jphys:019880049090155500�. �jpa-00210835�
High-pressure magnetization of the heavy-Fermion system CeRu2Si2 .
J. Voiron (1), J.-M. Mignot, P. Lejay, P. Haen and J. Flouquet
(1) Laboratoire Louis Néel (*), CNRS, B.P. 166X, 38042 Grenoble Cedex, France CRTBT (*), CNRS, B.P. 166X, 38042 Grenoble Cedex, France
(Requ le 29
mars1988, accepté le 24 mai 1988)
Résumé.
2014L’aimantation de CeRu2Si2 monocristallin à basse température
aété mesurée
souspression hydrostatique jusqu’à 6 kbar. Les résultats révèlent
unedécroissance extrêmement rapide de la susceptibilité magnétique ~~ (T ~ 0) pour H suivant l’axe c, à raison d’environ 2014 17 % par kilobar. On constate
uneforte corrélation (~~ (0 ) Tmax
~cst.) entre la variation
enpression de la susceptibilité à T
=0 et la température du
maximum de susceptibilité. Les données pour ~~ (T) T peuvent être représentées par
unecourbe unique rapportée à
unevariable réduite T/Ts (P),
enaccord
avecles théories Kondo à
uneimpureté. L’anisotropie magnétique ~~ ~ décroît
comme ons’y attend pour
unsystème s’approchant du régime de valence intermédiaire, mais d’autres explications sont également envisagées. Les résultats sont comparés à d’autres
études du même matériau
soushaute pression ainsi qu’aux effets observés dans certains de
sesalliages.
Abstract.
2014The low-temperature magnetization of single-crystal CeRu2Si2 has been investigated under hydrostatic pressures up to 6 kbar. The results reveal
anextremely rapid decrease of the magnetic susceptibility ~~ (T ~0) for H applied along the c-axis, at
arate of about 201417% per kbar. A strong correlation (~~ (0) Tmax ~ const. ) is found between the pressure-variations of the susceptibility at T
=0 and the temperature of the susceptibility maximum. The data for ~~ (T) T
canbe represented by
asingle
curvein terms
of the reduced variable T/Ts (P), in accordance with single-impurity Kondo theories. The magnetic anisotropy ~~/~ decreases,
asexpected for
asystem approaching the mixed-valence regime, but alternative
explanations
arealso considered. The results
arecompared to other high-pressure studies
onthe
samematerial
and to the effects produced by alloying.
Classification
Physics Abstracts
75.30M - 62.50
-75.40C
-75.30G
1. Introduction.
The cerium-based ternary silicides [1] belonging to
the tetragonal ThCr2Si2 structure exhibit a large variety of low-temperature behaviours, which in-
clude magnetic ordering (CeRh2Si2) [2], mixed val-
ence (CeOs2 Si2 ) [3], and heavy-fermion (HF) super-
conductivity (CeCu2Si2) [4]. The compound with
ruthenium CeRu2Si2 can be categorized as a
«
medium-heavy-fermion
»material from the value of its linear specific-heat coefficient y=
350 mJ mole - K- 2 [5, 6]. This system was reported
to exhibit quite remarkable magnetic properties [7].
Its susceptibility is strongly anisotropic depending
on whether the applied field is oriented parallel or
normal to the c-axis. In the former case, XII approxi- mately obeys a Curie law above - 70 K, then reaches
(*) Laboratoire associd a l’Universit6 Joseph Fourier,
Grenoble.
a weak maximum around Tmax = 10 K and for
T-+ 0 tends to a high value (,y 0 11 == 3.5 10-2 emu/mole Ce), characteristic of the correlated
Fermi-liquid state. On the other hand, the suscepti- bility for H _L c assumes much smaller values, and in
a X -1 vs. T plot, exhibits a Curie-Weiss behaviour with a large negative 0 below room temperature, followed by a pronounced downward curvature
around - 100 K. The anisotropy ratio X / X J.. in-
creases from - 2.5 at 200 K to 13-15 at 4.2 K, with a faint maximum near T,,ax-
Whereas the magnetic isotherms M (H ) are essen- tially linear with applied field down to - 10 K, positive curvatures gradually develop at lower tem- perature for Hllc, leading to a steplike anomaly
around HM = 8 T at T = 1.5 K. This behaviour,
which is suggestive of some kind of metamagnetism
is further associated with a sharp positive peak in the magnetoresistance [7]. In contrast, X1 remains field
independent up to 18 T and p (H -L c ) increases only
Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphys:019880049090155500
1556
weakly with the applied field. Recent neutron-dif- fraction experiments [8] provided no evidence for an
ordered magnetic structure in this compound, but
rather indicated short-range antiferromagnetic (AF)
correlations with moments along the c-axis to exist among neighbouring cerium sites up to about 60 K.
It is interesting to note that the maximum in
p (Hllc ) persists over the same temperature range.
These results point to a rather unconventional behaviour of the Fermi-liquid state in the presence of an external field. From what we know about this
compound, it seems unlikely that they can be explained by simply invoking the quenching of the
AF couplings by the applied field : even at H
=0,
the system is already in a complicated state where
the normal development of a long-range structure
has been inhibited by demagnetizing processes (Kon-
do effect, s-f mixing, etc.). Furthermore, it is well known that crystalline anisotropy plays an important
role in defining the ground state of non-cubic cerium
compounds. An important point is that very similar effects have also been reported for UPt3 [9] (though
at much higher fields), so that they appear to characterize a new crossover situation which has not
yet been considered in current theories but might
occur in a larger class of HF systems.
It is therefore an urgent task to better document the relationship existing between the various Fermi-
liquid parameters at H
=0 and the way the system responds to an external field. This was undertaken in the present study by measuring the magnetization of CeRU2Si2 as a function of pressure up to 6 kbar. The results are presented in the following and character- istic Grüneisen parameters are derived. Anisotropy
effects and their pressure dependence will receive
particular attention since the measurements were
performed on a single-crystalline specimen for Hllc and H L c. Comparisons will also be made with data obtained for other quantities (p (P, T), V (H))
and in the case of alloy systems.
2. Experiments.
The single crystal used for this study was cleaved
from an ingot grown by a Czochralski technique in a
triarc furnace, under purified argon atmosphere.
The constituents were high-purity elements (Ce :
99.99 %, Ru : 99.999 %, Si :
>99.999 %). The crys- tal presented large cleavage planes which were
checked by x-ray diffraction to be normal to the c-
direction. In order to allow measurements with H either parallel or perpendicular to the tetragonal axis, additional plane faces were cut perpendicular
to the basal plane. The parallelepiped-shaped speci-
men, with dimensions of approximately 0.4 x 0.5 x
0.5 mm3, was the one used for the magnetostriction
measurements in a capacitance cell reported in
reference [10]. The magnetization data for this
sample (Fig. 2 in Ref. [10]) agreed with previous results, including the critical field (HM = 8.3 and
7.9 T at 4.2 and 1.3 K respectively), and the ani- sotropy ratio X II /X 1 = 14 at 4.2 K.
Hydrostatic pressures up to 7 kbar were generated
in a copper-beryllium cell using compressed helium
as a pressure-transmitting medium. The pressure inside the experimental chamber was measured with
a calibrated thermally-compensated manganin gauge located in the pressure generator which is connected to the cell by a capillary tube. At low temperatures, the helium gas solidifies and pressure corrections
were computed using the phase diagram of helium.
Magnetic fields up to 7 T were produced by a superconducting solenoid at the Service National des
Champs Intenses, and the magnetization was
measured by the conventional extraction technique.
The background contribution from the pressure cell
was determined in a separate experiment and sub-
tracted from the data.
3. Results.
The magnetization of our single crystal was measured
at various pressures with the field applied either parallel or normal to the c-axis. The corresponding
curves for T
=4.2 K are shown in figure 1. Pressure is seen to produce a drastic decrease of M(H) for
both field directions.
Let us focus first on the case where H is parallel to
the easy axis (H// c). In this case, the magnetization
in 6 T is reduced by a factor of 3 with only 6 kbar. At
ambient pressure, a positive curvature of M(H) is observed, in agreement with previous data, due to the approach of the steplike transition (pronounced
maximum of 8M/8N) at HM = 8 T. At 6 kbar, on
the other hand, no deviation from a straight line can
be detected any more. This difference indicates that the transition has shifted to higher magnetic fields,
as already inferred from previous magnetoresistance
measurements [11] : in the latter study, HM was
found to increase to 18 T for P
=5 kbar.
The low-field susceptibility XII deduced from the linear part of the magnetic isotherms at 4.2 K is displayed in figure 2 as a function of pressure.
Relying on the shape of the XII vs. T curves (see below), we will assume these values to approximate
the Pauli susceptibility Xo II of the compound at
T
=0. The data can be represented quite accurately by an exponential law with a rate of variation of
rjj(X)i a ln XoII /aP = - 171 Mbar-1.
Applying the field in the basal plane results in much weaker effects. Indeed, it was noted previously
that the heavy-fermion character of CeRu2Si2 mani-
fests itself in the magnetic properties (large Pauli susceptibility X o, maximum in X (T),
«metamagnet- ism ») predominantly for Hllc, whereas weak, struc-
tureless variations are observed for H 1.. c [7]. How-
Fig. 1.
-Magnetization
curvesof single-crystal CeRU2S’2 at T
=4.2 K under pressure : (a) field applied along the tetragonal c-axis ; (b) field normal to the c-axis.
Fig. 2.
-Pressure dependence of the low-field suscepti- bility of CeRu2Si2 at 4.2 K (Hllc and H ..L c) and 49 K
(HI! c).
ever, the point here is that even the relative variation of X , is comparatively small (r Ix) = a In X ..L / aP
=-
70 Mbar-l). Consequently, the magnetic ani- sotropy X 11 /X -L decreases rapidly from 14 at P
=0
to 8 at 6 kbar (Fig. 3). The non-4f terms in
Fig. 3.
-Pressure decrease of the magnetic anisotropy (xll Ix, ) of CeRu2Si2 at 4.2 K.
x 0’ as estimated from measurements on LaRU2Si2 [12], would represent less than one percent of the total susceptibility, and no attempt was thus made to subtract them out.
The temperature dependence of the low-field susceptibility X II for various pressures is presented in figure 4. One sees that the decrease of Xo is corre- lated with an increase of the temperature Ta,, of the susceptibility maximum. This behaviour suggests to
cast the pressure-dependence of XII in terms of a
reduced temperature variable TS (P ) by writing the product X II T as :
Fig. 4.
-Temperature variation of the initial suscepti- bility of CeRU2S’2 parallel to the c-axis at various press-
ures :