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HAL Id: jpa-00210719

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Submitted on 1 Jan 1988

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Low temperature properties of Yb1.2-xEuxMo6S 8 under pressure

J. Beille, B. Cheaito, M.S. Torikachvili, M.B. Maple

To cite this version:

J. Beille, B. Cheaito, M.S. Torikachvili, M.B. Maple. Low temperature properties of Yb1.2-xEuxMo6S 8 under pressure. Journal de Physique, 1988, 49 (3), pp.481-484. �10.1051/jphys:01988004903048100�.

�jpa-00210719�

(2)

Low temperature properties of Yb1.2-xEuxMo6S8 under pressure

J. Beille

(1),

B. Cheaito

(1),

M. S. Torikachvili

(2, *)

and M. B. Maple

(2)

(1) Laboratoire Louis Néel, CNRS, 38042 Grenoble Cedex, France

(2) Institute for Pure and Applied Physical Sciences, University of California, San Diego, La Jolla, CA 92093, U.S.A.

(Reçu le 22 juillet 1987, accept6 le 17 novembre 1987)

Résumé. 2014 Les propriétés des composés pseudoternaires Yb1.2-xEuxMo6S8 ont été étudiées à l’aide des

mesures de résistivité électrique et de susceptibility magnétique ac sous pression hydrostatique jusqu’à 20 kbar

et quasi hydrostatique jusqu’à 100 kbar. Un diagramme de phase de température-pression-concentration d’Eu

montrant les phases cristallographiques, normales et superconductrices de ces composés a été construit.

Abstract. 2014 The properties of Yb1.2-xEuxMo6S8 compounds have been investigated by means of electrical resistivity and ac magnetic susceptibility measurements under hydrostatic pressure up to 20 kbar and quasi- hydrostatic pressure up to 100 kbar. A temperature-pressure-Eu concentration phase diagram showing the crystallographic, normal and superconducting phases of these compounds was constructed.

Classification

Physics Abstracts

72.15 - 74.10 - 74.70

1. Introduction.

Most ternary rare-earth R

molybdenum

chal- cogenides with nominal

composition R.,M06X8 (where x

= 1.0-1.2 ; X = S,

Se)

are

superconducting

and their

superconducting

transition temperatures

Tc’s

show a systematic variation with R

[1]

that can

be accounted for in terms of the theory of Abrikosov and Gor’kov

(AG) [2].

Exceptions to this systematics

include

Cel.2MO6X8

and

Eul.2MO6X8 (X

= S and

Se)

which do not exhibit

superconductivity,

and also

Ybl.2MO6S8,

which has a

Tc

much higher than expected

[1].

Recent

crystal

structure refinement

studies on single

crystals

of

RxM06S8 (R

= Ce, Eu, Ho, and

Yb)

indicate an upper limit for the R concentration x = 1.0,

[3, 4]

which suggests that the sintered specimens with x > 1.0 utilized in the early

work as well as on this one contained

impurity

phases. Baillif et al.

[5]

found that a structural

phase

transition at - 109 K prevents

superconductivity

from occurring in

EuM06S8

at ambient pressure.

This structural transformation can be

suppressed by

hydrostatic pressure

[6],

and pressure-induced super-

conductivity in

EuM06S8

occurs at a

T, [7-9]

which is

(*) Present address : Department of Physics, San Diego

State University, San Diego, CA 92182, U.S.A.

also much higher than what one would expect from the AG theory, as is the case for

Ybl.2MO6S8

at zero

pressure. While most R ions in the ternary

R.,M06X8

compounds are trivalent, Eu

[10]

and Yb

[4, 11-12]

are in nearly divalent states, and it is

possible

that

the high Tc values of - 7.3 K for

Ybl.2Mo6S8 (sintered chunk)

and - 14 K for

Eul.2MO6S8 (extrapolated

value to zero pressure on a melted

sample) [8]

are

associated with the large unit cell volume due to the divalent character of the Yb and Eu ions, as suggested by Sergent et al.

[9],

and it is therefore not

surprising that these two compounds do not follow

Abrikosov-Gor’kov’s

systematics

for trivalent R in

RM06S8 compounds.

It has been

suggested

that the

crystallographic

transformation in

EuM06S8

at -109 K may be

accompanied by the formation of a

charge density

wave

(CDW)

which removes a

portion

of the Fermi

surface

[13].

High pressure

experiments

on sintered

Snl.2-,,EU,,MO6S8

samples

[13]

revealed a pressure

dependence of Tc that

suggested

that the

portion

of

the Fermi surface removed by the CDW decreases

with pressure, resulting in an increase in the

density

of states at the Fermi level and a

corresponding

increase in Tc. However, measurements of electrical

resistivity

vs. temperature under hydrostatic pressure

on a

high quality

melted sample of

EuM06S8

indi-

Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphys:01988004903048100

(3)

482

cated that

superconductivity

sets in

abruptly

with Tc - 12 K as soon as the pressure is

sufficiently high

to suppress the

crystallographic

transformation com-

pletely

(Per --

13.2

kbar ) [6].

This suggests that a CDW which may occur in the triclinic phase does not

coexist with

superconductivity.

A recent

study

of Yb 1.2 -

xEuxMo6Sg pseudotemary

compounds revealed that the upper critical magnetic

field Hc2 of

Ybl.2Mo6S8

is

substantially

enhanced by partial substitution of Eu for Yb

[14].

As in

Snl,2 - XEuxMo6S8 [15], Pbl - xEUxMo6S8 [15],

and

Lal,2 -xEuxMo6S8 [16],

the enhancement of

Hc2

in

Ybl.2 - xEUxMo6S8 [14]

was attributed to the com-

pensation of the

applied

magnetic field

by

a

negative exchange

field due to an

antiferromagnetic exchange

interaction between the conduction electron

spins

and the Eu 2+

magnetic

moments, via a mechanism

first suggested

by

Jaccarino and Peter

(JP) [17].

The

data and a theoretical calculation of

Hc2(T)

suggest that

Ybl.2-xEuxMo6Sg compounds

with x - 0.5 are good candidates for

magnetic

field induced supercon-

ductivity,

provided

high

quality homogeneous

sam- ples could be

prepared [14].

Reported herein are the results of an investigation

that we carried out on Yb-Eu

pseudoternary

molyb-

denum sulfide

compounds

with nominal

composition Yb1.2 - xEuxM06Sg

by means of measurements of electrical

resistivity

p and ac magnetic

susceptibility

Xac under hydrostatic pressure up to 20 kbar and

quasi-hydrostatic

pressure up to 100 kbar. Prelimi- nary results were discussed in reference

[18].

2. Experimental details.

The

Ybl.2 - xEUxM06S8

compounds were prepared by sintering according to the description in reference

[14].

Low

frequency

ac electrical

resistivity

and ac

magnetic susceptibility

measurements under

hydros-

tatic pressure were carried out at the

University

of California,

San Diego (UCSD)

and Louis Neel

Laboratory (LNL)

in

self-clamped

Be-Cu pressure cells utilizing a 1:1

isoamyl

alcohol: n-pentane

mixture as a pressure

transmitting

medium. A

Bridgman

anvil cell

capable

of

achieving quasi-hyd-

rostatic pressures up to - 140 kbar

[19]

was used at

LNL for the

resistivity

measurements under

quasi- hydrostatic

pressure. Since the electrical resistance of samples extracted from the sintered

pellets

was

strongly

sample

dependent,

no attempt was made to

determine absolute values of

resistivity.

3. Results and discussion.

Curves of electrical

resistivity

versus temperature for the five

Ybl,2 - xEuxMo6S8

compounds with x = 0, 0.4, 0.6, 0.8 and 1.2 at

atmospheric

pressure are

displayed

in figure 1. The behaviour of p

(T)

evolves

from metallic-like in

Ybl.2MO6S8

to a behaviour in which the

resistivity

shows a broad minimum as Eu is

Fig. 1. - Electrical resistivity vs. temperature for Ybl.2 _ xEuxMo6S8 compounds with x = 0, 0.4, 0.6, 0.8 and 1.2 at atmospheric pressure. The solid lines are guides to

the eye.

substituted for Yb,

presumably

due to the onset of

the triclinic distortion. The

resistivity

of the Eu-rich

Ybl.2 -

,Eu.,Mo6S8

compounds at low temperatures is

about two orders of magnitude higher that at room temperature.

Defining

the temperature at which the triclinic distortion occurs as the temperature Ts at

which the derivative

dp /dT

first exhibits a discon- tinuity upon

cooling,

a phase

diagram

can be con- structed, in which the

boundary

between the rhombohedral and the triclinic

phases

can be

display-

ed as a function of Eu concentration, as shown in figure 2a. The

dependence

of Tc on x determined

from the

midpoint

of the transitions in X ac and p is

also

displayed

in

figure

2a. The detailed behaviour of

Tc (x)

is shown in figure 2b, where the vertical

bars represent the temperature interval between 10 % and 90 % of the transition from the normal to the

superconducting

state.

Fig. 2. - (a) Crystallographic and superconducting tran-

sition temperatures T,, and Tc, respectively, versus x for Ybl.2-.,EU.,Mo6S8 compounds. The values of T, were

inferred from discontinuities in ap /aT upon cooling and

the values of Tc were determined from the midpoints of

transitions in p (A) and X ac (N) ; (b) superconducting

transition temperature Tc vs. Eu concentration x for sintered pellets of Yb1.2 - xEuxMo6Sg compounds.

(4)

The behaviour of p

(T )

for

YbO.2Eul.OM06S8

under

various

hydrostatic

pressures between 0 and 20 kbar

can be seen in figure 3. The effect of pressure is to

depress

T, very

rapidly

and to suppress the upturn of the resistivity at low temperatures. At 7 kbar

p

(T) displays

a broad minimum ant - 67 K followed

by

sharp drop

at - 5 K due to the onset of supercon-

ductivity, as confirmed

by

X ac measurements. The pressure

dependence

of Tc determined from resistivi- ty measurements is

displayed

in the inset of

figure

3.

Superconductivity is

quickly

established in a narrow

pressure range and Tc achieves a maximum near

10 kbar. At higher pressures,

T,

decreases almost

linearly

with pressure at a rate of -0.13K/kbar,

which is close to the rate found for

EuM06S8-

Curves p

(T)

for

Ybo,6Euo.6Mo6Sg

under various

quasi-hydrostatic

pressures between 4.4 kbar and 103.5 kbar are

displayed

in figure 4. At 4.4 kbar,

which is the lowest pressure at which electrical contact between the sample and the leads could be

Fig. 3. - Electrical resistivity vs. temperature for Ybo.2Eu1.0Mo6SS at hydrostatic pressures between 0 and 20 kbar. The pressure dependence of T, extracted from

resistivity measurements ( ) is displayed in the inset.

Fig. 4. - Curves of electrical resistivity vs. temperature for Ybo,6Euo.6Mo6Sg at quasi-hydrostatic pressures between 4.4 kbar and 103.5 kbar.

established, the

resistivity

exhibits a broad minimum

at - 115 K, followed by an increase in p as the temperature is lowered and a

drop

at - 8 K that is associated with the onset of

superconductivity.

How-

ever, the

superconducting

transition was not com-

plete

down to 1.7 K, the lower temperature limit of the apparatus. As the

quasi-hydrostatic

pressure was further increased, the minimum in p

(T)

was progres-

sively suppressed.

Although

a

drop

in p ant - 8 K suggests the onset of

superconductivity

at 9.7 kbar,

the

superconducting

transition was not complete

down to 1.7 K either. The

incompleteness

of the

superconducting

transitions is

probably

associated

with pressure

inhomogeneities.

No

superconductivity

was observed above 20 kbar. A temperature-hydros-

tatic pressure

phase diagram

for

Ybo.6Euo.6Mo6Sg

was constructed and is

displayed

in

figure

5a, and

the pressure

dependence

of Tc is displayed in figure 5b.

Fig. 5. - (a) Hydrostatic pressure dependence of T, and Tc for Ybo,6Euo.6Mo6Sg, showing the distinction between the rhombohedral and the triclinic phases ; (b) pressure dependence of T,,. Data points denoted by triangles (A) are from electrical resistivity measurements, and by squares (0) from ac magnetic susceptibility

measurements.

4. Conclusions.

The Yb-Eu pseudoternary

molybdenum

sulfide com- pounds with nominal

composition Ybl,2-xEuxM06S8

exhibit remarkable

crystallographic

and supercon- ductive properties that are very sensitive to pressure.

The compound

Ybl.2Mo6Sg

is

superconducting

at

zero pressure with 7c - 7.3 K. Upon partial substitu-

tion of Eu for Yb, Tc decreases with Eu concen-

tration until superconductivity is

completely

sup-

pressed at x -- 0.7. The effect of pressure on Yb-rich

Ybl _ xEuxMo6Sg compounds

is to depress

Tc

at a rate

similar to

Ybl.2MO6S8.

At intermediate compositions Tc is first enhanced

by

pressure, reaches a maximum and then starts to decrease. The Eu-rich compounds,

which are not

superconducting

at ambient pressure, become

superconducting

in a narrow pressure range, above which Tc is

depressed by

pressure. The

temperature TS at which the rhombohedral-triclinic

crystallographic

distortion that prevents supercon-

(5)

484

Fig. 6. - Three dimensional phase diagram of Ybl.2-,,EU.,MO6S8 compounds displaying the pressure and concentration dependences of T, and T,. Data points

denoted by triangles (A) are from electrical resistivity

measurements, and by squares (0) from ac magnetic susceptibility measurements.

ductivity from occurring at ambient pressure takes

place

in

EUM06S8,

and which determines the onset

of the non-metallic behaviour, is suppressed by

pressure and by

substituting

Yb for Eu. A three- dimensional phase diagram of the

Ybl,2-xEuxM06Sg pseudoternary compounds

in which Ts and

Tc

are displayed as a function of pressure and concentration is shown in

figure

6.

In light of the recent

availability

of

single

crystals

of

EuM06S8

and

YbM06S8 [3-4],

an attempt to grow

Yb1 - xEuxM06Sg single

crystals and a study of the

effect of pressure on these compounds at low temperatures as well a search for

magnetic

field

induced

superconductivity

at intermediate compo- sitions is in order.

Acknowledgments.

Research at UCSD was supported

by

the US Depart-

ment of Energy under Grant No. DE-FG03- 86ER45230. Research at Louis Neel Laboratory was supported by the DRET under Grant No. 84/109.

The authors would like to thank Chris Seaman for

preparing the figures.

References

[1] MAPLE, M. B., DELONG, L. E., FERTIG, W. A., JOHNSTON, D. C., MCCALLUM, R. W. and SHEL-

TON, R. N., in Valence Instabilities and Related Narrow-Band Phenomena, Ed. R. D. Parks (Plenum, New York) 1977, p. 17.

[2] ABRIKOSOV, A. A. and GOR’KOV, L. P., Sov. Phys.

JETP 12 (1961) 1243.

[3] PENA, O., HORYN, R., POTEL, M., PADIOU, J. and SERGENT, M., J. Less-Common Met. 105 (1985) 105 ;

PEÑA, O., HORYN, R., GEANTET, C., GOUGEON, P., PADIOU, J. and SERGENT, M., J. Solid State Chem. 63 (1986) 62 ; and

PEÑA, O., GEANTET, C., HORYN, R., POTEL, M., PADIOU, J. and SERGENT, M., Mater. Res. Bull.

22 (1987) 106.

[4] PEÑA, O., GOUGEON, P., SERGENT, M. and HORYN, J., J. Less-Common Met. 99 (1984) 225.

[5] BAILLIF, R., DUNAND, A., MULLER, J. and YVON, K., Phys. Rev. Lett. 47 (1981) 672.

[6] DECROUX, M., TORIKACHVILI, M. S., MAPLE, M. B., BAILLIF, R., FISCHER, ~. and MULLER, J., Phys. Rev. B 28 (1983) 6270.

[7] CHU, C. W., HUANG, S. Z., LIN, C. H., MENG, R. L., WU, M. K. and SCHMIDT, P. H., Phys.

Rev. Lett. 46 (1981) 276.

[8] HARRISON, D. W., LIM, K. C., THOMPSON, J. D., HUANG, C. Y., HAMBOURGER, P. D. and LUO,

H. L., Phys. Rev. Lett. 46 (1981) 280.

[9] SERGENT, M., CHEVREL, R., ROSSEL, C. and FISCHER, ~., J. Less-Common Met. 58 (1978)

179.

[10] PELIZZONE, M., TREYVAUD, A., SPITZLI, P. and FISCHER, ~., J. Low Temp. Phys. 29 (1977) 453.

[11] BONVILLE, P., CHEVREL, R., HODGES, J. A., IM-

BERT, P., JEHANNO, G. and SERGENT, M., in the Proceedings o f the Conference o f the Appli-

cations of the Mösbauer Effect, Jaipur (India),

Dec. 14-18, 1981.

[12] JORGENSEN, J. D., HINKS, D. G., NOAKES, D. R., VICCARO, P. J. and SHENOY, G. K., Phys. Rev.

B 27 (1983) 1465.

[13] LACOE, R. C., WOLF, S. A., CHAIKIN, P. M., HUANG, C. Y. and LUO, H. L., Phys. Rev. Lett.

48 (1982) 1212.

[14] TORIKACHVILI, M. S., BEILLE, J., LAMBERT, S. E.

and MAPLE, M. B., J. Low Temp. Phys. 65 (1986) 389.

[15] FISCHER, ~., DECROUX, M., ROTH, S., CHEVREL, R. and SERGENT, M., J. Phys. C 8 (1975) L474.

[16] TORIKACHVILI, M. S. and MAPLE, M. B., Solid State Commun. 40 (1981) 1.

[17] JACCARINO, V. and PETER, M., Phys. Rev. Lett. 9

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