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MAGNETORESISTANCE OF FeS1.14 SINGLE

CRYSTALS FOR B // c

E. Vitoratos, S. Sakkopoulos

To cite this version:

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JOURNAL DE PHYSIQUE

Colloque C8, Supplement au no 12, Tome 49, decembre 1988

MAGNETORESISTANCE OF

FeS1.14

SINGLE CRYSTALS FOR

B

//

c

E. Vitoratos and S. Sakkopoulos

Department of Physics, University of Patras, GR-261 10, Patras, Greece

Abstract. - Measurements of the transverse magnetoresistance on natural single crystals of pyrrhotite FeS1.14 revealed a phenomenon of the order The shape of the curves Ap/ p (0) vs. B for different temperatures is explained and the magnitude of the magnetoresistance can be adequately forseen by the s-d model.

T h e o r y a n d material

A quantitative theory of magnetoresistance in heavily-doped antiferromagnetic semiconductors has been developed by Nagaev et al. based on the s-d

model [I, 21. The basic idea is that indirect exchange via the conduction electrons tends to establish a ferro- magnetic ordering a fact that differenciates the mag- netization of regions of unequal electron concentration due t o impurities 131. These spatial fluctuations of magnetization cause a particularly strong scattering of the carriers.

This theory predicts that,

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for B << B,, where B, is the magnetic field which po- larizes completely the electron-spins. A is the s-d ex- change parameter, p is the Fermi energy of the carriers, nA the critical concentration of electrons at which the antiferromagnetic order becomes unstable, n the con- centration of carriers and M is the crystal magnetic moment per atom. We have that M = (B.S)

/

BF where B is the magnetic field, S the spin of the Fe atom and BF the saturation magnetic field, at which both sublattices of the antiferromagnet become paral- lel to each other. For B

>

B, the magnetoresistance

ceases to be a function of the field, reaching a satura- tion value given by the equation:

The two equations above predict a magnetoresis- tance which is negative for n

<

0.1 nA and positive for n

>

0.125 nA in all magnetic fields B

<

BF. For intermediate carrier densities 0.1 nA

<

n

<

0.125 n ~ ,

Ap

/

p ( 0 ) is negative for B

<<

B, becoming posi- tive as B approaches B,. After reaching saturation

for B N

B,,

the magnetoresistance becomes negative again for B

>

BF.

Experimental data on the rare earth compounds EuSe, EuS, EuTe [4, 51 and Gd2S3 [6] are in excellent agreement with this theory. It is not known though if this is also true for transition element semiconducting compounds, because magnetoresistance data are lack- ing. This prompted us to carry out magnetoresistance measurements on natural single crystals of pyrrhotite.

Natural pyrrhotite FeS1.14 is a heavily-doped [7, 81 ferrimagnetic semiconductor with a distorted NiAs structure, in which successive planes perpendicular to the c-axis are occupied exclusively by iron atoms with their magnetic moments antiferromagnetically aligned. The iron vacancies are ordered in every second plane forming a superstructure [9] and making the compound ferrimagnetic.

Spectroscopical data give the value A = 0.25 eV for the s-d exchange parameter in high-spin Fe, from which an A S = 0.5 eV is concluded. On the other hand, from Hall effect and thermopower measurements a Fermi energy /I = 0.14 eV was deduced for pyrrhotite

[lo,

111, which is less than half the s-d exchange energy. Measurements a n d results

The transverse magnetoresistance was measured by the four probe DC method for temperatures ranging from 88 to 607 K, beyond the N6el point TN 600 K of pyrrhotite and for magnetic fields from 0 to 7 000 G in 500 G intervals with B

//

c. Three typical curves at different temperatures are presented in figure 1. Discussion and conclusions

The critical carrier concentration n~ is given by the equation, nA = ( 4 k T ~ )

/

AS^^) where k is the Boltz-

mann constant and a the distance between nearest atoms in the lattice [3]. For pyrrhotite, where TN

-

600 K, S = 2, A = 0.25 eV and a = 3.1

x

lo-'

cm, the last equation gives nA = 3.0

x

lo2'

crnW3.

According to the theory, the magnetoresistance is negative for low magnetic fields, becoming positive for higher fields, only if the carrier concentration n lies in

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C8 - 194 JOURNAL DE PHYSIQUE

Fig. 1. - Transverse magnetoresistance for B

//

c, as a function of B at three temperatures. The experimental uncertainties are indicated. The first three experimental points for weak magnetic fields of the curves at T = 308 K and T = 376 K are fitted by equation (1) with n = 3.8 x

lo2' cm-3 and n = 4.0 x 10"

the range 0.1 n A

<

n

<

0.125 n A . For n A = 3.0 x

10'' ~ m - ~ this shape of the magnetoresistance curve must be observed only for 3.0

x

1021

<

n

<

3.8 x

10'' ~ m - ~ .

From Hall effect measurements on natural single crystals of pyrrhotite, a carrier concentration n =

3

-

8 x

loz1

~ m - ~ was determined [12, 131. Besides, the shape of the magnetoresistance curves at T = 308

and 376 K in figure 1 suggests that n must lie in the range 3.0 - 3.8 x 10'' ~ m - ~ , as it is predicted by the theory above. Taking into account the approximate character of n A and n calculation, we can say that the

shape of the magnetoresistance curves agrees well with the experimentally deduced carrier concentration.

The theory gives the exact shape of the magnetore- sistance curves either for B

<<

B, or B

>

B,. In the

intermediate region, in which the majority of our ex- perimental points lies, the shape of the curves is not analytically given. According to the theory [14], B, =

2 2 / 3 C 1 ~ ~

/

AS. For pyrrhotite, which is characterized

by a high magnetic anisotropy [15], BF = 100 kG, for

B

//

c and BF = 30 kG, for B l c and the last equation

gives B, = 50 kG and 17 kG for the two orientations respectively. In both cases the maximum B = 7 kG

used in the experiments, is too weak t o reach satura- tion.

Equation (1) fits very well the first experimental points of the curves a t T = 308 K and 376 K with n = 3.8 and n = 4.0 x 10'' cme3 respectively. More- over, the fact that the magnetoresistance takes higher values for higher temperatures a t B

<<

B,, can be ex-

plained as a result of an increase of n and BF with

temperature, according to equation (1).

The fact that the shape of the magnetoresistance curves is sensitive to the carrier concentration, can give a possible explanation of the oscillatory shape of the curve at T = 606 K. Because of the strong s-d exchange interaction, the change of magnetization induced by a magnetic field can affect appreciably the splitting of energy bands into sub-bands of

+

and - spins, leading to a corresponding change of n with B.

In conclusion we see that the theory outlined above can predict the magnitude of the magnetoresistance and in most cases the exact shape of the curves, for

FeS1.14.

[I] Kashin, V. A. and Nagaev, E. L., JETP Lett. 21

(1975) 56.

[2] Zil'bervarg, V. E. and Nagaev, E. L., Sov. Phys.

Solid State 18 (1976) 1460.

[3] Kashin, V. A. and Nagaev, E. L., Sou. Phys.

JETP 39 (1974) 1036.

[4] Shapira, Y., Foner, S., Oliveira, N. F., Jr. and Redd, T. B., Phys. Rev. B 10 (1974) 4765. [5] Shapira, Y., Kautz, R. L. and Reed, T. B., Phys.

Lett. 47A (1974) 39.

[6] Andrianov, D. G., Drozdov, S. A. and Lazareva,

G. V., Sow. Phys. Solid State 21 (1979) 1253. [7] Sakkopoulos, S., Vitoratos, 'E. and Argyreas, T.,

J. Appl. Phys. 55 (1984) 595.

[8] Gosselin, J. R., Townsend, M. G . and Tremblay, R. J., Solid State Commun. 19 (1976) 799. [9] Tokonami, M., Nishiguchi, K. and Morimoto, N.,

Am. Mineral. 57 (1972) 1066.

[lo] Sakkopoulos, S. and Theodossiou, A., 'J. Appl.

Phys. 45 (1974) 5379.

[ l l ] Tsatis, D. and Theodossiou, A., J. Phys. Colloq.

France 41 (1980) C5-371.

[12] Theodossiou, A., Phys. Rev. 137 (1965) A1321. [13] Pomoni, K. and Theodossiou, A., J. Appl. Phys.

53 (1982) 8835.

[14] Nagaev, E. L., Physics of Magnetic Semiconduc-

tors (Mir Publishers, Moscow) 1983, pp. 63, 234. [15] Sato, K., Yamada, M. and Hirone, T., J. Phys.

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