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VOLUME DEPENDENCE OF Sn2+-TRANSFERRED HYPERFINE FIELDS IN EUROPIUM
MONOCHALCOGENIDES
M. Abd Elmeguid, G. Kaindl
To cite this version:
M. Abd Elmeguid, G. Kaindl. VOLUME DEPENDENCE OF Sn2+-TRANSFERRED HYPERFINE
FIELDS IN EUROPIUM MONOCHALCOGENIDES. Journal de Physique Colloques, 1979, 40 (C2),
pp.C2-310-C2-312. �10.1051/jphyscol:19792109�. �jpa-00218478�
JOURNAL DE PHYSIQUE Colloque C2, suppl&ment au n o 3, Tome 40, mars 1979, page C2-3 10
VOLUME
D E P E N D E N C E O F sn2+-TRANSFERREDHYPERFI NE F1 ELDS IN
EUROPIUM
MONOCHALCOGENI DES
M. Abd Elmeguid and G. ~aindl*AbteiZmg flir Physik und Astronomic, Ruhr-UniversitBt Bochwn, 0-4630 Bochwn, Germany
* ~ n s t i t u t fiir Atom- und F e s t k o ~ e r p h y s i k , Freie U n i v e r s i t a t Berlin, 0-1000 Berlin, & m y
Rdsum6.- Les champs hyperfins transferds B sur des impuretds sn2+ dans les composGs magn6tique- ment ordonnds EuS et EuTe ont 6t6 mesurds ekhgonction de la pression jusque 6 4 kbar par spectrom6- trie Gssbauer de l l 9 ~ n . La valeur absolue de Bth croTt beaucoup plus vite dans EuS que dans EuTe quand le volume diminue. Les r6sultats sont discugbs sur la base d'un modsle dlBchange 5 deux pa- rametres.
Abstract.-The transferred hyperfine fields Bthf at sn2+ impurity atoms in magnetically ordered EuS and EuTe were measured as a function of pressure up to 64 kbar by '19sn ~gssbauer spectroscopy. In EuS the magnitude of B was observed to increase much fasterwith decreasing volume than in EuTe.
The results are discus%6 in terms of a two-parameter exchange model.
h e magnetic properties of the europium chal- cogenides EuCh (with Ch : 0, S, Se, and Te) have been studied extensively in the past /1,2/. Due to their simple NaC1-structure and the spin-only magne- tism of E U ~ + they are considered model substances of Heisenberg magnets. When described in a two-parame- ter exchange model both the ferromagnetic nn exchan- ge constant J1 and the antiferromagnetic superexchan- ge constant J 2 have been shown to vary in a systema- tic way over the chemical series.131 and as a func- tion of interatomic distance 14, 51 : when the lattice parameter is reduced by external pressure J1 increases strongly while J2 shows only a weak in- crease.
Recently, Bykovetz has studied transferred hyperfine fields at ll9sn impurity atoms at substi- tutional cation sites in EuS, EuSe, and EuTe well below the respective magnetic ordering temperatures /6/. The systematic variations of the nn transferred field B1 and particularly of the nnn supertransfer- red field B2 over the chemical series were found to differ quite drastically from those observed for Ji and J 2 in the pure Eu chalcogenides / 3 / . We report here on a high-pressure MEssbauer study 0 6 sn2+
transferred hyperfine fields in EuS and EuTe, aimed at a comparison with existing data on pure Eu chal- cogenides 151.
The experiments were performed with a high- pressure setup with BrC anvils allowing ~Essbauer transmission experimnts to be performed at liquid- helium temperature with low gamma ray energies. A similar setup has been described in the literature / 7 / . A superconducting lead manometer / 8 / was
employed for in-situ pressure measurements.
The substituted samples containing about 1 at% lL9sn (enriched to 92 2) were prepared by solid- state reaction between 1 1 9 ~ n ~ h (with Ch = S or Te) and the pure EuS and EuTe, respectively. The EU'+
contaminations of the samples were checked by 15'~u Mgssbauer spectroscopy and found to be less than 2%
in either case. A 2-mCi CaSn03 source was used for the l l '~n Mijssbnuer experiments.
Some typical spectra of Euo.ggSno.olS at 4.2 K and at various pressures are shown in figure 1. The increase of the magnetic hyperfine splitting with pressure is clearly visible. The relative line in- tensities observed are strongly influenced by a tex- ture of the absorber. Similar ll9sn spectra were recorded for Euo.qsSno.olTe at 4.2 K and 1.5 K.
The pressure dependences of the effective hy- perfine field Beff and of the isomer shift S were derived from spectra taken at 4.2 K (EuS) and at
1.5 K (EuTe), respectively. While Beff varies appre- ciably with pressure, the observed changes of S are small and will not be discussed here (EuS : dS/dP = +0.003(1) mm/s per kbar); EuTe : dS/dP = +0.001(1) m / s per kbar). The effective sn2+ hyperfine fields listed in table I were extrapolated to 0 K assuming proportionality between Beff and the host magneti- zation /g/ and using the known pressure coefficients of the magnetic ordering temperatures 15, 10, 1 l/.
In the present case Beff is made up of two contributions : Beff = Bthf + Bdip. The dipolar fields Bdip in Eu chalcogenides are of the order of 0.4 T and were taken from reference 1 6 1 . In the last column of table I the tranferred hyperfine fields
Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphyscol:19792109
Bthf are listed. In a two-parameter exchange model only nn B1 and nnn B2 contributions to Bthf are con- sidered. In EuS (ferromagnetic) these fields add up to Bthf = 12B1 + 6B2, while in EuTe (antiferromagne- tic, MnO-type) only the nnn shell, containing 6 E U ~ + ions, contributes : Bthf = -6B2. With Bthf being negative in EuS a positive sign has to be assumed for EuTe /6/.
The magnitudes of Bthf are plotted in figure 2 as a function of the lattice parameter. To this purpose values of the low-temperature compressibi- lities of EuS ( K = 0.9x10-~ kbar-l) and of EuTe
( K = 1 . ~ X I O - ~ kbar-l) were extracted from referen-
ces /10/ and /12/. The dotted line of figure 2 con- nects the antiferromagnetic B (equal to -6B2) of
thf
EuTe and EuSe and includes a linear extrapolation to EuS.
+ +
present results4
Fig. 1 : ' 1 9 ~ n MSssbauer spectra of Euo.ggSno.olS at 4.2 K and at various pressures. The solid lines are the results of least-squares fits of six Lorent- zian lines to the data.
Table I : Effective Sn2+ fields B ff in EuS and EuTe extrapolated to 0 K, and derfved values for the transferred hyperfine fields B
thf' P
(kbar) Be ff Bthf
(T) (T)
Eu0.99Sn0. O I S
0 -5.26(5) -5.7 8(8)
20(2) -6.34(6) -6.87(8)
41 ( 3 ) -6.90(6) -7.44(8)
64(4) -7.81(6) -8.36 (8)
Euo.ssSno.o~Te
0 4.21 (7) 3.88(9)
21 (2) 4.87(8) 4.54(10)
38(3) 5.30(9) 4.96(11)
54(4) 5.51(11) 5.16(1 )
-
-\
A Bykovetz 119761,
L +(lkborm 20 kbar
I
Fig. 2 : Magnitudes of Sn2+ transferred hyperfine fields Bchf (extrapolated to 0 K) as a function of the lattice constant. The ambient-pressure results of Bykovetz /6/ are also included. The dotted line represents a linear extrapolation of the antiferro- magnetic Bthf to EuS (marked by X).
0 I
-
U 6.0.-
&a
C 2,
v 5.0 E b
-
cE
4a-From its slope the volume dependence of Bthf, caused by chemical variation of the anions, is derived : (dBthf/dln~)ch = -3.6 T. From the slopes of the so- lid lines in figure 2 values for the volume depen- dences of the magnitudes of Bthf induced by pressu- re are obtained : (dBthf/dlnV) = -17(2)T for EuTe,
P
and (dBthf/dlnV) = -45(4)T for EuS. These pressure- P
induced changes of Bthf are by factors of 4.7 (EuTe) and 12.5 (EuS), respectively, larger than(dBthf/
dlnV)ch, supporting a view where the increase of
- \ 4
0 kbor- *...
'... -..0
kbor..
A....'... '".... 'y ....,\
0 kbar
-
EuS EuSe EuTe
I , , l , , ,
- -
the lattice parameter within the chalcogen series reflects mainly the different anion radii.
In pure Eu chalcogenides the nnn E U ~ + trans- ferred field
~t~
decreases from EuTe to EuSe with the chemically-induced decrease of the lattice pa- rameter /13/, while it increases slightly under external pressure 151. On the other hand, the Sn2+transferred field B? increases from EuTe to EuSe and increases quite drastically with external pres- sure (see Fig.2). Obviously, is more sensitive to changes of the lattice parameter than ':B and less to changes in covalency. The decrease of
5.8 6 0 62 6 L 6.6
Lottlce c w t o n t [A)
C2-312 JOURNAL DE PHYSIQUE
from EuTe to EuSe is then interpreted by covalency changes while the observed increase of "!B is domi- nated by "chemical" pressure. This different beha- viour of
BP
andBE^
is due to the different orbi- tals involved in the supertransfer mechanism via the ligand p orbitals : while for Eu the quite extended 5d orbitals are most important /3/ the transfer to the sn2+ sites should be dominated by the 5s elec- trons of sn2+. It should be mentioned here, that the 21.6 keV " ~ E U isomer shift exhibits an almost identical behaviour as B? as a function of pressu- re and chemically-induced changes of the latticeReferences
/l/ Methfessel, S. and Mattis, D.C., in "Handbuch der Physik" (Springer-Verlag, Berlin) 1968, Vol. 18/1.
/2/ Wachter, P., Crit. Rev. Solid State Sci.
3
(1972) 189.
/3/ Kasuya, T., IBM J. Res. Dev. (1970) 214.
/ 4 / Schwob, P., Phys. Kond. Mater.
10
(1969) 186./5/ Klein, U.F., Moser, J., Wortmann, G. and Kal- vius, G.M., Physica 86-88B (1977) 118.
/6/ Bykovetz, N., Solid State Conrmun.~(1976) 143.
/7/ Schilling, J.S., Klein, U.F. and Ho1zapfel.W.B.
Rev. Sci. Instrum.
45
(1974) 1353.parameter /13/. This may be due to the fact that the /8/ Eichler, A. and Wittig, J.,Z. Angew. Phys.
2
observed changes of
sEU
are mainly caused by a (1968) 319.compression of the Eu 5s2 shell /13/. /9/ Zinn, W., J. blagn. Mat.3 (1976) 23.
found EuTe
.
/10/ Shrivastava, V.C. and Stevenson, R., Can. J.
The volume dependence of Bthf at sn2+ was
Phys.
5
(1968) 2703.to be about 3 times larger in EuS than in
/l]/ Schwob, P. and Vogt, O.,Phys.Lett. (1967) This indicates quite appreciable nn contribu- 242.
tions B1 to Bthf in EuS, in contrast to the discus- /l21 Levy, F. and Wachter. P., Solid State Conunun-B sion in reference /6/. A more quantitative separa- (1970) 183.
tion of the B1 and B p contributions and their volu- /l31 Klein, U.F., Wortmann, G. and Kalvius, G.M., J. Magnet. Magn. Mat.
2
(1976) 50.me dependences must wait for Sn2+ field measurements in EuTe and EuSe in externally applied magnetic fields and with external pressure.
Acknowledgement.- The authors gratefully acknowledge valuable discussions with S. Methfessel, H. Micklitz.
and W. Zinn. This work was partly supported by the Sonderforschungsbereich 161 of the Deutsche For- schungsgemeinschaft.