ARTICLE IN PRESS

Journal of Magnetism and Magnetic Materials 320 (2008) 671–682

www.elsevier.com/locate/jmmm

Magnetic structure and phase diagram of the frustrated spinel

Cd1xZnxCr2Se4
E. Loudghiria, A. Belayachia,, M. Noguesb, M. Taibic, M.M. Cruzd, M. Godinhod
a
Laboratoire de Physique des Matériaux, Faculté des Sciences, Université Mohammed V, B.P. 1014 Rabat, Morocco
b
Laboratoire de Magnétisme et d’Optique de l’Université de Versailles (URA 1531), Batiment, Fermat, 45 Avenue des Etats Unis,
78035 Versailles Cedex, France
c
Laboratoire de Physico-Chimie des Matériaux associé à l’AUF (LAF 502), Ecole Normale, Supérieure Takadoum, B.P. 5118 Rabat, Morocco
d
Dept. Fisica/CFMC-UL, Fac. Ciências, Universidade de Lisboa, Campo Grande, Ed.C8, 1749-016 Lisboa, Portugal
Received 1 June 2007; received in revised form 5 August 2007
Available online 12 August 2007

Abstract

In attempt to characterise the magnetic ordering in the whole composition range of the Cd1xZnxCr2Se4 system, various magnetic
measurements were performed on both crystalline and polycrystalline samples with 0pxp1. The magnetic properties of the system are
typical of a ferromagnet below x ¼ 0.4 and of a complex antiferromagnet one above x ¼ 0.6. In this work the intermediate region was
carefully studied. The variations of both M(T) and wac at low fields suggest that transitions from ferromagnetic to Gabay–Toulouse
ferromagnetic-spin-glass mixed phase at low temperature occur in the range 0.41pxp0.58. The high-temperature susceptibility
measurements show that for the whole concentration range the system obeys Curie–Weiss laws. The results can be explained by the
coexistence of competing interactions (ferromagnetic between nearest neighbours and antiferromagnetic between higher order
neighbours) and disorder due to the random substitution between zinc and cadmium ions in the tetrahedral sites of the spinel lattice.
An experimental magnetic phase diagram of the system is established.
r 2007 Elsevier B.V. All rights reserved.

PACS: 75.30.Kz; 75.40.Cx; 75.40.Gb; 75.50.Lk

Keywords: Spinel selenide; Phase transistion; Long-range order; Re-entrant spin-glass

1. Introduction neighbours. The substitution and random distribution of

Magnetic materials having a random mixture of
ferromagnetic and antiferromagnetic interactions have
attracted a lot of attention. In the mixed spinel
Cd1xZnxCr2Se4, two important frustration effects are
present: the topological frustration in presence of anti-
ferromagnetic interactions and the competition between
n.n. ferromagnetic Cr–Se–Cr interactions J1 and high-
order-neighbours antiferromagnetic Cr–Se–(Zn,Cd)–Se–Cr
interactions J2. Zn and Cd are involved as an interme-
diate in superexchange interactions between higher-order
Corresponding author. Tel.: +212 67 07 36 36; fax: +212 37 77 89 73/
+212 37 67 11 19.
E-mail address: belayach@fsr.ac.ma (A. Belayachi).
Zn and Cd in tetrahedral sites result in disorder of
distribution of exchange interactions and therefore in
fluctuations of the J1/J2 ratio.
CdCr2Se4 is known to be a ferromagnetic semiconductor
[1,2] with Curie temperature TCE130 K and paramagnetic
Curie temperature ypE200 K. The chromium ion Cr3+
occupies the octahedral sites in the spinel B sublattice
and the Cd2+ occupies the tetrahedrally coordinate
A sublattice. The nearest neighbour exchange interaction
for the magnetic Cr3+ ions is via Se2 ion in the 901
superexchange position [3]. The magnetic moment per
Cr3+ and the Lande factor g, at 4.2 K, are respectively
2.9970.02 mB and 1.98370.003 [4]. ZnCr2Se4 has a
complex helical antiferromagnetic structure with a first-
order transition at T1 ¼ 21 K at which the helimagnetic

0304-8853/$ - see front matter r 2007 Elsevier B.V. All rights reserved.
doi:10.1016/j.jmmm.2007.08.005
 ARTICLE IN PRESS
672 E. Loudghiri et al. / Journal of Magnetism and Magnetic Materials 320 (2008) 671–682
macro-domains break into metamagnetic micro-domains.
The transition from metamagnetism to paramagnetism
occurs at T ¼ 45 K which is the true Néel temperature [5],
but since by magnetic susceptibility measurements only the
transition at 21 K is observed this temperature is currently
labelled as TN. The paramagnetic Curie temperature is
ypE100 K [6]. For their interesting electrical and optical
properties, CdCr2Se4 and ZnCr2Se4 have also been the
subject of many experimental and theoretical studies [7].
Some theoretical and numerous experimental studies
have been devoted to the system Cd1xZnxCr2Se4. The
magnetic susceptibility measurements show a linear varia-
tion of the Curie temperature yp with x [8]. Due to the large
number of interaction parameters, the difference between
the positive Cr–Se–Cr and the negative Cr–Se–Se–Cr
interactions in ZnCr2Se4 and CdCr2Se4 cannot be esti-
mated from experimental data without speculative assump-
tion about the relative strength of the fourth interaction [9].
The measurements of magnetic moment and magnetic
susceptibility performed by Busch et al. [10] show that the
magnetic properties of the system Cd1xZnxCr2Se4 are field
dependent which can explain the difference between the
results of Baltzer et al. [8] and Lotgering [9]. Using high-
frequency permeability on single crystals Makhotkin et al.
[11] concluded that the main change resulting from the
replacement of the Cd with the Zn ions occurs in the long-
range exchange interactions Cr–Se–A–Se–Cr (A ¼ Zn,
Cd). Neutron diffraction investigations on the system
Cd1xZnxCr2Se4 were carried out [12]. It is concluded that
with decreasing zinc concentration, the transition from
helimagnetic structure to ferromagnetic state proceeds via a
disordered magnetic phase. For xo0.4 there is a ferro-
magnetic order while for x40.6 the predominant state is
antiferromagnetic, but no clear explanation of the nature
of the state between 0.4oxo0.5 has been given. The
investigations of Myagkov et al. [13,14], using dynamic
magnetic susceptibility and remanent magnetisation, seem
to show the possibility of existence of a spin-glass order for
x0.4. A preliminary magnetic phase diagram has been
proposed [15] and no evidence of paramagnetic to spin-
glass transition appears in the region 0.4oxo0.6 but
rather a perturbed order occurs for 0.5oxo0.6. Using the
mean field theory and the spin wave theory, the exchange
integrals for x ¼ 0.35, 0.41 and 0.45 were calculated to the
third nearest neighbours [16,17]. A critical analysis has
been performed on the samples x ¼ 0.35, 0.45 and 0.55.
The results show that the critical exponents for xp0.45 are
similar to the values expected for 3D Heisenberg ferro-
magnets. For the first time, a re-entrant ferromagnetic-
spin-glass transition has been identified for x ¼ 0.55. The
magnetic properties indicate clearly a more disordered
magnetic structure with critical exponents different from
the classical case [18]. The exponents found for the re-
entrant Cd0.45Zn0.55Cr2Se4 sample are b ¼ 0.5 and d ¼ 2.8,
i.e. a slight increase of b and a net decrease of d with
respect to the Heisenberg ferromagnet values. The ferro-
magnetic critical region in the concentration range
0.35pxp0.58 was studied by the high-temperature series
expansions extrapolated with the Pade approximant
method [19]. Taking into account the exchange integrals,
the transfer integrals were calculated [20]. A phase diagram
of the system Cd1xZnxCr2Se4 has been computed by
considering the bond-diluted Ising model on the spinel B
lattice with competitive exchange interactions [21]. The
quenched randomness may cause fundamental changes in
low-temperature magnetic behaviour in this system [22].
Nevertheless, there is a lack of definite information about
the different transitions in the middle concentration range.
We have undertaken a detailed analysis of the phase
transitions in the system Cd1xZnxCr2Se4, and particularly
in the range 0.4pxp0.6. From our data, the magnetic
phase diagram, in which the characteristic temperatures are
plotted against Zn concentration x, can be established.
A comparison with the above-mentioned papers is also
given.
2. Samples preparation and composition analysis
Different methods were used to prepare the crystalline
samples, depending on Zn and Cd concentrations: vapour
liquid transport (VLT) [23], high-temperature solution
growth (HTSG) [24] and chemical vapour transport [25]. In
VLT, MSe (M ¼ Cd, Zn or a mixture) and CrCl3, in the
ratio 1:2, respectively, are separately cold-pressed to pellet
shape and placed at one of end of a sealed silica vial. The
vial is placed in the furnace at a temperature of 925 1C and
a temperature gradient is established such that the tip of
the tube is about 50 1C cooler than the region containing
reactants; the furnace is inclined 201 to horizontal to
promote collection of liquid in which crystals form at the
tip of vial. In HTSG, a mixture of CrCl3+2MSe (M ¼ Cd,
Zn) is slowly cooled from 950 to 700 1C in 2 weeks, the
crystals growing in the molten mixture. In the chemical
vapour transport (CVT or CVD) crystals of mixed
Zn–CdCr2Se4 powder have grown using Cl2 containing a
few HCl as transport agent in a temperature gradient
between 850 and 800 1C.
The crystal composition was determined by electron
microprobe analysis. Generally, the composition of crystals
is different of that starting mixture. VLT and HTSG give
crystals richer in Zn. Only chemical vapour transport
seems to give crystal composition near the starting one.
For the magnetic study, as the crystals do not span the
whole range of composition, samples in powder form
were prepared by the classical ceramic method. Powder of
Cr2Se3, ZnSe and CdSe, in the correct proportions,
were mixed, cold-pressed and treated at 800 1C in vacuum
quartz tube.
The purity and the composition of the samples (powder
and grinded crystals) were confirmed by X-ray measure-
ments. The lattice constants are reported in Table 1.
For both crystalline and powder samples, the lattice
constant of Cd1xZnxCr2Se4 system varies with the
composition in accordance with the Vegard’s law.
 ARTICLE IN PRESS
E. Loudghiri et al. / Journal of Magnetism and Magnetic Materials 320 (2008) 671–682 673

Table 1 constant C and the paramagnetic Curie temperature y.

Nature of the samples and the lattice constant of the system Fig. 1 presents the (1/w, T) plots for some Cd1xZnxCr2Se4
Cd1xZnxCr2Se4
samples. All the samples show a curved (1/w, T) plot, which
Sample x Nature Lattice constant is characteristic of the existence of short-range order as
previously reported by Lotgering [9]. By lowering the
CdCr2Se4 0 Crystal 10.73670.005 temperature, short-range order progressively installs. In the
Cd0.65Zn0.35Cr2Se4 0.35 Crystal 10.65470.005
case of inhomogeneous growth of the clusters, the magnetic
Cd0.59Zn0.41Cr2Se4 0.41 Powder 10.64170.005
Cd0.55Zn0.45Cr2Se4 0.45 Crystal 10.63270.005 order is established first in the larger clusters while it starts
Cd0.52Zn0.48Cr2Se4 0.48 Crystal 10.62570.005 to take form in the smaller clusters. This will correspond to
Cd0.45Zn0.55Cr2Se4 0.55 Powder 10.60870.005 a distribution of the transition temperatures [18] and the
Cd0.42Zn0.58Cr2Se4 0.58 Crystal 10.60070.005 transition from the paramagnetic state to an ordered state
Cd0.40Zn0.60Cr2Se4 0.60 Powder 10.59370.005
Cd0.35Zn0.65Cr2Se4 0.65 Powder 10.57970.005
(F or AF) is smoothed. This behaviour of the magnetic
Cd0.28Zn0.72Cr2Se4 0.72 Crystal 10.56270.005 susceptibility can be easily understood by determining the
ZnCr2Se4 1 Crystal 10.49570.001 Kouvel–Fisher exponent: geff ¼ (TTC)w(dw1/dT). Out-
side the critical regime, geff(T) shows a non-monotonic
behaviour which has been predicted for disordered
A structural determination [26] for the single crystal with ferromagnets by the correlated molecular field theory,
x ¼ 0.49 showed that cadmium and zinc are randomly Monte Carlo simulation and it has been confirmed
distributed in the tetrahedral sites. experimentally for a large number of systems [27]. The
detailed analysis performed on the samples in the
3. Experiments concentration range 0.45pxp0.6 seems to follow the same
behaviour [18].
The high-temperature magnetic susceptibility wdc was The Curie constants were converted to effective
pffiffiffiffi magnetic
measured by a DMS 4 magnetometer in the temperature moments meff using the relation meff ¼ 2:84 C (in CGS
range 300–600 K and applied field of 1 T. units). These moments along with the paramagnetic Curie
The magnetisation isotherms were carried out in the temperatures are listed in Table 2. The values of the
temperature range 4.2–300 K, either with an axial extraction effective moment obtained are in very good agreement with
technique up to 15 T (Service National des Champs Intenses meff ¼ 3.87 mB calculated for the Cr3+ spin only state. The
at Grenoble) or with a vibrating sample magnetometer up to positive values of y indicate that the interplanar exchange
1.8 T. The hysteresis loop measurements were performed, interaction is ferromagnetic. No linear variation of y is
with the vibrating sample magnetometer (VSM) or a detected for the concentration range 0.35pxp0.72 in
SQUID, in the same ranges of temperature and field. The disagreement with previous works [8,10] (Table 2).
low field dc magnetisation measurements were performed
with a VSM equipped with a coil-winding (0–30 mT) in
the temperature range 4.2–300 K. For dc measurements, the 300
samples were first cooled down in zero field up to 4.2 K, the
field was applied and the measurements taken with increasing 180

the temperature (ZFC. curves). Then the samples were cooled 250
160
θ (K)

down again at constant field and a new set of measurements

done with increasing the temperature (FC curves). For 140
((1- ). ) (mol.emu )
-1

thermoremanent measurements, the field cooling procedure 200

120
was used from room temperature down to the measurement
temperature where the sample is kept at constant tempera- 0.3 0.4 0.5 0.6 0.7
150 1-x
ture for a waiting time tw ¼ 250 s. Then the field was
-1
χ

switched off and the TRM(T, t) measured during 1800 s. x = 0.35

x

Below room temperature, alternative current magnetic x = 0.48

100
susceptibility wac was measured for frequencies between
x = 0.55
10 Hz and 10 kHz, in an ac magnetic field of 0.1 mT. At a
fixed frequency, the influence of a low external dc magnetic 50
x = 0.60
field (0–20 mT) was also studied.

4. Magnetic measurements data 0

0 100 200 300 400 500 600
4.1. High-temperature susceptibility T (K)

Fig. 1. Plot of w1 against temperature for the system Cd1xZnxCr2Se4.

The high-temperature susceptibility measurements were Inset: the variation of the paramagnetic temperature y as function of the
analysed by plotting 1/w against T to determine the Curie temperature.
 ARTICLE IN PRESS
674 E. Loudghiri et al. / Journal of Magnetism and Magnetic Materials 320 (2008) 671–682
Table 2
Magnetic moments and Curie temperature y for 0.35pxp0.65
x meff
0.35 3.9
0.45 3.9
0.55 4.0
0.60 4.0
0.65 4.0
4.2. High field magnetisation
Fig. 2 shows the field dependence of the magnetisation of
the system Cd1xZnxCr2Se4 for x ¼ 0.55. In order to
determine the chromium moment, for each temperature the
M vs. 1/H were extrapolated to 1/H ¼ 0 to obtain Mext;
these values were plotted against T and extrapolated to
T ¼ 0 to determine the saturated moment. Using the
same procedure for each sample, the same saturation
magnetisation was obtained corresponding to the same
experimental moment per Cr.at of 2.970.1 mB. This
saturation magnetic moment, close to 3 mB/Cr.at,
agrees with the one measured for x ¼ 0 and is consistent
with the value obtained from band calculation for this
compound.
Nevertheless, for all the samples above the Curie
temperature TC (high-temperature regime), the isotherms
M(H) present a slight curvature for H4HL, HL depending
on x, indicating that a pure paramagnetic regime is
not reached until 300 K in accordance with the high-
temperature susceptibility measurements. This pattern of
behaviour is also observed in many frustrated spinels [28],
indicating that the short-range order exists above the
ordering temperature. In this case, the transition
from paramagnetic state to the magnetic one takes place
through a large temperature range due to the occurrence
of clusters.
4.3. Hysteresis loop measurements
The hysteresis loops measurements have been used to
determine the coercive field Hc, the remanent magnetisation
Mr and the maximum slope (DM/DH)max of the loop at
H ¼ Hc as function of temperature. The loops were
obtained for each sample in temperature range 4.2–80 K,
after zero field cooling the sample from room temperature to
4.2 K. The variations with temperature of the coercive field
Hc, the remanent magnetisation Mr and the maximum slope
(DM/DH)max are shown in Fig. 3a–c.
In the ferromagnetic region (xo0.4), the data are
characteristic of a pure ferromagnetic regime [15]. For
Cd0.52Zn0.48Cr2Se4, at low temperature an important
increase of Hc occurs. It is well-known that in classical
ferromagnets high coercive fields are sign of domain wall
blocking; this may be true here also, but with blocking
mechanisms related to local frustration effects. The plot of
6
y
185
175
150
4
125
115
M (μ )
B
x = 0.55
T = 2.3 K T = 48 K
2
T = 7.5 K T = 58 K
T = 13 K T = 66 K
T = 24 K T = 80 K
T = 35 K T = 100 K
0
0 5 10 15
H (T)
Fig. 2. High field magnetisation isotherms for x ¼ 0.55.
ln(Hc) vs. 1/T (Fig. 4a) shows an exponential variation of
the coercive field with a slope change at T ¼ 15 K
indicating two magnetic regimes before the sample behaves
paramagnetically at high temperature. This exponential
behaviour can be explained by the properties of a complex
structure of domains and domain walls, associated with the
relaxation of the transverse spin component St. At low
temperature, the relaxation is slow. The cost in energy to
move the walls is important and the barrier energy minima
therefore is high. On the contrary, for T415 K, the energy
barrier is lower, the relaxation is fast and the equilibrium
state is quickly reached, the behaviour being similar to a
classical ferromagnet [29]. The remanent magnetisation
has also an exponential behaviour (Fig. 4b), where
two different regimes are identified as function of the
temperature. This type of variation has been observed
for the thermoremanent magnetisation (TRM) of
certain spin-glasses and small particles systems where a
thermally activated process governs the properties [30].
The maximum slope (DM/DH)max of the hysteresis loop is
constant for 15 KpTp40 K and falls down at 42 K. Below
15 K a drop of (DM/DH)max is observed as in re-entrant
systems.
Cd0.45Zn0.55Cr2Se4 behave as x ¼ 0.48 sample but with
some differences. As for Cd0.52Zn0.48Cr2Se4, in the
temperature range 4.2–20 K, Hc has values expected for
polydomain ferromagnet and follows an exponential law
indicating that the domain wall motion is governed by
thermally activated phenomena. Above 35 K, Hc keeps
non-zero value with a broad maximum near 50 K and
vanishes at 55 K; this behaviour is not consistent with a
classical ferromagnet and arises at a temperature higher
 ARTICLE IN PRESS
E. Loudghiri et al. / Journal of Magnetism and Magnetic Materials 320 (2008) 671–682 675

c 5
4
102(Δ M/ΔH)max

2
3

Ln (Hc )
0
b
1.5 1
x = 0.48
Mr(emu.g-1)

x = 0.55 x = 0.48
1.0 x = 0.58 0 x = 0.65
x = 0.60
x = 0.65

0.5 -1

0.0 -2
0.0E+0 7.5E-2 1.5E-1 2.3E-1 3.0E-1
60
a 1/T

2
Hc(mT)

40

20
0

0 x = 0.48
0 10 20 30 40 50 60 x = 0.65
-2
Ln(Mr )

Fig. 3. Evolution of Hc, Mr and (DM/DH)max with temperature for

0.48pxp0.65.

than that expected for such a transition. This behaviour -4

will be discussed later. The variation of Mr(T) can also be
fitted by exponential law in the temperature range
4.2–20 K. Mr(T) keeps constant value until 40 K, then
decreases and vanishes as Hc. The curve of (DM/DH)max
presents a broad maximum near 25 K, and falls down at
low temperature. The decrease of (DM/DH)max is indicative
of decrease of order, but for this composition the decrease
is higher than in the case of x ¼ 0.48.
For Cd0.42Zn0.58Cr2Se4, in the experimental limits,
hysteresis loop could not be observed above around 20 K.
The results show a low value of Hc around T ¼ 15 K; then
Hc increases sharply with lowering temperature. From
15 K, the onset of strong irreversible behaviour in the
magnetisation process is observed. Both Hc(T) and Mr(T)
variations obey an exponential law. (DM/DH)max presents
a maximum at T27 K, and decreases regularly with
decreasing temperature.
For the two samples Cd0.40Zn0.60Cr2Se4 and
Cd0.35Zn0.65Cr2Se4, the hysteresis loop characteristic
values are lower than for the samples with smaller Zn
content. Also exponential law variations were found
(Fig. 4a and b) and different behaviour of (DM/DH)max
can be identified.
-6
0.0E+0 1.0E-1 2.0E-1 3.0E-1
1/T
Fig. 4. Logarithm of Hc vs. T1 for x ¼ 0.48 and 0.65.
4.4. Low field magnetisation
The characteristic behaviour of the ZFC and FC
magnetisation curves for Ha ¼ 30 mT has been previously
published [15]. For 0pxp0.4, the magnetisation curves
behave as a typical ferromagnet, M keeping constant
values at ToTC. For the critical concentration range
0.48pxp0.6 and Ha ¼ 5 mT, the typical behaviour is
presented in Fig. 5. The ZFC–FC curves exhibit field-
dependent irreversibilities in the whole temperature range
where hysteresis loops are observed.
In the range 0.41pxp0.5, the samples behave also
ferromagnetically but present at low temperature
 ARTICLE IN PRESS
676 E. Loudghiri et al. / Journal of Magnetism and Magnetic Materials 320 (2008) 671–682
0.3 x = 0.48, ZFC
x = 0.48, FC
x = 0.58, ZFC
x = 0.58, FC
x = 0.60, ZFC
x = 0.60, FC
0.2
M (emu.g-1)
Ha= 0.5 mT
0.1
0.0
0 30 60 90
T (K)
Fig. 5. Variation of the low field magnetisation with temperature for
x ¼ 0.48, 0.58 and 0.60.
(TE15 K) a decrease of the ZFC magnetisation and large
irreversibility phenomena. The FC–ZFC branching point is
strongly field-dependent and decreases with increasing
applied field.
The plots for 0.5oxo0.6 do not show a plateau but
rather a broad maximum around T ¼ Tm, the values being
dependent on both composition and applied field. The
M(T) curves do not show the distinct features of sharp
kinkpoint plot for ferromagnetic materials. This seems to
indicate a spin-glass like behaviour (with a broad distribu-
tion of freezing temperature) rather than an antiferro-
magnet at Tm. The branching point is also composition-
dependent. It seems that for x40.55, the irreversibilities
are no more observed at temperatures higher than Tm. The
Curie temperature TC, where the system shows paramag-
netic to ferromagnetic has been determined by the
maximum of the absolute value of the first-order derivative
of the magnetisation with respect to temperature and this is
at the inflexion point of M vs. T data. For x40.55, it is
very difficult to extract the transition temperature from the
magnetisation curves since the behaviour is rather of
antiferromagnet type.
For x ¼ 0.6, the behaviour seems rather be due to an
almost antiferromagnetic sample, but the Tm value (20 K)
is still too high to be identified as a TN transition (TN for
ZnCr2Se4 is 21 K) and small irreversibilities cannot be
excluded around Tm. For x ¼ 0.65, the lower Tm value
(17 K) can be identified as a TN, the irreversibilities
detected below 10 K indicate a re-entrant antiferromag-
netic transition.
Finally for 0.65oxp1, the magnetisation curves
have the characteristic shape of the ones for ZnCr2Se4
antiferromagnet with slightly lower TN temperatures. For
the measuring field of 5 mT, the ZFC–FC irreversibility is
of the same size order of the experimental accuracy and
cannot be attributed to a re-entrant behaviour below TN.
4.5. wac susceptibility measurements
The alternative current susceptibility wac measurements
are the most useful tool to show the dynamical properties
of the disordered systems. Some typical examples obtained
for Cd1xZnxCr2Se4 system are presented in Fig. 6.
4.5.1. 0.4op0.5 range
As a function of temperature, the samples behave as
typical re-entrant ferromagnetic systems showing two
magnetic transitions (two peaks in the w0ac and w00ac data),
for example, x ¼ 0.48 in Fig. 6a: one at TC associated with
the paramagnetic to ferromagnetic transition, and the
other at lower temperature Tfg associated with the
ferromagnetic to spin-glass transition. The w0ac maxima
shift towards lower temperatures with decreasing frequency
(Fig. 7). These shifts, similar to the ones of the w00ac maxima,
are of the order of DTfg/Tfg ¼ 2% per decade of frequency,
which is typical of a spin-glass like material (Fig. 8).
The frequency dependence of Tfg can be fitted with an
Arrhenius law f ¼ f0 exp(Ea/kT) or a Vogel–Fucher law
f ¼ f0 exp(Ea/k(TT0)). The fitted parameters of the
Arrhenius law, f0 ¼ 4.3  1018 Hz and Ea/k ¼ 461 K, have
no physical meaning. For the Vogel–Flucher law, the
fitted values are f0 ¼ 4.6  106 Hz, the activation energy
Ea/k ¼ 28.4 K and T0 ¼ 9.370.1 K. In magnetically inter-
acting small particles, the variation of the blocking
temperature TB can be represented in first approximation
by a Vogel–Fulcher law, and T0 is small compared to TB,
whereas for spin-glass systems, T0 is close to Tg. In our
case, the relative size of the shift and the closeness of T0
and Tfg characterises rather a spin-glass like transition.
Various criteria of the frequency dependence of Tfg
have been suggested to distinguish between a true
thermodynamic transition (true spin-glass) or a dynamic
non-equilibrium process (progressive freezing of cluster
moments) [31]. The obtained parameters: DTfg/TfgD log f
¼ 0.07, (TfgT0)/Tfg ¼ 0.3 and Ea/kTfg ¼ 2.2(Tfg ¼
12.8 K at 995 Hz), indicate an intermediate behaviour
between a cluster regime and a true spin-glass regime; the
observed re-entrant transition to spin-glass state being
explained as a freezing of finite clusters which destroys the
ferromagnetic order.
Fig. 9 shows the results of the ac susceptibility obtained
at a constant frequency, by applying various dc external
fields (0, 1.5, 5 and 20 mT). With increasing field Ha, the
maximum at high temperature of w0ac and w00ac is progres-
sively suppressed while the peak at low temperature is not
strongly affected.
4.5.2. 0.5oxo0.6 range
In this concentration range, a transition from short-
range order to a typical ferromagnetic order is no more
 ARTICLE IN PRESS
E. Loudghiri et al. / Journal of Magnetism and Magnetic Materials 320 (2008) 671–682 677

6E-2 Cd0.52Zn0.48Cr2Se4
f = 995 Hz
x = 0.48
0.04 x = 0.55
x = 0.60

(emu.g-1.Oe-1)
4E-2
χ'ac (emu.g .Oe )
-1 -1

ac
0.02 2E-2

'
χ
f = 10 Hz
f = 95 Hz
f = 995 Hz
f = 9995 Hz
0E+0
0 20 40 60 80
0.00 T (K)
0 20 40 60 80
T (K) 3E-2
f = 10 Hz
0.10 f = 95 Hz
f = 995 Hz
f = 995 Hz f = 9995 Hz
x = 0.48 2E-2
(emu.g-1.Oe-1)

0.08 x = 0.55
x = 0.60
10 χ"ac (emu.g-1.Oe-1)

0.06
1E-2
ac
"
χ

0.04

0E+0
0.02 Cd0.52Zn0.48Cr2Se4

0 20 40 60 80
T (K)
0.00
0 20 40 60 80 Fig. 7. Temperature and frequency dependencies of wac susceptibility
T(K) (Hac ¼ 1 Oe; f ¼ 10, 95, 995 and 9995 Hz) for x ¼ 0.48: (a) w0ac and (b) w00ac .

Fig. 6. Temperature dependence of wac for x ¼ 0.48, 0.55 and 0.60

(F ¼ 995 Hz, Hac ¼ 1 Oe): (a) w0ac and (b) w00ac .
observed. The w0ac presents only a broad peak centred
around 25 K, while w00ac presents several peaks at very low
temperature. We note the presence of a small shoulder in
w0ac behaviour and a peak in w00ac at Tclu72 K (Fig. 6b) for
x ¼ 0.55 and 65 K for x ¼ 0.58. This shoulder and the
peak occur at a temperature well above an expected Curie
temperature and cannot be taken as a transition to an
ordered state. This can explain the existence of hysteresis
loop until 55 K.
At low temperature, w00ac presents two peaks: the first near
Tfg1 ¼ 7 K and the second for Tfg2 ¼ 16 K for x ¼ 0.55
(8 and 16 K for x ¼ 0.58). At these temperatures, a rapid
decrease of w0ac is observed, probably due to the disap-
pearance of long-range ferromagnetic order. The main
reason will probably be the onset of AFM interactions and
frustration at TC. The presence of double-peaked structure
in the temperature dependence of the w00ac , and the change in
peak position with a biasing field in the vicinity of
the re-entrant spin-glass transition can be considered to
be reminiscent of two re-entrant phase boundaries,
Almeida–Touless and Gabay–Toulouse, predicted by the
isotropic vector spin model [32–34].
In this concentration range, the susceptibility data point
to the existence of a spin-glass like state at low
temperature. The trend with x composition reveals that
the introduction of zinc ions, reinforcing the relative
 ARTICLE IN PRESS
678 E. Loudghiri et al. / Journal of Magnetism and Magnetic Materials 320 (2008) 671–682

20 and the transition temperature of 16 K indicates spin-glass

x = 0.48 character for the installing phase. As expected, a decrease
of the ordering temperature with applied dc field is detected
x = 0.58 since it favours the more ordered phase.

4.5.3. 0.6pxo0.7 range

16
The same kind of analysis has been performed for this
concentration range. The real part of ac susceptibility shows
only a broad maximum at Tm ¼ 20 K for x ¼ 0.6 (Fig. 6a)
Tg (K)

and 18 K for x ¼ 0.65, while w00ac presents several peaks. At

high temperature, we note the presence of a small shoulder in
w00ac which is strongly frequency and composition dependent,
12
reminiscent of ferromagnetic interaction associated with
the presence of ferromagnetic clusters. For x ¼ 0.6:
55pTclup65 K, and for x ¼ 0.65: 45pTclup55 K. The
variation of Tclu with composition can be related to the
relative concentration of Cd ions inside the cluster, greater
8 for small x values leading to a predominance of ferromag-
10 100 1000 10000 netic interactions inside the cluster. With decreasing tem-
f (Hz) perature, w00ac presents a small sharp peak at low temperature.
The peak is located at the inflection point of the w0ac drop,
Fig. 8. Frequency dependence of freezing temperature Tfg ¼ f(ln(f)).
which can be identified as TN. This w00ac small sharp peak is
associated with a spin-glass like behaviour. The weak
frequency dependence along with the fact that a magnetic
6E-2 dc field does not affect significantly the susceptibility values is
Zn Cd Cr Se χ' 0 T
0.48 0.52 2 4
χ' 1.5 mT
consistent with the onset of antiferromagnetic order.
95 Hz
χ' 20 mT
χ" 0 T 4.6. Thermoremanent magnetisation
χ" 1.5 mT
4E-2 χ" 20 mT
The time dependence of dc magnetisation is important to
χ ac (emu.g-1.Oe-1)

reveal the spin dynamics in spin-glass and re-entrant-spin-

2E-2
0E+0
0 20 40
T (K)
Fig. 9. Temperature dependence of wac susceptibility with external bias
field Hdc for x ¼ 0.48.
strength of the higher order neighbours antiferromagnetic
interactions with respect to the n.n. ferromagnetic one,
destabilises the ferromagnetic order, which remains
strongly perturbed. The resulting moments block with
decreasing temperature. The reduction of the strength of
the ferromagnetic interactions when Zn ions are introduced
is clearly reflected by the decrease of the magnitude of w0ac .
Applying a Vogel–Fulcher law to the frequency depen-
dence for the x ¼ 0.58 compound, the values Ea/k ¼ 27.9 K
and T0 ¼ 11.5 K are obtained. The closeness between T0
glass systems. TRM(T, t) have been performed on the
samples for 0.35pxp0.65 with an applied field of 50 mT in
the temperature range 6–60 K. Two approaches have been
used to fit the experimental data.
We first fitted the data with logarithmic function:
TRM ¼ M 01  S 1 lnðtÞ, (1)
where S1 is the magnetic viscosity and t the measuring time.
The second approach is based on the phenomenological
logarithmic decay function:
60 80
lnðTRMÞ ¼ lnðM 02 Þ  S 2 lnðtÞ. (2)
The fitted data to Eqs. (1) and (2) are presented in
Fig. 10. For x ¼ 0.55 and 0.58, with increasing tempera-
ture, M01 and S1 first decrease, then show a slight increase
before to gradually decrease to almost zero value at
T460 K. In the second approach, Eq. (2), the behaviour is
different since S2 increases with temperature as in small
particles and spin-glass regimes, then reaches a maximum
before to decrease rapidly. This unusual behaviour has
been previously reported for local canted state ferrites [35].
In this concentration range, the ferromagnetic regime is
highly perturbed and a cluster regime occurs below 45 K as
can be seen from the variation of the coercive field and ac
susceptibility. The viscosity behaviour can be interpreted
from the relaxation of the transverse spin component St.
 ARTICLE IN PRESS
E. Loudghiri et al. / Journal of Magnetism and Magnetic Materials 320 (2008) 671–682 679

0.20 fitted both by Eqs. (1) and (2). In the first case, M01 and S1
decrease with increasing the temperature, while in the
M0 x = 0.55 second case S passes through a maximum near 7 K.
1

0.15 M0 x = 0.55 5. Data analysis and discussion

2

5M0 x = 0.60
1
On the basis of our data many magnetic phases can be
M0 (emu.g-1)

5M0 x = 0.60 identified depending on the concentration and temperature

2

0.10 ranges: a pure paramagnetic regime, short-range order

based on cluster regime, pure or perturbed ferromagnetic
states, pure or perturbed helical antiferromagnetic states
and re-entrant or spin-glass like state.
0.05 To establish the magnetic phase diagram Ti vs. x, the
samples can be divided in several domains following the
concentration of Zn: a ferromagnetic concentration range
for xp0.4, re-entrant properties for 0.4oxp0.5, mixed
0.00 phases for 0.5oxp0.6 and an antiferromagnetic concen-
0 15 30 45 60
tration range for x40.6.
T(K)

5.1. Ferromagnetic concentration range

3.0
2.0
S1 x = 0.60 The TC values decrease monotonically with increasing
2.5 1.5 S2 x = 0.60 Zn concentration up to 0.4. In this region, the monotonic
decrease of TC is attributed to the increase of the
S

1.0
antiferromagnetic super-exchange integral Cr–Se–(Zn,Cd)
2.0 0.5 –Se–Cr. The ferromagnetic exchange integral Cr–Se–Cr
may be affected by a slight variation of the distance dCr–Cr
0.0
S (a.u)

1.5 4 8 12 16 between neighbouring chromium. This distance varies

T (K) linearly with lattice parameter (the composition x). Since
no anomaly was observed in the low field magnetisation
1.0 S1 x = 0.55 curves at temperatures lower than TC, there is no evidence
S2 x = 0.55 of transition to a re-entrant state.
0.5
5.2. Re-entrant properties: 0.4oxp0.5

0.0 As in the ferromagnetic concentration range, the

0 10 20 30
T(K)
Fig. 10. TRM(T, t) of Cd0.45Zn0.55Cr2Se4 and Cd0.4Zn0.6Cr2Se4 as
function of temperature.
At low temperature, the characteristics of the hysteresis
loop follow exponential variations vs. temperature. This
indicates that the properties are governed by a thermally
activated process, therefore S increases with temperature.
However, the St relaxation decreases when T increases and
then S decreases because the relaxation takes place between
two states which become almost similar when the St
relaxation is fast. This behaviour indicates that different
time responses can be assigned in the temperature range
6–60 K with regard to the magnetic state. The existence
of two temperature regions has been reported for
ZnCr1.6Ga0.4O4 [29] where exponential decay has been
fitted above and below the freezing temperature.
For x ¼ 0.6 and 0.65, no TRM has been detected above
15 K for x ¼ 0.6 and 10 K for x ¼ 0.65. The data have been
40 50 60
magnetisation reaches saturation for fields close to 1 T.
The moment per chromium ion is found to be 2.970.1 mB.
Below the Curie temperature TC, the coercive field Hc
has values consistent with a polydomain ferromagnet. At
low temperature, an increase of Hc occurs as observed
in many frustrated systems, which can be explained by
the Dzyaloshinsky–Moriya interaction which causes
anisotropy, pinning the domain walls. In this region, the
temperature dependence of Hc follows an exponential
law indicating that the domain wall displacement depends
on a thermally activated process. By lowering the
temperature, the w0ac presents a sharp pick at the ordering
temperature TC and develop a plateau of long-range
ferromagnetic ordering, presents a second pick at Tfg and
falls down at low temperature. For w00ac we note the presence
of two peaks: a broad one at higher temperatures,
consistent with the onset of ferromagnetic behaviour,
and another one, relatively sharp, at low temperatures,
associated with the onset of a spin-glass phase. Two models
are used to explain the re-entrant properties. The first is an
homogeneous model based on the mean field theory
 ARTICLE IN PRESS
680 E. Loudghiri et al. / Journal of Magnetism and Magnetic Materials 320 (2008) 671–682
[32–34] in which by cooling the system from high
temperature the successive phases are: paramagnetic,
homogeneous ferromagnetic, homogeneous randomly
canted ferromagnetic state resulting from the freezing of
the transverse component, and finally a spin-glass state
characterised by strong irreversibility. The second is an
inhomogeneous model based on a percolation approach
with the coexistence of a ferromagnetic state and magne-
tically isolated clusters in the sample [36]. The re-entrant
spin-glass phase is located in region that coexist with
ferromagnetic ones.
5.3. Mixed phases domain 0.5oxp0.60
In this concentration range, a spin clusters regime is
assumed below about 60 K with clusters that can be
sufficiently small to include only a few domains. Hc is much
higher than the values observed for polydomain samples.
The maximum observed in the Hc(T) at high temperature
can be explained as follows. In the high-temperature
Curie–Weiss regime, an interaction between spin exists
but the spins relax independently. When the temperature
decreases, short-range order can occur progressively
between the spins leading to the formation of small spin
clusters. Inside the cluster, the spins can be strongly
correlated. It is clear that the topological frustration
governed by the ratio J1/J2 is the main reason for the
cluster formation. The cluster sizes and their evolution
depend on both the substitution concentration and
temperature. From theoretical point of view, the existence
of spin cluster inside the matrix is expected [37,38]. This is
correlated with the appearance of small monodomain
clusters separated from the matrix. Further decreasing the
temperature, the spin clusters grow, further increasing
the coercive field because of high energy barriers governing
the Bloch wall moving. This trend continues to evolve until
most clusters begin to coalesce while a decrease in the
coercive field is observed. A large maximum is observed in
the low field dc magnetisation and irreversibilities are
present up to the ordering temperature. These irreversi-
bilities are strongly field dependent, Tirr increasing with
decreasing Ha. The irreversibilities in the curves for a given
Ha can be directly related to the limit field of existence of
the hysteresis loop for a given temperature [39]. In this
concentration range, the ferromagnetic order, if any, is
more and more perturbed as x increases. The order is
neither a pure ferromagnetic order nor an helical one; we
observe that the critical exponents begin to deviate from
the classical values [18]. Specific heat measurements
performed on a powder sample with composition
x ¼ 0.55 showed the absence of peak or anomalies in the
temperature range 3–25 K. On the other hand, an
antiferromagnetic order was found by Sadykhov et al.
[12] for x40.5 (TN ¼ 16 K, x ¼ 0.5). In this concentration
range the ac susceptibility strongly increases around a
temperature which we call TC. However, w0ac susceptibility
does not reach the inverse of the demagnetising factor as
expected for a ferromagnet. We note the presence of two
peaks in w00ac considered to be reminiscent of two re-entrant
phase boundaries. According to the Heisenberg mean-field
model predictions, in this concentration range by lowering
the temperature, one should observe a first transition at a
temperature TGT (the Gabay–Tou1ouse transition) each
spin should begin to increase their static transverse-
moment components without change of the ferromagnetic
order parameter. At a yet lower temperature TAT (the de
Almeida–Thouless transition), a crossover from weakly
irreversible to strongly irreversible behaviour should
occurs. The sharp onset of irreversible behaviour that we
observe at Tfg1 indicates the crossover. The two aspects of
spin-glass ordering (frozen-in random spin orientations
and strong irreversibility) which occur together at Tg in a
standard spin-glass appear in this model at distinct
temperatures. We must to point out that in this concentra-
tion range the magnetic properties are very sensitive to
slight changes in the composition and hence it appears
difficult to do a direct comparison between samples
(originating from different authors) for which the accuracy
in the initial composition is different. We can confirm that
until x ¼ 0.55 the ferromagnetic interactions are still
predominant [18] and the freezing observed at low
temperatures, where the antiferromagnetic interactions
also becomes effective, should be non-classical in type,
involving regions (where the ferromagnetic interactions
dominate) which are weakly correlated between them
because of the frustration. In this composition region, we
prefer to define as ‘‘mixed phase’’ the magnetic state as
some residual perturbed ferromagnetism may persist within
the magnetic regions. The existence of true spin-glass state
in the system Cd1xZnxCr2Se4, previously reported by
Myagkov et al. [13,14], cannot be taken into account.
In our measurements any sample shows only one cusp
and more the observed frequency dependence is not
characteristic of a true spin-glass transition in the whole
concentration range. However, the results of the frequency
dependence of the ac susceptibility are rather indicative
of freezing cluster process. From all observed properties
for 0.5oxo0.6, the corresponding state may be considered
as intermediate between a classical order and a true
spin glass.
5.4. Antiferromagnetic concentration range
For 0.6oxo0.7, there is no well established order
because of the strong frustration. The samples behave
as a perturbed or re-entrant antiferromagnetic system. The
presence of a small shoulder in w0ac behaviour and a peak in
w00ac at high temperature is indicative of short-range order
above the Néel temperature TN. At low temperature,
To10 K, the properties seem to be characteristic of
re-entrant antiferromagnetic system or freezing cluster
regime.
When xX0.7, with increasing the applied magnetic field,
all samples behave as a helimagnet with a Cr moment of
 ARTICLE IN PRESS
E. Loudghiri et al. / Journal of Magnetism and Magnetic Materials 320 (2008) 671–682 681

2.9 mB/at.Cr, as in ZnCr2Se4. The structure is antiferro- Table 3

magnetic at low temperature, with a slight increase of TN Different transition temperatures for Cd1xZnxCr2Se4 system
with zinc concentration until TN ¼ 21.5 K for x ¼ 1. These x Tfg (K) (1/2) TC (K) TN (K) Tclu (K)
results are in agreement with others studies [8–15].
0 128
0.35 70
5.5. The magnetic phase diagram
0.41 62
0.45 55
The magnetic phase diagram of Cd1xZnxCr2Se4 0.48 13 52
deduced from our data analysis is presented in Fig. 11. 0.55 16/7 42 70
The re-entrant transition has been characterised by ac 0.58 16/8 35 65
0.60 14/9 25 60
susceptibility, scaling analysis and thermomagnetic mea-
0.65 10 16 50
surements. The Curie temperature for the ferromagnetic 0.72 17
region and the re-entrant region has been determined using 0.80 18
the scaling analysis (Table 3). This phase diagram shows 1 21
that for small substitution 0pxp0.4 the predominant state
is ferromagnetic. For 0.41pxp0.5, the system show
re-entrant properties but the ferromagnetic order is less between the n.n. ferromagnetic and n.n.n. antiferromag-
predominant. With increasing zinc concentration, the netic interactions induce mixed state below a certain
system becomes more perturbed. With lowering the temperature Tfg in which the longitudinal spin component
temperature the system evolves towards a cluster phase remains ferromagnetically and the transverse component St
regime. When 0.61pxo0.7, the structure is a perturbed presents a spin-glass state. Above Tfg and below the
helimagnetic one with re-entrant antiferromagnetic transi- paramagnetic transition the order is ferromagnetic. The
tion at low temperature. Finally for xX0.7, the system magnetic properties seem to demonstrate that some
becomes helimagnetic according to previous works. In magnetic perturbation subsist in this temperature range.
contrast to earlier phase diagrams [12–14,16] the different When x40.5, the properties are modified leading to more
magnetic phases have been determined accurately. The disordered states characterised by strong irreversibilities as
phase diagram determined by Afif et al. [21,22] using Ising for a spin-glass like state but no paramagnetic-spin-glass
model cannot describe correctly the system as it is a 3D transition has been observed. Finally, we conclude that for
Heisenberg system. the system Cd1xZnxCr2Se4 the spin-glass like properties
are typical of system with spin cluster rather than a true
6. Conclusions spin-glass. ZnCr2Se4 has a complex helical antiferromag-
netic state with TN ¼ 21 K, therefore not strong enough
Starting from a ferromagnetic state, re-entrant proper- interaction is supplied in comparison with the ferromag-
ties are observed for 0.41pxp0.50. The competition netic interaction with TC ¼ 130 K in CdCr2Se4. The
competition between the positive exchange integral J1
and the n.n. negative exchange integral J2 in
TC long range FM Cd1xZnxCr2Se4 is not sufficient to lead to a true spin-
120
TN long range AFM glass state.
Tfg2 GT-line
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