Journal of Alloys and Compounds 649 (2015) 142e150

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Journal of Alloys and Compounds

journal homepage: http://www.elsevier.com/locate/jalcom

Magnetic properties of Ge1
x
yPbxMnyTe cluster-glass system

A. Podgo
rni a, L. Kilanski a, *, K. Szałowski b, M. Go

rska a, R. Szymczak a, A. Reszka a,
V. Domukhovski , B.J. Kowalski , B. Brodowska , W. Dobrowolski a, V.E. Slynko c,
a a a

E.I. Slynko c
a
Institute of Physics, Polish Academy of Sciences, al. Lotnikow 32/46, 02-668 Warsaw, Poland
b
d
z, ul. Pomorska 149/153, 90-236 Ło
Department of Solid State Physics, Faculty of Physics and Applied Informatics, University of Ło
d
z, Poland
c
Institute of Materials Science Problems, Ukrainian Academy of Sciences, 5 Wilde Street, 274001 Chernovtsy, Ukraine

a r t i c l e i n f o a b s t r a c t

Article history: We present studies of magnetic properties of Ge1
x
yPbxMnyTe bulk crystals with chemical composition
Received 14 May 2015 varying in the range of 0.180 < x< 0.311 and 0.019 < y < 0.136. Two transitions, one at temperatures
Accepted 25 June 2015 below 20 K and the other between 44 and 105 K, are observed. The transitions are associated with the
Available online 3 July 2015
presence of two magnetic subsystems having different chemical compositions e the host lattice and
clusters. The transition at higher temperatures is identified as a transition from a paramagnetic state to a
Keywords:
spin-glass-like state. The observed magnetic order is interpreted in terms of the carrier mediated
Semimagnetic-semiconductors
ferromagnetism, assuming an exchange interaction among magnetic ions in both subsystems. The
Ferromagnetic-materials
Cluster-defects
experimental results are analyzed theoretically with good accuracy within the spin-wave-theory-based
model of a disordered two-phase ferromagnet with the long-range RudermaneKitteleKasuyaeYosida
interaction. The magnetic exchange constant, Jpd, having values from 0.47 eV to 0.80 eV gives spin-glass
transition temperature, TSG, values close to the experimental values for the Ge-rich phase. The magnetic
order observed for the Pb-rich phase is also due to the carrier mediated magnetic interaction. The
experimental transition temperatures are fitted with Jpd value ranging from 0.22 eV to 0.28 eV.
© 2015 Elsevier B.V. All rights reserved.

1. Introduction
Transition metal (TM) doped IVeVI diluted magnetic semi-
conductors (DMS) such as Ge1
xTMxTe alloys attracted recently a
significant interest due to their potential applicability in spintronics
[1]. IVeVI DMS offer unique advantages over IIIeV materials due to
several unique properties. The solubility of magnetic impurities in
IVeVI bulk DMS is two orders of magnitude higher than in bulk
IIIeV DMS. Moreover, the Mn ions in IVeVI DMS are isoelectronic
dopants (two s-electrons like in Pb and Ge) and the solubility of Mn
in IVeVI compounds is much higher than, e.g. of Fe. In addition, Pb-
based IVeVI materials have the highest mobilities in this group of
semiconductors. In view of the above characteristics the optimi-
zation of the magnetic and transport properties of IVeVI DMS is
very important for the development of semiconductor spintronics.
The Pb-based IVeVI semiconductors with their not-distorted
* Corresponding author.

rni), kilan@ifpan.edu.pl
E-mail addresses: podgorni@ifpan.edu.pl (A. Podgo
(L. Kilanski).
rocksalt structure are also interesting from the point of view of
the basic research, since some of them turned out to be topological
insulators [2].
First experimental studies of magnetism of bulk Ge1
xMnxTe
were done over 40 year ago by Rodot [3]. Ferromagnetic order with
the Curie temperature, TC z 167 K, in Ge1
xMnxTe with 50 at. % of
Mn was observed by Cochrane et al. [4] Long range carrier mediated
ferromagnetism due to RudermaneKitteleKasuyaeYosida [5]
(RKKY) interactions is present in IVeVI DMS such as Ge1
xMnxTe
since these materials: (i) naturally grow with high concentration of
conducting holes due to the presence of cation vacancies [6] and (ii)
have relatively high Mn-ion e conducting hole exchange constant,
Jpd, ranging from 0.8 to 0.9 eV for bulk Ge1
xMnxTe crystals [4,7],
and 0.7 eV for thin Ge1
xMnxTe layers [8]. Recently, significant
attention was put into the studies of thin Ge1
xMnxTe layers. The
nonequilibrium methods of thin layer growth, such as molecular
beam epitaxy (MBE), allowed introduction of a large variation of
Mn-content into the high-quality GeTe layers [9e12]. In the
Ge1
xMnxTe system with x ¼ 0.46 Lechner et al. [13] observed TC as
high as 200 K. Recently, complex compounds based on quaternary
IVeVI alloys have been shown to offer more degrees of freedom

http://dx.doi.org/10.1016/j.jallcom.2015.06.208
0925-8388/© 2015 Elsevier B.V. All rights reserved.

rni et al. / Journal of Alloys and Compounds 649 (2015) 142e150
A. Podgo 143

with respect to the control of the magnetic and electrical properties
of the alloy [14,15]. Development of complex IVeVI based DMS
gives possibilities to gain further understanding of the physical
mechanisms responsible for their magnetic properties. Thus,
further studies devoted to this topic are necessary.
The present paper undertakes the problem of understanding the
nontrivial magnetic properties of Ge1
x
yPbxMnyTe bulk DMS with
chemical composition varying in the range of 0.180 < x < 0.311 and
0.019 < y < 0.136. Two magnetic transitions are observed in all our
samples: one at temperatures below 20 K and the other between 44
and 105 K. Dynamic and static magnetic measurements reveal that
the spin-glass-like state is observed in this system below 105 K.
Two similar Ge1
xPbxTe based phases with significantly different
chemical compositions, x, are found to be responsible for the
magnetic states in these crystals. The main purpose of this paper is
to investigate the influence of the Ge:Pb ratio on the magnetic
exchange constant, Jpd, of the two magnetic phases present in the
Ge1
x
yPbxMnyTe alloy. The experimental results are analyzed
theoretically with good accuracy within the spin-wave-theory-
based model of a disordered ferromagnet with the long-range
RKKY interaction as well as the Sherrington-Southern model.
2. Basic characterization
The Ge1
x
yPbxMnyTe bulk crystals were grown by the modified
Bridgman method. The applied modifications are similar to those
used by Aust and Chalmers in order to improve quality of alumina
crystals [16]. The main change of the growth technique consisted of
installation of additional heating elements to create radial tem-
perature gradient along crystallization surface. Such modification
changed the angle between the crystallization front and the growth
direction by about 15  . The applied modifications reduced the
number of crystal blocks in the as-grown crystals from a few down
to a single one.
The chemical composition of our crystals was determined by the
energy dispersive x-ray fluorescence technique (EDXRF). We used
the Tracor Spectrace 5000 EDXRF spectrometer. The maximum
relative error of the EDXRF technique does not exceed 10% of the
calculated value of x or y. The as-grown ingots were cut into thin
slices (about 1 mm thick) perpendicular to the growth direction,
mechanically polished, chemically cleaned, and etched prior to
further characterization. Each slice was characterized with the
EDXRF method. The obtained results indicate that the chemical
composition of the slices changes continuously along the growth
direction. From all our samples we selected the ones with the
chemical composition showing the smallest changes in each indi-
vidual slice and covering the widest range of x and y values. The
chemical content of the samples selected for the present studies are
gathered in Table 1.
The structural characterization of Ge1
x
yPbxMnyTe consisted of
the standard powder x-ray diffraction (XRD) measurements done
at room temperature using Siemens D5000 diffractometer. The
analysis of the diffraction patterns was done with the use of the
Rietveld refinement method [17]. The XRD results show that all our
crystals consist of two similar NaCl-like structure phases. The main
phase has the rock-salt crystal structure showing distortion to the
rhombohedral structure with the values of the lattice parameter, a1,
and the angle of distortion, a, similar to those of the bulk GeTe
crystals, i.e., 5.98 Å and 88.3 , respectively [18]. The second phase
crystallizes in the cubic rock-salt structure with the value of the
lattice parameter, a2, close to the value reported for bulk PbTe
crystals [19], i.e. a2 z 6.46 Å, and shows no signature of a rhom-
bohedral distortion. The XRD results clearly show that our samples
consist of Ge-rich host lattice and Pb-rich clusters.
The chemical segregation of our Ge1
x
yPbxMnyTe crystals was
studied with the use of a scanning electron microscopy (SEM)
coupled with energy dispersive x-ray spectrometer system (EDX).
The field emission Hitachi SU-70 Analytical UHR FE-SEM scanning
electron microscope and Thermo Scientific NSS 312 energy
dispersive x-ray spectrometer system equipped with silicon drift
detector were used. Prior to the SEM-EDX measurements the
sample surface was mechanically polished and chemically cleaned
in order to reduce the surface roughness and remove impurities.
The simultaneous use of the SEM and EDX techniques allowed us to
obtain images of the samples and localized elemental information.
The SEM-EDX results, in agreement with the XRD data, indicate the
presence of two different phases inside all of our crystals. The
exemplary SEM-EDX results for the Ge0.794Pb0.196Mn0.055Te crystal
in the form of the SEM image and the EDX spectra measured for the
selected, two kinds of typical areas on the sample are shown in
Fig. 1. The chemical compositions of the two phases (shown on the
inset to Fig. 1 and gathered in Table 1) indicate a large difference in
the amount of substitutional elements between the host lattice and
the clusters. For each sample the chemical composition was
measured for a series of spots on the crystal, selected for both the
GeTe-based crystal matrix, and for PbTe-rich cluster areas. Clusters
may have different thicknesses or the cluster at the surface may
have been cut in such a manner that it has a varying thickness.
Therefore the SEM imaging does not provide reliable information
about the thickness of each cluster. The EDX electron beam probes
the volume of the sample beneath the surface with the penetration
depth of about 500 nm. It is then probable that the chemical
composition can be affected in several spots by the influence of
both phases. In order to reduce the above problems, the most
divergent data are skipped. The averaged Pb and Mn molar frac-
tions (x and y, respectively) obtained by EDXRF and the molar
fractions of matrix (xmtx and ymtx) and cluster areas (xclr and yclr)
obtained by EDX are gathered in Table 1. In many cases the Pb
content in the clusters, xclr, is almost an order of magnitude higher
than xmtx. Manganese ions are present both in the host lattice and
the cluster regions.
The elementary magnetotransport studies including the

Table 1
Results of a basic characterization of Ge1
x
yPbxMnyTe crystals (obtained at room temperature) including (i) the average chemical composition, x and y, obtained using the
EDXRF spectrometer, (ii) the average chemical composition of the matrix e xmtx and ymtx, and clusters e xclr, yclr, and (iii) the electrical resistivity rxx, carrier concentration n, and
mobility m.

x ± Dx y ± Dy xmtx ± Dxmtx ymtx ± Dymtx xclr ± Dxclr yclr ± Dyclr n ± Dn (1020 cm
3) m ± Dm (cm2/(V s))
0.232 ± 0.02 0.019 ± 0.002 0.038 ± 0.004 0.020 ± 0.002 0.731 ± 0.07 0.006 ± 0.001 8.8 ± 0.9 15.4 ± 2.0
0.196 ± 0.02 0.055 ± 0.005 0.054 ± 0.010 0.094 ± 0.020 0.531 ± 0.10 0.055 ± 0.006 6.2 ± 0.6 14.1 ± 1.0
0.196 ± 0.02 0.061 ± 0.006 0.041 ± 0.004 0.187 ± 0.020 0.693 ± 0.07 0.070 ± 0.007 5.6 ± 0.6 11.7 ± 1.0
0.254 ± 0.03 0.074 ± 0.007 0.045 ± 0.005 0.076 ± 0.008 0.612 ± 0.06 0.059 ± 0.006 6.0 ± 0.6 8.2 ± 0.8
0.183 ± 0.02 0.074 ± 0.007 0.055 ± 0.020 0.063 ± 0.005 0.503 ± 0.20 0.042 ± 0.012 6.6 ± 0.7 12.8 ± 1.0
0.180 ± 0.02 0.074 ± 0.007 0.055 ± 0.010 0.091 ± 0.030 0.677 ± 0.05 0.050 ± 0.007 4.6 ± 0.5 2.0 ± 0.2
0.311 ± 0.03 0.081 ± 0.008 0.111 ± 0.040 0.126 ± 0.004 0.408 ± 0.20 0.088 ± 0.030 8.1 ± 0.8 3.5 ± 0.4
0.294 ± 0.03 0.136 ± 0.010 0.097 ± 0.070 0.170 ± 0.020 0.614 ± 0.10 0.113 ± 0.030 9.9 ± 1.0 1.6 ± 0.2
144
rni et al. / Journal of Alloys and Compounds 649 (2015) 142e150
A. Podgo
Fig. 1. The SEM secondary-electron image of the Ge0.794Pb0.196Mn0.055Te crystal and EDX spectra measured at selected spots (marked with circles). The characteristic x-ray emission
lines related to transitions to La, Ma, and Ka shells of Ge, Pb, Mn and Te elements are marked with labels.
resistivity and the Hall effect measurements for our samples were
performed at selected temperatures between 4.3 K and 300 K. The
standard six-contact dc-current Hall configuration and static
magnetic field B ¼ 1.5 T were used. The temperature dependence of
the resistivity component parallel to the current direction, rxx, was
measured in the absence of the external magnetic field for all
investigated samples. All our samples show low resistivity
rxx z 10
3 … 10
4 U cm. The temperature dependence of rxx for
T > 50 K shows features characteristic of degenerate semi-
conductors, i.e., metallic behavior for all our samples. Such feature
is characteristic of GeTe based DMS [6]. At low temperatures,
T z 40 K, a minimum in the rxx(T) dependence is clearly visible. It
may be related to the magnetic-impurity scattering processes in the
samples. The Hall effect measurements allowed us to determine the
temperature dependence of the carrier concentration,
n ¼ ðRH eÞ
1 , where RH is the Hall constant and e is the elementary
charge. All the samples show p-type conductivity with high carrier
concentration values n > 4  1020 cm
3 (see Table 1). The n was
almost temperature independent for our samples proving that the
thermal activation is not the main mechanism leading to the
appearance of conducting carriers in a material. The comparison of
the n values obtained at room temperature for the samples with
different chemical compositions leads to the following conclusions:
(i) we observe a small and non-monotonic increase of n as a
function of the Pb content, x, (ii) n does not seem to depend on the
Mn-content, y. The influence of the Pb content on the carrier con-
centration can be easily explained as an introduction of vacancies
and antisite defects into the crystal lattice during alloying of the
compound [20]. However, since our samples consist of two phases,
there are at least two major effects that could in principle influence
the calculated values: (i) carrier scattering occurring at inter-phase
regions and (ii) a difference in the Hall constant and Hall mobility
between the two phases. It is highly probable that in both phases
there is a high Hall carrier concentration and a low mobility. It is
impossible to separate them. We do not observe significant changes
of n as a function of the Mn content, y, due to the fact that Mn is an
isoelectronic dopant in IVeVI semiconductors. The values of the
Hall carrier mobility, m ¼ ðe,n,rxx Þ
1 , are gathered in Table 1. All
our samples have low mobility m < 20 cm2/(V s) at room
temperature. The m values show a small and non-monotonic
decrease as a function of both x and y. The carrier mobility de-
creases as a function of T, which is a signature of phonon scattering
mechanism.
3. Magnetic properties
The magnetic properties of Ge1
x
yPbxMnyTe samples were
studied with the use of dynamic and static susceptibility and static
magnetization measurements. We used LakeShore 7229 Suscep-
tometer/Magnetometer and Quantum Design XL-5 magnetometer
systems.
3.1. Low field results
The low-field dynamic susceptibility measurements were done
with the use of LakeShore 7229 Susceptometer/Magnetometer
system. At first the temperature dependence of the ac magnetic
susceptibility, cac, in the presence of an applied ac magnetic field
with the amplitude equal to 10 Oe and the frequency f ¼ 625 Hz,
was measured. The measurements were performed over a wide
range of temperatures from 1.4 K to 300 K. The results of the
temperature dependent dynamic susceptibility measurements in
the form of the temperature dependence of the real part of the ac
susceptibility Re(cac) for the selected Ge1
x
yPbxMnyTe samples
with different chemical compositions are presented in Fig. 2. The
obtained Re(cac(T)) curves show two peaks for each crystal. The
high-temperature maxima are located in the temperature range
between 40 and 100 K. The low-temperature maxima appear below
20 K. The behavior of the susceptibility indicates that we observe a
transition to an ordered state. Symmetrical shapes of the peaks
indicate that we do not observe a paramagneteferromagnet tran-
sition. In order to determine the type of the observed magnetic
order more detailed ac susceptibility measurements have to be
done.
We focused our studies on the temperature region from 40 K to
130 K where the maxima in the Re(cac(T)) curves are observed. We
measured the Re(cac(T)) dependence for four different frequencies
of the ac magnetic field: fi ¼ 7, 80, 625, and 9980 Hz. The shift of the

rni et al. / Journal of Alloys and Compounds 649 (2015) 142e150
A. Podgo 145

indicate a spin-glass-like state with the RM values close to those

Fig. 2. The temperature dependence of the real part of the ac magnetic susceptibility,
cac, obtained for the selected Ge1
x
yPbxMnyTe samples with different chemical
compositions xmtx and ymtx (shown in legend). The upper right corner inset shows
exemplary Re(cac(T)) dependence obtained for Ge0.794Pb0.196Mn0.055Te sample placed
in a magnetic field of different frequencies (shown in labels) and the upper left inset is
the low temperature region close up.
position of the maximum in the Re(cac(T)) dependence on the
temperature scale with the changing frequency of external mag-
netic field is a well known behavior characteristic of spin-glass and
superparamagnetic systems. In our samples all the observed peaks
shift to higher temperatures with the increase of f (an exemplary
result presented in the inset to Fig. 2). In order to distinguish be-
tween the spin-glass-like state and the superparamagnetic state we
calculated the phenomenological parameter proposed by Mydosh
as a good criterion for such an analysis [21], expressed in the
following form:
obtained for our samples. Thus the peaks in the cac(T) dependence
can be convincingly identified as a signature of a spin-glass-like
state.
The freezing temperature, TF, defined as a position of the peak in
the cac(T) dependence for each measured frequency of the ac field
depends on the magnetic field frequency. In order to properly
determine the TSG value it is necessary to extrapolate the TF(f)
dependence to f / 0. The TSG obtained in this way should be
comparable to the static magnetic susceptibility and thus deter-
mine the spin-glass-like transition temperature in a precise way.
The calculated values of TSG are gathered in Table 2.
The discussion of the changes of TSG with the amount of mag-
netic impurities has to take into account that our Ge1
x
yPbxMnyTe
crystals form two phase system. Both phases, Ge- and Pb-rich, due
to their different chemical composition should have different
values of the magnetic exchange-constant, Jpd. For Ge1
xMnxTe Jpd
reached values up to 0.9 eV, while for Pb1
xTMxTe with x ¼ 0.01
Jpd ¼ 0.18 eV (Ref. [24]). Since our samples consist of two magnetic
subsystems characterized by different Jpd values, the temperature
dependence of the ac susceptibility indicates two magnetic tran-
sitions in each sample (see Fig. 2). Since the main phase is the
matrix with high Ge-content (with possibly higher Jpd value), we
can associate the high temperature spin-glass-like transition tem-
perature TSG with this phase and correlate TSG with the amount of
Mn in the matrix, ymtx. The transition observed at T < 20 K can be
related to the second phase, e.g., clusters with high Pb content. The
TSG(ymtx) dependence does not show a well defined trend. It is due
to a fact that the spin-glass-like transition temperature due to
carrier mediated magnetic interactions depends on several struc-
tural, magnetic and transport parameters. Thus, a much more
complicated analysis with the use of theoretical modeling has to be
employed in order to explain and reproduce theoretically the
experimental values of TSG. An analysis based on theoretical and
semi-empirical model will be shown in Section IV.
The temperature dependence of the ac magnetic susceptibility
at temperatures well above TSG for our samples can be described
with the use of a modified CurieeWeiss law:

DTF C
RM ¼ ; (1) Reðcac Þ ¼ þ cdia ; (2)
ðTF ÞDlogðf Þ T
q

where TF represents the freezing temperature at a frequency fi,
DTF ¼ TF(fi)
TF(fj), and Dlog(f) ¼ log(fi)
log(fj). The TF(fi) values are
determined from the position of the maximum in the Re(cac(T))
dependence measured at the frequency fi. The calculated values of
the RM factor obtained for our samples (gathered in Table 2) are
close to 10
2 and do not change much with the chemical compo-
sition of our samples. The RM values are close to 0.01, i.e. the value
characterizing canonical spin-glasses like CuMn or FeAu [21].
Furthermore, other TM-alloyed IVeVI DMS, i.e., Pb1
x
ySnxMnyTe
(Ref. [22]), Ge1
x
ySnxMnyTe (Ref. [6]), and Ge1
xCrxTe (Ref. [23])
with the Curie constant, C, defined as
C ¼ g2 m2B SðS þ 1ÞyC
W ; (3)
where q is the paramagnetic CurieeWeiss temperature, g is the
effective spin splitting factor, g ¼ 2 for Mn, mB is the Bohr magneton,
S is the spin of the Mn, yC
W is the magnetically active Mn content,
and cdia is the diamagnetic susceptibility of the nonmagnetic
Pb1
xGexTe host crystal. All IVeVI semiconductors containing
nonmagnetic ions are standard diamagnetic materials. In PbTe

Table 2
Results of the magnetometric measurements including the Mydosh factor RM, the spin-glass-like transition temperature TSG, the CurieeWeiss temperature q, the Curie constant
C, and magnetically active Mn content yC
W.

x y RM ± DRM TSG ± DTSG (K) q ± Dq (K) C ± DC (10
4) yC
W ± DyC
W

0.232 0.019 0.015 ± 0.004 75.8 ± 0.3 137 ± 3 0.8 ± 0.1 0.004 ± 0.001
0.196 0.055 0.008 ± 0.006 92.5 ± 0.4 80 ± 2 13.0 ± 0.2 0.067 ± 0.001
0.196 0.061 0.007 ± 0.002 88.8 ± 0.1 82 ± 4 8.6 ± 0.3 0.044 ± 0.001
0.254 0.074 0.008 ± 0.005 92.7 ± 0.3 68 ± 4 10.3 ± 0.1 0.054 ± 0.001
0.183 0.074 0.002 ± 0.001 88.8 ± 0.1 95 ± 4 8.7 ± 0.3 0.044 ± 0.002
0.180 0.074 0.015 ± 0.018 64.9 ± 0.7 49 ± 2 9.9 ± 0.1 0.050 ± 0.001
0.311 0.081 0.015 ± 0.003 44.0 ± 0.1 72 ± 1 12.0 ± 0.1 0.066 ± 0.001
0.294 0.136 0.015 ± 0.009 65.3 ± 0.5 45 ± 1 18.3 ± 0.1 0.099 ± 0.001
146
rni et al. / Journal of Alloys and Compounds 649 (2015) 142e150
A. Podgo

cdia ¼
3  10
7 emu/g (Refs [25] and [26]) and in GeTe

cdia ¼
3  10
7 emu/g (Ref. [27]). Corrections of the experimental
data taking into account the contribution of the sample holder were
applied (the signal from the sample holder was measured prior to
each sample characterization). The experimental cac(T) depen-
dence obtained at T ranging from 200 K up to 325 K for all our
samples was fitted to the Eq. (2) with C and q as the fitting pa-
rameters. We obtained good fits of the modified CurieeWeiss law
to the experimental Re(cac(T)) curves. The obtained values q and C
are presented in Table 2.
It should be pointed out, that in the molecular-field approxi-
mation the parameters q and C obtained from the CurieeWeiss law
are actually related to all interactions between magnetic ions in the
sample. In our fits of high-temperature magnetic susceptibility to
the CurieeWeiss law it was not possible to separate satisfactorily
contributions from different phases to the parameters q and C.
Therefore, these parameters are not related to either the matrix or
the clusters but carry information about the combined properties of
both systems.
The calculated q values cannot be easily correlated with the
average amount of Mn in the alloy. It is also visible, that q values are
either lower or higher than TSG, depending on the alloy composi-
tion, without any obvious trend. The large difference between the
values of q and TSG is a signature of a presence of additional regions
in the samples with different Mn-content than the estimated yclr or
ymtx. The presence of such regions can be observed in Re(cac(T))
dependence as a slight change of slope above the temperature of
the maximum.
The value of the Curie constant obtained during the fitting of
Re(cac(T)) with Eq. (2) can be used to calculate from Eq. (3) the
amount of magnetically active Mn ions present in each sample. In
our estimation we assumed that the manganese ions contributing
to the magnetic susceptibility are the Mn2þ ions with S ¼ 5/2. The
obtained yC
W values are gathered in Table 2. The amount of
magnetically active Mn ions, yC
W, is smaller than the average
content, y. It is a signature of the increase of structural and mag-
netic disorder in our samples. A part of manganese ions may remain
in a different charge state than the Mn2þ and have S < 5/2. It is also
possible that some Mn ions can occupy interstitial positions in the
cation lattice. These ions may be very strongly electrically and
antiferromagnetically coupled to other Mn ions and be magneti-
cally inactive. Such effect has been observed in other DMS like
Ga1
xMnxAs [28,29]. The Mn ions may be also magnetically inactive
if they happen to be in GeeMn nanoclusters [30].
The dc magnetometery was used to study magnetization M vs. T
of the Ge1
x
yPbxMnyTe crystals. At first, the temperature depen-
dence of the magnetization was measured in the range of low
magnetic fields H ¼ 50e1000 Oe using a SQUID magnetometer.
Measurements were performed over a wide temperature range
T ¼ 2e250 K in two steps, i.e. with the sample cooled in the pres-
ence (FC) and the absence (ZFC) of the external magnetic field. The
contribution of the sample holder was subtracted from the exper-
imental data. The results showed that up to 1000 Oe the isothermal
magnetization M(H) curves were nearly linear allowing us to
calculate the dc magnetic susceptibility, cdc ¼ vM/vH, and its
changes with temperature for each Ge1
x
yPbxMnyTe sample. The
results of the estimation in a form of temperature dependencies of
both ZFC and FC static susceptibility cdc for two selected samples
are presented in Fig. 3. The ZFC cdc(T) dependence shows a
maximum between 40 and 80 K. Another maximum is observed
below 25 K. In the cdc(T) we observe a large separation between the
FC and ZFC curves for T < 100 K. The cdc(T) curves lead to conclu-
sions similar to the ac susceptibility results, i.e. that we observe the
spin-glass-like state in our Ge1
x
yPbxMnyTe crystals. The M(T)
results will be discussed in detail in the subsequent paragraphs and
Fig. 3. DC susceptibility, cdc, as a function of temperature for selected
Ge1
x
yPbxMnyTe samples with different chemical compositions.
used for the determination of the magnetic exchange constants in
both magnetic subsystems present in our samples.
3.2. High field magnetization
The isothermal magnetization, M, measurements were done in
the presence of a static magnetic field with values H  90 kOe.
Measurements were performed under isothermal conditions at
selected temperatures below 200 K. The Weiss extraction method
implemented in the LakeShore 7229 magnetometer system was
used. The exemplary M(H) curves measured at 4.5 K for the samples
with different chemical compositions are plotted in Fig. 4a. For each
sample the magnetization rises abruptly with rising magnetic field
up to about 5 kOe, then the further increase is slow and even at the
magnetic field as high as H ¼ 90 kOe M does not reach saturation.
That indicates a presence of more than one type of magnetic in-
teractions in the crystals. If the material were paramagnetic with
ferromagnetic (FM) interactions only, the M(H) dependence at the
4.5 K would reach saturation in H below 90 kOe. The lack of satu-
ration indicates a presence of a strong antiferromagnetic coupling,
probably due to pairing of Mn-ions. The competition between the
ferromagnetic and antiferromagnetic interactions causes a disorder
necessary for the appearance of the spin-glass-like magnetic state
in our crystals.
Detailed isothermal measurements of magnetic hysteresis loops
were performed at selected temperatures below 200 K. Hysteresis
loops obtained for a selected sample measured at isothermal con-
ditions at selected temperatures are presented in Fig. 4b. Well
defined magnetic hysteresis loops are observed in all the investi-
gated crystals at temperatures T < TSG. The presence of magnetic
hysteresis in a spin-glass-like system is a sign of the appearance of a
domain structure in a material. The presence of magnetic hysteresis
was reported in many typical metallic spin-glasses such as AuFe
with 8% of Fe atoms [31] or NiMn with 21% at. Mn (Ref. [32]). The
square-shape of the hysteresis loops points out the fact that the
distribution of the cluster sizes in our samples is uniform. The
presence of tails in the hysteresis loops indicates that a small
fraction of clusters has sizes significantly different from the average
size. The magnetic hysteresis loops measured at temperatures
below 100 K are used to define the temperature dependencies of

rni et al. / Journal of Alloys and Compounds 649 (2015) 142e150
A. Podgo
Fig. 4. Results of the isothermal magnetization measurements including: (a) magnetization curves obtained at T ¼ 4.5 ± 0.1 K for the samples with different chemical compositions
(see legend), (b) magnetic hysteresis loops obtained at different temperatures for the exemplary Ge1
x
yPbxMnyTe crystal with x ¼ 0.294 and y ¼ 0.136, and the temperature
dependencies of (c) coercive field HC and (d) remnant magnetization MR for the selected Ge1
x
yPbxMnyTe samples with different chemical compositions, x and y (see legend).
the coercive field, HC, and the spontaneous magnetization, MR, (see
Fig. 4c and d). The HC and MR obtained at T ¼ 4.5 K change values
from 160 Oe to 870 Oe and from 0.5 emu/g to 3.0 emu/g, respec-
tively, for the samples with different chemical compositions. There
is no clear correlation between the obtained HC and MR parameters
and the average Mn or Pb content in the samples. Both HC and MR
are decreasing linear functions of the temperature for T < TSG, and
for T z TSG the hysteresis loops vanish. The temperatures at which
both HC(T) / 0 and MR(T) / 0 are close to the estimated TSG values.
4. Exchange integral estimation
4.1. Temperature dependence of magnetization
The results of the low-field magnetization measurements, M(T),
for selected samples will be used in order to determine the mag-
netic exchange constants for both magnetic subsystems present in
the samples. By visual inspection of the measured M(T) de-
pendencies for FC conditions, we can distinguish between two
classes of behavior. The first one is characteristic of the sample with
x ¼ 0.294 and y ¼ 0.136, in which we deal only with a single
magnetically ordered system. As is seen in Fig. 5a, where a set of
temperature dependencies of magnetization under FC conditions is
presented for that sample, the slope of the M(T) curve is varying
Fig. 5. Magnetization M obtained experimentally (points) and fitted to the Bloch law
(lines) as a function of temperature for selected Ge1
x
yPbxMnyTe samples with: (a)
x ¼ 0.294 and y ¼ 0.136 and (b) x ¼ 0.196 and y ¼ 0.061.
147
monotonically in a way which resembles the prediction of the Bloch
law, being a sure sign of the presence of long-range magnetic order
in the sample, perturbed by thermally excited spin waves. On the
contrary, for two other samples (with x ¼ 0.196, y ¼ 0.061 and with
x ¼ 0.180, y ¼ 0.074) we observe non-monotonic changes of the
M(T) curve slope (as visible in Fig. 5b for x ¼ 0.196 and y ¼ 0.061).
They can be interpreted as a result of the existence of two sub-
systems ordering magnetically below two significantly different
characteristic temperatures. These subsystems can be identified
with Mn ions in matrix and in clusters, respectively.
For the sample with a single magnetically ordered subsystem
(Fig. 5a), we assume that the system which orders magnetically is
composed of Mn ions in the matrix. The dependence of magneti-
zation on temperature can be written as the Bloch law
MðTÞ ¼ M1 ½1
ðT=TSW 1 Þ3=2 , where M1 is the spontaneous
magnetization at T ¼ 0 K and TSW 1 is the characteristic temperature
for the first magnetic subsystem. TSW 1 can be extracted from the
experimental data. It is visible in Fig. 5a that the temperature
dependence of the FC magnetization can be fitted to the Bloch law
for the range of temperatures lower than approximately half of the
critical temperature. The values of the characteristic temperature,
TSW 1, obtained from such fits are indicated in Fig. 5a. It is visible
that the temperature increases slightly with increasing FC field,
therefore, the value obtained for the lowest field 50 Oe was
accepted for further calculations.
For the samples with two subsystems, ordering magnetically
below two significantly different characteristic temperatures, we
use a different approach for modeling of M(T). According to our
model, the subsystem consisting of Mn-ions in the matrix is char-
acterized by a considerably high ordering temperature, TSW 1, and
thus the temperature dependence of magnetization for it can be
described with MðTÞ ¼ M1 ½1
ðT=TSW 1 Þ3=2  (solid line in Fig. 5b for
x ¼ 0.196 and y ¼ 0.061). At temperatures about an order of
magnitude lower than TSW 1 but higher than TSW 2 the subsystem of
ions in clusters is not ordered and does not contribute to the total
sample magnetization. On the other hand, at temperatures below
TSW 2 magnetic order emerges among magnetic impurities in
clusters as well. For such low temperatures the magnetization of
the remaining subsystem (matrix) can be treated as constant. Let us
mention that the application of the Bloch law to the matrix sub-
system (1) can be somewhat more approximate than to the cluster
subsystem (2), since for (1) it is applied in the range of relatively
higher temperatures (but still less than a half of TSW 1) than for the
case of the cluster subsystem (when the range of temperatures
extends from zero temperature). However, such a procedure is
148
rni et al. / Journal of Alloys and Compounds 649 (2015) 142e150
A. Podgo

conditioned by the existence of two subsystems with significantly
different ordering temperatures, so that the excitations just in the
matrix can be singled out only at temperatures higher than the
ordering temperature of the cluster subsystem. Therefore, the
magnetization of the subsystem of Mn ions in the matrix acts as a
source of a constant external magnetic field applied under FC
conditions. The total sample magnetization in the low-temperature
range can be fitted with a dependence
MðTÞ ¼ M1 þ M2 ½1
ðT=TSW 2 Þ3=2  (dashed line in Fig. 5b), where
M2 is the spontaneous magnetization at T ¼ 0 K and TSW 2 is the
characteristic temperature of the second magnetic subsystem. Data
ranges used for both fits exclude magnetization tails which arise for
temperatures close to TSW 1 and TSW 2 due to nonzero external field
and exchange interaction between both subsystems. Like in the
case of the previous sample, we performed the fits only for the
lowest FC field of 50 Oe. Please note that the logarithmic temper-
ature scale in Fig. 5a and b is used to emphasize the low-
temperature features of M(T) dependencies.
The characteristic temperatures TSW 1 and TSW 2 resulting from
fits to the experimental M(T) curves for all the considered samples
are contained in Table 3.
The characteristic temperature TSW i for a given subsystem can
be expressed as


4pDi 4S 3=2
TSW i ¼ ; (4)
kB a2s zð3=2Þ
where Di denotes spin wave stiffness in the ordered subsystem, kB is
the Boltzmann constant, z(3/2) x 2.612 is the Riemann zeta func-
tion, while as is the lattice constant. We used as ¼ 5.98 Å, the lattice
constant of GeTe. The value of Di can be calculated within a model
assuming that the driving force for long-range magnetic order is
the indirect RKKY coupling between magnetic ions, which yields
1 X
Di ¼ yeff i S JRKKY ðRk ÞR2k : (5)
6
k of Jpd written in Table 3 involve the uncertainty in determination of
The summation here is over all the positions in the lattice which
can be occupied by magnetic ions (and Rk are relative distances of
these sites from a selected site at the origin). In our calculations we
assume that the Mn ions occupy approximately the sites of the fcc
lattice (thus neglecting the rhombohedral distortion) and the yeff i is
the concentration of Mn ions in a given subsystem which orders
magnetically. It is known that the concentration of magnetic ions
which contribute to the ordered state is lower than their total
concentration, for example because of the existence of antiferro-
magnetically coupled nearest-neighbor pairs and larger clusters. In
order to take this factor into account, we assume that yeff i is equal
to the EDX-measured concentration of Mn in a given subsystem
rescaled by the ratio yC-W/y for a given sample, i.e. yeff i ¼ yiyC-W/y,
where yi ¼ ymtx or yclr. Such a procedure is justified by the fact that
yCW is sensitive only to the presence of magnetically active ions
(averaged over the whole sample). We note here that we are not
able to determine separately the concentration of magnetically
active ions in both subsystems. The rescaled concentrations used in
calculations are collected in Table 3.
The exchange integral of RKKY coupling is expressed after
Ref. [33] as:
  m* Jpd
2 a6 k4
s F
JRKKY Rij ¼ NV
32p3 Z2
     
sin 2kF Rij
2kF Rij cos 2kF Rij Rij
  4 exp
; (6)
2kF Rij l
where NV ¼ 4 is the number of valleys in the valence band of GeTe,
m* ¼ 1.2me is the effective mass of the charge carriers (holes), and
Rij is the distance between magnetic ions. The Fermi wavevector is
kF ¼ ð3p2 n=NV Þ1=3 for the concentration of holes equal to n. In or-
der to account for scattering of the charge carriers by the impu-
rities, we include an exponential damping factor in the expression
for JRKKY, parameterized by the mean free path l ¼ mZkF/e. In the
present case its value cannot be extracted from the conductivity
measurements with help of the Drude model of conductivity, due
to the highly inhomogeneous character of the samples, influencing
nontrivially the transport properties. From our Hall effect data with
m < 20 cm2/(V s) we estimated, within our experimental accuracy,
the approximate value of l ¼ 10 Å. The only free parameter which
remains is the exchange interaction energy between Mn spins and
hole spins, Jpd, which can be determined from the experimental
values of TSW i. The values of Jpd exchange integrals for both matrix
and cluster magnetic subsystems obtained from the values of TSW 1
and TSW 2 using Eqs. 4e6 are collected in Table 3. On the basis of
analysis of M(T) dependencies, it can be concluded that for the Ge-
rich phase (corresponding to the matrix) the value of Jpd is close to
0.6 eV. On the other hand, for the Pb-rich phase (clusters) it takes
the values of approximately 0.2 … 0.3 eV. This energy range lies
slightly above the value known for Pb0.99Mn0.01Te [24]. In spite of
some scatter of spin wave stiffness values for various samples, the
scatter of Jpd is much reduced. Let us mention that the uncertainties
TSW i from fitting procedure, the uncertainty of yeff i, and the un-
certainty of the Hall carrier concentration n.
4.2. Sherrington-Southern model
We have determined from our experiments the magnetic tran-
sition temperature, TSG, in the Ge-rich phase. The theoretical model
of the diluted magnetic system with RKKY interactions gives a TSG
in a good agreement with our experimental results. The model
proposed by Sherrington and Southern [34] (SS) can be used to
describe the coexistence of FM and SG states in diluted magnetic
semiconductor systems with RKKY interactions. The SS model
modified by Eggenkamp et al. (Ref. [22]) has been successfully
applied for the IVeVI semimagnetic semiconductors such as
Pb1
x
ySnxMnyTe [22] and Ge1
x
ySnxMnyTe [35] reproducing well
their magnetic behavior and allowing the determination of the
magnetic exchange constant, Jpd, for a range of crystal

Table 3
Parameters and results of fitting of the temperature dependence of magnetization for three samples to the Bloch law.

Sample i yeff i ± Dyeff i TSW i ± DTSW i Di ± DDi Jpd i ± DJpd i

(K) (meV Å2) (eV)

x ¼ 0.294, y ¼ 0.136 1 (matrix) 0.124 ± 0.025 37.6 ± 0.8 3.77 ± 0.08 0.61 ± 0.16
x ¼ 0.196, y ¼ 0.061 1 (matrix) 0.135 ± 0.031 89.2 ± 5.7 8.9 ± 1.0 0.55 ± 0.12
2 (clusters) 0.050 ± 0.012 5.1 ± 0.3 0.51 ± 0.05 0.22 ± 0.05
x ¼ 0.180, y ¼ 0.074 1 (matrix) 0.061 ± 0.027 66.8 ± 7.0 6.7 ± 2.2 0.64 ± 0.28
2 (clusters) 0.034 ± 0.009 6.8 ± 0.3 0.69 ± 0.10 0.28 ± 0.07

rni et al. / Journal of Alloys and Compounds 649 (2015) 142e150
A. Podgo
compositions. In the present work we adapted the modified SS
model proposed by Eggenkamp [22] to reproduce the observed
spin-glass-like state and to find the most appropriate values of the
magnetic exchange constant, Jpd. SS model assumes that the mag-
netic system is described by the Heisenberg Hamiltonian
P
H ¼
Jij Si Sj , in which each ion with spin S interacts with all other
i;j
spins. The interaction strength between two spins, Jij, has the
gaussian distribution. The interaction distribution is described with
P samples with x z 0.1 and n z 1021 cm
3 the transition temperature
the mean value, J0 ¼ JRKKY ðRk Þ, and the width, DJ, of the gaussian
k
P close to the theoretical TSG(yeff 1) curve for Jpd ¼ 0.47 eV and
distribution expressed as ð DJ Þ2 ¼ ½ JRKKY ðRk Þ
J0 2 . The SS model
k
allows us to calculate the spin-glass transition temperature, TSG,
using the following equation:


2DJ 2 SðS þ 1Þ 1=2
TSG ¼ S ðS þ 1Þ2 þ : (7)
3kB 2 The magnetic properties of Ge1
x
yPbxMnyTe bulk crystals with
In the above equation the RKKY indirect interaction is described
with the exchange constant JRKKY, which is expressed by the Eq. (6).
In our calculations we used the lattice parameters for pure GeTe
crystals. We assumed that in the investigated Ge1
x
yPbxMnyTe
crystals both the crystal and the band structure are similar to the
crystal and the band structure of GeTe. The valence band of GeTe is
nearly spherical with a maximum at the L-point of the Brillouin
zone and the energy gap of about 0.2 eV [36]. The results of our
calculations based on the SS model are presented in Fig. 6 in the
form of TSG temperatures as a function of the manganese content,
rescaled by the ratio yC-W/y, in the Ge-rich phase, ymtx, compared
with the experimental data. We calculated the TSG dependencies for
different values of Jpd. In Fig. 6 we show the representative results
for two values of Jpd corresponding to the two regions of x. Calcu-
lations of TSG were done with the values of the Hall carrier con-
centration indicated in the legend to Fig. 6. The calculated
transition temperatures increase with the Mn ion concentration.
The chemical compositions of the samples, especially
Fig. 6. The spin-glass transition temperature, TSG, (lines) calculated as a function of the
effective Mn molar fraction in the main phase of the alloy, yeff 1, for two different Pb-
content values: (a) xmtx z 0.05 and (b) xmtx z 0.1. The transition temperatures were
calculated for two different values of the exchange integral, Jpd, and different values of
the carrier concentration n (see legend). The experimentally determined values of TSG
for Ge1
x
yPbxMnyTe crystals with different chemical contents yeff 1 are plotted as
symbols.
149
GeMnTeePbMnTe ratio, should have significant impact on the value
of the exchange integral, Jpd. As we can see in Fig. 6a for the samples
with xmtx z 0.05 and different carrier concentrations the experi-
mental results lie in the region of transition temperatures TSG(yeff 1)
predicted by the SS model for Jpd ¼ 0.80 eV. However, the experi-
mental TSG do not seem to increase noticeably with the Mn-content.
This would be hard to explain in case of a canonical spin glass;
therefore we describe our system as a spin-glass-like state. For two
increases with the Mn-content and the experimental points lie
n z 1021 cm
3 (Fig. 6b). The estimated Jpd values reflect the fact,
that the magnetic exchange constant has much lower value for
Pb1
xMnxTe than for Ge1
xMnxTe.
5. Summary
chemical composition 0.180 < x < 0.311 and 0.019 < y < 0.136 grown
by modified Bridgman method are studied. The structural charac-
terization of our samples indicated that all our samples consist of
two similar Ge1
xPbxTe-based phases, one of which is Ge-rich and
the other is Pb-rich. All our samples show a magnetic order with
two transitions, one at temperatures lower than 20 K and the other
between 40 and 100 K. The observed magnetic transitions are
associated with the presence of two magnetic subsystems having
different chemical compositions e the host lattice and clusters. The
observed magnetic order is interpreted in terms of the carrier
mediated magnetic interactions in two magnetic subsystems. The
experimental results are analyzed theoretically within the spin-
wave-theory-based model of a disordered ferromagnet with long-
range RudermaneKitteleKasuyaeYosida interaction. The mag-
netic properties of our samples indicate, that even in the region of n
and yeff 1 where the ferromagnetic state could be expected, we
observe rather a spin-glass-like state. The comparison of the
experimental and theoretical TSG values indicates that most prob-
ably the magnetic exchange constant, Jpd, for the Ge-rich phase has
values from 0.47 eV to 0.80 eV. The carrier mediated magnetic
exchange constant for the Pb-rich phase has values from 0.22 eV to
0.28 eV.
Acknowledgments
The research was supported by the Foundation for Polish Sci-
ence e POMOST/2011-4/2 Programme co-financed by the European
Union within European Regional Development Fund. The research
was partly financed by the National Center for Science of Poland
under Decision No. DEC-2012/05/D/ST3/03161.
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