Solid State Communications 151 (2011) 1112–1116

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Solid State Communications

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Thermal expansion and magnetostriction of GdAg2 , and relations to the

magnetoelastic paradox
N. Mehboob a , M. Rotter b,∗ , M. Doerr c , E. Royanian a , H. Müller a , A. Grytsiv d , Y. Skourski e
a
Institut Für Festkörperphysik, Technische Universität Wien, 1040-Wien, Austria
b
Max Planck Institute for the Chemical Physics of Solids, Nöthnitzer Str. 40, 01187 Dresden, Germany
c
Institut für Festkörperphysik, Technische Universitat Dresden, D-01062 Dresden, Germany
d
Institute for Physical Chemistry, University of Vienna, A-1090 Wien, Austria
e
Hochfeld-Magnetlabor Dresden, FZ Dresden-Rossendorf, D-01314 Dresden, Germany

article info abstract

Article history: The antiferromagnet GdAg2 has been shown to be a good model system for the magnetoelastic paradox
Received 18 February 2011 (MEP), because it exhibits large symmetry conserving magnetoelastic strains and the antiferromagnetic
Received in revised form propagation vector breaks the tetragonal lattice symmetry (therefore a large symmetry breaking
5 May 2011
magnetoelastic strain can be expected in a single q magnetic structure). As in many similar Gd based
Accepted 16 May 2011
by P. Chaddah
compounds no symmetry breaking strain has been found in the experiment. In order to investigate
Available online 27 May 2011 this MEP further, we have measured magnetostriction and magnetization on a textured polycrystal. The
behaviour closely resembles that of GdNi2 B2 C, the prototype system for the magnetoelastic paradox
Keywords: (MEP). Our forced magnetostriction data indicate that the crystal distorts in applied magnetic field and
A. Magnetically ordered materials gives further evidence that the MEP is a low field effect. The observed phase transitions are in agreement
D. Thermal expansion with available specific heat and neutron diffraction data. Moreover, the saturation magnetic field was
measured in high pulsed magnetic fields and agrees well with the value calculated from the Standard
Model of Rare Earth Magnetism (SMREM).
© 2011 Elsevier Ltd. All rights reserved.

1. Introduction and Ag on the 4e sites [4]. The lattice parameters are a =

The interaction of lattice and correlated electrons is of funda-
mental importance for the understanding of magnetic frustration
and exotic superconductivity [1,2]. However, magnetoelastic ef-
fects are often neglected, because they are assumed to be small
or because the underlying mechanism has not been investigated
in detail. Gd based systems are ideal to study the magnetoelastic
exchange striction effects, because the Gd3+ ion has the 4f7 con-
figuration and possesses a huge spin moment but no orbital mo-
ment. Investigations of magnetoelastic effects in a large number of
Gd compounds showed, that the exchange striction effects may be
very large. However, in zero field these large effects seem always
to conserve the lattice symmetry. This surprising experimental ev-
idence has been called the magnetoelastic paradox [3].
GdAg2 is a prototype system for the magnetoelastic paradox
because magnetic order is accompanied by large magnetoelastic
effects. It crystallizes in the tetragonal MoSi2 -type structure (space
group I4/mmm), with Gd on the 2a sites (point symmetry 4/mmm)
∗ Corresponding author.
E-mail address: Martin.Rotter@cpfs.mpg.de (M. Rotter).
0038-1098/$ – see front matter © 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.ssc.2011.05.030
0.3716 nm, c = 0.926 nm. The z parameter of the 4e sites (point
symmetry 4/mmm) has been determined from neutron diffraction
experiments with the value zAg = 0.327 ± 0.004 [5].
From specific heat, resistivity, thermal expansion and magne-
tization measurements as well as first neutron powder diffraction
experiments, it is known that GdAg2 orders antiferromagnetically
below TN ≈ 22.7 K [5,6] followed by two first-order magnetic tran-
sitions at TR1 ≈ 21.2 K and TR2 ≈ 10.8 K. The magnetic ordering
temperature of GdAg2 is lower than that of TbAg2 (TN = 34.8 K),
which violates the de Gennes law (the ordering temperatures of
other members of the RAg2 (with R = Dy, Ho, Er series are 15 K, 8 K,
and 5.5 K respectively [7])). This has been referred to a change in
the conduction band due to the boundary situation of GdAg2 con-
cerning the crystal structure, i.e. only the RAg2 with heavy R, start-
ing from Gd, show the MoSi2 type of structure [5]. GdAg2 shows
large magnetoelastic effects in contrast to isostructural GdAu2 [8].
In magnetic systems with f 7 configuration (L = 0, S = 7/2)
the exchange striction is considered as the only source of
magnetostriction. If the symmetry of a compound is not low,
a general propagation vector q will have more than one
equivalent. All these equivalent propagation vectors form the star
of the propagation vectors. If the star is formed by more than
one propagation vector and the system undergoes a single q
 N. Mehboob et al. / Solid State Communications 151 (2011) 1112–1116
antiferromagnetic order, a symmetry breaking lattice distortion
(SBLD) is expected. This means, that some special cases such as
ferromagnetism or antiferromagnetism with propagation along
the tetragonal c direction will not lead to a SBLD. In case
of GdAg2 the propagation vector has been reported to be not
along c [5,9] and therefore a SBLD is expected for a single q
magnetic structure. Note that also for multiple q structures a
SBLD is expected [10] unless these are completely symmetric.
The ‘‘magnetoelastic paradox (MEP)’’ [3] is the experimental fact,
that up to now in no Gd compound such a SBLD has been found.
The magnetoelastic paradox has been explained theoretically by
a multiple q structure [10], however such a multiple q-structure
has not been observed up to now in experiment in any Gd based
antiferromagnet.
Previously we have published detailed studies on the existence
of the MEP in GdAg2 on the basis of X-ray diffraction data [8] with
further explanations provided by the example of GdNi2 B2 C [10].
The present work is a continuation of our previous research to
provide further information on the MEP in magnetic field by
dilatometeric measurements performed on a strongly textured
sample (note that for this system single crystals are not available).
Up to now only in GdNi2 B2 C the MEP has been investigated
in magnetic field. In GdNi2 B2 C the application of a magnetic
field leads to the appearance of a large orthorhombic distortion
of the tetragonal crystal in small magnetic fields. This result
is surprising not only because it is of fundamental interest
in explaining the magnetoelastic paradox, but also, because it
indicates, that antiferromagnets might be of technological interest
as high magnetostriction materials. Therefore we study the
forced magnetostriction in systems exhibiting the magnetoelastic
paradox. Earlier magnetization measurements performed on
GdAg2 were up to 30 T [11] without any information on saturation
magnetic field. Therefore another task of the present work was
to measure magnetization in high pulsed magnetic field and to
compare the observed value of saturation magnetic field with the
theoretical value calculated from the SMREM.
2. Experimental details
The sample of GdAg2 with a weight of about 1.5 g was prepared
by melting in a high frequency furnace under an argon atmosphere
on a copper hearth from elemental ingots with minimal purity
of 99.9 mass%. Titanium was used as a getter prior to melting.
The alloy was remelted two times in order to improve their
homogeneity. The mass loss of the alloys after melting was less
than 1%. Grinding served to remove the oxidized layer from the
surface cleaned GdAg2 . The sample was sealed in quartz tubes and
annealed at 800 °C for 4 days before quenching in cold water.
The sample was analysed by X-ray powder diffraction with a
Guinier–Huber image plate system (Cu–Kα 1 ; 8° < 2θ < 100°)
at the Institute of Physical Chemistry, University of Vienna, and
was found to be almost single phase with traces of impurities,
probably some oxides. The sample was cut in size of approximately
(2 × 1.84 × 1.78) mm. The sample is not sensitive to air so there
is no need to protect it.
Note it is very difficult to produce a single crystal of
GdAg2 because of incongruent formation of this phase and the
narrow region of crystallization (825 °C < T < 830 °C)
according to the phase diagram [12]. Therefore we studied a
strongly textured sample. Verification of the strong texture in
our GdAg2 sample was performed with a GADDS (General Area
Detector Diffraction System) instrument in the Institute of Physical
Chemistry University of Vienna. The sample was exposed to
Cu–Kα 1,2 radiation with sample to detector distance of 15 cm.
The measurements were made at 50° < 2θ < 70° with
continuous rotation of the specimen around ϕ with respect to
1113
plane containing the incident and diffracted beams. The exposure
time for each frame with frame window 2θ = 2° was 60 min.
Bright spots were observed on Debye–Scherrer rings at (213)
and (204) indicating that the polycrystalline sample has a strong
preferential orientation.
The magnetoelastic properties, in particular the thermal expan-
sion (= temperature dependence of the sample length in zero field)
and the forced magnetostriction (= field dependence of sample
length at constant temperature) were measured on the textured
polycrystalline GdAg2 sample by capacitive dilatometry using a
tilted plate miniaturized dilatometer [13] with a resolution of rel-
ative changes of sample length of about 10−8 in a superconduct-
ing magnet with a maximum field of 9 T. The thermal expansion
was measured in zero field with a sweep rate of 5 mK/s. The mag-
netostriction has been measured at selected temperatures (below
TN ) to see transitions in a magnetic field. The induction method
with a coaxial pick-up coil system was used to perform the mag-
netization experiments in the pulsed field magnet up to 60 T at the
Hochfeld Magnetlabor Dresden (HLD). The characteristic rise time
of the pulsed field magnet was about 10 ms.
3. Results and discussions
The zero field thermal expansion measurement in the 4.2–290 K
range of temperature is shown in Fig. 1. The thermal expansion
curve measured by dilatometry is shown as a solid curve. There
is a negative thermal expansion coefficient (contraction) between
4.2 and 23 K for one direction; above this temperature, a
positive thermal expansion coefficient is observed. This behaviour
illustrates the antiferromagnetic ordering at TN ≈ 22.7 K. The
increase of the sample length to low temperatures represents the
spontaneous magnetostriction caused by the magnetization in the
ordered state. Comparison of the dilatometric thermal expansion
1l/l (solid curve) with 1a/a, 1c /c and 1V /3V (data points with
error bars) measured by X-ray powder diffraction [8], indicate that
1l/l matches well with thermal expansion along a-axis (1a/a).
This implies that the material is strongly crystallographically
textured and the dilatometer measures the a-axis properties. On
the basis of this observation one could expect that in the other
direction of the sample i.e. perpendicular to 1l/l ≈ 1a/a
there should be some distribution of grains oriented along b (=a
tetragonal) and c-axis. This hypothesis was confirmed by the
thermal expansion data taken in the perpendicular direction as
shown Fig. 1 (dashed line).
Fig. 2 shows the temperature dependence of thermal expansion
1l/l under an applied magnetic field of 0, 1.5 and 9 T. In zero
field two transitions at temperatures of about 11 and 22.7 K are
observed. The transitions are more clear in the inset which shows
the derivative of the 1l/l curves with respect to temperature
and represents the thermal expansion coefficient (α). The first
transition at Tt = 10.8 K corresponds to a change in magnetic
structure as is proofed by neutron diffraction results [5], whilst the
2nd transition at 22.7 K corresponds to the Néel Temperature TN ,
which is also in agreement with the results reported earlier [5,9].
The transition at 21.3 K, which was observed in neutron diffraction
and specific heat measurements, is not observed in the present
measurement, because the transitions at 21.3 and 22.7 K are very
close and our measurement resolution is not high enough and the
footprint of this transition in the magnetoelastic strain is small.
Comparing the temperature dependence of thermal expansion
1l/l under an applied magnetic field of 0, 1.5 and 9 T, it can be
seen that almost all the curves have the same behaviour and by
increasing applied magnetic field, the negative thermal expansion
increases. At a temperature near TN = 22.7 K the thermal
expansion changes from negative to positive. The value of thermal
expansion at 4 K in going from 0 to 1.5 T is about 4.8 × 10−5 (see
1114 N. Mehboob et al. / Solid State Communications 151 (2011) 1112–1116
Fig. 1. Comparison between the thermal expansion of GdAg2 as measured by the
dilatometer along different orthogonal directions of a textured sample (solid and
dashed lines) and by powder X-ray diffraction (from literature, points with error
bars) [8].
Fig. 2. Thermal expansion of GdAg2 in applied fields µ0 H = 0, 1.5, and 9 T
parallel to 1l/l. Dashed line 0 T is in comparison with 1.5 T. Inset shows the thermal
expansion coefficient (α ) at µ0 H = 0, 1.5 and 9 T.
Fig. 3. Longitudinal forced magnetostriction of textured GdAg2 sample at different
temperatures.
Fig. 2) which corresponds exactly to the value of magnetostriction
measured at 4 K and at 1.5 T as shown in Fig. 3.
Fig. 3 shows the longitudinal magnetostriction at seven
different temperatures (4, 8, 10, 15, 22, 26, and 33 K) in magnetic
fields up to 9 T. Because of the preferred orientation of the
crystal grains (texture), the magnetostriction mostly resembles
the behaviour of the a-axis, i.e. λ‖ ∼ (1a/a). The arrows in
the figure show whether the field was ramped up or down. The
magnetostriction starts positive from 4 to 10 K. A steep increase
in magnitude of λ‖ at 4 and 8 K occurred up to magnetic fields of
1–2 T which we interpret as an indication of a symmetry breaking
lattice distortion. It is reminiscent of the magnetoelastic paradox
observed in GdNi2 B2 C, where an orthorhombic distortion of the
tetragonal crystal appeared upon the application of a small field
in the tetragonal plane [3].
Above about 2 T the magnitude of λ‖ at 4–10 K increases
with very weak slope and exhibits a broad maximum at µ0 H =
5.5 T. Above 5.5 T, the magnitude of λ‖ decreases steadily the
magnetic field and saturation is not achieved up to 9 T. The
magnetostrictive effect is negligibly small above 10 K in a low
field but at higher field, negative magnetostriction is observed.
However, none of isotherms reaches the saturation in an applied
field of 9 T. Note that for the exchange striction model the
magnetostrictive signal may be expected to be proportional to the
square of the magnetization, which rises approximately linear with
the magnetic field until the saturation field (at low temperatures,
see below). The magnetostrictive effect at 22 K is larger than
at other temperatures for field above 3 T. We suggest that this
behaviour can be explained by the increase of the magnetic
susceptibility near TN : for temperature approaching T ≤ TN ,
the field induced spin reorientation transition to ferromagnetism
occurs at smaller fields and thus the saturation magnetostriction
(associated with the field induced ferromagnetic state) may be
achieved at lower fields. This may explain the larger slope in the
forced magnetostriction for temperatures near TN .
Fig. 4 presents the magnetostriction perpendicular to the
external field (λ⊥ ) at different temperatures (4, 8, 10, 15, 22,
and 33 K). Because of the texture, the magnetostriction again
may be considered as measured along the a-axis λ⊥ ∼ (1a/a)
while the field is applied perpendicular to it, but not along a
specific crystallographic direction. This makes the interpretation
more difficult. From the longitudinal signal and by analogy to
GdNi2 B2 C we may expect an orthorhombic distortion at 2 T leading
to some negative contribution in the transversal magnetostriction.
Increasing the field further should remove this distortion leading to
a positive contribution to the magnetostriction. Those grains with
field more along c direction seem to contribute with a negative
transversal magnetostrictive signal, which may be expected from
the spontaneous magnetostriction shown in Fig. 1. The isotherms
from 4 to 15 K have initially a negative slope and then increase with
positive slope up to a field of 5 T, the slope becomes again negative
at higher fields. Near the Néel temperature, the magnetostriction
increases linearly with negative slope and reaches the value of
about λ = −6 × 10−5 at 9 T. These larger magnitude may be
explained (as in the longitudinal magnetostriction) by the lower
transition field to the ferromagnetic state for temperatures near TN .
Taking the absolute values we get λ⊥ = 2λ‖ at 22 K for maximum
applied field.
Fig. 5 shows the comparison of magnetostriction along the
textured a-direction parallel (λ‖ ) and perpendicular (λ⊥ ) to
the magnetic field measured at 4 K. Both magnetostrictions
are of opposite sign and the longitudinal magnetostriction
(λ‖ ) is approximately 2.5 times larger than the transversal
magnetostriction (λ⊥ ). In Gd based systems without a symmetry
breaking lattice distortion the magnetostriction 1a/a should be
independent of the direction of the applied magnetic field as
 N. Mehboob et al. / Solid State Communications 151 (2011) 1112–1116
Fig. 4. Transversal forced magnetostriction of textured GdAg2 sample at different
temperatures.
Fig. 5. Comparison of the longitudinal and transversal magnetostriction curves of
the textured GdAg2 at temperature 4 K.
reported for orthorhombic GdCu2 [14]. However, in the present
case the magnetostrictions depend (for fields up to 2 T) strongly
on the direction of the applied field. This is in accordance with
the appearance of a symmetry breaking lattice distortion in GdAg2
occurring at application of an in plane magnetic field. From
GdNi2 B2 C we conjectured that the magnetoelastic paradox is only
present in zero field and may be lifted by a small magnetic field [3].
Our new data on GdAg2 supports this conjecture. Note that this
effect has only been observed in GdNi2 B2 C up to now and has been
explained theoretically by a transition from a zero field multiple
q structure to a single q structure in a magnetic field [10]. A
small hysteresis along and perpendicular to the magnetic field at
temperatures of 4 and 8 K in the data is also noticed.
To further investigate the hysteresis behaviour we measured
the steady field dependent magnetization at 4 K. The data show
no hysteresis as shown in Fig. 6. Therefore the hysteresis in
the magnetostriction is not associated with a corresponding
effect in magnetization. In order to explain the hysteresis effect
in magnetostriction we suggest two possible scenarios: (i) a
1115
Fig. 6. Steady state field dependent magnetization at T = 4 K (measured in PPMS).
The inset shows the hysteresis at low field.
coexistence of the low field and high field state or (ii) the
reorientation of antiferromagnetic domains. Concerning (ii) we
remark that also in a multiple q structure there may exist domains,
if it is not completely symmetric. Such a nonsymmetric double q
structure has been actually suggested in the case of GdNi2 B2 C [10]
and might lead to a tiny distortion of the tetragonal plane, which
is below the detection limit of the X-ray powder diffraction
experiment. Also in GdAg2 the hysteresis is about 1l/l = 1.0 ×
10−5 . Such a small orthorhombic distortion cannot be excluded in
the zero field state and is a factor of 20 smaller than the anomalies
in the lattice constants 1l/l ∼ 5 × 10−4 . The term MEP refers to
the observation, that any distortion of the crystal lattice is not of
the same magnitude as the anomalies in the lattice constants [3].
We want to emphasize that we could not measure a single
crystal of GdAg2 and therefore in the transversal magnetostriction
the direction of the applied field is in the ac plane, but different for
each grain in the sample. Therefore, we expect that the transversal
magnetostriction 1a/a with field along b (=a) will show a larger
and more first-order-like transition at 2 T than the transversal
signal shown in Fig. 5.
In order to get direct information about the magnetization
process of GdAg2 some magnetization measurements were
performed in high magnetic fields. Fig. 7 shows the graph of low
temperature pulsed field magnetization of GdAg2 as a function
of magnetic field µ0 H. It is linear without any obvious phase
transition signature up to the saturation field Hs = 37 T. The
saturation moment is about 7 µB /Gd3+ which is close to the
moment of the free ion.
In comparison to the experimental data, the saturation
magnetic field can be calculated with the standard model of rare-
earth magnetism. The Hamiltonian for the system can be derived
as follows.
Since for a Gd3+ the 4f shell is half filled so the orbital moment
is L = 0 and the 4f charge density is spherical, hence in first-order
perturbation theory there is no crystal field effect. Therefore, the
magnetic Hamiltonian for 4f, the Gd3+ system is a sum of isotropic
exchange (RKKY), the classical dipolar and the Zeeman interaction:
1− α 1 − α αβ β
H =− Ji (ij, ε)Ji · Jj − Ji JCD (ij)Jj
2 ij 2 ijαβ
−
− g J µB Ji · H. (1)
i
In expression (1) the 4f moment of the ith Gd+3 ion is represented
by the three components of the angular momentum operator
Jαi (α = 1, 2, 3). gJ = 2 is the Lande factor for Gd+3 with total
angular momentum J = 7/2 and µB the Bohr magneton.
1116 N. Mehboob et al. / Solid State Communications 151 (2011) 1112–1116

By using these values in Eq. (7) we obtain the value of the

saturation field Hs = 37 T. This calculated value agrees very well
with the experimental value found from magnetization in pulsed
magnetic fields. We may expect the disappearance of the SBLD for
the field induced ferromagnetic state in applied fields >37 T.

4. Conclusions

Magnetostriction, magnetization and thermal expansion mea-

Fig. 7. Isothermal magnetization at T = 4 K (measured in pulsed field at HLD).
The classical dipolar interaction constants can be calculated as;
β β
αβ (Rαi − Rαj )(Ri − Rj ) − δαβ |Ri − Rj |2
JCD (ij) = (g J µB )2
|Ri − Rj |5
Here Ri denotes the position vector of the ith Gd ion, which is
known from the crystal structure.
In order to calculate the saturation field we use the following
equation for the Néel temperature TN , the paramagnetic Curie
temperature Θp and the saturation field Hs for the transition from
the antiferromagnetic to the field induced ferromagnetic state,
surements on a GdAg2 textured polycrystalline sample were
performed in order to investigate the magnetoelastic paradox in
applied magnetic field. We estimated the saturation magnetic field
Hs from the Curie and Neel Temperatures by applying the standard
model of rare earth magnetism: the value of the saturation mag-
netic field is Hs = 37 T in good agreement with experimental value
determined in pulsed magnetic fields. Thus GdAg2 seems to behave
like a standard Gd3+ based antiferromagnet on a tetragonal lattice.
It exhibits large magnetostrictive effects and is a good example for
the MEP. Our forced magnetostriction data indicates, that the mag-
netoelastic paradox exists only in zero field and an orthorhom-
bic distortion may be induced in GdAg2 by application of a small
magnetic field. These results are similar to GdNi2 B2 C and support
. (2)
our conjecture that such behaviour of the MEP may be common
to all Gd antiferromagnets with a symmetry breaking propagation
vector. This conjecture needs still more support by further magne-
tostriction experiments on other prototype systems in small mag-
netic fields. However, the biggest challenge for experiments will
be to find evidence for the multiple q nature of the ground state of
systems showing the MEP.

J (J + 1) Acknowledgement
Θp = J (0). (3)
3kB
Part of this work has been supported by EuroMagNET under the
J (J + 1) EU contract no. 228043.
TN = J (q). (4)
3kB
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