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Physica B 359361 (2005) 12461248

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Magnetic state of pyrochlore Gd2 Mo2 O7 studied by

pressure-dependent magnetization measurement
H.C. Kima,, Younghun Job, J.-G. Parkb, S.W. Cheongc, M. Uhlarzd,
C. Peidererd, H.V. Lohneysend
a

National Research Laboratory for Material Science, Korea Basic Science Institute, 52 Yeoeun-Dong, Yusung-Ku, Daejeon 305-333,
Republic of Korea
b
Department of Physics, SungKyunKwan University, Suwon 440-746, Republic of Korea
c
Department of Physics and Astronomy, Rutgers University, Piscataway NJ 08854, USA
d
Physikalisches Institut, Universitat Karlsruhe, D-76128 Karlsruhe, Germany

Abstract
We studied the magnetic state of pyrochlore Gd2 Mo2 O7 by pressure-dependent magnetization MH and magnetic
relaxation measurements up to 16 kbar. The ferromagnetic saturation behavior seen in the MH curve was
substantially weakened by applying pressure and, at the same time, hysteresis behavior in the magnetization becomes
pronounced with pressure. Relaxation in the magnetization, although absent at ambient pressure, emerges upon and
increases with pressures. These ndings of the suppression of the ferromagnetism and the appearance of a metastable
spin glass phase is consistent with the previous results of rare-earth substitution studies.
r 2005 Published by Elsevier B.V.
PACS: 75.30.Kz; 64.60.My; 61.50.Ks
Keywords: Pyrochlore compound; Pressure; Metastable magnetic state

Pyrochlore compounds are characterized by

their three-dimensional geometrically frustrated
structure. Studies of pyrochlore molybdates
R2 Mo2 O7 (R rare-earth element) have shown
that magnetic properties of these compounds are
very sensitive to variations in the ionic size of the
Corresponding

author.
Tel.:
+82 42 865 3493;
fax:+82 42 865 3469.
E-mail address: chankim@kbsi.re.kr (H.C. Kim).
0921-4526/$ - see front matter r 2005 Published by Elsevier B.V.
doi:10.1016/j.physb.2005.01.373

rare-earth element [1]. Our previous studies of

(Gd1x Dyx 2 Mo2 O7 by DC and AC susceptibility
measurements showed the magnetic ground state
can also be changed by external pressure [2]. In
this work, we investigated the low-temperature
magnetic state of ferromagnetic Gd2 Mo2 O7
T C 70 K by magnetization and magnetic
relaxation measurements under high pressures to
further elucidate correlation between the magnetic
ground state and the lattice constant.

ARTICLE IN PRESS
H.C. Kim et al. / Physica B 359 361 (2005) 12461248

Sn, which is used as a manometer in our set-up.

Previous studies using substitutions have shown
that the ground state of pyrochlore Re2 Mo2 O7 is
very sensitive to variations in the ionic size of rareearth ions or to a resultant change in the lattice
constant. With substitution of rare-earth elements
having smaller ionic radius or likely applying
externally applied pressure, the ferromagnetic
ground state becomes unstable and the metastable
magnetic behavior of a spin glass (SG) type gets
clearly visible [1,2]. Similarly, a bigger hysteresis
loop at higher pressure, we think, is another
indication of the metastable spin glass phase.
In order to conrm further the metastable
magnetic behavior induced by pressure, we measured magnetic relaxation under pressures up to
16 kbar after switching on the magnetic eld of
500 Oe following zero-eld-cooling to 2.4 K. Fig. 2
shows the result of pressure-dependent magnetic
relaxation measured at 2.4 K. At ambient pressure
the sample shows no relaxation at all in the
magnetization measured for 2 h. However, upon
application of pressures, the magnetization begins
to show logarithmic time dependence. This logarithmic relaxation behavior is a typical spin-glass

1.3
20

16

M (B/f.u.)

1 bar
3.8 kbar
10.4 kbar
16 kbar

M(t)/M(0)

12

1.2

M (%)

Samples studied in this work are high-quality

single-phase polycrystals of Gd2 Mo2 O7 : Highpressure magnetization measurements were made
at 2.4 K using a BeCu pressure cell with a vibrating
sample magnetometer (Oxford Instruments Plc.).
Pressure inside the pressure cell was determined
from the superconducting transition temperature
of a pure Sn. For magnetic relaxation measurements, the sample was rst zero-eld-cooled to
2.4 K before a magnetic eld of 500 Oe was applied
and then magnetization was measured for 2 h.
Fig. 1 shows MH of Gd2 Mo2 O7 measured at
2.4 K under pressures up to 16 kbar. The magnetization measured at ambient pressure shows clear
ferromagnetic saturation behavior. For example,
the magnetization is 14:2mB =f:u: at 1 T and the
saturated magnetization (not shown here) is
15:33mB =f:u: at 12 T. Considering the full magnetic
moment 7mB of Gd3 ions, the saturated
magnetization value indicates that the sub-lattice
of Gd moments is ferromagnetically ordered at
2.4 K and there should also be ferromagnetic
coupling between Gd moments and Mo moments:
Mo moments is already ferromagnetically ordered
(FM) below 70 K [3]. With increasing pressure, the
ferromagnetic saturation behavior is weakened
and hysteresis behavior in the magnetization,
which is almost absent at ambient pressure,
becomes prominent. The small anomaly at low
elds is due to the superconducting properties of

1247

10

0
0

4
8
12
Pressure (kbar)

16

5
6

1.1

3
2

-4

1.0

-8
-12

1
-1.0

-0.5

0.0
Temperature (K)

0.5

1.0

Fig. 1. Magnetization MH of Gd2 Mo2 O7 measured at 2.4 K

under pressures up to 16 kbar. The arrow indicates the
increasing pressure.

10
time (min)

100

Fig. 2. Magnetic relaxation measured at 2.4 K under pressures

of (1) 1 bar, (2) 3.8 kbar, (3) 6.6 kbar, (4) 10.4 kbar, (5) 12 kbar,
(6) 16 kbar. Inset shows the pressure dependence of the
relaxation rate.

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H.C. Kim et al. / Physica B 359 361 (2005) 12461248

feature [4]. Interestingly enough, the relaxation

rate increases with pressure with a maximum
around 10 kbar before nally getting saturated
above 12 kbar. The inset of Fig. 2 shows the
pressure dependence of a total change in the
magnetization after 2-h measurements with respect
to the initial magnetization value. In the same way,
the magnetic hysteresis loop displays very small
pressure dependence above 12 kbar. From these
results, we can conclude that the ferromagnetic
state of Gd2 Mo2 O7 becomes unstable with pressure and eventually is made of a metastable spinglass type at higher pressures.
That the relaxation in the magnetization shows
a maximum at the intermediate pressure range is
interesting in comparison with the rare-earth
substitution effects. When doping smaller Dy ion
in (Gd1x Dyx 2 Mo2 O7 ; relaxation in the magnetization is found to show a maximum at x 0:1;
while the ferromagnetic phase is monotonically
decreased with x (not shown here). This result
together with the present pressure studies implies
that the relaxation in the magnetization is most
pronounced near the FMSG phase boundary.

To summarize, we have investigated the magnetic state of pyrochlore Gd2 Mo2 O7 by magnetization MH and magnetic relaxation Mt
measurements under pressures up to 16 kbar. The
ferromagnetic state is considerably weakened with
pressures and eventually turns into a metastable
spin-glass phase at higher pressure. The magnetic
relaxation effect is found to be most prominent
near the FMSG phase boundary. All our
observations with pressure studies are consistent
with the previous rare-earth substitution effects
[1].
The works at KBSI were supported by NRL
fund.

References
[1]
[2]
[3]
[4]

T. Katsufuji, et al., Phys. Rev. Lett. 84 (2000) 1998.

H.C. Kim, et al., Acta. Phys. Pol. B 34 (2003) 1429.
Y. Yasui, et al., J. Phys. Soc. Japan 70 (2000) 284.
J.A. Mydosh, Spin Glasses: An Experimental Introduction,
Taylor & Francis, London, 1993.