Physica B 320 (2002) 94–96

Dynamical effects in magnetic and transport properties

of phase separated La0.5Ca0.5Mn0.95Fe0.05O3
L. Granja, E. Indelicato, P. Levy, G. Polla, D. Vega, F. Parisi*
! Nacional de Energ!ıa Atomica,
Departamento de F!ısica, CAC, Comision ! Av. Gral Paz 1499 (1650), San Mart!ın Buenos Aires, Argentina

Abstract

We have measured transport and magnetic properties of polycrystalline La0.5Ca0.5Mn0.95Fe0.05O3, a phase separated
manganite with ferromagnetic ground state. Cooling rate dependences and time relaxation were found; the coexistence
of ferromagnetic and charge ordered regions determines a dynamics which influences physical properties. We show that
a dynamical contribution to the resistivity can account for the observed cooling rate dependence and ageing effects on
this phase separated manganite. r 2002 Elsevier Science B.V. All rights reserved.

Keywords: Manganites; Phase separation; Relaxation

The issue of phase separation (PS), i.e., the
simultaneous presence of submicrometer ferro-
magnetic (FM) regions and charge ordered (CO)
ones, is now arising as the most interesting one in
the physics of the manganese-oxide-based com-
pounds [1]. In PS compounds with the FM
ordering temperature lower than the charge order
antiferromagnetic (COAF) one (TC oTco ), as
La5/8
yPryCa3/8MnO3, the state of the system
close below TC is characterized by the coexistence
of isolated FM clusters embedded in insulating
regions; these clusters grow as the temperature is
lowered, and the insulator–metal transition is
obtained when the FM phase reaches the percola-
tion threshold [2]. A similar behavior is obtained
by doping with Cr at the Mn site in the half-doped
manganite Pr0.5Ca0.5MnO3, [3] with otherwise
COAF ground state. As was previously shown,
[4] doping with Fe the Mn site of La0.5Ca0.5MnO3
also renders it into this ‘‘TC oTco ’’ category.
*Corresponding author. Fax: +54-11-4754-7121.
E-mail address: parisi@cnea.gov.ar (F. Parisi).
0921-4526/02/$ - see front matter r 2002 Elsevier Science B.V. All rights reserved.
PII: S 0 9 2 1 - 4 5 2 6 ( 0 2 ) 0 0 6 5 1 - 8
The PS phenomena has given place to the study
of a variety of physical properties associated with
time dependent effects: cooling rate dependence of
resistivity, time relaxation in both magnetization
and resistivity, etc. [5].
In this work we present a study of dynamical
effects in the PS compound La0.5Ca0.5Mn0.95-
Fe0.05O3. Polycrystalline samples of this com-
pound were synthesized by the sol–gel technique.
DC resistivity was measured using the four-probe
technique, magnetization was measured using a
commercial SQUID.
Fig. 1 displays magnetization and resistivity as a
function of temperature. MðTÞ increases continu-
ously between 100 and 50 K, reaching a low-
temperature plateau which reveals mostly a FM
state. In accordance, the resistivity seems to dis-
play an insulator–metal transition at Tp E80 K.
Both Tp and the sample resistivity between 85
and 55 K were found to be very sensitive to the
cooling rate vc (inset Fig. 1), indicating that
dynamical effects are influencing the transport
response. Following this fact, we studied the time
 L. Granja et al. / Physica B 320 (2002) 94–96 95

40 40 ageing, the resistivity merges smoothly the curve

obtained at that cooling rate without temperature

Resistance (kΩ)
1.0 30 2 K/min
30 stabilization steps. This effect is similar to that
20

Resistance (kΩ)
found in the dissipation of some disordered
M ( µB )

0.2 K/min
10
20 ferromagnets and spin glasses [6], and has been
0.5 0
60 80
named ‘‘rejuvenation’’. Another striking feature is
Temperature (K) 10 that the slope of the rðTÞ curve below 80 K is
highly dependent on the previous history of the
0.0 0 sample. For instance, while qr=qT > 0 is found at
0 50 100 150 200 T ¼ 71:5 K when cooling continuously, suggesting
Temperature (K) metallic behavior, a typical insulator response is
Fig. 1. Temperature dependence of the magnetization obtained if, after 1 h ageing at that temperature,
(H ¼ 1000 Oe) and resistivity (H ¼ 0) on cooling for La0.5- cooling is resumed (Fig. 2).
CaMn0.95Fe0.05O3. Inset: temperature dependence of the In what follows, we work out a simple
resistivity when cooling at 2 and 0.2 K/min. phenomenological model to describe the main
features shown in Figs. 1 and 2. We start assuming
40 that at TC an inhomogeneous FM state appears,
1.15 consisting in the coexistence of isolated FM
clusters of definite size within a non-FM host. At
1.10
30 TD ¼ 85 K the FM clusters start to grow against
M(t)/M(0)
Resistance (kΩ)

1.05 the host material; the equilibrium size of the

20 clusters increase as T is lowered. The process
1.00
followed by the clusters to reach their equilibrium
10 100 1000
time (s)
size can be thought as a stepwise movement of the
10 phase boundaries through energy barriers. The
height of these barriers can be considered as
0 dependent on T and on the difference between the
40 50 60 70 80 90 actual cluster size and its equilibrium value, key
Temperature (K) ingredients also found in the description of
domain growth in random systems [7]. These kind
Fig. 2. Temperature dependence of the resistivity on cooling
continuously at 0.2 K/min (solid line) and with intermediate of models (called hierarchical constrained dyna-
stops of 1 h (open symbols). Inset: time dependence of the mics) are successful to predict slow logarithmic
magnetization at 80 K (H ¼ 1000 Oe). relaxation in several physical systems [8].
Before the FM clusters reach percolation thresh-
old, the resistivity re of the sample can be modeled
relaxation of the resistivity at several temperatures as a series circuit:
in the mentioned range. We used vc ¼ 0:2 K/min as
re ðT; vc Þ ¼ nðT; vc ÞrFM ðTÞ
the cooling rate to approach and depart from the
values at which the temperature was stabilized for þ ð1
nðT; vc ÞÞrCO ðTÞ; ð1Þ
1 h (Fig. 2). A decrease in the resistivity was where rFM ðTÞ and rco ðTÞ are the resistivities of the
observed at all tested temperatures. The relaxa- constitutive media and nðT; vc Þ is an effective
tions follow a logarithmic time dependence, and cluster length, a measure of the relative fraction
are as high as an 18% in 1 h at 73.8 K. A related f ðT; vc Þ of the FM phase. The slope of the
behavior was observed in the relaxation of the resistivity curve has two components. On one
magnetization at 80 K, characterized by a slow hand, a static contribution given by
increase of MðtÞ (inset of Fig. 2). 
qre qr qr
A noticeable fact is that, when the cooling ¼ nðT; vc Þ FM þ ð1
nðT; vc ÞÞ CO ;
process is resumed with vc ¼ 0:2 K/min after qT st qT qT
96 L. Granja et al. / Physica B 320 (2002) 94–96
which is typically less than zero in the non-
percolative regime. On the other hand, a ‘‘dyna-
mical’’ term given by
 regime, determined mainly by vc ; and the resistivity
qre qnðT; vc Þ
¼ ðrFM ðTÞ
rCO ðTÞÞ
qT dyn qT
related to the change of the size of FM clusters.
This term gives a positive contribution to the
resistivity slope in all the temperature range in
which f ðT; vc Þ changes with T:
As the system is cooling down at a rate vc below
TD ; the appearance of energy barriers at the
clusters surface prevent their free growth, and the
FM fraction f ðT; vc Þ no longer follows its equili-
brium value f ðT; 0Þ; larger differences correspond-
ing to higher vc : This fact accounts (Eq. (1)) for the
overall increase in the resistivity as vc is increased
(Fig. 1, inset). Two regimes can be distinguished
regarding the temperature dependence of the
cluster growth. Just below TD ; f ðT; vc Þ increases
slower than f ðT; 0Þ; yielding a low dynamical
contribution, i.e., larger (negative) slopes are
achieved with higher vc : As the difference between
f ðT; 0Þ and f ðT; vc Þ becomes larger, the rate at
which the FM clusters grow increases, and the
dynamical contribution approaches the static one.
Both terms are of the same magnitude at Tp ; and
below the dynamical contribution is even larger
than the static one. A positive slope resembling
‘‘metallic-like’’ behavior is then obtained below
Tp ; although the FM clusters do not percolate.
The history-dependent resistivity slope obtained
after a relaxation process is consistent with the
above described scenario. By ageing at a given
temperature f ðT; vc Þ slowly approaches its equili-
brium value f ðT; 0Þ and the growth dynamics
becomes partially frozen. When the cooling
process is resumed a small dynamical contribution
is obtained, compared with that of the non-stop
cooling process, because of the ‘‘clamping’’ of the
interface. The main contribution to the resistivity
derivative comes then from the static part, giving
rise to the ‘‘insulator like’’ response obtained after
ageing. On further cooling, the frozen-in state is
released, the system falls again in the dynamical
curves (with and without ageing) merge in a single
one.
Summarizing, we have presented crucial evi-
dence of the importance of the cluster dynamics
in the transport properties of the PS manganite
La0.5Ca0.5Mn0.95Fe0.05O3. This fact adds a new
variable to be taken into account to correlate
magnetic and transport properties in compounds
presenting the PS phenomena. When dynamical
effects are present the amount and spatial
distribution of the FM phase (percolative or
not) is insufficient to account for metallic
or insulator behavior. Finally, the ‘‘rejuvenation’’
effect found in the resistivity behavior after
ageing is a novel feature in the physics of
manganites, further investigation about it is being
performed.
Acknowledgements
Project partially financed by CONICET,
! Antorchas and Fundacion
Fundacion ! Balseiro.
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