Low-temperature transition to a metallic state in „ La
0.5
Pr
0.5
…
0.7
Ca
0.3
MnO
3
films
N. A. Babushkina and L. M. Belova
*
Institute of Molecular Physics, Russian Research Center ‘‘Kurchatov Institute,’’ Kurchatov Square 1, Moscow, 123182 Russia
D. I. Khomskii
Materials Science Center, University of Groningen, Nijenborgh 4, 9747 AG Groningen, The Netherlands
and Lebedev Physics Institute, Leninskii Prospect 53, Moscow, 117924 Russia
K. I. Kugel
Scientific Center for Applied Problems in Electrodynamics, Izhorskaya Street 13/19, Moscow, 127412 Russia
O. Yu. Gorbenko and A. R. Kaul
Chemistry Department, Moscow State University, Vorobievy Gory, Moscow, 119899 Russia
Received 15 July 1998
The electrical resistivity of epitaxial (La
0.5
Pr
0.5
)
0.7
Ca
0.3
MnO
3
films deposited on single crystalline LaAlO
3
substrates was studied at temperature and magnetic fields ranging from 4.2 to 300 K and from 0 to 3 T,
respectively. On cooling from room temperature at zero magnetic field, the films demonstrate at first the
behavior typical of the charge-ordered CO insulating state, whereas below 40 K they undergo the transition
to a metal-like state with slowly decreasing resistivity. On heating from 4.2 K, the films remain metallic and
their resistivity ( T ) coincides with the cooling curve only at T 80 K. This hysteretic behavior fully repro-
duces itself at repeated cooling-heating cycles. Near the low-temperature transition to a metal-like state the
charge ordering CO is metastable and the resistivity exhibits the relaxation phenomena. The applied magnetic
field as low as H=1 T suppresses CO, and the temperature hysteresis gradually disappears. The ( T ) mea-
surements at nonzero fields reveal a pronounced colossal magnetoresistance effect with the resistivity drop by
a factor exceeding 10
6
at H=3 T. It was also found that relatively small dc voltages ( 3 V) can cause the
switching from CO to a metal-like state within the metastability range in the vicinity of 40 K when the charge
ordering can be rather easily suppressed. Within this range, the current-voltage characteristics are highly
nonlinear, with a memory effect: after switching the sample remains metallic even if the voltage is lowered.
The observed effects are interpreted in terms of strong competition between charge ordering and ferromagnetic
spin ordering. This competition can give rise to different kinds of spatial inhomogeneities involving the
charge-ordered state, which should manifest themselves most clearly in the vicinity of the low-temperature
transition to the metal-like state. The behavior of resistivity before the transition gives indications of the
two-phase state. The transition itself can be a manifestation of a percolative nature of conductivity in this
regime. S0163-18299906209-8
I. INTRODUCTION
Magnetic oxides with metallic conductivity, especially
those characterized by the colossal magnetoresistance
CMR exhibit a whole wealth of interrelated phenomena
such as metal-insulator transitions, orbital or Jahn-Teller
ordering, charge ordering, double exchange, lattice and mag-
netic polarons, etc. see, e.g., Ref. 1. This interplay provides
a better insight into the origin of magnetism, the nature of
electronic states, and transport phenomena in these materials.
The compounds where the transition points corresponding to
different types of ordering are close to each other are of
special interest because small composition changes and rela-
tively weak applied fields can produce rather pronounced
effects.
A good example of such materials is presented by the
doped rare-earth manganites (La
1 -y
R
y
)
1 -x
A
x
MnO
3
( R
=Pr, Nd; A =Ca, Sr. These manganites are very sensitive
to composition variations and can be switched, for example,
from the insulator to the metallic state under effect of pres-
sure, magnetic and electric fields, and even x-ray
irradiation.
2–4
A dramatic manifestation of these phenomena
is the metal-insulator transition induced by
16
O →
18
O iso-
tope substitution.
5–7
The unusual behavior of these manganites stems from the
strong competition between two possible types of states: a
charge-ordered CO state where Mn
3 +
and Mn
4 +
are local-
ized at separate sublattices this state is insulating and usu-
ally antiferromagnetic and a charge-delocalized CD ferro-
magnetic state with a metal-like conductivity. Note that
Mn
3 +
is the Jahn-Teller ion, and the corresponding distor-
tions of MnO
6
octahedra can give rise to the orbital ordering
and to the additional stabilization of the CO state.
Above a certain characteristic temperature both CO and
CD states transform to a charge-localized CL paramagnetic
phase. The CD-CL transformation is accompanied by a sig-
nificant increase in the electrical resistivity, and it is rather
sensitive to the applied magnetic field giving rise to the
CMR. For the CL state, it is usually assumed that charge
carriers are polarons localized due to lattice distortions of the
PHYSICAL REVIEW B 1 MARCH 1999-II VOLUME 59, NUMBER 10
PRB 59 0163-1829/99/5910/69947/$15.00 6994 ©1999 The American Physical Society