Structural, transport, magnetic, and dielectric properties of La1− x Te x MnO3 (x= 0.10 and 0.15)
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Transcript of Structural, transport, magnetic, and dielectric properties of La1− x Te x MnO3 (x= 0.10 and 0.15)
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Journal of Materials ScienceFull Set - Includes `Journal of MaterialsScience Letters' ISSN 0022-2461 J Mater SciDOI 10.1007/s10853-012-7112-9
Structural, transport, magnetic, anddielectric properties of La1−x Te x MnO3(x = 0.10 and 0.15)
Irshad Bhat, Shahid Husain, Wasi Khan& S. I. Patil
1 23
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Structural, transport, magnetic, and dielectric propertiesof La12xTexMnO3 (x 5 0.10 and 0.15)
Irshad Bhat • Shahid Husain • Wasi Khan •
S. I. Patil
Received: 3 October 2012 / Accepted: 22 December 2012
� Springer Science+Business Media New York 2013
Abstract In this study, we have investigated the struc-
ture, temperature-dependent resistivity, magnetization, and
dielectric properties of La1-xTexMnO3±d (x = 0.10 and
0.15). X-ray diffraction analysis confirms the rhombohe-
dral crystal symmetry with space group R3c. For both the
samples, the temperature dependence of magnetization
plots show paramagnetic-to-ferromagnetic phase transition.
The Curie temperature (Tc) and magnitude of magnetiza-
tion increase with the Te concentration. Field-dependent
magnetization produces the asymmetric hysteresis loop
that has been attributed to the magneto crystalline anisot-
ropy induced by lattice distortion and the rare earth spin
coupling at room temperature. Temperature-dependent
resistivity plots exhibit metal–insulator transition (MIT)
and charge-ordering state. These plots have been fitted
using variable range hopping model, and the density of
states [N(EF)] has been estimated. Magnetoresistance is
measured as a function of temperature in the field of 1T,
5T, and 8T. The dielectric constant shows an anomaly near
MIT. The dielectric constant exhibits a peaking behavior
with the applied frequency and the temperature dependence
of dielectric constant attains colossal values at high
temperatures.
Introduction
Perovskite manganites Ln1-xKxMnO3 (Ln = rare earth
ion; K = divalent or tetravalent ions) have been a subject
of vivid interest in recent years because of their exotic
electronic and magnetic properties [1–5]. Most interesting
properties of the manganese perovskite arise from the
competition between ferromagnetic (FM) double exchange
(DE) and antiferromagnetic (AFM) super exchange, with
the ratios of these competing interactions being determined
by intrinsic parameters such as doping level, average ‘‘A’’
size cation radius hrAi, cation disorder, and oxygen stoi-
chiometry. These materials exhibit high magnetoresistance
for certain composition ranges [5]. Besides the colossal
magnetoresistance (CMR), charge-ordering (CO) phe-
nomena [6] has also attracted a lot of interest. Earlier
studies show that CO state and the concomitant spin and/or
orbital-ordering (OO) are favored when the long range
coulomb interaction and/or a strong lattice interaction due
to Jahn–Teller (J–T) distortion overcomes the kinetic
energy of the electron [7–9]. Wider ‘‘eg’’ bandwidth, i.e.,
larger average A site radius (rA) favors lower TCO because
the mobility of the itinerant electrons through the lattice is
higher, while narrower bandwidth induces an opposite
trend. Such, CO phenomenon has been observed when the
concentration of the charge carriers takes the rational val-
ues of the periodicity of the crystal lattice [10–12]. In the
picture of Millis et al. [13] the Jahn–Teller effect leads to
the opening of a gap at the Fermi level, which together with
the DE gives at least a qualitative description of the
experimental observation. The strong electron–phonon
interaction arising from the Jahn–Teller splitting of the
‘‘Mn’’ d level plays a crucial role. Although optical,
magnetic, thermoelectric power, dc conduction measure-
ment studies on these materials suggest a high possibility
I. Bhat (&) � S. Husain
Department of Physics, Aligarh Muslim University,
Aligarh 202002, India
e-mail: [email protected]
W. Khan
Department of Applied Physics, Z.H. College of Engg. &
Technology, Aligarh Muslim University, Aligrah 202002, India
S. I. Patil
Department of Physics, University of Pune,
Ganeshkhind 411007, Pune, India
123
J Mater Sci
DOI 10.1007/s10853-012-7112-9
Author's personal copy
of conduction due to a hopping process of small polarons
[14–16].
In general, doping of LaMnO3 with divalent or tetra-
valent ions derives the manganese ions into a mixed
valence state. The effect of tetravalent ion doping at La site
of the LaMnO3 like Ce4?, Zr4?, Sn4?, and Te4? has been
reported earlier [17–24]. These reports include x-ray pho-
toemission spectroscopy (XPS) and Hall effect measure-
ments have revealed that Te ions are in the tetravalent state
and the manganese ions exist in a mixed valence state of
Mn2? and Mn3? in La1-xTexMnO3 (x = 0.10 and 0.15)
[19–21]. The introduction of Te drives manganese Mn3?
ions of LaMnO3 into a Mn2? ions, which is equivalent to
introducing electron into the eg band. The mixed phase of
Mn3?/Mn2? is the key component to understand the CMR,
charge-ordering effects, and the transition from the FM
metal to paramagnetic (PM) semiconductor in such
systems.
The transition metal oxides (manganites) of the type
ABO3 where (A = rare earth ion and B = transition metal
ion) also show ferroelectric behavior [25–27]. Large
dielectric constants are expected for ferroelectrics in a
narrow temperature range close to transition temperature or
in systems where we observe dielectric response based on
the mechanism of hopping of charge carriers that diverge
toward low frequencies. Recently, a new class of materials
exhibiting a colossal dielectric constant (CDC) (e0[ 103)
has also gained considerable attention because of its
application in high-e0 electronic materials, such as random
access memories. Fundamental interest was initiated by the
observation of CDC behavior in some high Tc compounds
[28–30]. During the last decade, similar observations of
CDC behavior have been reported in an increasing number
of materials, such as transition-metal oxides [31–35].
Several theoretical and experimental results previously
reported have claimed that internal barrier layer capacitor
(IBLC) [36–39] and surface barrier layer capacitor (SBLC)
[40, 41] are the two special influential factors giving rise to
the CDC behavior. It is believed that such barrier layers
may get developed at grain boundaries or at the planar
defects and at the interface between the metallic electrode
and the bulk sample, giving rise to the formation of
Schottky barriers.
The role of grain boundaries is expected to be drastically
enhanced in compounds with a mixed-phase character, not
only owing to their inherent character, but also because
they can act as accumulative pinning centers for structural
defects. Earlier studies [42, 43] on low-frequency dielectric
properties of doped manganite reveal that these properties
are affected by barrier-layer capacitor microstructure, cre-
ated because of the oxidation of grain boundaries, which
forms an insulating layer. Various theories have excluded
the possibility of the intrinsic origin of high dielectric
constant [44, 45]. These studies conclude that the internal
inhomogeneity plays the major role. It is suspected that
such inhomogeneity arises from crystal twinning or some
internal domain boundaries. In view of the above, we have
focused on the problem to study the structural, transport,
magnetic, and dielectric properties of Te-doped LaMnO3.
It is one of the lesser studied materials as far as the
dielectric properties are concerned.
Experimental
The standard solid-state reaction route is used to prepare
the samples of La1-xTexMnO3 (x = 0.10 and 0.15). Stoi-
chiometric amounts of La2O3, TeO2, and MnO2 are mixed,
ground, and heated at 1050 �C for 20 h. After first heat
treatment, these samples are ground again and sintered at
1100 �C, with two intermediate grindings. The powder
x-ray diffraction pattern is recorded using a x-ray diffrac-
tometer with Cu Ka (k = 1.5406 A) radiation at room
temperature. Magnetization versus temperature measure-
ments and the magnetic hysteresis measurements were
carried out using vibrating sample magnetometer. The
resistivity as a function of temperature is measured with
four-probe technique. The dielectric constant measurement
is performed on the Novo control, Alfa-A high-perfor-
mance frequency analyzer. The samples were palletized in
disk shape at a pressure of 6 ton/cm2, and silver paste was
sputtered on their surfaces to ensure good electrical contact
with the electrode capacitor.
Results and discussion
Structural analysis
The room temperature x-ray diffraction (XRD) patterns
confirmed single-phase nature of the samples. The com-
pound La1-xTexMnO3 (x = 0.10 and 0.15) has a rhombo-
hedral crystal structure with space group R3c. The crystallite
sizes of the samples calculated using Debye–Scherrer’s
formula are found to be 346 and 377 A, for x = 0.10 and
0.15, respectively. The structural parameters were refined by
the standard Rietveld technique [46]. The experimental and
calculated XRD patterns for La0.9Te0.1MnO3 and
La0.75Te0.15MnO3 with conventional Rietveld parameters
are shown in Fig. 1. The lattice parameters and the unit cell
volume of both the samples are tabulated in Table 1.
The unit cell volume increases with Te concentration.
This is consistent with the earlier reports [19–21, 47] since
it is known that the radius of Te4? is about 0.097 nm and
that of the La3? is 0.1216 nm. The part of substitution of
Te4? ion for La3? ions should cause the reduction in the
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ionic size hrAi of the rare earth ion, which will cause the
cell constriction and the distortion in the MnO6 octahedron,
resulting in the decrease of Mn–O–Mn bond angle from
180�. However, we have found that an increase in the Mn–
O–Mn bond angle from 160.7� to 163.4� and small changes
in Mn–O bond lengths (dMn–O * 1.96 for x = 0.10 and
dMn–O * 1.95 for x = 0.15) with the increasing Te con-
centration result in the increase in volume. Another reason
for this increase may be the oxygen stoichiometry (d) in
La1-xTexMnO3±d, and consequently the respective valence
states of ions present at A and B sites.
Figure 2 shows the Fourier transform infrared (FTIR)
spectrum for La1-xTexMnO3 (x = 0.10 and 0.15) at room
temperature. Since rare earth manganites of type (ABO3),
such as LaMnO3, are known to have a distorted crystal
structure with Mn (central atom) octahedral surrounded by
its nearest neighbor six O ions. It is believed that MnO6, in
its ideal form has six vibrating modes, two of which are
reported to be IR active [48–50].
The irrational bands present around 606 and 418 cm-1 for
La0.9Te0.1MnO3 and the bands 607 and 409 cm-1 for
La0.75Te0.15MnO3, are the characteristics of the perovskite
structure [48]. The bands at 606 and 607 cm-1 are attributed
to the Mn–O stretching vibrations mode (ts), and the bands at
418 and 409 cm-1 are corresponding to the Mn–O–Mn
deformation (bending) vibrations mode (tb). We have
observed a shift in the tb with the increase in Te doping. The
tb mode shifts slightly toward the lower wavenumber (cm-1)
region, and a very small shift of 1 cm-1 toward higher
wavenumber is observed in ts. Since both the bands are
sensitive to the octahedral distortion in MnO6, the lowering
of symmetry arising from the Jahn–teller effect results in
Mn–O–Mn bond length to vary which produces the slight
shift in bending vibration mode tb. The relative intensity of
two vibrating modes is influenced not only by the distortion
surrounding the MnO6 octahedron, but also by the local
fluctuation of the electron density at the A (La) site.
Magnetization
Fig. 3 shows the temperature dependence of magnetization
plots for Te-doped LaMnO3. The Curie temperatures (Tc) are
found to be 210.15 and 211.43 K for x = 0.10 and x = 0.15
concentrations, respectively. The increase in Tc with the
increasing Te content may be attributed to the strengthening
of the interaction of the lattice constriction and bond angle
increase, which strengthens the FM coupling between Mn
Fig. 1 X-ray diffraction patterns of La0.9Te0.1MnO3 and La0.8Te0.2MnO3.
The experimental data points are indicated by stars, and the calculated
profile by solid traces. The lowest curve shows the differences between
the experimental and the calculated data. The vertical bars indicate the
expected reflection positions for rhombohedral structure
Table 1 Lattice parameters and unit cell volumes (V) of
La1-xTexMnO3 (x = 0.10 and 0.15) at room temperature
Concentration (x) Lattice parameters V (A´
)3
a (A´
) c (A´
)
x = 0.10 5.511 13.321 350.36
x = 0.15 5.514 13.325 350.84
Fig. 2 FTIR spectra for La1-xTexMnO3 (x = 0.10 and 0.15) samples
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ions. The values of metal–insulator transition (MIT) tem-
perature Tp for both the compositions obtained from the
resistivity measurement are lower than the values of corre-
sponding Tc; this could be due to the increase of carrier
density with the increasing Te concentration and is a com-
mon characteristics of electron-doped compounds [17, 51].
Another reason could be the size effects at rare earth site
(A site) and the variation of Mn–O–Mn bond angle, since the
substitution of Te at rare earth site varies hrAi and causes the
distortion in the MnO6 octahedron; consequently, the
Mn–O–Mn bond angle increases, which may influence the
FM-DE and AFM super-exchange interaction differently,
and hence the increment in Tc. The magnetization has dras-
tically increased with Te concentration, and can be attributed
to the competition between the DE and the core spin inter-
action. This competition leads to the parallel alignment of
core spins as the doping level increases. The exchange
interaction of the Mn–Mn depends on the bond angle and the
bond length. The decrease of Mn–O length and increase of
Mn–O–Mn bond angle will make Mn–Mn exchange inter-
action stronger, leading to a higher Tc and higher magneti-
zation value. The decreases in magnetization at lower
temperatures signifies the existence of AFM-insulating
clusters along with the FM metallic clusters, which results in
the magnetic inhomogeneity and domain wall [52, 53].
The hysteresis curves for magnetization versus magnetic
field at room temperature are shown in Fig. 4. The asym-
metric reversal magnetization has been noticed in our
samples La1-xTexMnO3 (x = 0.10 and 0.15), which may
indicate the presence of FM and AFM clusters, since such
coexistence of FM and AFM domains is often the cause for
the asymmetric magnetization hysteresis and their inter-
action can strongly influence the reversal mechanism of the
magnetization, modifying nucleation and annihilation of
the vortex. Our results show a shift of the hysteresis loop
toward negative fields. The magnetization reversal mech-
anism depends upon the orientation of the cooling field
with respect to the twinned microstructure of the antifer-
romagnet, and on whether the applied field is increased to
(or decreased from) a positive saturation field. The reversal
magnetization occurs via either domain wall motion or
magnetization rotation on opposite sides of the same hys-
teresis loop. We believe that the asymmetric magnetization
in both the samples may be due to the magneto crystalline
anisotropy [54–56] induced by lattice distortion and the
rare earth spin coupling at room temperature. There are two
aspects of lattice distortion in the context of the magnetic
anisotropy of manganites: one is the global strain, which is
a general feature for many manganites and determines the
anisotropy of the uniform rotation of the spin magnetic
moments; and the other one is the alternating local dis-
tortion of the magnetic anisotropy energy known as one of
the common mechanisms responsible for the non-collinear
magnetic order. If La spin coupling has a contribution to
the magnetic anisotropy, then it is most likely due to the
interaction of La, 4f electron spin with 3d-electron Mn
spin, which weakens the magnetization as well as induces
the magnetic anisotropy. The charge-ordering and mag-
netic anisotropy, which is induced by lattice distortion and
the rare earth spin coupling at room temperature, could
behave in an AFM-ordered or FM-insulating state. We
have observed an enhancement in the magnetization with
the increasing Te concentration.
Fig. 3 Magnetization versus temperature plots for a La0.9Te0.1MnO3
and b La0.85Te0.15MnO3 samples
Fig. 4 The magnetization versus field at room temperature for
a La0.9Te0.1MnO3 and b La0.85Te0.15MnO3 samples. The insets show
the enlarged view for the same
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Transport Analysis
The temperature-dependent resistivity q(T) plots for
La1-xTexMnO3 (x = 0.10 and 0.15) are shown in Fig. 5.
On decreasing the temperature, these compounds first
undergo a PM (insulating) to FM (metallic) phase transi-
tion at transition temperatures Tp = 203 and 209 K,
respectively, then resume the semiconducting behavior. A
wide charge-ordered region centered between 70 and
140 K is observed in both the samples which could be due
the coexistence of the AFM and FM spin clusters, and the
competition between them yields charge-ordering charac-
teristics. Such phase coexistence features are explained in
the framework of electronic phase separation scenario,
predicted for the manganites [57]. This behavior is attrib-
uted to the structural inhomogeneous characteristic of the
strongly correlated electronic systems that govern the
electric and magnetic properties. The insulating behavior
results from the single ion J–T distortion as well as the
blocking of hopping by strong Hund’s coupling to the
paramagnetically disordered Mn spins. A shift in the MIT
and charge-ordering transition temperature (TCO) is
observed with the increasing Te doping amount. It is well
documented in the literature [58, 59] that the strong
increase of the resistivity with decreasing temperature can
be described by the Mott’s variable range hopping (VRH)
model [60–62]. In this model, it is assumed that the charge
carriers move along a path described by the optimal pair
hopping rate from one localized state to another. To
investigate the electronic transport mechanism, we have
fitted the resistivity q(T) data with thermally activated
conduction (TAC) model, q(T) = q0(T) exp(Ea/kBT);
Small polaron hopping (SPH) model, q(T) = q0(T) T
exp(Ea/kBT); and three-dimensional Mott’s VRH model,
q(T) = q0(T) exp(To/T)1/c—with c = 2 or 4—predicting
the charge transport by tunneling of electrons or holes [63];
c = 4 has been considered as indicative for isotropic
charge transport. Efros and Shklovski [64, 65] proposed an
alternative explanation for c = 2 in Mott’s three-dimen-
sional model where the coulomb interaction between the
charges is taken into account.
We have found that VRH model is much superior to
other models in describing the carrier transport in our
system. The fitted results are shown in Fig. 6 a, b. We have
found VRH model responsible for the transport properties
below (T [ TCO) as well as above (T \ TCO) charge-
ordered regions. The most convincing results (straight line)
are observed for log q against 1/T1/4 below MIT in both the
samples, which are typical for three-dimensional VRH
Fig. 5 lnq(T) versus T plots for La1-xTexMnO3 (x = 0.10 and 0.15)
samples
Fig. 6 lnq(T) versus 1/T1/4 plots for a La0.9Te0.1MnO3 and
b La0.85Te0.15MnO3 samples. Solid line shows Mott’s VRH model
fitting, and the inset shows the VRH fitting below the transition
temperature
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model. The value of resistivity increases above the arbi-
trary temperature (TA) with the temperature decreasing
further. A small metallic region has been observed between
203 and 196 K for La0.90Te0.10MnO3 and between 209 and
198 K for La0.85Te0.15MnO3 before resuming semicon-
ducting behavior with the temperature decreasing further. It
is a known fact that VRH transport behavior does require
the appearance of random potential; hence, due to the large
anisotropic lattice distortion of MnO6 octahedron in
La1-xTexMnO3 (x = 0.10 and 0.15) caused by charge
ordering, it will trap the electrons below TCO, and hopping
across the grain boundaries contributes toward transport
process at low temperatures. The To (characteristic tem-
perature) occurring in the VRH relation can be related to
the carrier localization length, using the expression
To = 24/(kBN(EF)pL3) [66]. The value of the localization
length should be comparable to Mn–O bond distance for
VRH type of conduction; in the present case, the mean
Mn–O bond lengths for x = 0.10 and 0.15 calculated from
XRD data are dMn–O = 1.96 A and dMn–O = 1.95 A,
respectively. The values of To and density of states N(EF)
are tabulated in Table 2. It is clear from the Table 2 that
the characteristic temperature (To) shows the minimum
value in charge-ordered region for both the samples, which
indicate less-disordered state and hence attains higher
values of density of states near Fermi level N(EF). The Chi-
square values indicate the quality of the fitted data. The
magnetoresistance as a function of temperature is measured
in the presence of the magnetic field 1T, 5T, and 8T as
shown in Fig. 7. Sharp and broad peaks can be attributed to
the coexistence of the AFM and FM clusters, contributing
to the spatially metallic and insulating areas in the studied
temperature range, which is believed to occur in materials
where the electron density is commensurate to the number
of lattice sites. Under the applied field, the resistivity gets
suppressed, especially near the (I–M) transition as well as
in the charge-ordered region. Under 8T magnetic field, the
maximum MR ratios reached are about 70 and 67 % for
x = 0.10 and 0.15 concentrations, respectively, in the
vicinity of charge-ordered region.
Dielectric Properties
Low-frequency dielectric properties of doped manganites
have been the subject matter of earlier studies [67, 68]. We
have studied the effects of frequency and temperature
dependence on dielectric functions for both the samples.
Table 2 Values of
characteristic temperature To,
density of states at the Fermi
energies N(EF), and Chi-square
(v2) determined from fitting of
resistivity temperature data for
La1-xTexMnO3 (x = 0.10 and
0.15)
Concentration (x) Temperature ranges To (K) N (EF) (eV-1 cm3) 9 1020 v2
x = 0.10 Below Tp 560 9 105 2.09 0.9996
T \ Tco 485 9 104 24.2 0.9959
Ta [ T [ Tco 7.86 1.49 9 107 0.9800
T [Ta 437.71 2.68 9 105 0.9996
x = 0.15 Below Tp 660 9 105 1.78 0.9996
T \ Tco 677 9 104 17.4 0.9952
Ta [ T [ Tco 7.7 1.52 9 107 0.9240
T [ Ta 1923.48 6.11 9 104 0.9965
Fig. 7 Temperature dependence of magnetoresistance (MR) with
magnetic fields of 1T, 5T, and 8T for a La0.9Te0.1MnO3 and
b La0.85Te0.15MnO3
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Figs. 8 and 9 show the variation of dielectric constant with
frequency and temperature, for La1-xTexMnO3 (x = 0.10
and 0.15). Dielectric constant e0 can be expressed as
e0 = ea ? ed ? el, where ea is associated with the dis-
placement of ionic charge distribution relative to their
nuclei and contribution at higher frequencies; the lattice
contribution (el) arises from displacement of ions and their
charge distributions; and ed gives the dipolar contribution
associated with the charge carrier hopping. Dielectric
constant as a function of frequency shows a peak behavior;
e0 first decreases for specific low-frequency region up to
2 kHz, above which a dispersion maxima starts to develop
giving a broad peak between 400 kHz and 1.25 MHz and
attains the colossal values of dielectric constant (CDC).
The height of the dispersion peak shows a decrease with
the decreasing temperature, the signature of dipolar relax-
ation. The interface and the grain boundaries control the
behavior of e0 at lower frequencies: the thinner the grain
boundary layers, the higher the value of e0. The peaking
behavior of e0 with frequency can be explained using
Rezlescu model [69]. According to this model, the peaks of
e0 curves can be ascribed to the presence of collective
contribution to the polarization from two different types of
charge carriers—both intrinsic and extrinsic effects con-
tribute to the overall dielectric response. Intrinsic effects
are related to charge condensation that takes place in some
systems with cations of variable valances such as Mn3?–
Mn2?/Mn4? and Ni2?–Ni3? [70, 71]. External factors lead
to the interfacial polarization produced in grain boundaries
and contact sample electrodes [72]. An increase in
dielectric constant has been observed with the increasing
temperature as depicted in Figs. 8b and 9b, suggesting the
thermal effects on charge carriers which orient themselves
after getting liberated, thereby enhancing the space-charge
Fig. 8 a. Frequency dependence of dielectric constant (e0) at
different temperatures for La0.9Te0.1MnO3. b Temperature depen-
dence of the dielectric constant (e0) at different frequencies for
La0.9Te0.1MnO3. Inset shows the enlarged view near transition region
Fig. 9 a Frequency dependence of dielectric constant (e0) at different
temperatures for La0.85Te0.15MnO3. b Temperature dependence of the
dielectric constant (e0) at different frequencies for La0.85Te0.15MnO3
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polarization and hence the overall dielectric constant. We
have observed anomaly in dielectric constant near the MIT
temperature. A decrease in dielectric constant near MIT
has been observed, and above which, it rises rapidly to
higher values, upon decreasing the resistivity further,
suggesting a correlation between the two phenomena. It is
pertinent to mention that the higher values of the dielectric
constant is attributed mainly in space-charge polarization
mechanism, known to predominate in heterogeneous
structures, in which a material is assumed to be composed
of different regions (grain and grain boundaries).
The conductivity of grains is considered relatively better
than that of grain boundaries because the charge carriers
encounter different resistances so that accumulation of
charges at separating boundaries occurs, and hence, the
dielectric constant values increase. Earlier reports interpret
high dielectric responses like CDC as an artifact emerging
from Schottky effect at the electrode contacts [69].
M. Sanchez-Andjar et al. [73] suggest the dielectric
behavior as a consequence of the formation of polar entities
at the temperature of the charge condensation, due to an
asymmetric charge distribution, intermediate between site-
centered and bond-centered types as described by Efremov
et al. [74] for real half-doped manganites.
Loss tangent
Figure 10 shows the temperature dependence of loss tan-
gent at different frequencies. We have observed high
dielectric loss, with relaxation dispersion peaks centered at
different temperatures for both the samples, which is the
direct consequence of the semiconducting nature of these
Fig. 10 Temperature dependence of loss tangent (tand) at different frequencies for a La0.9Te0.1MnO3; and b La0.85Te0.15MnO3 samples
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materials, having high dc resistivity. These loss peaks can
be discussed within the framework of the Maxwell–
Wagner model which refers to interfacial polarization
occurring in electrically inhomogeneous systems [75]. The
presence of oxygen non-stoichiometry in our samples can
be thought of as a possible source of inhomogeneity. It is
known that when an electric current passes through inter-
faces between two different dielectric media, because of
their different conductivities, surface charges pile up at the
interface [76], and the system shows a Debye-like relaxa-
tion process under an external alternating field [75]. Dou-
ble-dissipation peak behavior can be seen at the
frequencies of 1.25 MHz, 625 kHz, 312 kHz, and 156 kHz
for La0.90Te0.10MnO3, and can be interpreted by the hop-
ping of localized carriers and the thermally excited relax-
ation processes. We have noticed only single peak at low-
frequency toward low-temperature region, but with the
increase in frequency of the applied field above 7800 Hz, a
secondary dissipation peak starts to develop toward the
higher-temperature region, thereby minimizing the char-
acteristic dissipation peak formed at low-temperature
region. While, in the case of La0.85Te0.15MnO3, a different
scenario has been observed: the characteristic height of the
peak starts to develop with the decrease in frequency, and a
complete phase transition can be observed at 155 kHz near
MIT in La0.85Te0.15MnO3. The dissipation energy (loss)
decreases with the increasing frequency of the applied
field. The decrease in loss tangent with the increasing
frequency can be attributed to the dc conductivity. The loss
tangent increases with the increasing concentration as
depicted in Fig. 10. It should be noted that the temperature
at which the dielectric constant begins to increase rapidly is
approximately equal to that at which the dielectric loss
dispersion starts.
Fig. 10 continued
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Conclusion
We have systematically investigated the structural, mag-
netization, electronic transport, and dielectric properties for
La1-xTexMnO3 (x = 0.10 and 0.15). The samples are
found to be in single phase as confirmed by Rietveld
analysis. Both the samples exhibit the PM–FM phase
transition accompanied by MIT temperature. However,
with further decrease in temperature, the samples show the
insulating phase characteristics accompanied with the
charge-ordered region at low temperature. The Curie
temperature Tc, the charge-ordering transition temperature
TCO, and the MIT have been found to increase with Te
doping. Asymmetric magnetization and the shifting in
hysteresis loop have been noticed. The VRH model has
been found useful in discussing the transport properties
(resistivity). Dielectric constant exhibits a peak response
with frequency and attains colossal values at higher tem-
peratures for both the samples.
Acknowledgements The authors are greatly thankful to the UGC-
DAE Consortium for Scientific Research, Indore and the Center ofExcellence in Materials Science (Nanomaterials), Department of
Applied Physics, Aligarh Muslim University, Aligarh for providing
the experimental facilities. The authors are also thankful to Dr. R.K.
Kotnala, the National Physical Laboratory, New Delhi for providing
facilities in respect of magnetic measurements.
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