Journal of Magnetism and Magnetic Materials 547 (2022) 168928

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Journal of Magnetism and Magnetic Materials

journal homepage: www.elsevier.com/locate/jmmm

Evidence of finite magneto-electric coupling in SmFeO3 – PbTiO3

solid solutions
Mehak Arora a, Shubhpreet Kaur a, Kanika Aggarwal b, Sunil Kumar a, Parambir Singh Malhi c,
Mandeep Singh a, Anupinder Singh a, *
a
Department of Physics, Guru Nanak Dev University, Amritsar 143005, Punjab, India
b
Department of Physics, Science Block, S.L.I.E.T, Longowal, Sangrur-148106, Punjab, India
c
Department of Chemistry, Guru Nanak Dev University, Amritsar 143005, Punjab, India

A R T I C L E I N F O A B S T R A C T

Keywords: Present work proposes new insights in the field of multiferroics and its properties. The substitution of SmFeO3 in
Ferroelectrics PbTiO3 (Pb1-xSmxTi1-xFexO3, x = 0.21, 0.22, 0.23, 0.24 and 0.25) over a range of composition has been syn­
Solid state reaction thesized and explored for multiferroicity. The properties such as ferroelectric, magnetic as well as coupling
Multiferroics
between these two have been investigated at room temperature. An in-depth study is carried out to detect the
Magneto-electric coupling
magneto-electric coupling in all the samples through magneto-dielectric, magnetization after electric poling and
magneto-pe. The magneto- pe measurement gives the indication of multiferroic nature of all the samples. The
maximum value of coupling coefficient (γ) and magneto-dielectric response (MDR) of about 10.3 g2/emu2 and
13.09 at 1.5 T respectively for sample × = 0.24 has been achieved by magneto-dielectric properties. Moreover, a
comparative higher shift (~0.061 emu/g) in magnetization has been observed after electric poling.

1. Introduction: memory device applications [6,16–19]. The magnetic behavior in PT is

usually generated by substituting transition metal cations (Mn3+, Fe3+,
Multifunctional materials attract great interest due to their unique Ni2+,Co2+) at Ti4+ site [20]. However, this substitution of transition
functionalities which render them useful for a variety of novel applica­ metal cations is reported to enhance leakage current [20]. It has been
tions [1–3]. Out of all these materials, magneto-electric multiferroics are further established that, the substitution of rare earth ions (R3+) at A-site
being increasingly explored [4,5]. These special type of materials are of PT based materials suppress the leakage current [21,22]. The rare
essentially those which exhibit simultaneous magnetic and electric earth cations are generally substituted into ferroelectric perovskites by
ordering [6]. The presence of partially filled d-orbitals are responsible forming their solid solutions with rare earth orthoferrites (RFeO3, where
for magnetic behavior, while the presence of empty d – orbitals con­ R = Sm, La, Nd) [23,24]. SmFeO3 (SF) is an important rare earth ferrite
tributes to the ferroelectric behavior of multiferroics [7,8]. The multi­ having perovskite structure. Its crystal structure is orthorhombic and
functionality of these materials leads to their significant potential space group is Pbnm [25]. Its Neel temperature (TN) and spin reor­
applications such as memory devices (FeRAMs, MRAMs) [9,10], spin­ ientation temperatures are reported to be ~ 670 K and 480 K, respec­
tronics, sensors and biomedical applications [11–14]. Mixed perovskite tively [26,27]. PT-SF solid solutions offer a potential possibility of
(doping dn ion in ferroelectric material) is one of the widely used realizing efficient multiferroic materials. Few studies have been re­
approach to synthesize high performance multiferroic materials [15]. ported on PT-SF solid solutions. Barranco et al. reported dielectric
Lead titanate (PT) is a very important ferroelectric material which can studies of Pb0.88Sm0.08Ti0.48Mn0.02O3 sample [28]. In another, they re­
be used as a suitable base material for synthesizing mixed perovskite ported structural and electric behavior of Pb0.88Sm0.08TiO3 ceramic
multiferroics. It has high Curie temperature (Tc ~ 490 ◦ C), high ferro­ sample [29]. Increased Sm doping was found to lead to decreased tet­
electric and very high dielectric constant as compared to other ferro­ ragonality in these studies. Further, in these studies, the B- site doping
electric materials. Due to its high dielectric and ferroelectric properties, was either not carried out or was substituted with Mn ions. Also, the
PT based materials show extensive utility for sensors, transducers and ferroelectric and magnetic studies were not reported. Singh et al. [30]

* Corresponding author.
E-mail address: anupinders.phy@gndu.ac.in (A. Singh).

https://doi.org/10.1016/j.jmmm.2021.168928
Received 25 August 2021; Received in revised form 20 November 2021; Accepted 1 December 2021
Available online 9 December 2021
0304-8853/© 2021 Elsevier B.V. All rights reserved.
M. Arora et al. Journal of Magnetism and Magnetic Materials 547 (2022) 168928

influence of Sm and Fe on the magnetoelectric coupling of

Pb1-xSmxTi1-xFexO3 has been supported by a series of experimental
measurements.

2. Experimental:

Solid solutions of Pb1-xSmxTi1-xFexO3 (x = 0.21, 0.22, 0.23, 0.24 and

0.25) were prepared by conventional solid state reaction method. The
raw materials Sm2O3, PbO, TiO2 and Fe2O3 (from Sigma Aldrich, 99.9%
pure) were weighed in stoichiometric proportions and mixed well using
mortar pestle for 2 h. The powder was transferred to bottles containing
acetone and zirconia balls and subject on milling for 24 h. For phase
formation, the mixed powders were calcined at 1000 ◦ C for 12 h in high
temperature furnace. Thereafter, powders were mixed with PVA binder
(2 wt%) to form circular pellets of 10 mm diameter and 1 mm thickness
with the help of hydraulic press. Afterwards, pellets were sintered at
1150 ◦ C (after optimization studies) for 2 h in lead environment using
closed crucible arrangement to reduce weight loss due to lead volatility.
Fig. 1. X-ray diffractograms of Pb1-xSmxTi1-xFexO3 for × = 0.21, 0.22, 0.23, The X-ray Diffraction (XRD) data of these sintered samples were recor­
ded using Shimadzu (Maxima) diffractometer in the range 20 – 80 at a
◦ ◦
0.24, 0.25 samples.
step size of 0.02 and scan speed of 2 /min using Cu Kα anode (λ = 1.54
◦ ◦

Å). The surface morphology of all the samples was investigated using FE-
SEM (Supra 55) from Carl Zeiss at 2 kX magnification with InLens de­
tector. A set up based on Archimedes principle, was used to measure the
density of prepared samples. The electric and magnetic properties were
measured by using automatic PE loop tracer from Marine India and
Vibrating Sample Magnetometer (VSM) EZ9 from MicroSense respec­
tively. The impedance analyzer (E4990A) from KEYSIGHT TECHNOL­
OGIES was used to determine the dielectric properties whereas
magneto-electric studies such as magneto-dielectric, magneto-polariza­
tion and magnetization after electrical poling were made by performing
polarization versus electric field measurement in the presence of mag­
netic field using PE loop tracer.

3. Results and Discussions:

3.1. X- ray Diffraction:

Fig. 2. The splitting of peaks for × = 0.21–0.25 in the range (a) 44.4 – 48.0
◦ ◦

Structural investigation of Pb1-xSmxTi1-xFexO3 samples, (x = 0.21,

and (b) 55 – 60 .
◦ ◦

0.22, 0.23, 0.24, 0.25) has been carried out by X-ray diffraction tech­
nique. The diffractograms of all the samples are shown in Fig. 1. The
reported the multiferroic properties of (Pb0.8Sm0.2) (Ti0.8Fe0.2)O3 solid sharp and intense peaks depict the crystalline behavior of all the sam­
solutions and he observed the effect of processing parameters (sintering ples. The splitting of peaks for × = 0.21–0.24 between 44.4 – 48.0
◦ ◦

temperature) in the prepared samples. He optimized the sintering tem­ (Fig. 2a) and 55 – 60 (Fig. 2b) is suggestive of the tetragonal phase of
◦ ◦

perature at which solid solutions exhibits enhanced multiferroic prop­ these samples. This may be because of the base material PT which
erties whereas structural and magnetic properties of (1-x)Pb possesses tetragonal structure. The figure also indicate that the tetrag­
(Zr0.45Ti0.55)-(x)SmFeO3, 0.10 ≤ x ≤ 0.15 have been reported by Ran­ onal distortion decreases with × and disappears for × = 0.25. This
deep et al. [31]. From these studies, it is clear that PT-SF solid solutions disappearance of tetragonal splitting might be due to the fact that with
have either been explored up to × = 0.20 only. The possibility of increase in × (Sm concentration), the crystal structure transforms into
extending the composition (beyond × > 0.20) still exits. It further needs pseudo cubic at × = 0.25. Thus, visual inspection of the XRD data in
to established that at which value of × , the (PT)1-x – (SF)x system these 2θ ranges suggests tetragonal structure for × = 0.21–0.24. The
transforms to pseudo cubic structure. Similarly, in these studies the further confirmation of structural phase in these samples has been done
coupling between magnetic and electric has either not been explored or by Rietveld refinement using Fullprof software. All the samples from ×
only demonstrated using magneto-pe studies. Magneto-dielectric studies = 0.21–0.25 have been refined using tetragonal phase having P4mm
are more often used to describe the presence of M− E coupling [32]. symmetry. The initial atomic co-ordinates and structural parameters of
However, Catalan et al. [33] reported that the magneto – dielectric different atoms were kept same as those reported by Sunil et al. (having
response (MDR) can also results from factors other than M− E coupling. P4mm symmetry) [34]. Peak shape was modeled using Thompson Cox
Hence, the main aim of the present study is to synthesize and charac­ Hasting function and a sixth order polynomial was used to describe the
terize the multiferroic properties of Pb1-xSmxTi1-xFexO3 (x = 0.21, 0.22, background. Various parameters such as lattice parameters, zero shift,
0.23, 0.24, 0.25) solid solutions using solid state reaction route. The scale factor, refine able atomic positions and Biso were successively

2
M. Arora et al. Journal of Magnetism and Magnetic Materials 547 (2022) 168928

Fig. 3. (a-e) represents the refined X-ray diffractograms of Pb1-xSmxTi1-xFexO3 for × = 0.21–0.25 samples respectively.

Table 1
Rietveld refined parameters of composition Pb1-xSmxTi1-xFexO3 for × = 0.21–0.25 samples.
Composition x ¼ 0.21 x ¼ 0.22 x ¼ 0.23 x ¼ 0.24 x ¼ 0.25

Space Group P4mm (tetragonal) P4mm (tetragonal) P4mm (tetragonal) P4mm (tetragonal) P4mm (tetragonal)
a (Å) 3.9192 3.9190 3.9184 3.9196 3.9218
c (Å) 3.9658 3.9649 3.9581 3.9495 3.9310

Pb/Sm 0/0/0 0/0/0 0/0/0 0/0/0 0/0/0

Fe/Ti 0.5/0.5/0.5038 0.5/0.5/0.51967 0.5/0.5/0.51821 0.5/0.5/0.50822 0.5/0.5/0.50550
OI 0.5/0/0.07350 0.5/0.5/0.04380 0.5/0.5/0.04064 0.5/0.5/0.03907 0.5/0.5/0.03892
OII 0.5/0/0.536 0.5/0/0.48900 0.5/0/0.54084 0.5/0/0.47713 0.5/0/0.51239
V(Å3) Polarization(µC/cm2) 60.9151 60.8951 60.77210 60.6772 60.46080
10.01 9.45 6.34 3.19 1.75
Rexp χ2 (GOF) 7.88 9.08 8.26 8.09 7.92
3.22 3.59 3.98 3.58 3.71

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M. Arora et al. Journal of Magnetism and Magnetic Materials 547 (2022) 168928

refined. The refinement process was continued till the minimization of

discrepancy factors. The refined data for all the samples is shown in
Fig. 3(a-e). The refined data shows a nice match with the experimental
data. All the refined parameters are listed in Table 1.. The variation of c/
a ratio, lattice parameters and cell volume as a function of composition
is given in Fig. 4(a-c). The figure clearly shows that c/a ratio becomes
nearly equals to 1 for × = 0.25 samples which shows cubic nature of the
sample. Also, the lattice parameters (a & c) and cell volume (V) decrease
non - linearly with composition x. This observed decrease may be due to
the mismatch in the ionic radii of Sm3+ (1.08 Å) and Fe3+ (0.60 Å) as
compared to Pb2+ (1.19 Å) and Ti4+(0.605 Å) ions and hence results in
decrease in tetragonality [29,35].

3.2. Morphological studies

The morphological studies of the prepared samples were carried out

using Field emission scanning electron microscopy (FE-SEM) and the
micrographs are shown in Fig. 5(a-e). All the images were recorded at a
magnification 2kX using InLens detector. The well-defined and uniform
grain growth in all the samples can be easily visualized. The ImageJ
software was used for the determination of the grain size. The experi­
mental density of all the samples was measured using a set up based on
Archimedes Principle. The value of the obtained grain size, standard
deviation, experimental density and theoretical density of all the sam­
ples is tabulated in Table 2.. The table clearly shows that grain size and
experimental density increase with increasing SF concentration.

3.3. Dielectric Properties:

The temperature dependent dielectric constant (εʹ) and dielectric loss

(tanδ) for all the samples in the range 303 K ≤ T ≤ 823 K at different
frequencies (1 kHz ≤ f ≤ 100 kHz) were measured. The εʹ and tanδ
versus temperature profiles of all the prepared samples are shown in
Fig. 6(a-e) and 7(a-e) respectively. It is clear from the figure that all the
samples exhibit ferroelectric transition (TcFE), accompanied by dielectric
anomaly in the higher temperature range. Further it found that TcFE
shifts below room temperature (in × = 0.25 sample) from 412 K (in ×
= 0.21 sample). The 6 s2 lone pair present in Pb is responsible for the
tetragonality in PbTiO3 by introducing strain in the lattice. Since XRD
results has revealed that the doping of Sm3+ at Pb2+ reduces the c/a
ratio and has lowered the tetragonality, the effect of lone pair of Pb
spontaneously decreases with increase in doping. Such a change in
structure from tetragonal to cubic is also reflected from phase transition
profile. The decrease in εʹ and tanδ shows that the SF substitution require
less thermal energy for the ferroelectric/ paraelectric phase transition
[36,37]. Therefore, the × = 0.25 sample has shown the value TcFE below
room temperature .The c/a ratio and TcFE have been plotted as a func­
tion of composition (x) and are shown in Fig. 6(f). The calculated values
of the εʹ and tanδ (at TcFE) are mentioned in Table 3.. It is clear from the
table that the maximum value of dielectric constant as well as tanδ
decrease with the composition (x).

3.4. Ferroelectric Properties:

The room temperature polarization versus electric field loops for all
the samples Pb1-xSmxTi1-xFexO3 (for × = 0.21–0.25) were measured and
given in Fig. 8(a-e). It can be clearly seen from the figure that loops are
almost saturated for × = 0.21 and 0.22 sample (Fig. 7 (a,b)) and
increasingly non-saturated for × = 0.23 and 0.24 (Fig. 7(c,d)) and it
became lossy for × = 0.25 sample (Fig. 7(e)). It is worth mentioning
Fig. 4. The variation in (a) c/a ratio, (b) lattice parameters and (c) cell volume
that the polarization in lead based materials is generally attributed to
as a function of composition.
hybridization of titanium and oxygen ions in 3d and 2p states [38]. The
observed shape of the loops indicate that the electric dipoles in × = 0.21
and × = 0.22 samples have an almost instantaneous (nearly ideal)
response to applied ac field whereas the dipoles in × = 0.23 and × =
0.24 samples have a more gradual response. The observed remnant

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M. Arora et al. Journal of Magnetism and Magnetic Materials 547 (2022) 168928

Fig. 5. (a-e) shows scanning electron micrographs for composition Pb1-xSmxTi1-xFexO3 for × = 0.21–0.25 samples.

polarization (Pr) for × has been found to decrease from 17.42 µC/cm2 to
Table 2 3.88 µC/cm2. The decreasing Pr values can be directly correlated with
The value of the obtained grain size, standard deviation, experimental density decreasing tetragonality as shown in Fig. 8(f).
and theoretical density of composition Pb1-xSmxTi1-xFexO3 for × = 0.21–0.25
samples.
3.5. Magnetic properties
Sample Average Standard Experimental Theoretical
Grain Size Deviation Density(gcm¡3) Density
(μm) (σ) (gcm¡3) The room temperature magnetization (M) versus magnetic field (H)
x= 5.411 0.068 6.40 7.94
studies of Pb1-xSmxTi1-xFexO3 (for × = 0.21–0.25) has been carried out
0.21 and the M− H loops are shown in Fig. 9(a-e).The figure clearly reveals
x= 7.673 0.092 6.69 7.96 the presence of non–saturating loops with increasing remnant polari­
0.22 zation (Mr) and coercivity (Hc). By the virtue of substitution of Fe3+ ion
x= 8.285 0.097 7.40 7.97
which has five unpaired electron in d-shell, the samples attributed to
0.23
x= 11.977 0.115 7.69 7.98 magnetic order. The magnetic parameters of × = 0.21–0.25 samples
0.24 retrieved from M− H data are given in Table 4.. Unlike the ferroelectric
x= 12.245 0.150 8.08 7.99 properties, the magnetic properties of these samples exhibit an
0.25 increasing trend. The increase in magnetic behavior of these samples is
directly correlated with increasing Fe content coming from increased SF
concentration. The highest Mr and Hc values have been observed to be

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M. Arora et al. Journal of Magnetism and Magnetic Materials 547 (2022) 168928

Fig. 6. (a-e) gives the temperature dependent dielectric constant (εʹ) of composition Pb1-xSmxTi1-xFexO3 for × = 0.21–0.25 samples and (f) shows the variation of
TcFE and c/a ratio with composition(x).

samples is generally reported by studying the magneto-dielectric

Table 3 response (MDR) of these samples. Therefore, in addition to magneto-
The values of the εʹ and tanδ (at TcFE) of composition Pb1-xSmxTi1-xFexO3 for ×
dielectric studies, we have also performed magneto-polarization
= 0.21–0.25 samples.
(MPE) and magnetization after electrical poling.
Composition TcFE (in K) εʹ (at TcFE) Tanδ (at TcFE) c/a

x = 0.21 412 3942 0.074 1.0118 3.6.1. Magneto-Dielectric properties

x = 0.22 388 3883 0.044 1.0117 The MDR of these samples was determined by performing εʹ vs fre­
x = 0.23 385 2167 0.040 1.0101 quency measurements of × = 0.21–0.24 samples at 0 T, 0.5 T, 1 T, 1.5 T
x = 0.24 356 2000 0.027 1.0076
x = 0.25 – – – 1.0020
fields. The data is shown in Fig. 10(a-d). Also, the measurement has been
repeated several times at regular intervals, and it was found that there is
no variation in data with respect to time. It is clear from the Fig. 10, εʹ
0.341 emu/g and 1.41 kOe in × = 0.25 sample. However, this sample decreases with increasing frequency for given magnetic field and de­
has pseudo cubic (exhibits lossy P-E loop) crystal structure. creases at given frequency with increasing magnetic field in all samples.
The reduction of εʹ with magnetic field at a given frequency is indicative
3.6. Magneto-Electric coupling of negative MDR. The phenomenon of magneto-electric coupling in
multiferroic materials is basically due to the coupling of magnetic and
The coupling between magnetic and electric components of these electric domains. The magnetic domains get strained due to application

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M. Arora et al. Journal of Magnetism and Magnetic Materials 547 (2022) 168928

Fig. 7. (a-e) gives temperature dependent tangent loss (tanδ) of composition Pb1-xSmxTi1-xFexO3 for × = 0.21–0.25 samples.

of external magnetic field which in turns induces the stress on ferro­ lated using Ginzburg- Landau-Dehonshire theory [42] and expressed as:
electric domains by generating electric field. This whole mechanism
β β
results in change in dielectric permittivity of the material after applying Φ = ϕo + αP2 + P4 − PE + αP2 + M4 − MH + γP2M2 (2)
2 2
magnetic field [39,40]. The %age change in dielectric constant with
applied field is termed as magneto-dielectric response (MDR). The MDR where ϕo is reference potential, α, αʹ, β, βʹ and γ are related coupling
values for all the samples were calculated using the following formula: coefficients. The γP2M2 term arises due to coupling between electric and
magnetic components of the material [43]. The magneto-electric
MDR% =
ε’(H) − ε’(0)
X100% (1) coupling results in being proportional to γM2 as:
ε’(0)
ε’ (H) − ε’ (0)
Here, εʹ (H) and εʹ (0) are the values of dielectric constant at applied ∼ γM (3)
ε’ (0)
magnetic field and in the absence of magnetic field, respectively. This
results in lowering of the dielectric constant of the material [41]. It is Here M2 is square of magnetization and γ is the magneto-electric
clear that × = 0.24 sample exhibits highest MDR%. coupling coefficient. The value of γ has been calculated by linear
The thermodynamic potential in multiferroic system can be calcu­ fitting of equation (3) [43]. The obtained MDR values and fitted γ values

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M. Arora et al. Journal of Magnetism and Magnetic Materials 547 (2022) 168928

Fig. 8. (a-e) shows the room temperature polarization versus electric field loops of composition Pb1-xSmxTi1-xFexO3 for × = 0.21–0.25 samples and (f) shows the
variation of Pr and c/a versus composition.

for × = 0.21, 0.22, 0.23, 0.24 have been tabulated in Table 5.. Since, the 3.6.2. Magnetization after electric poling
sample × = 0.24 has shown the maximum MDR value. Therefore, the The impact of electric field poling on the magnetic properties of × =
detailed investigation of MDR vs frequency profile for this sample (x = 0.21–0.24 samples was also investigated in order to check whether the
0.24) only has been carried out in the range − 1.5 T ≤ Field ≤ +1.5 T. electric field induces any magnetic changes in these samples or not. In
The Fig. 11(a,b) represents the effect of positive and negative field on this regard, the pellets were broken into two pieces for each composi­
MDR values. The obtained values of MDR with varying fields at fixed tion. One of these pieces was electrically poled at an applied voltage of 2
frequencies (100 Hz, 1 kHz, and 10 kHz) are shown in Fig. 11(c). It is kV while the other piece was kept unpoled. The sample is mounted in
clear that highest value of γ is observed for × = 0.24 sample (Recall that such a way that the direction of applied electric field while electric
MDR % was also maximum for this sample). The reason for the poling remains same as the direction of applied magnetic field. The first
maximum value of γ for × = 0.24 sample could be its TcFE being just quadrant M− H loops (Virgin Curve) of these unpoled and poled samples
above room temperature. were measured for each composition. The typical plot for × = 0.21–0.24
sample is shown in Fig. 12(a-d). The plots clearly reveal that the virgin

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M. Arora et al. Journal of Magnetism and Magnetic Materials 547 (2022) 168928

Fig. 9. (a-e) shows the room temperature magnetization (M) versus magnetic field (H) graphs of composition Pb1-xSmxTi1-xFexO3 for × = 0.21–0.25 samples.

magnetization of the samples. The difference in magnetization (ΔM),

Table 4 measured at 8000 Oe for × = 0.21, 0.22, 0.23, 0.24 has been observed
The magnetic properties retrieved from M− H data of composition to be 0.04 emu/g, 0.044 emu/g, 0.050 emu/g, 0.061 emu/g respec­
Pb1-xSmxTi1-xFexO3 for × = 0.21–0.25 samples. tively. Clearly, x = 0.24 samples exhibit highest shift in magnetization
Composition Remnant Magnetization (Mr) (emu/g) (Recall that this sample also exhibited highest magneto-dielectric
x = 0.21 0.098 response).
x = 0.22 0.137
x = 0.23 0.201 3.6.3. Magneto-polarization
x = 0.24 0.280 In view of findings by Catalan et al. [33] that magneto-dielectric
x = 0.25 0.341
changes could also be the consequence of factors other than M− E
coupling, we also carried magneto-pe measurements over these samples.
curves do not overlap and the poled samples have higher magnetization In this regard MPE measurement over × = 0.21–0.24 samples were
as compared to unpoled samples. Since in multiferroic materials, po­ carried out in 0 T, 0.5 T, 1 T, 1.5 T. The measurements for (x = 0.21–0.24
larization and magnetization are coupled together. Therefore, the samples) are shown in Fig. 13(a-d). The data clearly reveals that electric
alignment of electric dipoles by electric poling results in enhancement in polarization decreases under the influence of applied magnetic field.

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M. Arora et al. Journal of Magnetism and Magnetic Materials 547 (2022) 168928

Fig. 10. (a-d) shows the plots of εʹ vs frequency measurements of × = 0.21–0.24 samples at 0 T, 0.5 T, 1 T, 1.5 T fields.

4. Conclusion:
Table 5
The obtained MDR values at different fields (0.5 T, 1Tand 1.5 T) and fitted γ
Pb1-xSmxTi1-xFexO3, (x = 0.21, 0.22, 0.23, 0.24 and 0.25) have been
values of composition Pb1-xSmxTi1-xFexO3 for × = 0.21–0.24 samples.
fabricated using solid state reaction method. The tetragonal structure
Composition MDR(%) at MDR(%) at MDR(%) at γ (g2/ with P4mm symmetry has been determined by X- Ray diffraction data
(x) 0.5 T 1T 1.5 T emu2)
for × ≤ 0.24. The FE-SEM results shows the uniform grain growth in all
0.21 2.46 3.28 3.41 5.6 the samples. A good agreement with XRD data has been established by
0.22 1.75 1.88 2.03 7.8
the ferroelectric transition temperature which decrease from 412 K to
0.23 6.10 7.92 10.33 8.1
0.24 11.71 12.76 13.09 10.3 351 K for × = 0.24 (for × = 0.25, TcFE < room temperature). The
decrease in polarization and increase in magnetization has been
explained through the c/a ratio and Fe3+ content respectively. The
This is also indicative of M− E coupling in these samples. The MPE magneto-dielectric and magnetization after electric poling studies sug­
response is usually measured as: gested that sample × = 0.24 exhibits highest magneto-electric response
Pr(H) − Pr(0) of 13.09 at 1.5 T and coupling coefficient (γ) of 10.3 g2/emu2.
MPEresponse = X100% (4)
Pr(0)
CRediT authorship contribution statement
where Pr(H) and Pr(0) represent electric polarization in presence and
absence of magnetic field (H) respectively. The MPE response at 1.5 T of Mehak Arora: Investigation, Data curation, Software, Conceptuali­
× = 0.21, 0.22, 0.23, 0.24 has been measured out to be − 15.46, − 14.13, zation, Writing – original draft. Shubhpreet Kaur: Conceptualization.
− 9.90, − 9.53 respectively. Clearly, x = 0.21 sample exhibits highest Kanika Aggarwal: software. Sunil Kumar: Writing – review & editing.
MPE response. Undoubtly, the obtained results reveal that all the sam­ Parambir Singh Malhi: Visualization. Mandeep Singh: Investigation,
ples have exhibited promising MPE response. Generally, the magnetic Validation. Anupinder Singh: Supervision.
poling induced stress in the material which impose electric field on
electric dipoles and hence variation in polarization comes into picture Declaration of Competing Interest
[44]. With this regard, the sample which has shown maximum polari­
zation in the absence of magnetic poling exhibits more variation under The authors declare that they have no known competing financial
magnetic field. Hence, for × = 0.21 sample, the MPE response has interests or personal relationships that could have appeared to influence
attained maximum value. the work reported in this paper.

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M. Arora et al. Journal of Magnetism and Magnetic Materials 547 (2022) 168928

Fig. 11. The plots (a) and (b) represents the effect of positive and negative field on MDR values and figure (c) represents the variation of the MDR% with range of
magnetic field (− 1.5 T ≤ Field ≤ +1.5 T).

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Fig. 12. The first quadrant M− H loops (Virgin Curve) of unpoled and poled samples of composition Pb1-xSmxTi1-xFexO3 for × = 0.21–0.24 samples.
M. Arora et al. Journal of Magnetism and Magnetic Materials 547 (2022) 168928

Fig. 13. The variation of polarization (P) as a function of applied electric field (E) with and without magnetic field of composition Pb1-xSmxTi1-xFexO3 for × =
0.21–0.24 samples.

Acknowledgements tuned by magnetic fields, Nat. Commun. 4 (1) (2013), https://doi.org/10.1038/

ncomms3051.
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Arora also wishes to thank Rusa-2.0 and DST-SERB for providing [13] C.M. Leung, J. Li, D. Viehland, X. Zhuang, A review on applications of
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