Applied Physics A (2023) 129:779

https://doi.org/10.1007/s00339-023-07052-8

Analysis of interphase magnetoelectric coupling

in ­Bi0.9La0.1FeO3–MgFe2O4 composites
Muhammad Hamza Maqbool1,2 · Zaffar Iqbal3 · Sidra Zawar2 · Ayesha Khalid1 · Shahid M. Ramay4 · Shahid Atiq1

Received: 10 July 2023 / Accepted: 5 October 2023 / Published online: 18 October 2023
© The Author(s), under exclusive licence to Springer-Verlag GmbH, DE part of Springer Nature 2023

Abstract
Multiferroic materials have grabbed great attention of researchers due to their distinctive feature of magnetoelectric coupling
with vast applicability in advanced multifunctional devices. To achieve considerable value of magnetoelectric coupling, the
samples of La-doped ­BiFeO3 and ­MgFe2O4, which were initially synthesized via hydrothermal method, were then embedded
into the (1–x)Bi0.9La0.1FeO3 + xMgFe2O4 composites using a ball-milling process. The presence of rhombohedrally distorted
cubic perovskite structure of La-doped ­BiFeO3 having R3c space group symmetry and spinel cubic structure of ­MgFe2O4
with Fd-3m space group symmetry was confirmed using X-ray diffraction analysis. The microscopic images of the composite
samples show a slight variation in grain size with least porosity observed for the composite of x = 0.5. The elemental map-
ping assured the presence of all elements in the prepared composites that were in accordance with the stoichiometric ratios.
The ferroelectric analysis exposed that the x = 0.2 composition had shown the highest efficiency of 52% for energy storage
devices. The linear magnetoelectric response of the composite samples along with small values of switching charge density
observed at x = 0.3 inferred this particular composite quite preferable for data storage applications.

Keywords Multiferroics · Bi-phasic composites · Magnetostriction · Piezoelectric · Data storage devices

1 Introduction temperature in C ­ r2O3 was much smaller than its ferroelectric

Multiferroic materials exhibit two or more ferroic orderings
simultaneously within the same phase, and particularly,
the combination of ferroelectric and ferromagnetic order-
ings, that have gained significant impact in multifunctional
devices [1]. Multiferroic materials have variety of applica-
tions that include micro-sensors, ME sensors, microtrans-
ducers, memory storage devices, and spintronics [2–5].
The reason behind these vast applications is the magneto-
electric (ME) effect which was first observed in C ­ r2O3 by
Dzyalonshinskii-Moria. However, the magnetic transition
* Shahid Atiq
satiq.cssp@pu.edu.pk
1
Centre of Excellence in Solid State Physics, University
of the Punjab, Lahore, Pakistan
2
Department of Physics, University of Jhang, Jhang, Pakistan
3
Department of Physics, University of Houston, Houston,
USA
4
Physics and Astronomy Department, King Saud University,
Riyadh, Saudi Arabia
transition temperature [6, 7]. ­ABO3-type perovskite family
of multiferroic materials having rare-earth or alkaline met-
als at A site and transition metals at B site in their structure.
However, it is significant to mention that ­BiFeO3 (BFO) is
a sole single-phase ABO3-type perovskite with both ferro-
electric and anti-ferromagnetic orderings simultaneously in
a single phase above room temperature (RT) [8]. In BFO,
the origin of ferroelectricity is the stereochemical activity
of ­6s2 loan pair of ­Bi3+ ions with high Curie temperature
(TC = 1103 K). While, anti-ferromagnetic behavior comes
from unpaired 3d electrons of F ­ e3+ ions having Neel’s tem-
perature (i.e., TN = 643 K) [9, 10]. Despite all these specific
characteristics, there are some limitations associated with
BFO, which hinders its commercialization for device fab-
rication [11, 12]. These limitations are due to leaky ferro-
electric behavior and weak magnetic behavior of BFO based
on its intrinsic G-type anti-ferromagnetism that results into
insignificant ME coupling [13, 14]. Although the research-
ers have tried to resolve this issue by doping or substituting
both A and B sites of BFO with different transition and rare-
earth metals, that has somehow lessened its leakage current

13
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779 Page 2 of 11
shortcomings, yet these alterations could not address the
issue of weak ME coupling.
Many methods like strain engineering and chemical
substitution were suggested to tune the magnetic response
and ME coupling in BFO, but these approaches worked up
to limited extent [15, 16]. Partial substitution of transition
metals like Mn, Ni, Cu, and Zn in BFO not only affects the
magnetic features but also plays a significant role in reducing
the leakage current and improving the structural stability of
BFO [17]. As a matter of fact, ferroelectricity is generated
due to empty or completely filled d-shell orbitals while fer-
romagnetism requires partially filled d-shell, so it seemed
quite impossible to achieve both these attributes in single-
phase materials. Therefore, a practical approach to achieve
significant ME coupling is mediated by making BFO-based
composites with other compounds to achieve considerable
ME coupling for multifunctional devices. Since BFO is a fer-
roelectric material with an anti-ferromagnetic ordering, it is
mandatory to have counterpart ferro- or ferrimagnetic phase
within a single composition that ultimately tends to enhance
ME coupling. Among magnetic materials, ferrites are of
great interest due to their enormous magnetic properties.
Atuchin et al. used flux crystal growth method to synthesize
barium hexaferrite (­ BaFe12O19), which belongs to MFe12O19
ferrite family having magnetoplumbite crystal structure
[18]. Vinnik et al., utilized solid-state reaction method for
synthesizing pure ­BaFe12O19 and Ti-doped ­BaFe12-xTixO19
(x = 0.5, 1, 2) solid solutions [19]. Using a sol–gel auto-
combustion approach, Naheed et al. synthesized Y-type
hexagonal ferrite samples having a chemical composition
of ­Ba2Co2Fe12−xPrxO22 (x = 0.0, 0.025, 0.05, 0.075, and 0.1)
[20]. Due to their thermal and chemical stability, relatively
high Curie temperature, high doping level, and prominent
magnetic, catalytic, and electronic properties, they are used
in various engineering and energy technologies, micro-
electronics, radio technology, and modern day applications
like microwave communication, inductor devices, storage,
and recording components [18, 19]. Sharma et al. used a
low-cost sol–gel auto-combustion process to fabricate and
characterize the nano-crystalline S ­ m0.96Ce0.04Fe1−xNixO3
samples with x = 0, 0.1, 0.2, and 0.3. Their results showed
that the Urbach energy increased with increasing Ni con-
tents and there was a considerable red shift in the energy
band-gap. As Ni content was increased, remanent magneti-
zation, coercive field, and maximum magnetization values
increased, as well [21]. ­MgFe2O4 (MFO) is an n-type soft
magnetic material having spinel structure and has its appli-
cations in the field of photoelectrical, magnetic technologies
and sensors [22–24]. It shows a relatively high resistivity in
comparison with other ferrites of this kind [25]. It is used
as a magnetic component in multiferroic composites, which
makes it easier to control electric polarization when using
weak magnetic fields. Hence, a composite of ­BFO3 and
13
M. H. Maqbool et al.
MFO was therefore regarded as appropriate components for
muliferroic materials in terms of ferroelectric and magnetic
characteristics [26]. Metal matrix, concrete composite, and
polymer matrix are few examples of the diverse features of
composite materials and their structure that are covered by
composite technology. Composites, which are heterogene-
ous systems made up of two or more components that dif-
fer in their physical characteristics, chemical composition,
and separation within the material by a boundary that is
easily defined, have recently drawn a lot of interest [6, 27].
They are characterized by physical characteristics that are
not shared by their constituent components. Their primary
distinction between alloys and chemical compounds is that
the structural components in them are not combined at the
molecular or atomic level. Components for use in electro-
magnetic devices can be made more affordable and con-
trolled using ferrite-ferroelectric composites. Such mul-
tiferroic composites serve as the building blocks for the
development of multifunctional devices, including sensors,
transducers, spintronics, and terahertz radiation. The crea-
tion of all-in-one devices with promise for storage devices,
logical operations, and optical active and electromechanical
systems can result from the development of such ferrite–fer-
roelectric composites [6, 28]. Therefore, the present work is
focused on the preparation of ­Bi0.9La0.1FeO3 (BLFO) and
MFO by hydrothermal method. Then, a composite series of
(1–x)BLFO + xMFO (x = 0.2, 0.3, 0.4 and 0.5) was prepared
by the solid-state ball-milling method to analyze systemati-
cally ME coupling. In these composites, MFO as magnetic
component and BLFO as a ferroelectric component were
chosen to improve the magnetic and ferroelectric features
to enhance ME coupling in the prepared composites for effi-
cient utilization in multistate applications.
2 Experimental
To prepare (1–x)BLFO + xMFO (x = 0.2, 0.3, 0.4 and 0.5)
composite samples, first, BLFO and MFO were synthesized
using hydrothermal method. The metal nitrate precursors
that include iron-nitrate nonahydrate [Fe(NO3) 3·9H 2O,
pur ity ≥ 98% ], magnesium-nitrate hexahydrate
[Mg(NO3)2·6H2O, purity ≥ 99%], lanthanum-nitrate hexa-
hydrate [La(NO3)3·6H2O, purity ≥ 98%], and bismuth-nitrate
pentahydrate [Bi(NO3)3·5H2O, purity ≥ 98%] purchased
from Sigma-Aldrich, were utilized. The stoichiometrically
calculated fuelling agents that include urea (­ CH4N2O) and
glycine ­(C2H5NO2) along with metal nitrates were dissolved
in deionized (DI) water to make a homogenously transpar-
ent solution. The solution was placed on a hot plate at 95 ºC
and stirred at 200 rpm using a magnetic stirrer. Meanwhile,
the pH of the solution was maintained around 10 using the
dropwise addition of 6 M KOH, which was further stirred
Analysis of interphase magnetoelectric coupling in ­Bi0.9La0.1FeO3–MgFe2O4…
for 50 min. The secondary phases of BFO are reduces while
keeping the pH at 10 or above [29]. Afterward, the solution
was shifted to a Teflon-lined autoclave and heated at 200 ºC
for 7 h. This heated solution was slowly cooled down to RT
and washed using a centrifuge. The resulting precipitates
were washed many times with DI water and a furnace was
used to dry the samples for 10 h at 80 ºC. The dried samples
were homogenized up to fine powder using an Agate mortar
and pestle. Both BLFO and MFO were synthesized sepa-
rately by the same method. The BLFO powder was calcined
at 550 ºC for 2 h, while MFO was calcined at 700 ºC for 3 h
to ensure the crystalline phases. After calcination, both the
individual samples were mixed via ball-milling chamber for
8 h at different stoichiometric ratios to achieve homogene-
ous mixture of BLFO and MFO in each composition. After
that, the pellets were made by an Apex hydraulic press and
sintered for 250 ºC for 1 h before further analysis. The syn-
thesis process for the composite samples is shown in Fig. 1.
The individual phases of BLFO and MFO in the com-
posite samples were identified using a Bruker D8 Advance
X-ray diffractometer (XRD), for confirming the composite
formation. A Nova-Nano SEM-450, field emission scanning
electron microscope (FESEM) was utilized to analyze the
surface morphology. An attached energy-dispersive X-ray
(EDX) Oxford’s instrument was used to evaluate the element
composition of composite samples. A Radiant Tech., (USA)
precision multiferroic tester with Helmholtz coils was used
to determine the ferroelectric response and ME coupling of
composite samples.
3 Results and discussion
The XRD patterns of (1–x)BLFO + xMFO at x = 0.2, 0.3, 0.4,
and 0.5 are shown in Fig. 2a. The identified intense peaks
were indexed according to analytical approach described
Fig. 1  Schematic illustration of sample synthesis
Page 3 of 11 779
by B.D. Cullity [30]. At x = 0.2, the peaks appeared at 2θ
values 22.39°, 31.81°, 39.44°, 45.76°, 51.34°, 57.02°, and
66.95° corresponding with hkl values (100), (110), (111),
(200), (210), (211), and (2–20) were well matched with
ICSD card no. 01–071-2494, that confirmed the presence
of BFO having rhombohedrally distorted cubic perovskite
structure with R3c space group symmetry[31]. Other peaks
that appeared at 2θ values 30.15°, 35.50°, 37.08°, 43.14°,
53.56°, 62.67°, and 67.10° corresponding with hkl values
(220), (311), (222), (400), (422), (440), and (442) are well
matched to the ICSD card no. 01-071-1232, and it assured
the presence of normal spinel structure of MFO with Fd-3m
space group symmetry [32]. This confirms the synthesis of
desired bi-phasic composite at x = 0.2. It seems quite evi-
dent from the diffraction patterns recorded at x = 0.3 that the
intensity of the peaks correspondent to BLFO is decreased,
while that related to MFO component is enhanced. Further-
more, at x = 0.4, the MFO peak intensity is further enhanced,
and at x = 0.5, the highest intensity peaks of spinel phase
MFO could be observed, which confirmed the formation
of bi-phasic composites with selected content ratios [33,
34]. The peaks related to BLFO are represented by (♣)
symbols, while spinel phase MFO is denoted by (♥) sym-
bols. For better visualization of Bragg angles correspond-
ing with hkl values, the indexed pattern at x = 0.5 is shown
in Fig. 2b. The cell parameter√values were evaluated using
the relation, i.e., a = 𝜆∕2sin𝜃 h2 + k2 + l2 , while for crys-
tallite size the Scherrer relation D = 0.9 𝜆∕𝛽cos𝜃 was used
[35]. Here, λ represents the wavelength of Cu Kα radiation
(i.e., 0.1546 nm), while θ represents the Bragg angle and
β represents full width at half maxima. The cell parameter
for BLFO and MFO phases remained almost same at all
compositions, and it confirmed the structural stability after
composite formation [36]. For further confirming the invari-
ancy of the cell parameters, a plot having almost no peak
shift can be observed in Fig. 2c [37, 38]. However, a small
13
779 Page 4 of 11 M. H. Maqbool et al.

Fig. 2  a XRD patterns of (1–x)BLFO + xMFO at x = 0.2, 0.3, 0.4, and 0.5, b indexed pattern of x = 0.5 composite, c plot indicating no shifting of
peaks, and d–g Rietveld’s refinement plots at x = 0.2, 0.3, 0.4, and 0.5 composites

variation in the crystallite size from 11.5 to 12.6 nm was
observed for BLFO, while for MFO, it varied from 20.9
to 23.4 for x = 0.2–0.5. The bulk density, estimated by the
relation 𝜌B = m∕V , first reduced from 2.15 to 2.02 g ­cm−3
by the change of MFO content (x) from x = 0.2 to 0.4, and
then increased to 2.11 g/cm3 for x = 0.5. This variation in 𝜌B
might be attributed to non-uniformity in composite pow-
der samples in pellet form [39], while the X-ray density
(𝜌x = NM∕VN A) showed a systematic reduction from 5.23
to 4.97 g ­cm−3 for x = 0.2–0.5. The %porosity was calculated
using the relation: % Porosity = (1 − ρB/ρx) ×100 that varied
from 59 to 58% by gradually enhancing the spinel phase
contents (x) in the composite samples. All above-mentioned
parameters, including cell parameters, crystallite size, 𝜌B, 𝜌x ,
and % Porosity are provided in Table 1.
For further assurance of phase composition development,
the Rietveld's refinement was implemented by the use of
X'pert HighScore Plus software, as shown in Fig. 2d–g. The
difference plot between observed intensity (Io) and calculated
intensity (Ic) provides the information about phase purity of
the composite samples. An enhancement in MFO phase with
reduction in BLFO could be seen in the refinement plot.
The small intensity difference between the two XRD plots
might occurred due to some factors like vacancies, tempera-
ture effect, or defects in the samples. The refinement factors
such as weighted-R profile (Rwp), R-expected profile (Rexp)
achieved through refinement process provides goodness of
fit (χ2) values, i.e., χ2 = Rwp/Rexp. The observed χ2 values for
all samples from x = 0.2–0.5 remained to be closer to 1 that
confirmed the proper formation of the required crystalline
phases. The values of Rwp, Rexp and χ2 for all composite
samples are listed in Table 2.
The magnetic and electric characteristics of ferrites are
significantly affected by the shape and size of the grains
[40]. The morphology of the composite samples was studied
by analyzing FESEM images taken at 200,000× magnifi-
cation, as shown in Fig. 3a–d. The surface roughness was
observed which might be due to gas evaporation occurred

Table 1  Lattice constants, Substitution Lattice constant Crystallite size (nm) X-ray density Bulk density Porosity (%)
crystallite size, X-ray density, contents (x) (nm) (g/cm3) (g/cm3)
bulk density, and porosity of
(1–x)BLFO + xMFO composite BLFO MFO BLFO MFO
samples
0.2 3.96 8.38 11.50 20.90 5.23 2.15 59
0.3 3.96 8.38 13.70 32.60 5.12 2.03 60
0.4 3.96 8.38 12.30 24.70 5.05 2.02 61
0.5 3.96 8.38 12.60 23.40 4.97 2.11 58

13
Analysis of interphase magnetoelectric coupling in ­Bi0.9La0.1FeO3–MgFe2O4…
Table 2  Rietveld’s refined x Rwp Rexp
structural parameters of (1–x)
BLFO + xMFO composite 0.2 2.48 1.68
samples
0.3 8.29 3.13
0.4 7.53 3.45
0.5 6.29 3.15
during sintering from the surface of the samples. It is obvi-
ous that the pores are present in the structure and irregular
shaped particles are distributed uniformly over the surface
[41, 42]. A Java-based Image-J software was used for meas-
uring the grain size of composite samples. At x = 0.2, some
of the grains had hexagonal shapes, while the particles were
dominantly irregular with an average grain size of 131 nm,
as shown in Fig. 3a. At x = 0.3, the average grain size was
about 111 nm, having less porosity compared to x = 0.4 but
greater than other two compositions, as shown in Fig. 3b. At
x = 0.4, the average grain size slightly decreased to 95 nm,
as shown in Fig. 3c. While, at x = 0.5, for the highest spinel
phase contents, the composite depicted least porosity com-
pared to all other compositions having an average grain size
of 114 nm, as depicted in Fig. 3d. The small change in the
grain size caused small variation in the composite porosity.
The large and small grains observed in FESEM images may
be attributed to the presence of two distinctive phases in as-
synthesized composites [43, 44]. The density and number
of small grains were enhanced by increasing MFO content
in the composite, because the average size of MFO is much
lower than BLFO. Meanwhile, some significant agglomera-
tion was observed in the composite samples [45, 46].
For the elemental analysis, a small scanned area of the
x = 0.5 composite was taken, as shown in Fig. 3e. This
elemental mapping assured about the presence of desired
Fig. 3  a–d FESEM images of (1–x)BLFO + xMFO at x = 0.2, 0.3, 0.4, and 0.5 taken at ×200,000 magnification, and e small area scanned for the
sample with x = 0.5, to trace the elements f Bi, g La, h Mg, i Fe, and j O via elemental mapping
Page 5 of 11 779
χ2 elements in the composite samples [31, 44]. These images
are established from a wireless distribution system (WDS)
1.47
which gives a real image of the surface in terms of the pre-
2.64 sent elements. In this elemental mapping, the data are digi-
2.13 tally recorded and used for locating the spot analysis. The
1.99 bright region shows the presence of particular elements in
that region, while the dark region represents the absence or
minimal concentration of those elements in the specified
region, as depicted in Fig. 3e. The presence of Bi, La, Mg,
Fe, and O elements in the composite samples is verified in
Fig. 3f–j. The specific region in these colored spectra indi-
cates the presence of constituent elements in both BLFO and
MFO that validates the element presence in the composites
according to nominal composition.
The ferroelectric characteristics of the composites were
studied by analyzing polarization versus electric field
(P–E) hysteresis loops taken at ± 20 kV/cm, as shown in
Fig. 4a. The P–E loops do not seem to be saturated even
at high values of electric field, due to large leakage current
of BLFO [47]. Tang et al. reported that, at higher electric
field, the high value of leakage current produced break-
down voltages in BFO-based ceramic composites [48].
The oxygen vacancies floated and concentrated at domain
walls, and it reduced the polarization due to domain
switching blockage [49]. The charging and discharging are
evaluated by plotting P–E loops in 1st quadrant for all the
composites, as shown in Fig. 4b. The fluctuating behavior
of polarization by enhancing applied electric field (Ef) at
different voltages for x = 0.5 composite is shown in Fig. 4c.
It was observed that, by increasing Ef, the electric dipoles
is aligned more systematically, and that is resulted into
large polarization values. However, the shape of P–E loops
at different voltages almost showed the same trend. The
analysis of these P–E loops provided maximum
13
779 Page 6 of 11 M. H. Maqbool et al.

Fig. 4  a Polarization (P) vs electric field (E), P–E loops, b charge density (WL) at various contents (x), f %efficiency at various contents
discharge curves, c response of P vs E at various voltages, d remanent (x), g current–voltage plot, and h conductivity plot for bi-phasic com-
polarization (Pr) and maximum polarization (Pm) with various substi- posites
tution content (x), e recoverable energy density (WR) and energy loss

Table 3  Maximum polarization (Pm), remanent polarization (Pr), Table 4  Energy density (WT), recoverable energy density WR,
and coercivity (Ec) of bi-phasic composites (1–x)BLFO + xMFO at and energy loss density (WL) and %efficiency (%η) of (1–x)
x = 0.2, 0.3, 0.4, and 0.5 BLFO + xMFO at x = 0.2, 0.3, 0.4, and 0.5
Sr. no. x Pm (µC/cm2) Pr (µC/cm2) Ec (kV/cm) Sr. no. x WT (µJ/cm3) WR (µJ/cm3) WL (µJ/cm3) (%η)

1 0.2 108 88 10 1 0.2 1080 560 520 52

2 0.3 143 118 12.2 2 0.3 1430 500 930 35
3 0.4 214 183 12.9 3 0.4 2140 620 1520 29
4 0.5 187 162 12.7 4 0.5 1870 500 1370 27

polarization (Pm), remanent polarization (Pr), and coerciv-
ity (Ec) values. A plot between Pm and Pr vs substitution
is provided in Fig. 4d. The lowest recorded values of Pm,
P r and E c of 108 µC/cm 2 , 88 µC/cm 2 and 10 kV/cm,
respectively, were observed at x = 0.2. While at x = 0.3, a
sudden variation in Pm, Pr and Ec values was observed to
be 143 µC/cm2, 118 µC/cm2, and 12.2 kV/cm, respectively.
At x = 0.4, the highest recorded values of Pm, Pr, and Ec
were 214 µC/cm2, 183 µC/cm2, and 12.9 kV/cm, respec-
tively. Surprisingly, at x = 0.5, there was a decrease in Pm,
Pr, and Ec values as 187 µC/cm2, 162 µC/cm2, and 12.7 kV/
cm, respectively. All values of Pm, Pr, and Ec are provided
in Table 3. These P–E loops can measure the efficiency of
the material for utilization in energy storage devices,
which can be calculated by the following prescribed rela-
tions; for total energy density (WT = ½ E ×Pm), recoverable
P
energy density ( WR = ∫ Pm Edp ), energy loss density
r
(WL = WT − WR ), and %efficiency by the following rela-
tion; %𝜂 =WR/WT ×100 . The deviation of WR and WL for
the different substitutions in composites is shown in
Fig. 4e. At x = 0.2, the calculated values of WR and WL
were 560 µJ/cm 3 and 520 µJ/cm 3, respectively, with the
highest %𝜂 ⁓52%. At x = 0.3, the WR value decreased to
500 µJ/cm 3 and WL increased to 930 µJ/cm 3 along with
decrease in %𝜂 ⁓35%. Whereas, at x = 0.3, the calculated
values of WR and WL were 620 µJ/cm3 and 1520 µJ/cm3,
respectively, with the highest %𝜂 ⁓29%. At maximum spi-
nel phase contents, i.e., at x = 0.5, the observed values of
WR and WL were 500 µJ/cm3 and 1370 µJ/cm3, respectively.
This composite showed the largest value of WL, and so, it
possessed the least %𝜂 ⁓27%. For comparative analysis,
the %𝜂 vs substitution graph is provided in Fig. 4f. In this
study, it is suggested the x = 0.2 composite, where 80%
BLFO and 20% MFO are mixed, is the most preferable for
energy storage devices, having highest %𝜂 ⁓52%. The cal-
culated values of W T, WR, WL, and %𝜂 of the composites
are provided in Table 4. The incomplete P–E loops are due
to high value of oxygen vacancies and leakage current, and
conduction mechanism as well [50, 51].
The plots between current and voltage (I–V) at RT for
(1–x)BLFO + xMFO (x = 0.0, 0.1, 0.2, 0.3, 0.4, and 0.5)

13
Analysis of interphase magnetoelectric coupling in ­Bi0.9La0.1FeO3–MgFe2O4…
composites are shown in Fig. 4g. The curves reveal char-
acteristic trends as expected from a semiconductor material
and extends equally in both positive and negative directions
[52]. The low leakage current values are observed that could
be attributed to two different parameters; one is the oxygen
vacancies production and other is the structure formation.
Although most of the oxygen vacancies were removed dur-
ing sintering, some of the vacancies were present in the sam-
ple [53]. The amount of oxygen vacancies is also increased
due to the addition of MFO in the composites. It might be
the cause of the increase in radiative recombination [27].
The enhancing values of current with increasing concentra-
tion of MFO in the composites can be observed in Fig. 4g.
The composite samples at x = 0.2 and 0.3 showed leakage
current value of ⁓10–8 A, while at x = 0.4 sample showed
the highest value of leakage current beyond 1­ 0–8 A, and at
x = 0.5, the leakage current again decreased by enhancing the
MFO content (x). The amount of current also depends upon
the porosity and roughness of the surface, and at x = 0.4,
the porosity is maximum which is also evident from SEM
images. This increasing current caused an increase in the
conductivity of the prepared samples with an increasing
amount of MFO till x = 0.4, and then decreased at the same
electric field due to which the dielectric losses and leak-
age current becomes higher. In Fig. 4h, the conductivity is
displayed for all the prepared samples, showing the same
trend as current and having a maximum value for the x = 0.4
composite.
BFO is typically thought of as a weak ferromagnetic
material because of the unpaired Fe spins. Additionally,
anti-ferromagnetic (AFM) spiral spins and finite spin cycloid
distortion play an important role for the reduction in these
ferromagnetic features [31]. Figure 5a illustrates the mag-
netic characteristics of (1–x)Bi0.9La0.1FeO3 + xMgFe2O4
composites sintered at 250 ºC, recorded at room tempera-
ture at less than 18 kOe applied magnetic field. M–H loops
suggest that all of the synthesized samples exhibit weak fer-
romagnetic behavior at RT. Interesting characteristics may
be seen in the M–H hysteresis loops of prepared composites.
These composites have the typical magnetic hysteresis loops
Fig. 5  a Variation in M–H loops
obtained from VSM, and b
comparison of Ms and Mr and
variation in the coercivity for of
(1–x)BLFO + xMFO at x = 0.2,
0.3, 0.4, and 0.5
Page 7 of 11 779
of magnetic materials, proving that they have magnetically
ordered structure [54]. The inclusion of MFO has a signifi-
cant impact on the saturation magnetization (Ms), remanent
magnetization (Mr), and coercivity (Hc) of the composite,
and is shown in Fig. 5b. Strong dipolar interaction is the
main cause of smaller dispersion values of particles, which
reduces Mr/Ms ratio [55, 56]. The Ms of all the samples
have been achieved by 14.5 kOe with values in the range of
6–17.2 emu/g. The Mr values also increased with increas-
ing concentration of MFO in the composites and ranges
1.6–4.5 emu/g, while the coercive field remains same for all
the prepared composites. For the growth in MFO content
from 20 to 50%, the magnetic saturation of the composites
increased from 6.15 to 17.18 emu/g, while the remanent
magnetization increased from 1.68 to 4.41 emu/g. The maxi-
mum value of Mr and Ms are observed for 50% concentration
of MFO in the composites. The magnetic characteristics of
the samples are significantly improved when the addition
of MFO in pure BFO increases. It shows that the BFO and
MFO phases have strong exchange coupling interactions
with in the system, which can be characterized by Mr/Ms
ratio [51]. Although the produced composites Mr/Ms are
below 0.3 in this case, coupling in the system is still present.
Another assignable component that affects the Mr/Ms ratio
is the interparticle dipolar interaction. Table 5 includes the
magnetic properties of the synthesize composites. Linear
combination of BFO and MFO phases, along with the spin
orientations in the composite interface also contributes to the
increased magnetization of the composites. The ferroelectric
Table 5  Saturation magnetization (Ms), remanent magnetization (Mr),
coercivity (Hc), and Mr/Ms ratio of (1–x) BLFO + xMFO at x = 0.2,
0.3, 0.4, and 0.5
Sr. no. x Ms (emu/g) Mr (emu/g) Hc (Oe) Mr/Ms
1 0.2 6.15 1.68 327 0.27
2 0.3 8.79 2.35 335 0.27
3 0.4 12.33 3.23 329 0.26
4 0.5 17.18 4.41 339 0.26
13
779 Page 8 of 11
polarization in BFO is caused by a stress produced and trans-
ferred from the surface of the magnetostrictive MFO to the
composite interface between the BFO and MFO. The single-
phase multiferroic BFO experiences moderate magnetism.
As a result, the overall magnetization of the multiferroic
(1–x)BLFO + xMFO composite system increases [51, 56].
The fast-switching capability of ferroelectric materials
is purely based on Pr values to develop the energy storage
devices. To measure the precise Pr values in ferroelectric
materials, Scott introduced the positive up and negative
down (PUND) sequence in which the sample was exposed
to the alternate pulses of external electric field by adjusting
the pulse width of 1 ms and pulse delay of 1 s [57]. Total
polarization is measured after each pulse and it is the sum of
switching polarization and polarization caused by the leak-
age current that can be calculated by the following equa-
tion; P ∗= Pswitching + Pleakage [58]. The value of remanent
polarization was measured with switching ( P∗r ) and with-
out switching ( P∧r ) after each pulse. The positive and nega-
tive values of P∗r and P∧r are plotted in the form of PUND
sequence which is plotted in Fig. 6a–d, and these sequences
were used to measure the switching charge density (QSW).
It has been observed that value of P∗r are greater than P∧r
which are attributed to the leakage current that provides
ease to evaluate QSW values from the prescribed relation;
QSW = P∗ P∧ . Here, P∗ and P∧ represent the maximum value
of polarization with and without switching, respectively
[59]. The calculated values of maximum polarizations with
and without switching, i.e., P∗r , P∧r along with QSW values,
are summarized in Table 6. The small QSW values in the
studied composites highlight their fast-switching capability
for the next-generation ferroelectric switching devices.
Magnetoelectric coupling in spinel–perovskite compos-
ites is of fundamental and technological importance and
provides a mean of transformation of electric energy to
magnetic energy and vice versa which decide their utili-
zation in many particular applications. The ME coupling
of any material can be computed by its coupling coeffi-
cient αME = 𝜕p∕𝜕H where 𝜕p is the induced polarization
occurred at applied magnetic field (H). This phenomenon
Fig. 6  Positive up and negative down (PUND) sequence of (1–x)BLFO + xMFO with x = a 0.2, b 0.3, c 0.4, and d 0.5
13
M. H. Maqbool et al.
Table 6  Polarization values with switching (P*) and without
switching (P^), along with switching charge density (Qsw) of (1–x)
BLFO + xMFO at x = 0.2, 0.3, 0.4, and 0.5
Sr. no. x P* (nC/cm2) P^ (nC/cm2) Qsw (nC/cm2)
1 0.2 0.1156 0.1149 0.0007
2 0.3 0.1456 0.1454 0.0002
3 0.4 0.2327 0.2304 0.0023
4 0.5 0.1948 0.1942 0.0006
is the key feature of multiferroic materials. The ferroelec-
tric behavior of BFO is due to the leaning of lone pair
electrons of Bi ions along the diagonal, while its magnetic
response is insufficient due to their canted spin structure
[60]. This canting spin makes a complete loop in a space
of diameter 62 nm and thus reduces the magnetic character
of BFO which could be enhanced by controlling the par-
ticle’s size of BFO i.e., < 62 nm. The variation in linear
polarization by applied magnetic field showed the ME cou-
pling of prepared composites, as shown in Fig. 7a–d. The
formation of composites quenched the cycloidal spin in the
crystal structure and depicted high values of the coupling
coefficient [61]. The ferroelectric attributes originated
from Fe–O–Fe bonds and ferromagnetic characteristics of
spinel phase commutatively enhanced the ME coupling of
the composites. The values of ME coupling can also be
enhanced by un-wounding the spiral structure. In fact, the
MFO magnetic particles in BFO matrix, when exposed to
external magnetic field, generate a stress at the intergranu-
lar boundaries via magnetostriction. This magnetostriction
induced the polarization in the ferroelectric phase through
piezoelectric phenomenon which was the underlying phe-
nomenon of magnetoelectric coupling in the composite
materials. The graphs in Fig. 7a–d reveal a linear ME cou-
pling in all the compositions where coupling coefficient
is increased with increasing magnetic field that provides
its potential applications in magnetic sensors, spintronic
devices, and data storage devices [62, 63].
Analysis of interphase magnetoelectric coupling in ­Bi0.9La0.1FeO3–MgFe2O4…
Fig. 7  Linear M–E coupling response for (1–x)BLFO + xMFO composite samples with x = a 0.2, b 0.3, c 0.4, and d 0.5
4 Conclusion
In this work, BLFO and MFO were synthesized via hydro-
thermal method, followed by ball milling to form the (1–x)
BLFO + xMFO at x = 0.2, 0.3, 0.4, and 0.5 composites.
The XRD analysis confirmed the presence of rhombo-
hedrally distorted cubic structure of BLFO and spinel
cubic structure MFO having R3c and Fd-3m space group,
respectively. The average crystallite sizes in BLFO and
MFO were 12.52 and 25.40 nm, respectively. The high-
est porosity of 61% was observed at x = 0.4. The grain
size decreased over the range of x = 0.2–0.4 having aver-
age grain size values of 131, 111, and 95 nm, and then
increased at x = 0.5, having average grain size value
114 nm. The element mapping confirmed the presence of
all constituent of all elements of BLFO and MFO, that was
in accordance with stoichiometric ratios of the compos-
ites. The maximum calculated values of P m and Pr were
214 µC/cm2 and 183 µC/cm2, respectively, at x = 0.4, as
determined from P–E loops. The highest %η of ⁓52% was
recorded at x = 0.2. The calculated QSW value was maximal
at x = 0.4 and minimal at x = 0.3, having 2.3 × ­10–3 nC/
cm2 and 2.3 × ­10–4 nC/cm2 values, respectively, as found
through the PUND sequence. The composite at x = 0.3
is highly preferable in fast-switching applications due to
smaller values of switching charge density. These com-
posites could be used in data storage devices, magnetic
sensors, and spintronic devices.
Acknowledgements The authors would like to acknowledge the
Researchers Supporting Project number (RSP2023R71), King Saud
University, Riyadh, Saudi Arabia.
Author contributions MHM: conceptualization, data curation, formal
analysis, and writing—original draft. ZI: formal analysis, software, and
methodology. SZ: data curation and investigation. AK: formal analysis
and software. SMR: data curation, investigation, and software. SA:
conceptualization, project administration, supervision, and writing—
review and editing.
Data availability statement Data will be available on request.
Page 9 of 11 779
Declarations
Conflict of interest The authors declare that they have no such finan-
cial or other competing interests to declare that could be there to influ-
ence the work presented in this article.
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