Nano-Structures & Nano-Objects 36 (2023) 101035

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Nano-Structures & Nano-Objects

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

Enhancing high frequency magneto-dielectric performance with

exchange-coupled garnet/spinel ferrite
(Y3 Fe5 O12 /Mg0.4 Cd0.4 Co0.2 Fe2 O4 ) composites
∗
Anjori Sharma a , , Dipesh b , Hamnesh Mahajan a , Neha Aggarwal c , Subhojyoti Sinha d ,
∗
A.K. Srivastava a ,
a
Department of Physics, Lovely Professional University, Phagwara, Punjab 144411, India
b
Division of Research and Development, Lovely Professional University, Phagwara, Punjab 144411, India
c
Department of Electronics Technology, Guru Nanak Dev University, Amritsar, Punjab 143005, India
d
Department of Physics and Nanotechnology, SRM Institute of Science and Technology, Kattankulathur, Tamil Naidu 603203, India

article info a b s t r a c t

Article history: Yttrium iron garnet ferrite (YIG), with good magnetic and dielectric properties, was mixed with doped
Received 21 June 2023 magnesium spinel ferrite (Y3 Fe5 O12 (x)/Mg0.4 Cd0.4 Co0.2 Fe2 O4 (1-x) (x = 0.3, 0.6, 0.9)) to attain high
Received in revised form 24 July 2023 permittivity and permeability with low magneto-dielectric losses. We have reported the synthesis
Accepted 10 August 2023
and enhanced structural, magnetic and magnetodielectric properties of composites for miniaturized
Keywords: antenna applications. The X-ray diffraction (XRD) patterns of all the composites were analysed using
Ferrites the Rietveld method, which confirmed that they exhibited a crystalline structure with a cubic spinel
Exchange-coupling and cubic garnet phase. XRD spectra confirm that the spinel ferrite phase dominates over the garnet
Permittivity ferrite phase in the x = 0.3 composite, whereas it is the opposite for the other composites. In contrast
Permeability to the parent ferrites, it has been observed that the composites (x = 0.3, 0.6, 0.9) exhibit a higher
Dielectric and magnetic losses value of the crystallite size ‘D’ and a lower value of the lattice constant ‘a’. The composite with the
x = 0.3 composition has the least porosity and a high relative density. From field emission scanning
electron microscopy (FESEM), it has been ascertained that the materials possess a grain size ranging
from 0.57 to 0.8 µm, with a larger grain size for the x = 0.9 composite, while the x = 0.3 composite
has the smallest grain size. Transmission electron microscopy (TEM) scans have corroborated the
FESEM micrographs’ findings, indicating that the grains within the composites’ structure exhibit
agglomeration. The calculated values of inter-planar spacing of the samples using high-resolution TEM
(HR-TEM) matches well with the XRD results. A magnetic study reveals that the composite with x =
0.3 has a good exchange-coupling, the highest coercivity value of 99.2 Oe and a magnetization value of
41 emu/g. The composite with x = 0.3 also has the highest permittivity value of ∼19.5, a permeability
value of ∼2.8, but low dielectric and magnetic losses of ∼0.009 and ∼0.002, respectively. These low
losses and a high miniaturization factor of ∼7.2 at high frequency (14 GHz) make it a potential
candidate for high-speed satellite antenna applications.
© 2023 Elsevier B.V. All rights reserved.

1. Introduction However, miniaturization of the antenna size whilst maintain-

In this era of cutting-edge, revolutionizing technology in the
communication industry, miniaturized smart innovative devices
are in huge demand. Miniatured antenna in the device design is
one of the prime sectors of focus in this context [1]. Antennas
are devices that receive and transmit electromagnetic signals.
In communication technology, the device antenna size plays a
very crucial role in determining its compactness and portability.
∗ Corresponding authors.
E-mail addresses: anjori.sharma1995@gmail.com (A. Sharma),
srivastava_phy@yahoo.co.in (A.K. Srivastava).
ing high efficiency is a bottleneck of modern antennas [2–4].
The miniaturization of antennas is tough because the bandwidth
and gain depend on the size of the antennas.
√ Theoretically, the
miniaturization factor is determined by ε ′ µ′ [5], where ε ’ and
µ’ represent the real parts of dielectric permittivity and mag-
netic permeability, respectively. So, the effective way to achieve
miniaturization as well harvest good performance is to design the
antennas with materials of high permittivity (ε ’) and permeability
(µ’), but with low dielectric and magnetic losses. Ferrites, with
the desired dielectric and magnetic properties, are an important
class of material which are now being considered as potential
candidates for the same. Ferrites are ceramic oxides and apart

https://doi.org/10.1016/j.nanoso.2023.101035
2352-507X/© 2023 Elsevier B.V. All rights reserved.
A. Sharma, Dipesh, H. Mahajan et al.
from their various applications, such as in microwave devices,
transformer core and in memory device applications, they are
also promising materials for antenna miniaturization with high
efficiency [6,7]. From a literature review, it is evident that ferrite-
based nanocomposites are very useful to enhance the individual
existing properties of ferrites, also if the nanocomposite has dis-
tinct phases [8–12], it can lead to an exchange bias effect or
exchange coupling. This could raise to the superparamagnetic
limit, which is a pivotal parameter for device miniaturization
[13,14]. Also, the inter-diffusion of cations and interface engi-
neering in ferrite composites can leads to the remediation of
different properties [15,16]. It is noteworthy that ferrite com-
posites exhibit excellent magneto-dielectric coupling, low losses,
chemical stability and high resistivity [17]. Ferrites are generally
of three types: hexagonal ferrite, spinel ferrite and garnet ferrites.
Hexaferrites exhibit good magnetic properties and have a higher
value of the imaginary part of complex permittivity, but this
results in higher losses in the material [18]. High losses are the
biggest drawback of their use in antenna applications.
Garnet ferrites are the best choice for antenna applications,
the reason for this is their excellent magnetic, electromagnetic
and dielectric properties, along with their low magnetic and
dielectric losses [19–23]. Among garnet ferrites, yttrium iron
garnet (YIG) is one of the widely investigated magneto-dielectric
materials for microwave devices. Garnet ferrites have the chem-
ical formula R3 Fe5 O12 , where R is any rare-earth element. In
general, the iron ions (Fe3+ ) occupy the 16a octahedral and 24d
tetrahedral sites, while the rare earth cations (R3+ ) frequently
occupy the dodecahedral 24c site. YIG offers high resistivity, low
losses, tuneable magnetic saturation and a narrow ferromag-
netic resonance bandwidth [24]. Among all the ferrites, spinel
ferrites are very important materials in terms of their practi-
cal and fundamental prospective [25,26]. Generally, all spinel
ferrites possess high insulating properties with varying mag-
netic properties. The rationale behind it is their fundamental
properties that occur because of exchange coupling in Fe3+ -O2− -
Fe3+ , Me2+ -O2− -Fe3+ and Me2+ -O2− -Me2+ cations and anions
bonding [27]. Spinel ferrites have the chemical formula AFe2 O4 .
Here A is a divalent ion, such as Fe+2 , Mg+2 , Mn+2 Ni+2 or
Co+2 . They are also very useful for antenna applications be-
cause of their good magnetic and dielectric properties, with very
low dielectric losses at higher frequencies [28,29]. Due to low
coercivity, low anisotropy, low losses, average saturation mag-
netization and large initial permeability [30–32], these materials
are suitable for many practical applications, like in microwave
devices, heating inductors, microwave heating, lithium-ion bat-
teries, water remediation and biomedical applications [33–35].
Magnesium (Mg) based spinel ferrites are of more interest for an-
tenna substrates because of their chemical and physical stability
and enhanced magnetic and dielectric properties. In addition to
this, the properties of such ferrites can be easily modified by par-
ticular ion substitutions [36]. Gan et al. have studied the magnetic
and dielectric properties of cadmium (Cd) substituted magne-
sium ferrite Mg1−x Cdx Co0.05 Fe1.95 O4 (x = 0, 0.2, 0.3 and 0.4). It
has been determined that the samples (Mg1−x Cdx Co0.05 Fe1.95 O4 )
have low dielectric losses, tan(δε ), and magnetic losses, tan(δµ),
values (tan(δε ) ≈ 0.0008, tan(δµ) ≈ 0.03 for x = 0.3) [37].
Bhongale has worked on cadmium substituted magnesium ferrite
(Mgx Cd1−x Nd0.03 Fe1.97 O4 (x = 0, 0.2, 0.4, 0.6, 0.8 and 1.0)) for
the substrate of a microstrip patch antenna [29]. The substituted
magnesium ferrite gave lower values of the magnetic and dielec-
tric losses in the X band. This further suggests that by cadmium
substitution, the material becomes suitable for antenna applica-
tion. Bassami et al. have studied the magnetic and mechanical
properties of cobalt-substituted magnesium-zinc ferrite [38]. It
has been investigated that with cobalt substitution, the magnetic
2
Nano-Structures & Nano-Objects 36 (2023) 101035
properties of the parent spinel ferrite are enhanced. The reason
for this is the strong magnetic anisotropy property of the cobalt
(Co+2 ) ion in the B sites.
Previous studies have already reported on exchange-coupled
nanocomposite ferrites, especially hard/soft ferrites for microwave
devices [39–44]. The main motivation of the research work is to
explore soft/soft ferrites composites (i.e., Mg spinel ferrite and
yttrium iron garnet ferrite) due to their lower losses and high
magneto-dielectric properties. From the above surveyed litera-
ture it has been found that garnet ferrite and Cd, Co doped Mg
spinel ferrite exhibit magneto-dielectric properties, but up to cer-
tain frequency garnet ferrites and Mg doped spinel ferrites have
shown some limitations. So, this research work aims to enhance
the magneto-dielectric properties in the form of composites. In
addition to their microwave applications, these composite ferrites
can exhibit a magneto-dielectric nature with high permittivity
(εr ) and permeability (µr ). This makes them potential candidates
to replace dielectric-only substrates in antenna miniaturization.
However, most of the dielectric studies on these composites have
focused on low frequencies up to 1 GHz [45,46]. The investi-
gation of the magneto-dielectric behaviour of such composites
at higher frequencies, specifically in the range of 12–18 GHz,
has been limited and requires further exploration. The study of
ferrites composites in the Ku band is very important because
most of the antennas used in satellites operate in this band
range. The international space station (NASA) uses a tracking data
relay satellite which operates in the Ku band. In this presented
work, we have synthesized composites of garnet ferrite (YIG) and
magnesium substituted spinel ferrite (Mg0.4 Cd0.4 Co0.2 Fe2 O4 ) via a
sol–gel auto combustion method and have studied the structural,
morphological, dielectric and magnetic properties. The sol–gel
auto combustion method was used because it provides better
homogeneity to the solution, cheaper precursors are required and
it has countless advantages over other methods [47]. The syn-
thesized ferrite samples have shown very low losses with good
permittivity, permeability and higher miniaturization parameters
which makes them suitable for antenna application in the Ku
band (12–18 GHz).
2. Experimental procedure
2.1. Materials preparation
The sol–gel auto combustion method was adopted to pre-
pare yttrium iron garnet (Y3 Fe5 O12 ) and magnesium substituted
spinel ferrites (Mg0.4 Cd0.4 Co0.2 Fe2 O4 ). The precursors, yttrium(III)
nitrate [Y(NO3 )3 .6H2 O], cadmium(III) nitrate [Cd(NO3 )3 .6H2 O],
cobalt(III) nitrate, with 99.999% traces, were procured from Sigma-
Aldrich, whereas ferric(III) nitrate [Fe(NO3 )3 .9H2 O], magnesium(III)
nitrate [Mg(NO3 )3 .6H2 O] and citric acid (C6 H8 O7 .H2 O), with a
purity of 98%, were procured from Loba Chemie. A significant
amount of ferric nitrate and yttrium nitrate powders were taken
in a 1.67 molar ratio (Fe/Y) for YIG preparation. Similarly, for
the formation of spinel ferrite, all the metal cation nitrates (M
= Mg, Cd, Co) and ferric nitrate were taken in 2 molar ratios
(Fe/M). The weighted amounts of these salts were measured in
consonance with the stoichiometric ratio of citric acid to metal
cation in a 1:1 ratio (the amount of citric acid equals the moles of
metals) and added to 100 ml of distilled water. The solution was
magnetically stirred for half an hour to get a homogeneous clear
solution. Ammonia solution was then added slowly to maintain a
pH value of 7. The solution was then continuously stirred and
heated simultaneously at 70 ◦ C until it turned into a gel. The
obtained gels were subjected to heating in the presence of air
at temperatures ranging from 200 to 250 ◦ C. During this heating
process, the gels swelled up and eventually burned, resulting in
A. Sharma, Dipesh, H. Mahajan et al.
Fig. 1. (A) XRD pattern of the samples and (B) shift in the 2θ value with the variation in composition.
the formation of dried powders. These dried powders were then
sintered in a muffle furnace at a temperature of 1200 ◦ C for a
duration of 7 h. In order to prepare the composites, the powders
of YIG and MgCdCoFe were initially coarsely crushed using a
mortar and pestle before being used. Then, the synthesized YIG
and MgCdCoFe powders were weighed based on the desired
weight percentages. These powders were blended together using
a simple mechanical or physical blending technique [48,49]. The
blending process involved using a mortar and pestle to mix the
powders for a duration of 45 min. This blending step resulted
in the preparation of composites of YIG(x)/MgCdCoFe(1-x) with
weight percentages (wt%) of x = 0.3, 0.6 and 0.9.
2.2. Characterizations
A powder X-ray diffractometer (XRD: Bruker D8 Advance) was
used to study the phase and crystal structure of the nanocompos-
ites. Using Rietveld analysis in the FullProf suite and pseudo-Voigt
as the peak profile function, all experimental XRD patterns were
fitted. The morphology and compositions of the samples were
analysed using a Field Emission Scanning Electron Microscope
(FESEM) coupled with Energy Dispersive X-ray analysis (EDX).
Specifically, the FESEM instrument used was the JEOL JSM-7610F
Plus, while the EDX system employed the OXFORD EDX LN2. In
order to enhance the conductivity of the samples for imaging, an
Au sputter coater, specifically the JEOL Smart Coater, was utilized.
These techniques allowed for the examination of the surface
morphology and elemental composition of the samples. The mi-
crostructure of the powders was examined using a Transmission
Electron Microscope (TEM), specifically the JEM-1200EX model.
TEM analysis allowed for a detailed investigation of the internal
structure and finer features of the powders at a microscopic scale.
A vibrating sample magnetometer (VSM-EZ9) was used for the
analysis of important magnetic properties of the prepared com-
posite samples. Pellets of 2 mm thickness, pressed according to
Ku-band waveguide (0.622 in × 0.311 in), were used to study the
high frequency magneto-dielectric properties of the nanocom-
posites with the help of an Agilent software module 85071,
3
Nano-Structures & Nano-Objects 36 (2023) 101035
vector network analyzer (VNA). The scattering parameters were
used to derive the values of electromagnetic parameters, such as
complex permittivity and complex permeability, by utilizing the
Nicolson-Ross-Weir model.
3. Results and discussions
3.1. Phase and structural study
The XRD patterns of the prepared samples, i.e. YIG, Mg0.4
Cd0.4 Co0.2 Fe2 O4 (MgCdCoFe) and YIG(x)/ MgCdCoFe(1-x) compos-
ites are shown in Fig. 1 (A) (a-0e). The obtained patterns were
compared and matched with the JCPDS card no. 430507 for
YIG and 221086 for MgCdCoFe, respectively. Diffraction peaks in
Figs. 1 (A) (a) and (b) reveal the pure phase formation of cubic
garnet ferrite with the space group Ia3D and cubic spinel ferrite
with the space group Fd-227, respectively. Fig. 1 (A) (c0-e) rep-
resent the XRD patterns of the composites. The diffraction peaks
of YIG and MgCdCoFe are present in all composites. This implies
that YIG and Mg0.4 Cd0.4 Co0.2 Fe2 O4 exist independently without
reacting with each other. However, for the x = 0.3 composite,
the highly intense peak of YIG at (420) becomes less intense,
implying that the spinel ferrite phase is dominating over the
garnet ferrite phase in the composite. This disparity in intensity
is obvious because the spinel ferrite phase is dominant for the x
= 0.3 composite, whereas for the x = 0.6 and x = 0.9 composites
the YIG phase dominates over the MgCdCoFe phase. The intensity
and number of diffraction peaks in the composite material are
determined by the quantity and identity of the respective phases
of the parent ferrites [50].
The extracted values of structural parameters like the lattice
constant ‘a’, micro-strain ‘ε ’ and crystallite size ‘D’ from the
diffraction patterns are tabulated in Table 1. Fig. 1 (B) represents
the shift in the 2θ value of the highly intense diffraction peak with
the Miller indices (hkl) value (420) of YIG in the YIG/MgCdCoFe
(from x = 0.3 to 0.9) composites. From Fig. 1 (B) and Table 1, it can
be concluded that by incorporating spinel ferrite (MgCdCoFe) in
garnet ferrite (YIG) the diffraction peak shift is towards higher
A. Sharma, Dipesh, H. Mahajan et al. Nano-Structures & Nano-Objects 36 (2023) 101035

Table 1
The calculated values of 2θ , β , hkl, the crystallite size(D), lattice parameter(a) and micro stain (ε ).
Sample Sample code 2θ ( ◦ ) β hkl D (nm) a εcal
YIG Y 32.01 0.25 420 32.1 2.49 –
Mg0.4 Cd0.4 Co0.2 Fe2 O4 M 35.39 0.22 311 36.9 8.40 –
(YIG)x-(Mg0.4 Cd0.4 Co0.2 Fe2 O4 )1-x (x = 0.3) YM0.3 32.46 0.17 420 Y M 12.32 2.8
42.1 26.4
YIG)x-(Mg0.4 Cd0.4 Co0.2 Fe2 O4 )1-x (x = 0.6) YM0.6 32.36 0.16 420 Y M 12.36 2.4
50.5 29.8
YIG)x-(Mg0.4 Cd0.4 Co0.2 Fe2 O4 )1-x (x = 0.9) YM0.9 32.35 0.16 420 Y M 12.36 2.3
51.4 32.2

Table 2
Measurement of the lattice constant (a) in different positions to show the formation of both phases in the composites for YIG(x)/MgCdCoFe(1-x) (x = 0.3 and 0.6).
YM0.3 YM0.6
YIG phase MgCdCoFe phase YIG phase MgCdCoFe phase
2θ hkl d a 2θ hkl d a 2θ hkl d a 2θ hkl d a
43.29 532 2.08 12.87 35.9 311 2.45 8.29 45.20 532 2.00 12.36 35.5 311 2.53 8.38
55.6 642 1.65 12.36 56.8 511 1.62 8.42 55.7 642 1.65 12.34 56.9 511 1.62 8.40
62.5 800 1.48 11.87 60.11 440 1.53 8.70 60.11 800 1.54 12.30 62.5 440 1.48 8.39

2θ values. This shift in angle further affects the value of the
lattice constant ‘a’, which was calculated using Eq. (1) [51] and
is given in Table 1. The values of the lattice constant in different
positions has been calculated (Table 2) to show the formation of
both phases in the composites.
a = d(h2 + k2 + l2 )1/2
Here ‘d’ is the inter-planar spacing which is calculated with the
help of Bragg’s law:
( ) nλ
dspacing Å = (2)
2 sin θ
Here the order of diffraction ‘n’ is equal to 1 and hkl is the Miller
indices. For YIG and MgCdCoFe, the Miller indices correspond to
the highest intensity peaks and for composites, it corresponds to
the YIG peak.
From the above equations (1) and (2) we can write:
nλ
a= (h2 + k2 + l2 )1/2 (3)
2 sin θ
Eq. (3) depicts that the lattice constant ‘a’ is dependent on the
angle (θ ). The decrease in the value of ‘a’ for the
YIG(x)/MgCdCoFe(1-x) (x = 0.3, and 0.9) composites is due to
the shift of angle towards the higher side. Also, the fluctua-
tion of the lattice constant of the composite from ideal YIG is
due to the variation in solubility between garnet and spinel
ferrite [52]. This mechanism can be elucidated on the account
of the inter-diffusion of cations into the YIG lattice sites in the
composites [53]. The inter-diffusion is possible as the ionic radii
of the Cd2+ ion (0.92 Å) (present in spinel ferrite MgCdCoFe)
is compatible with the ionic radii of the Y3+ ion (0.92 Å). The
cadmium ion can easily occupy the yttrium ion site, which can
decrease the lattice constants of pure YIG in the composite.
The crystallite size ‘D’ of the composites is calculated using
Scherrer’s formula (Eq. (4)) [54].
Kλ
D=
β cos θ
where K, λ and β are the Scherrer’s constant (0.9), the wavelength
of the X-ray source (0.15406 nm) and the full-width half maxima
(FWHM, units are radians), respectively. Here the value of ‘θ ’ for
the composites is taken to correspond to the value of ‘θ ’ for YIG.
From Table 1, it is also clear that the composites have a larger
value of ‘D’, contrary to the parent ferrites. This is because of the
nano-dimensional particle sizes of the prepared composites [55].
As the nano-dimensional composites have a higher possibility
of contact with other crystals [56], there is easy transport of
electrons from one crystal to another and therefore the crystal
size increases. With the inclusion of the spinel phase in the
composites, the value of ‘D’ increases for the x = 0.3 to 0.9
(1) composites from 42.1 to 51.1 nm and 26.4 to 35.2 nm for both
the garnet ferrite phase (Y) and the spinel ferrite phase (M),
respectively. The value of ‘D’ is less for the x = 0.3 composites,
which have a higher content of MgCdCoFe (70%) as compared to
YIG (30%). The lesser value of ‘D’ for the x = 0.3 composite may
be because the spinel ferrite is enhancing the crystal growth to
a further extent. After that, it is restricting the crystal growth
of YIG in the composite due to the presence of stress or strain.
As the MgCdCoFe content starts decreasing in the x = 0.6 to 0.9
composites, the crystal growth is enhanced and the crystallite size
increases. The micro-strain of the composites has been evaluated
by using Eq. (5) and the results are summarized in Table 1. The
lattice strain has been plotted via the Williamson-Hall (W-H) plot,
which is a first-order approximation to extricate lattice-strain
from the X-ray line broadening. Fig. 2 represents the W-H plot
for the composites.
β
ε= (5)
4 tan θ
Using the FullProf Suite programme, the observed XRD data
were refined via the Rietveld method in a two-phase model. The
observed and computed diffraction patterns of all the composites
by Rietveld refinement are shown in Fig. 3 (a–c). By reducing
the discrepancy between the calculated and observed diffraction
peaks, the XRD data of the garnet ferrite phase and spinel ferrite
phase present in the composites were refined. A very good agree-
ment between the calculated and observed XRD profile has been
established. For each of the composites, the values of several R-
factors, including Rexp (expected profile factor), Rp (profile factor),
Rwp (weighted profile factor), refined half-width parameters (U, V,
(4) W), goodness of fit (GoF), phase fractions (in composites) and chi
square (χ 2 ), are tabulated in Table 3. The low values of various
R-factors, along with the lower value of (χ 2 ), support the strong
agreement between the improved model and experimental data.
The refined values of the isothermal parameters and oxygen
positional parameters are shown in Table 3.
The GFourier programme was run to characterize and visualize
the electron density inside the unit cell. The one of the main
4
A. Sharma, Dipesh, H. Mahajan et al. Nano-Structures & Nano-Objects 36 (2023) 101035

Fig. 2. The Williamson-Hall plots for the approximation of micro-strain (ε ) for the composites (a) YM0.3, (b) YM0.6 and (c) YM0.9.

Table 3
Refined parameter, reliability factor (Rp ,Rwp ,Rexp ), refined half-width parameters (U, V, W) chi-square (χ 2 ) and good
of fit (GoF) of the prepared samples.
Parameters YM0.3 YM0.6 YM0.9
λ(Å) 1.54056 1.54056 1.54056
Cycles of 15 15 15
refinement
Step (◦ ) 0.02558 0.02558 0.02558
Profile function Pseudo-Voigt * Pseudo-Voigt * Pseudo-Voigt*
Rp (%) 15.6 15.2 13.5
Rwp (%) 10.5 11.7 12.5
Rexp (%) 8.7 9.4 9.7
U 0.00273 0.14976 0.05094
0.00114 0.03272 0.03272
V −0.00762 −0.00762 −0.04036
−0.00762 −0.04460 −0.04460
W 0.00543 0.00625 0.02163
0.00517 0.01798 0.01798
χ2 1.5 1.2 1.6
GoF 2.1 2.5 2.8
Fraction (%) Phase 1(YIG): 36.10 Phase 1: 57.50 Phase 1: 89.50
Phase 2(MgCdCoFe): 63.9 Phase 2: 42.50 Phase 2: 10.50
Space group of I a −3 d I a −3 d I a −3 d
phases fd-3 m fd-3 m fd-3 m

outcomes of the Rietveld refinement is electron density mapping.
For known or unknown crystals, the visualization is crucial for
identifying the atomic positions of constituent elements within
the unit cell; for example, thicker electron density contours in-
dicate the position of a heavier element among the unit cell
5
primary. The electron density maps can then be visualized as 2-D
or 3-D Fourier maps. Three-dimensional map uses a chicken-wire
style mesh to indicate a single level, in contrast to traditional two-
dimensional maps that depict varied densities using contours
(and occasionally colour). Fig. 4(a) displays the 2-D maps for the
A. Sharma, Dipesh, H. Mahajan et al. Nano-Structures & Nano-Objects 36 (2023) 101035

Fig. 3. Rietveld refinement of the composites (a) x = 0.3, (b) x = 0.6 and x = 0.9.

Fig. 4. (a) 2D electron density mapping (b) 3D electron density mapping of the x = 0.3 sample.

composite x = 0.3. The zero-level density contour is depicted in
white, however the reddish to orange-coloured sections denote
an increase in electron density levels close to the Y/Cd/Co and
Fe/Mg cations respectively. The 2D maps of the composites il-
lustrates the stark contrast in scattering densities between the
oxygen anion, Y/Cd/Co and Fe/Mg cations.
6
A 3-D Fourier image of each individual atom in the unit cell
for the composite (x = 0.3) is shown in Fig. 4(b). The pronounced
positive peaks associated with the heavy metals Y/Cd/Co are
present in the composites. There are some intermediate nuclear
density peaks that correspond to the Fe/Mg cations. The lower
density peaks correspond to oxygen (O) anions.
A. Sharma, Dipesh, H. Mahajan et al. Nano-Structures & Nano-Objects 36 (2023) 101035

Table 4 Table 5
Calculated X-ray density (Dx ), bulk density (Db ), porosity (P) and relative density Calculated grain size from the
(Dr) for the samples. micrographs of the samples.
Sample Dx Db (g/cm3 ) P% Dr (%) Sample Grain size (µm)
Y 5.03 4.82 4.05 96.0 Y 0.80 ± 0.003
M 5.41 4.83 10.7 89.2 M 0.70 ± 0.001
YM0.3 5.53 5.31 3.95 96.0 YM0.3 0.74 ± 0.001
YM0.6 7.58 6.42 15.2 84.8 YM0. 6 0.88 ± 0.001
YM0.9 9.67 8.25 14.7 85.3 YM0.9 0.97 ± 0.001

3.2. Density and porosity study
The value of X-ray density (Dx ), bulk density (Db ), porosity (P)
and relative density (Dr ) was calculated using Eqs. (6), (7), (8) and
(9) respectively [5,57] and the results are tabulated in Table 4.
MZ
Dx =
NA a3
where ‘M’ is the molecular weight of the sample, ‘Z ’ is the number
of molecules per unit cell (for spinel and garnet ferrite Z is 8), ‘N A ’
is Avogadro number (6.023 × 10−23 ) and ‘a’ is the lattice constant.
M known to be aided by oxygen exchanges within the material,
Db =
π r 2d
where ‘M’ is the mass of the pellet, ‘r’ is the radius and ‘d’ is the
thickness of the pellet.
Dx − Db
P =( ) × 100
Dx
(
Db
) grain formation. The secondary-phase of MgCdCoFe nanoparticles
Dr = × 100%
Dx
From Table 4, it is clear that all the prepared composites have
good bulk and relative density. This indicates that the sintering
temperature is sufficient for the preparation of YIG and MgCd-
CoFe. The YM0.3 composite has the least porosity and a high
relative density. This implies that the presence of 70% of MgCd-
CoFe enhances the densification of YIG in the composite. The
better densification in the composite is due to good packing [58].
3.3. Morphological study
A morphological study is important to understand the shape
and size of grains. The grain size and morphology of the samples
further affect the magnetic, dielectric and many other physical
properties. The morphological study was carried out with the
help of FESEM and TEM micrographs. Fig. 5 (a–e) represent the
FESEM micrographs of the prepared samples. Fig. 5(a) and (b)
represent the micrograph of the YIG and MgCdCoFe samples,
respectively. It has been found that YIG has roughly spherical-
shaped grains, whereas MgCdCoFe has cubic shaped grains. Fig. 5
(c–e) represent the micrographs of the YM0.3, YM0.6 and YM0.9
composites. It can be seen that two different morphologies of
grains (spherical and cubic) are present in all the composites.
The composite with x = 0.3 has less porosity contrary to other
composites because of the stronger packing of the garnet and
spinel ferrites. The spherical shaped YIG grains have some voids
or spaces, which are further occupied by the grains of MgCdCoFe.
For a higher packing mechanism, two conditions, (a) near about
30% fine and 70% coarse grains and (b) two different grain sizes
should be in the samples. In the synthesized samples the pores
can be seen from the micrographs [58]. The calculated porosity
matches the FESEM images. The grain size was calculated by
putting 10 intercept lines on the micrographs with the help of
ImageJ software. The line intercept method was followed to get
the values of the grain sizes, which is mentioned in Eq. (10) [51]
and tabulated in Table 5. Herein ‘L’ is the line length, ‘m’ is
magnetization and ‘n’ is number of intersects. The grain size of
the materials lies between 0.57 and 0.8 µm. The YM0.9 composite
has a larger grain size, whereas YM0.3 has the smallest least
grain size. The composites have a difference in grain sizes due to
(6) the grain boundaries migration between the two phases having
restricted solubility [59]. The restricted solubility of two ferrites
phases in the composites is because of the difference in the
morphology, crystallite size and presence of different ions with
different ratios. Due to which the two ferrites in the composites
can bond up to a certain limit. The process of grain growth is
(7) which take place at pores and grain boundaries. By transferring
electrons across multivalent cations more precisely and by reduc-
ing Fe3+ to Fe2+ ions at high sintering temperatures, this oxygen
transport is possible [60]. The above-discussed reduction with the
occurrence of Fe2+ ions, caused by the inclusion of MgCdCoFe,
(8)
prevents uncontrolled Fe2+ reduction, which in turn prevents
(9) obstructs the motion of grain boundaries, the MgCdCoFe ferrite
phase prevents the grain development of YIG in the composite
nanofibers. Since a two-phase system with mutually constrained
solubility typically results in grain expansion by grain boundary
migration, this process is known as long-range diffusion [61].
Each ferrite will have some degree of control over the grain
growth because of the separating effect brought by another phase
at the time of calcination. So, generally spinel ferrite influence the
growth of the garnet ferrite and vice-versa, which further restricts
the grain boundaries’ motion.
1.5 L
grain size = (10)
mn
Transmission electron microscopy (TEM) is the primary method
for investigating the internal microstructures or nanostructures of
any material. High resolution transmission electron microscopes
(HR-TEM) make it easier to image the crystal structure of samples
at the atomic level. Two samples (x = 0.3 and 0.6) were chosen
and investigated by transmission electron microscopy (TEM) at
high magnification in order to offer additional results on the
morphology of the grains in more detail. Fig. 6 (a and c) and
(b and d) represents the TEM image and high-resolution image
(HRTEM) of the composites x = 0.3 and 0.6, respectively. TEM
scans supported the FESEM micrographs’ observation that the
grains in the composites’ structure show agglomeration. Inverse
finite Fourier transform (IFFT) was used to calculate the d-spacing
of the HRTEM pictures and the planes indexed in the XRD pattern
are used as a guide. The inter-planar distance (d) measured from
the (420) peak in the XRD spectrum is confirmed by the inter-
planar distances for the two specimens in the HRTEM images. The
obtained values of the d spacing are 0.27 and 0.28 nm for the x
= 0.3 and 0.6 samples, respectively, which are shown in the inset
of Fig. 6(b) and (d). These values of the d spacing also withstand
with XRD observation. The composites have regular lattice planes.
The shapes of the particles are virtually spherical and cubic.
7
A. Sharma, Dipesh, H. Mahajan et al. Nano-Structures & Nano-Objects 36 (2023) 101035

Fig. 5. FESEM micrographs of (a) Y, (b) M, (c) YM0.3, (d) YM0.6 and (e) YM0.9 samples.

8
A. Sharma, Dipesh, H. Mahajan et al. Nano-Structures & Nano-Objects 36 (2023) 101035

Fig. 6. TEM micrographs of samples (a) YM0.3, (c) YM0.6 and HRTEM images of samples (b) YM0.3 and (d) YM0.6.

3.4. Composition study Table 6

The quantitative information about the composition for the composites YM0.3
and YM0.6.
To confirm the presence of all the elements in the prepared
Elements YM0.3 YM0.6
nanocomposites, EDX has been carried out. The spectra of the two
composites YM0.3 and YM0.6 are as shown in Fig. 7 (a and b). Weight % Atomic % Weight % Atomic %

From these spectra, it has been observed that both the composites O 20.65 47.1 7.72 22.89
Mg 4.61 5.8 1.89 3.69
have the presence of the desired elements without any other
Fe 60.84 39.8 74.42 63.22
undesirable elements. This confirms the successful synthesis of Co 6.62 4.11 7.73 6.22
the phase pure nanocomposites. The quantitative analysis of the Y 3.91 1.90 4.46 2.38
composition in terms of atomic and weight percentage has been Cd 3.37 1.10 3.78 1.60
tabulated in Table 6. Total 100 100 100 100

3.5. Magnetic properties study

The room temperature magnetic parameters of the prepared
samples were examined by employing a vibrating sample mag-
netometer (VSM). Important magnetic parameters, like rema-
nence magnetization (M r ), saturation magnetization (M s ), coer-
civity (H c ), squareness ratio (SQR), anisotropy constant (K eff ) and
9
magnetic crystalline anisotropy (H a ), were calculated through the
hysteresis curve (Fig. 8). These values are tabulated in Table 7.
Fig. 8 depicts that all the prepared samples exhibit S-shaped
magnetization versus applied field (M-H) loop, which indicates
superparamagnetic behaviour. There is no double magnetic phase
A. Sharma, Dipesh, H. Mahajan et al. Nano-Structures & Nano-Objects 36 (2023) 101035

Fig. 7. EDX spectra and elemental mapping of the (a) YM0.3 and (b) YM0.6 composites.

10
A. Sharma, Dipesh, H. Mahajan et al. Nano-Structures & Nano-Objects 36 (2023) 101035

Table 7
Important magnetic parameters deducted from the magnetization vs applied field loop.
Sample Hc (Oe) Mr (emu/g) Ms (emu/g) Keff (erg/cm3 ) Ha SQR
Y 31.2 ± 1.67 1.3 11.4 370.2 65.1 0.05
M 176.1 ± 1.37 10.6 44.0 8075.8 367.1 0.24
YM0.3 99.2 ± 0.94 5.3 41.0 4207.9 206.7 0.13
YM0.6 61.94 ± 0.50 7.6 40.7 2625.9 129.0 0.08
YM0.9 9.64 ± 0.53 0.41 27.1 271.8 20.1 0.01

with a bend in the hysteresis loops and no superimposition of

two loops has been observed. So, the prepared composites have
single smooth M-H curves (Fig. 8). This implies that exchange
coupling exists between the garnet and spinel ferrites [62]. The
reason for the formation of a single magnetic curve is that the
mechanical blending method has provided the proper mixing of
the two ferrites. This claim can be evident from the MH loop, as
in second quadrant the reversal of magnetization has no kink and
therefore there is no individual switching of the garnet and spinel
ferrites [63]. Such phenomena only occurs when the mixing of
ferrites has been done properly. The SQR values for all the pre-
pared samples are less than 0.5 and lie between 0.008 and 0.24,
indicating the existence of multi-magnetic domain structures.
It has to be noted that the prepared composites have a soft
magnetic nature because of lower Hc and higher Ms values. MgCd-
CoFe (M) has a higher value of Hc as compared to YIG (Y), because
of higher magneto-crystalline anisotropy (Ha ). The composite
YM0.3 has a smaller grain size, so it has a larger Hc value as
compared to the other composites. With an increase in grain Fig. 8. Magnetization (M) versus applied field curve for the samples.
size, Hc decreases because the single domain size of the grain
changes to a multi-domain structure and it requires a less mag-
netic field for magnetic alignments [64]. The Ms values for all in the 12 to 17 GHz frequency range. The permittivity of the
the composites are high as compared to YIG. This is because composites follows an oscillating trend which may be due to the
with the incorporation of MgCdCoFe, a disorder in spin, change in fluctuation in the polarization of the ferrites with variation in
surface morphology and anti-phase disorder takes place [65,66]. frequency. Singh et al. have also observed such a non-linear vari-
The lower coercivity of YM0.9 composites is promising for the use ation of the real part of the permittivity (ε ’) and described that
in switching devices, whereas the larger coercivity of the YM0.3 such behaviour is not of the relaxation or resonance type [67]. The
composite material shows potential suitability for utilization in polarization in the microwave frequency region is mainly due to
high-frequency applications. The values of Ha and Keff are greater the presence of different dipoles. These dipoles are formed from
for the YM0.3 composite as compare to the other composites. a variety of cations and anions present in the ferrite composites,
This means that it is harder to switch the magnetic field of like Mg2+ , Y3+ , Fe2+ , Fe3+ , Cd2+ , Co2+ and O2− . The strength of
the composite. The interparticle interactions, in addition to the different dipoles required different times to polarize, that results
magneto-crystalline and surface morphology, are a major factor in the non-linear behaviour of ε ’ [68–71]. The strength of the
for the variation of magnetic anisotropy (Keff ). Strong interpar- dipole is linked with the angles and inter-ionic distance, so as a
ticle interactions can have an impact on a system’s magnetic result non-monotonic variations have occurred in the composites.
behaviour and on Keff , especially when low magnetic fields and Xie et al. and Arora et al. have obtained spectral fluctuations due
low temperatures are present. to the equipment’s exceptional sensitivity and were viewed as
allowable measurement deviations [72]. The dispersion behaviour
To verify the presence of exchange-coupling between the soft
of the composites occurs beyond a frequency of 17 GHz. The
phases in the garnet and spinel ferrite nanocomposites, switching
composite YM0.3 has a higher permittivity value as compared to
field distribution curves (SFD) were plotted as the derivative of
YM0.6 and YM0.9. The values of ε ’ for the composites at 14.5 GHz
magnetization (dM/dH) against the applied magnetic field (H)
frequency are given in Table 8. For the YM0.3 composite the value
(Fig. 9). In the case of nanocomposites with strong exchange-
of ε ’ is ∼19.5. This is because of the lower porosity and high
coupling, a single peak is observed in the dM/dH plot. This in-
density of this composite [58].
dicates that the garnet and spinel phases are interacting strongly
Fig. 10 (B) illustrates the fluctuations of the real component of
with each other. However, in non-exchange coupled composites, the permeability (µ’) with frequency for all the composites. The
the SFD exhibits two distinct peaks, corresponding to the indi- variation also does not exhibit a frequency dispersion. The non-
vidual switching of the two soft magnetic spins (as shown in the linear variation of the real part of the permeability and frequency
inset of Fig. 9(c)). has been obtained in the 12 to 17 GHz range. In general, there
can be resonances due to magnetic domains which can cause a
3.6. Microwave dielectric and magnetic study for antenna non-monotonic frequency dependence of the permeability. Such
domain wall resonance occurs at 1 GHz [67,73,74], however our
3.6.1. Permittivity and permeability examined frequency range (12–18 GHz) is much larger than this
The variations of the real part of the dielectric permittivity (ε ’) frequency. So, domain wall resonance is absent in the prepared
and magnetic permeability (µ’) with frequency in the Ku-band for composites. Ferromagnetic resonance (FMR) may also be absent
the composites are shown in Fig. 10 (A) and 10 (B), respectively. in the frequency range for the ferrite composites.
From Fig. 10 (A), it has been observed that the dielectric spectra Pubby et al. have reported that the Co-Mg-Zr spinel ferrite
do not show dispersion behaviour (as explained by Koop’s theory) possesses ferromagnetic resonance at 32 GHz [75]. Othman et al.
11
A. Sharma, Dipesh, H. Mahajan et al.
Fig. 9. Switching field distribution curves of composites (a) YM0.3, (b) YM0.6 and (c) YM0.9.
have reported that the YIG composite possesses ferromagnetic
resonance at 20.91 GHz [76]. Sharma et al. have reported that
YIG ferrite gives ferromagnetic resonance at 20 GHz [77]. This
means that in the Ku band, the FMR of spinel ferrite and YIG will
be absent. From Table 8 it can be concluded that the composite
YM0.3 has a higher value of µ’ (∼2.8) as compared to the other
composites. The reason for the higher value of the permeability
is lower porosity and higher densification of the composite. The
permeability is dependent on grain size (D), saturation magneti-
zation Ms and magneto-crystalline anisotropy, as per the equation
µ∼Ms2 D/(K eff )0.5 . The YM0.3 composite has a higher value of Ms
and moderate grain size. The composite x = 0.3 exhibits the
highest value of magnetization (µ’). This suggests that there is a
strong exchange-coupling between the high and low permeable
phases in the composite. This strong interaction between the
phases could be the reason for the high magnetization observed
in the composite.
3.6.2. Dielectric and magnetic losses
The dielectric losses in samples occur due to vibrations of
dipoles. Dielectric tangent loss is an estimation of the energy
dissipation from an external electric field [6]. The loss associated
with the dielectric tangent is attributed to the phenomenon of
domain wall resonance, due to pores, grain boundaries and im-
purities present in the structure of ferrites [78]. The magnetic
loss in the samples is due to losses in hysteresis, domain wall
displacement (also known as resonance relaxation loss) and eddy
current loss. At higher frequencies, the losses are dependent
on morphology or grain sizes [7]. Fig. 10 (C) and (D) represent
the dielectric and magnetic losses in the composite from 12 to
18 GHz. Experimental observations indicate that all the compos-
ites exhibit lower values of both dielectric and magnetic losses. It
has been noticed that losses are approaching the negative values,
which is due to less signal to noise ratio or fixture error. Table 8
summarizes the dielectric and magnetic loss tangents of all the
composites at 14.5 GHz. The composite YM0.3 has the minimum
value of ∼0.009 for the dielectric loss tangent and ∼0.002 for the
magnetic loss tangent at 14.5 GHz. The reason for lower losses
is that the higher content of MgCdCoFe in the YIG composite
suppresses the overall grain growth. This decreases the porosity
and increases the density as the spinel ferrites segregate at the
grain boundaries of YIG, due to which the grain size reduces and
hence the losses also decrease [7].
3.6.3. Miniaturization factor of antenna
The miniaturization factor decides the compactness of the
antenna. The higher the miniaturization factor, the more the com-
pact size of the antenna is. The miniaturization factor is calculated
using Eq. (11) [79].
√ YIG/MgCdCoFe can be an excellent candidate for high frequency
ηi = ε ′ µ′
Nano-Structures & Nano-Objects 36 (2023) 101035
Table 8
Calculated permittivity, permeability, dielectric and magnetic loss tangent and
miniaturization parameters at 14.5GHz for the composites.
Sample ε’ µ’ tan δε tan δµ ηi
YM0.3 19.5 2.8 0.009 0.002 7.2
YM0.6 3.57 1.2 0.5 Negligible 1.7
YM0.9 3.90 1.1 0.12 Negligible 1.8
From the above equation, it is clear that the miniaturization fac-
tor ηi depends upon permittivity and permeability values. From
Fig. 10 (E), it is clear that the YM0.3 sample has larger values of
ηi as compared to the other composites. The values of ηi for all
samples at 14.5 GHz are presented in Table 8. The sample YM0.3
has the highest value of ηi (∼7.2) at 14.5 GHz.
4. Conclusions
Garnet ferrite (YIG) and spinel ferrite (MgCdCoFe) samples
have been synthesized using the sol–gel auto combustion method.
The composites of YIG/MgCdCoFe with composition x = 0.3 (30%
YIG, 70% MgCdCoFe), x = 0.6 (60% YIG, 40%) MgCdCoFe and x
= 0.9 (90% YIG, 10% MgCdCoFe) were prepared by a facile me-
chanical blending method. The Rietveld refined XRD graphs reveal
that both phases of YIG and MgCdCoFe are present independently
in the composites. The 2D maps of the composites illustrate the
stark contrast in scattering densities between the oxygen anion,
Y/Cd/Co and Fe/Mg cations. The composite with x = 0.3 has good
compactness because of the enhanced packing of the grains of
the two ferrites. The composite with x = 0.3, also results in
higher densification and lower bulk density as compared to the
other composites prepared. The obtained TEM images supported
the FESEM micrographs’ observation that the grains in the com-
posites’ structure show agglomeration. The calculated values of
the d spacing from HRTEM withstand with XRD observation. The
magnetic properties of the composites exhibit variations that
correspond to changes in the composition of the ferrites. The
x = 0.3 composite has the maximum Hc value, whereas the x
= 0.9 composite has the minimum value of Hc , which suggests
its potential application in switching devices. All the composites
offer a high value of saturation magnetization (Ms ). The YIG
and MgCdCoFe phases were shown to be well exchange linked
by coherent demagnetization curves (dM/dH) for the x = 0.3
and 0.6 composites. Among the composite studied, the x = 0.3
composite offers very good magneto-dielectric properties with
high ε ’ (∼19.5) and µ’ (∼2.8) values. It has to be noted here
that for this composite, the dielectric and magnetic losses are of
the order of 10−2 only. The miniaturization factor is also high for
the x = 0.3 composite. So, we conclude that the composite of
(11) Ku band antenna applications and for microwave devices.
12
A. Sharma, Dipesh, H. Mahajan et al. Nano-Structures & Nano-Objects 36 (2023) 101035

Fig. 10. Variation of (A) permittivity, (B) permeability with frequency, (C) dielectric loss tangent, (D) magnetic loss tangent and (E) obtained miniaturization factor
for samples at a frequency from 12–18 GHz.

13
A. Sharma, Dipesh, H. Mahajan et al.
CRediT authorship contribution statement
Anjori Sharma: Writing – original draft, Conceptualization,
Sample preparation, Formal data analysis. Dipesh: Software, Per-
formed XRD. Hamnesh Mahajan: Performed FESEM. Neha Aggar-
wal: Performed VNA. Subhojyoti Sinha: Language editing. A.K.
Srivastava: Editing manuscript, Data analysis, Conceptualization.
Declaration of competing interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
Data availability
No data was used for the research described in the article.
Acknowledgements
Anjori Sharma, Dipesh, Hamnesh Mahajan, Neha Aggarwal,
Subhojyoti Sinha, A.K. Srivastava
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