Current Applied Physics 29 (2021) 39–53

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Current Applied Physics

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

Review

Analysis of the role of M-type hexaferrite-based materials in

electromagnetic interference shielding
Shalom Ann Mathews, D. Rajan Babu *
Advanced Materials Research Centre, School of Advanced Sciences, Vellore Institute of Technology, Vellore, 632014, India

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

Keywords: M-type hexaferrite has attracted much attention for its large magneto-crystalline anisotropic energy, excep­
M-type hexaferrite tionally good chemical stability, corrosion resistance, high Curie temperature, and high coercivity. In this review
Spinel ferrites paper, our goal is to examine the microwave absorption properties and related studies of M-type hexaferrite-
Exchange-coupling
based materials. The microwave absorption properties of hexaferrite-based materials in the S, X, and Ku-band
Microwave absorption
are discussed with their corresponding reflection losses. Complementarity between magnetic loss and dielec­
Reflection loss
tric loss is found to have a great impact on the proper absorption of microwaves. The mechanisms corresponding
to the microwave absorption in different morphologies and structural adaptations of hexaferrite have been
elaborated in the article. The ongoing trends and future perspectives of these materials are also outlined.

1. Introduction synthesis reported for the preparation of metal oxide compounds. This
include techniques such as modified flux method [9–11], sol-gel
1.1. Ferrites: discovery, structure, and progress in applications [12–14], chemical co-precipitation [15,16], hydrothermal method
[17,18], solid-state reaction [19,20], etc. M-type hexaferrite has been
Investigated, studied, and applied in various fields for more than the under constant examination for its structural, morphological, and
past 50 years, ‘ferrites’ are one of the most inevitable parts of modern magnetic properties. Few of the very recent investigations into these
science and technology [1,2]. Ferrimagnetic transitional metal-oxides, hard ferrites include; the relation between the effect of different
better known as ferrites, have many forms of existence in nature, like annealing temperature and features such as microstructure, chemical
iron (III) oxide (FeO), maghemite (γ-Fe2O3), haematite (α-Fe2O3). homogeneity as well as morphological and magnetic parameters of
Magnetite/lodestone (Fe3O4) is the most abundant, naturally occurring, barium ferrite (BaM) nanoparticles as reported by Trukhanov et al. [21],
the strongest magnetic material on earth [3]. The earliest known usage Vinnik et al. reported the doping mechanism in M-type hexaferrite and
of lodestone dates back to the 12th century, by the Chinese. It was used the magnetic phase state of the doped BaM [22]. Li, Jun, et al. have put
as a part of the compass for navigation; also by the mariners for the easy forward an investigation on the co-substituted BaM and its microwave
placing of the North, instead of following the stars [4,5]. No studies were absorption capacity at lower frequencies [23]. Similarly, Lim et al. has
done on the ferrites until the 1930s. Prof. Takeshi Takei and Prof. Kato analysed the performance of the co-substituted strontium ferrite (SrM)
from Japan (1933), became the first to recognize the promising potential on the electromagnetic wave absorption properties [24]. Zandalazini
of the properties of ferrites. Later, soft and hard ferrites were produced et al. reported on the direct impact of the BaTiO3 on the magnetic pa­
on a large scale and commercialized by J.L. Snoek and Philips respec­ rameters of BaM by the formation of a double-layered thin-film structure
tively [6]. Two of the most common ferrites having different crystal [25]. On the other hand, cubic spinel ferrites take the chemical formula
symmetrical structures are hexaferrite and cubic spinels. Hex­ MO.Fe2O3, where M typifies a divalent ion. CoFe2O4, which falls under
agonal/hexaferrite are the magnetically hard materials with the chem­ the category of cubic ferrite structure, is the first useful ferrite that was
ical formula MFe12O19, here M represents Ba2+, Sr2+, and Pb2+ [7]. man-made. This was prepared by Kato and Takei in 1933 [5,6]. This type
Hexaferrites are largely used as permanent magnet materials, due to of ferrite is a soft magnetic material, with high magnetic saturation and a
their large magneto-crystalline anisotropy, high coercivity, high Curie very low coercive field. The low magneto-crystalline anisotropy of the
temperature, corrosion resistance, etc. [8]. There are many modes of soft material leads to a lower coercive field when an external magnetic

* Corresponding author.
E-mail address: [email protected] (D.R. Babu).

https://doi.org/10.1016/j.cap.2021.06.001
Received 6 January 2021; Received in revised form 21 May 2021; Accepted 5 June 2021
Available online 11 June 2021
1567-1739/© 2021 Korean Physical Society. Published by Elsevier B.V. All rights reserved.
S.A. Mathews and D.R. Babu Current Applied Physics 29 (2021) 39–53

field is applied. Few of the recent relevant reports on the spinel ferrites Me2W – BaMe2+ 3+
2 Fe16 O27
are; the correlation between the microstructural parameters and the
anti-cancer activity of rare-earth-doped Mn–Zn ferrites as studied by Me2Y - Ba2Me2+ 3+
2 Fe12 O22
Almessiere et al. [26], Liu et al. reported the technique of ‘electric
current-assisted synthesis method which lowered the sintering temper­ Me2Z – Ba3Me2+ 3+
2 Fe24 O41
ature and shortened the period required for the phase formation of
Where, Me2+ is Zn2+, Fe2+, Co2+, etc [68].
Ni–Zn ferrite [27]. Ghosh et al. explored that the appropriate incorpo­
These compounds have gained much interest because of their large
ration of rare-earth material into a spinel ferrite could lead to an ex­
anisotropic fields, high resistivity, and high permeability allowing their
change bias field between the ordered spins at the core and the
operation in devices at a higher frequency range [69]. The crystallog­
disordered spins at the surface and also enhance their
raphy of the hexaferrite is such that it embodies the stacking of three
magneto-crystalline anisotropy [28]. Almessiere et al. investigated and
layers which are called the R, S, and T blocks having two, three, and four
successfully identified rare earth substituted Ni–Cu–Zn spinel ferrite as a
anion layers respectively [70,71].
potential material to be used in radio-electronic devices [29]. The in­
clusion of Ni–Zn ferrites into the host matrix of polyaniline for micro­
1.3. M-type hexaferrites
wave shielding applications was reported by Kumar et al. [30]. Since the
focus of our review is M-type hexaferrite, an explanation of the spinel
M-type hexaferrite is one of the best and the most studied permanent
ferrite structure and its properties are not discussed in detail. Ferrite
magnetic material. This type of hexaferrite has the chemical formula
applications (both hexaferrites and spinel ferrites) are widely extended
MFe12O19, M denotes Ba, Sr, and Pb [72–74]. Since the discovery of
to various areas, such as in equipment used for telecommunication [31,
M-type ferrites in the Philips laboratories, Netherlands in the 1950s, the
32], magnetic recording devices [33,34], magnetic resonance imaging
influence of these ferrites in science and technology were investigated in
[35–37], targeted magnetic drug delivery [38–43], in gas sensing
detail [75,76]. Magnetically, these ferrites crystallize in an uniaxial di­
[44–46], hyperthermia [47–49], catalysis [50–52], microwave absorp­
rection parallel to c-axis [75]. They have been extensively researched
tion [53–55], giant magneto-impedance [56–58], environmental reme­
and commercialized because of some of their remarkable properties
diation [59–61], as transformer core materials [62,63], in biomedicine
such as a large anisotropic field of 1.7 T [74,77], high Curie temperature
[64–66]. Ferrite applications are schematically represented in Fig. 1,
[78], high resistivity [79], low dielectric loss [80], high chemical sta­
with examples.
bility [81,82], high coercive field [74], low cost [83], good corrosion
resistance [84], ferromagnetic resonance frequency above 40 GHz [85,
1.2. Hexagonal ferrites/Hexaferrites 86].
Barium ferrite (BaM) possesses the RSR*S* structural stacking. The
Hexagonal ferrites, commonly known as hexaferrite are of six types. ‘R’ represents a hexagonal symmetry and ‘S’, a spinel structure, and
The bonding between the atoms as well as the crystal structure of these these blocks are alternately stacked. The asterisk (*) depicts the 180◦
six compounds varies. The six planar hexaferrite structures namely, M-, rotation of their respective structures. The ‘R’ in this crystal structure
W-, X-, Y-, Z- and U- type were first described by Braun in 1957 [67]. constitutes a three-layer oxygen block with the composition BaFe6O−11
and ‘S’ encrusts a two-layered structure with the formula Fe6O+ 8 . These
M- BaFe3+
12 O19 structures are intertwined with each other, formulating BaFe12O19

Fig. 1. Schematic representation of a few application of ferrites, with examples.

40
S.A. Mathews and D.R. Babu Current Applied Physics 29 (2021) 39–53

[87–89]. Fe3+ ions are placed non-equivalently in five different crys­ increase in the technological efficiency of the gadgets/electronic
tallographic positions – octahedrally coordinated 2a, 4f2, and 12 k; equipment demands a ‘smarter’ design of materials used in this aspect.
tetrahedrally coordinated 4f1; and 2 b is penta-co-ordinated to form a This demand calls for some specificity in the requirements to develop
bipyramidal site [90,91] The schematic structural representation of material that is compatible with the equipment/gadget in use. ‘Thin,
M-type hexaferrite is given in Fig. 2. light, strong, wide’ denotes the basic properties for sequencing the
fabrication of a well-efficient MAM [99].
2. EMI shielding/microwave absorption The mechanisms inside a shielding material include absorption,
reflection, and transmission. The total shielding effectiveness of the
For the unperturbed functioning of an electronic equipment, non- shielding material is the sum of all these three processes [100,101],
interference of the electromagnetic waves in these devices are much which can be written as:
essential. This can be guaranteed by the usage of materials which would
SE = SEA + SER + SET (1)
absorb electromagnetic radiations that are primary as well as secondary
[92]. EMI shielding is the abbreviation used for electromagnetic inter­ where,
ference (EMI) shielding. This can be explained as the radiations being
shielded by either of the processes of absorption, reflection or multiple SET (dB) = 10log (1/T)
reflections. This phenomenon is also given the name of microwave ab­
SER (dB) = 10log (1/1-R) (2)
sorption since the procedure of absorption is much more efficient and
effective in its purpose, than the other processes. The materials used for SEA (dB) = 10log(1-R/T)
this sole purpose must be thickness limited [93], have a wide frequency
absorption band [94], must have a low density [95], possess high re­ The shielding due to multiple reflections, i.e, reflections within the
sistivity [96] to name a few. We could name the 21st century as an material is mostly dominated by the other mechanisms and often are
‘electronic era’ and as the name suggests, the overuse of electronic neglected. The discussion about the electromagnetic shielding mecha­
gadgets has led us to electronic pollution or rather ‘wave pollution’. The nism leads to the very relevant participation of the parameters of com­
abundance of devices operating in the GHz range adversely affect either plex permittivity and complex permeability. The reliability of the EMI
the equipment in use or that which is nearby it [97,98]. shielding capacity of material especially absorption is primarily
measured as a function of complex permittivity/permeability vs fre­
3. Concise presentation of the mechanisms involved in the quency plots [102]. The term “complex’ refers to that the said param­
absorption of electromagnetic radiation eters have both real and imaginary parts. The real part of the complex
permittivity and permeability represents the stored energy in the ma­
The immense increase in technology and communication has led to a terial and the imaginary part constitutes the energy lost through dissi­
tremendous rise in electromagnetic radiation, more specifically, mi­ pation as heat waves. The interaction of the incident EM waves and the
crowave radiation. This soar in the emission of EM waves has made it a material results in some changes in the material. The electric component
form of pollution, called by the names - ‘wave pollution’, ‘wireless of the EM wave incites two sets of currents, namely, displacement cur­
pollution’, etc. The need for decreasing radiation emission is being rent and conduction current. The displacement current emerges as a
addressed by the research society for over a decade. The everyday result of the bound charges (due to polarization), which directs to the
dielectric constant (ε′ - a real part of permittivity) of the material.
Whereas, the conduction current occurs as a consequence of the flow of
the charge carriers in the material, which brings about the dielectric loss
(ε”- imaginary part of the permittivity) [103]. The values of complex
permittivity and complex permeability are derived from the measure­
ment of scattering parameters (S-parameters) namely, reflectance S11
(or S22) and transmittance S21 (or S12). The schematic representation of
the S-parameters obtained from the vector network analyser (VNA) is
given in Fig. 3. Shielding effectiveness (SE) can be defined in simple
mathematical terms as the log of the ratio of the power of transmitted
EM waves through the material to the power of incident EM waves. The
power in this context can be equated to the intensity of the electric or
magnetic fields [104].

SE (dB) = 10 log10 PT/PI = 20 log10 ET/EI = 20 log10 HT/HI (3)

The absorptivity (A), transmissivity (T), and reflectivity (R) can be

stated as

A+T+R=1 (4)

where,

R = PR/PI = (S11)2 or (S22)2 (5)

2
T = PT/PI = (S21) or (S12) 2
(6)

PR= Power of the reflected wave

PT= Power of the transmitted wave
PI = Power of the incident wave

The microwave absorption performance of the material can be

Fig. 2. Structural overview of the M-type hexaferrite such as BaFe12O19, mathematically analysed by the transmission-line theory. The reflection
SrFe12O19 and PbFe12O19.

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S.A. Mathews and D.R. Babu Current Applied Physics 29 (2021) 39–53

Fig. 3. An illustration of (a) the interaction of the electric and magnetic waves and its direction of propagation
Fig. 3 (b) configuration of the S-parameters obtained and
Fig. 3 (c) the reach of EM waves (skin depth) with the increase in the thickness of the material.

loss (RL) of the single-layered material can be resolved as a function of 4. Other parameters crucial to the absorption of electromagnetic
the impedance of free space and input impedance at a given thickness of radiation
the absorber. Reflection loss is measured in terms of decibels (dB).
i) Conductivity and Dielectric properties
RL = 20log {(Zin-Z0)/(Zin + Z0)} (7)

Where, Zin = Z0(μr/εr)1/2 tanh{j[2πfd(μrεr)1/2]/c} (8) The volume content of ferrites influences the conductivity of the
composite material. The lesser the conductivity, the higher the skin
An in the case of multi-layered material with ‘x’ number of layers, depth due to low eddy current loss. This makes the material suitable for
then the input impedance of the xth layer can be expressed as: EM wave absorption [108]. Skin depth (δ) can be defined as the decrease
in the intensity of the incident EM wave to 1/e of its initial intensity. For
Zinx = Z0(μr/εr)1/2{[Zx-1+Z0(μr/εr)1/2tanh(j(2π/c)fd(μr/εr)1/2]/[Z0(μr/εr)1/2+Zx-
this reason, skin depth is an important factor in the absorption mecha­
1/2
1tanh(j(2π/c)fd(μr/εr) ]} (9)
nism by the material. This can be calculated using the equation:
Here, Zin = input impedance
δ = (2/ωμσac)1/2 (12)
Z0 = the impedance of free space
μr = relative permeability It is known from the studies that skin depth decreases with an in­
εr = relative permittivity crease in frequency and at higher frequencies, it is the surface conduc­
f = frequency tion that plays the role. Therefore, it can be inferred from the equation
d = thickness of the absorber material that for highly conductive, magnetic materials at higher frequencies, the
c = velocity of light in vacuum. skin depth can be less. When the skin depth is small, it leads to reflection
Zin equal to Z0, is the condition for impedance matching. Impedance from the surface of the material which results in a low absorption rate of
matching is one of the most relevant factors on which microwave ab­ the EM waves [109–111]. The interaction between the conductive part
sorption depends upon. Zero reflectivity of the electromagnetic waves of the material and the electromagnetic wave can be expressed in terms
from the absorber samples is ensured by impedance matching. And to of reflection loss as a function of the magnetic permeability and the
achieve this condition the ratio between input impedance and imped­ conductivity. The shielding effectiveness by absorption and reflection
ance of the free space must be equal to 1 [105,106]. The matching mechanism can be expressed as
thickness (tm) of the material can be determined from the quarter
wavelength mechanism. The matching thickness of the absorber mate­ SEA = 20(t/δ).log(e) = 20t(ωσμ’/2)1/2.log(e) (13)
rial is crucial for optimal absorption mechanism and this is dependent on and SER = 10log(σ/16ωε0μ’) (14)
the matching frequency (fm) [107].
respectively, where, t = thickness of the absorber, δ is the skin depth,
tm = nλ/4 = nc/[4fm(μrεr)1/2]; n = 1,3 and 5 (10)
σ is the conductivity of the material, ε0 is the permittivity of free space
Subsequently, the EM wave through a material (λ) can also be [112,113]. If the conductivity increases in the case of a composite, the
expressed as: value of permeability decreases (σr/μr). This leads to a larger (negative)
value of reflection loss. Whereas, the absorption loss can be distinctly
λ = λ0/ (|ε||μ|)1/2 (11) stated as the heat loss due to the interaction between the magnetic/di­
electric component of the absorbing material and the EM waves incident
λ0 = the wavelength in free space.
on them. In this case, absorption loss is a function of the product of σrμr,
|ε| = modulus of permittivity.
which indicates that both high values of permeability and conductivity
|μ| = modulus of permeability.
are required for a higher absorption loss. Studies reveal that reflection
The minimum reflection loss (RL) is related to the quarter wave­
loss-dominant shielding methods are much more efficient than the other
length (0.25λ) thickness of the absorber [102].
mechanisms. According to the different applications of the material in

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S.A. Mathews and D.R. Babu Current Applied Physics 29 (2021) 39–53

different frequency ranges, the range of conductivity is considered frequency, as the magnetic anisotropy of the hexaferrite is increased the
relevant. Conductivity value in the range of 10− 2 – 101 S/m is expected magnetization (spin) rotation takes charge and becomes accountable for
for materials is expected to shield EM waves effectively [100,114,115]. the complex permeability in the magnetic material. When the applied
The interaction between the conductive grains of the ferrite material and magnetic field is altered and the domain wall displacement and the
its weak conductive grain boundaries can be explained based on Koops rotation of the magnetization of the material lag behind it, then the loss
theory, based on the Maxwell-Wagner model of the two-layered struc­ in magnetic component (μ’’) is observed. The numerical closeness of ε′
ture of the dielectric material. The majority of Fe3+ ions and minority and μ′ is the desired factor in the set goal of impedance matching [125].
ions of Fe2+ hopping between the neighbouring grains is restricted by The hysteresis loss, ferromagnetic resonance loss, eddy current loss,
the resistive effect of the grain boundaries at lower frequencies. Thus, domain wall displacement, multiple scattering - all result in the mag­
electrons get collected at the boundaries, increasing the space charge netic loss of magnetic absorber material. In the microwave frequency
polarization inside the ferrite material. This mechanism is frequency and range, it is observed from various reports that, the eddy current loss and
temperature dependant and therefore at higher frequency and temper­ natural ferromagnetic resonance loss are involved prominently in the
ature, the hopping between the ferric and the ferrous ions becomes more contribution to the magnetic loss. Eddy current loss can be expressed as:
due to increased movement of the charge carriers. This leads to an in­
crease in conductivity at the grain boundaries and the conductivity of μ’’ = 2πμ0μ’2σd2f/3 (15)
the material increases remarkably [116–120]. When a conductive ma­ where σ denotes conductivity, f-frequency, μ0-permeability in a vacuum,
terial is added to a magnetic material, it leads to the shortening of the μ’ denotes the dielectric loss. In the case of dominance of eddy current
relaxation time during the change of the applied field. This battens the loss, it can be concluded that the part μ’’μ’− 2f− 1 is a constant [73,
dielectric loss of the nanocomposite [104]. It is reported that doping of 126–131]. Ferromagnetic resonance plays an important role in
Sr2+ instead of Ba2+, would increase the dielectric loss in the material contributing to the magnetic loss at a lower frequency. Theoretical
due to the increase in electrical conductivity [121]. studies show that losses due to eddy current effects do not depend on the
The mechanism of dielectric polarization which results in the operating frequency which suggests that this might be the major reason
dielectric properties of a material is quite similar to the conduction of for the magnetic loss in ferromagnetic absorbers [132]. The magnetic
charge carriers in the ferrite material. Both the mechanisms involve the parameters of a material are very significant in determining the
exchange of electrons between Fe2+ and Fe3+. So, this mechanism can be shielding efficiency of the material under consideration, here, hex­
explained in a similar manner. Dielectric properties of a material depend aferrite. The cationic distribution, the unpaired spins of the magnetic
on the frequency range in which it is measured, temperature, and also ions, super-exchange interaction of the cations in different lattice sites,
the different compositions of the material. The change in frequency magneto-crystalline anisotropy, compositional changes, along with
leads to a change in the electric field. The different mechanisms of po­ other factors – contributes to the magnetic behaviour in hexaferrite. The
larization play a significant role in tuning the dielectric parameters with magnetic response of a material can be easily drawn from the hysteresis
changes in frequency and temperature. These mechanisms include - loop, which is a plot of magnetization (M) vs. the externally applied
electric, ionic, dipolar, and space-charge polarization. While space- magnetic field (H). An ideal hard magnet would display a square hys­
charge polarization and dipolar polarization have an impact on the teresis loop. Squareness ratio (Mr/Ms) is a measure of how close the
dielectric properties at lower frequencies, electric and ionic polariza­ material is to idealistic. When the squareness ratio is or above 0.5, it can
tions are majorly responsible for the dielectric parameters at higher be assumed that the state of the material is in a single domain magnetic
frequencies. The dielectric constant of ferrite materials tends to decrease state [133]. The case is different when a hexaferrite is composited with a
or remain constant at higher frequencies, which is the expected behav­ soft ferrite. The behavioural pattern of the magnetic material changes
iour in ferrites. This is because, the dipolar polarization pertains at lower depending upon the spring exchange behaviour between the soft and the
frequencies whereas, the dipoles lag behind the direction of the alter­ hard magnets. As the exchange length between these two phases is
nating field at higher frequencies. With the increasing frequency, the increased, the interaction between them is compromised. The extent of
exchange of electrons lags behind the changing electric field, because of the reliability of the material for microwave absorption depends pri­
the smaller relaxation time. This decrease in the exchange of charge marily on the single-phase magnetic behaviour of the nanocomposite
carriers at the grain boundaries leads to a decrease in polarization. This [134]. (Discussed in section 5.1.1.). In this section, we have focussed on
leads to a decrease in the dielectric constant of the material. In the case the relation of the permeability of a material to the shielding effective­
of temperature dependency, the dielectric constant of ferrites is ness of a magnetic absorber.
observed to decrease with an increase in temperature. This is due to the
reason that after a certain temperature called the Curie temperature iii) Volume fraction of the ferrite content
(Tc), the material changes its magnetic ordering from ferromagnetic to
paramagnetic [122,123]. It is to be noted that with the increase in The absorption capacity of the material is closely related to its
dielectric material in a nanocomposite, the dielectric loss can be dielectric properties, which are affected by the volume percentage of the
considered as the loss of heat energy due to the combined effect of ferrite content in the composite. The concentration of the Fe2+ ions, to
conduction as well as due to the relaxation of the dipoles [95,124]. an extent, determines the variation in the dielectric properties. The
amount of ferrite content has an explicit impact on the conductivity of
ii) Magnetic property the composite material. In the case of ferrite/polymer nanocomposite,
the conductivity of the nanocomposite decreases with an increase in
As important as the dielectric parameters are to the absorber, ferrite content. The conductivity of the free charge carriers along the
permeability (magnetic energy component) plays a relevant role in the polymer chain is compromised by the insulating ferrite material. This
shielding capacity of the material. In the operating frequency range of leads to the decrease in free charge carrier density of the nanocomposite,
microwaves, M-type hexaferrite display high permeability, saturation thereby decreasing the electrical conductivity of the material [135]. The
magnetization, and magneto-crystalline anisotropic values, hence the relation between magnetic saturation of material and a single particle
importance of using the hexaferrite as a MAM. Permeability depends on expressed as:
two mechanisms, which are the domain wall displacement and the
magnetization (spin) rotation. The large magneto-crystalline anisotropy Ms = ϕms (16)
of the hexaferrite results in the magnetization rotation being the
clarifies that the magnetic saturation of the material (Ms) depends upon
dominant mechanism of the two. At a lower applied frequency, the
the volume percentage of the magnetic particles (ϕ) and the magnetic
domain wall displacement is found to be prominent. With the increasing

43
S.A. Mathews and D.R. Babu Current Applied Physics 29 (2021) 39–53

saturation of the single-particle (ms). When a polymer material is element, a change of crystallographic structural orientation can also
introduced to the ferrite material, depending upon the loading per­ take place [144]. This influences the extent of the absorption/shielding
centage of the ferrite material the magnetic parameters tend to change. mechanism. Vishal et al. [145] reported the design of strontium hex­
The diamagnetic order of the polymer material disrupts the ferrimag­ aferrite in the shape of a nano-disk for electromagnetic interference
netic order of the ferrite material, thus causing the Ms to decrease. shielding applications. The squareness ratio of this material exhibited a
Likewise, the Hc of the composite material is likely to change with the value of 0.608, implying a strong anisotropic symmetry favourable for a
alteration of charge density of the material which impacts the electron good MAM. The substitution of Ba2+ ions in the strontium ferrite lattice
spin and domain wall motion [136]. was found to densify the structure and increase the absorption rate than
the pure strontium ferrite [146]. Alireza et al. [147] justified that the
iv) Thickness of the absorber material substitution of Al3+ into the BaM structural lattice decreased the grain
size and transitioned the hexagonal plate-like structure into a
The thickness of the absorbent material is one of the several factors in rod-shaped structure. A maximum reflection loss of − 45 dB (where the
determining the minimum level of reflection loss. Alteration in the requirement for 99% of attenuation is ≤ to − 10 dB) was obtained for this
thickness of the material under study could impact the performance of substituted material. Mg–Sn doped strontium ferrite, as reported by
the absorption capacity of the material. Double layered material plays a Ghasemi et al. [148], claimed to have a greater surface area than the
significant role in improving the impedance matching of the material. pristine strontium ferrite material. The composite oxide was found to
Min et al. [137] reported the two-layered structure of BaFe12O19 and have lesser grain size (lesser particle size) which led to more defects on
graphite nanosheets which were employed to control the thickness and the surficial and the interfacial region. This caused the splitting of en­
enhance the absorption band of the material. The low permittivity ergy levels by morefold due to quantum confinement effect. When the
BaFe12O19 which would better the impedance matching was chosen as energy spacing between the levels is comparable to the incident mi­
the matching layer (d2) and the graphite sheets as the absorption layer crowave energy, it gets absorbed during the electronic transition from
(d1), backed by a metal plate. The matching layer ensures the maximum one energy level to another. Thus, increasing the electromagnetic
entrance of the incident microwaves into the absorption layer which in attenuation in the said material. A similar approach was made by Chen
turn lessens the reflection and transmission of the radiative waves. Ac­ et al. [14], in which La3+ was substituted to the Sr2+ site of M-type
cording to the study by Xu et al. [138], the coating thickness of the strontium ferrite and this justified the above mentioned impact of grain
absorber material is frequency dependant and can be expressed as: size shrinkage and increase in surface area of the nanocrystalline
structure. The influence of La3+ ions on the SrM lattice led to the partial
f = c/2πμ’’d (17) conversion of Fe3+ to Fe2+, increasing the electron hopping between the
where f is the frequency of operation, μ’’ is the magnetic permeability sites with different valence ions, thus enhancing the electric dipole po­
and d is the thickness of the absorber material. This feature can be larization. This increases the attenuation capacity of the material
regulated accordingly to be used in different frequency bands this tremendously. In this case, a minimum reflection loss of − 41.7 dB at a
enabling to modify the microwave absorption of the material. When the thickness of 2.3 mm.
material is to be operated at a higher frequency, the material can be
engineered at a lower thickness [139]. 5. An overview of the hexaferrite-based materials used for
microwave absorption
v) Shape and structural morphology of the absorber
The basic parameters to be looked upon in finding an efficient mi­
The shape of the absorber has an immense impact on the absorption crowave absorption are mentioned above. In this review article, the
capacity of the material under study. The increase in aspect ratio has focus is to inspect various methods and materials that have contributed
been reported to increase the minimum value of reflection loss and the to the research in microwave absorption studies.
bandwidth of the operating frequency. Wangchang et al. [140] reported
the design of a honeycomb microwave absorption material (HMAM) in 5.1. Summary of the interaction mechanism of prominent hexaferrite
ameliorating the efficiency of a microwave absorption material. The composites
effect of coating thickness, pore radius, the height of the honeycomb
structure on the reflection loss, and bandwidth of the frequency band 5.1.1. Hard/soft ferrite nanocomposites (magnetic absorbers)
was described in detail. One of the most effective analyses of the In recent years, much attention has been focussed on the hard/soft
structural morphology is the core-shell structure. The hard ferrite forms ferrite composite material.
the core and the soft spinel ferrite is coated on it as a shell. The closeness The combination of hard and soft magnetic phase ferrite materials
of the two phases is expected to guarantee the single-phase magnetic leads to the enhancement of the magnetic properties of the material.
behaviour of the MAM. The non-collinearity of the magnetic moments These are also considered beneficial in the arena of microwave ab­
between the phases leads to a decrease in the magnetic saturation of the sorption. Before we discuss the escalation of the use of the hard/soft
nanocomposite. The strong interphase exchange coupling between the ferrites in microwave absorption studies, the concept of ‘exchange
core and shell magnetic phases leads to better microwave absorption coupling behaviour’ should be explained. To procure the high saturation
[141]. The architecture of the material determines to an extent the magnetization property of the soft magnets and the high coercivity of
quality of the MAM. The very recent approach of 3-D printing of the the hard magnets, they are often made a composite, also referred to as
material ensures the time-effective method of controlling the shape and ‘spring exchange magnets’ [149,150]. The conceptualization of ‘ex­
structure of the material [142]. It has been observed that the degree of change coupling behaviour’ was first proposed by Kneller and Hawig.
crystallinity (average crystallite size and crystallite size distribution) is a They reported that the hard magnetic materials with the most superior
significant factor contributing to the exchange interaction between the properties contained rare earth material to a certain limit. Unfortu­
magnetic and dielectric parameters of the material under test. A very nately, rare earth material costs high, making it less accessible and
recent study done by Zdorovets et al. has elaborated on the conse­ useable on a commercial basis. On the contrary, the soft magnetic ma­
quences of the radiation damage on the structural parameters of the terials were relatively cheaper in price and less reactive. Therefore, the
material under consideration [143]. It is well known that when an ‘suitable dispersion’ of these hard and soft magnetic materials could
element substitution takes place in a material, the structural parameters merit better physical and chemical properties and these are also
are prone to change. With the increase in the doped/substituted cost-effective [151–153]. Microwave absorption of both hard and soft
ferrites was studied in detail over a period. The incorporation of a

44
S.A. Mathews and D.R. Babu Current Applied Physics 29 (2021) 39–53

second phase is often found to contribute to the enhancement of the microwave absorption by compositing both the materials [167]. The soft
dielectric properties of the material and this in turn collectively aug­ ferrite materials follow Snoek’s law:
ments the technological significance of the composite material [154,
2
155]. In this section, we prefer to discuss the hard/soft ferrite nano­ (μs − 1)fr = g × 4pMs (18)
3
composite and the mechanism of interaction between the phases. The
properties of a two-phase magnetic nanocomposite depend on the where μs is the permeability, fr is the resonant frequency, γ is the gy­
magnetic interaction between these two. These interactions are termed romagnetic ratio and Ms is magnetic saturation. The high Ms of the soft
dipolar and exchange interactions. The dipolar interactions comprise the ferrites subdues the permeability of the material, which plays an
soft-soft phase interaction and hard-hard phase interaction. Whereas, essential role in the microwave shielding mechanism. To overcome this
the exchange interaction deals with the association of hard and soft challenge, few strategies are often followed such as the effective mag­
phases of the nanocomposite [156–160]. Under the control of the netic saturation of the material is altered with the addition of a material
external magnetic field applied, the interaction between the magnetic with lower Ms, enhancing the permeability of the material by the
moments of the hard and the soft phases are aligned parallel to each incorporation of a low permittivity material and by the usage of com­
other, until the application of a reversed field. Application of the reverse bination materials with different magnetic anisotropy [168]. Due to
field assists the dipole moments of the soft phase to align towards the Snoek’s limitation, the operating frequency of the spinel ferrites is
direction of the moments of the hard phase. The schematic representa­ restricted. This could be dealt with, by compositing it with a hexaferrite.
tion of this behaviour is shown in Fig. 4. The lower the soft phase con­ The spring exchange coupling behaviour between the phases could raise
tent, the higher the dominance of the exchange interaction. But when the operating frequency of the microwave range [169]. When an
the soft magnetic phase of the nanocomposite is elevated, this interac­ external magnetic field is applied, if a smooth hysteresis loop is ob­
tion is gradually suppressed and dipolar interaction becomes prominent tained, the magnetic phases can be assumed to be well
[161–163]. The exchange coupling interaction is a phenomenon exchange-coupled exhibiting a single-phase magnetic behaviour. The
occurring at the surface interface of hard and soft grains. This associa­ behaviour of the nanocomposite depends on the distribution of the in­
tion of the hard/soft phases, as well as the magnetic moment alignment dividual phases, the grain size of the ferrite material, the shape of the
towards the application of the field, enhances the absorption capacity of particles, etc. The presence of a “kink”/“bee-waist” in common terms is
the nanocomposite [164]. This interaction is effective if the size of the the superimposition of both the hysteresis loops of the hard and the soft
soft grains is less than twice the width of the domain wall of the hard phases, suggesting that the spins of each phase rotate independently.
phase grains. The increase in the grain size would cause an enhanced The non-alignment of moments at the grain interphase of the two phases
interaction of the soft-soft phases, which could adversely affect the ex­ would result in the non-exchange coupling between the magnetic phases
change coupling [165,166]. Exchange length between the grains is [149,156,170,171]. Exchange coupling between the magnetic phases
another factor that could affect the extent of exchange coupling. can be further confirmed by the switching field distribution (SFD) which
The hexaferrite and the spinel ferrites are two of the best hard and is obtained by plotting dM/dH against the external magnetic field
soft magnetic phases that can be used as microwave absorption material. applied. If the SFD plot presents a single peak graph, then the nano­
The resonant frequency of spinel ferrites is in the range of MHz whereas, composite can be considered as well as exchange-coupled material.
the resonant frequency of hexagonal ferrites lies in the range of around Whereas, the appearance of double peaks would suggest the individual
30 GHz. Suitable dispersion of hard and soft magnetic phases allows the phase spin rotation, thereby indicating weak exchange coupling or
material to gain energy and efficiently work as a MAM [162]. The high non-exchange coupling [156,172].
permeability of the soft ferrites at low frequencies and low permeability The hexaferrite and the spinel ferrite system in the microwave
of the hard ferrites at high frequencies are used to the advantage of shielding mechanism can also be improved by employing doping/

Fig. 4. (a) Hysteresis loop representation of hard phase, soft phase and exchange-coupled hard/soft phases of the nanocomposite along with
Fig. 4 (b) the portrait of the shift of dipole moments of soft and hard phases with the reversal of magnetic field reversal.

45
S.A. Mathews and D.R. Babu Current Applied Physics 29 (2021) 39–53

substituting the material with suitable elements at the tetrahedral (A) crystalline ferrite material. This structural association causes a charge
site or at the octahedral (B) site. Doped M-type hexaferrite and com­ transfer because of the electrostatic interaction that is created. Due to
posite materials of the doped systems have been largely studied in this the weak domain wall movement resistance, more coupling occurs be­
arena in the previous years. Few of the doped M-type hexaferrite and tween the amorphous and crystalline ions. The more the coupling, the
doped hexaferrite in ferrite composite systems are BaCoxCuxZr2xFe12- less the availability of free Fe3+, which is a prominent factor affecting
4xO19 [173], SrFe9Mn1⋅5Ti1⋅5O19 [174], Sr0.9RE0.1Fe10Al2O19 [175], and the magnetic relaxation of the nanocomposite. This hurts the magnetic
SrFe10Al2O19/Co0⋅8Ni0⋅2Fe2O4 [149], (Ni–P)/BaNi0⋅4Ti0⋅4Fe11⋅2O19 saturation of the composite material [193]. Magnetic saturation and
[176], NiFe2O4@ SrCo0⋅2Fe11⋅8O19 [177] respectively. remanence will be thus found to decrease in the case of the composite,
The careful consideration of the element to be doped as well as the than its pure form [194].
oxidation state of the chosen element is relevant since it impacts the
magnetic parameters; such as a change in Curie temperature (Tc), 5.1.2.2. Hard ferrite/carbon derivative nanocomposite. Dielectric fillers
spontaneous magnetic moment, etc. and electrical parameters; such as are in much demand for their light density, high tensile strength,
resistivity, bandgap, etc. The coupling between the magnetic metals enhanced absorption capacity as well as the increase in the absorption
known as double/super-exchange interaction is controlled by their frequency band of the microwave absorbed than the traditional mate­
charge transfer properties as per the Goodenough-Kanamori rule. The rials used. Carbon-based materials such as graphene, reduced graphene
substitution of the +3 oxidation state element to the crystallographic oxide, nitrogen-doped graphene, carbon nanotubes-single walled and
site of an element with a +2 state would create an oxygen vacancy and multi-walled, etc. have grabbed much of the attention in research
vice-versa. This would result in an oxygen excess and deficit state recently. The high dielectric loss factor of these materials makes them a
respectively. The complex metal oxides witness the indirect exchange potential candidate for shielding applications. As mentioned in the
mechanism/super-exchange mechanism. The more oxygen vacancy, the previous section, the combination of magnetic loss and dielectric loss
less the exchange interaction between the metals. This perturbation in materials helps in the electromagnetic impedance matching.
the oxidation state would agitate the magnetic and dielectric order. Dielectric lossy materials such as carbon nanotubes (CNT), graphite,
Consequently, alteration in cell parameters, bond lengths, and weak fullerene, graphenol, graphene, graphene oxide, reduced graphene
exchange interactions take place [178–184]. oxide are a few in this genre that exhibits the best EMI shielding prop­
erties which when combined with magnetic materials balances the
5.1.2. Magnetic/dielectric absorber nanocomposite impedance matching of the composite system [195,196]. Excellent
properties exhibited by the graphene and reduced graphene oxide
5.1.2.1. Hard ferrite/polymer nanocomposite. Conducting polymers are (RGO), make it one of the best among the carbon-derived materials. The
a well-known dielectric material that is effective in its application as a development of skin effect due to high electrical conductivity when the
microwave absorber. These are often called ‘synthetic metals’ because it EM wave is incident on pure RGO causes an unfavourable impact on the
exhibits varied properties of both semiconductors and metals [185]. material. This influences its absorption capacity. The permittivity of
Modern electronic equipment thrives on its flexibility and light pure RGO does not balance its permeability, which is the major reason
weightiness. Polymers play an important role in this aspect. The inclu­ for impedance mismatch [197]. Despite the cons, its light density makes
sion of polymer matrix into the magnetic material complex finds its it an exceptional candidate for microwave absorption application. But
advantage and relevance in getting moulded into any desired shape and the impedance matching and dielectric properties of the graphene/RGO
size, of low density, being cost-effective, reducing the dielectric loss of alone cannot meet the requirements of an efficient MAM, in the case,
the complex, and above all contributing to the microwave absorption remedied by the ferrite/RGO (or graphene) composite. The synergy
mechanism most effectively. Polymer materials are often a few of the between the magnetic and the dielectric loss equips the
best materials considered for their low density which are advantageous magneto-dielectric composite to be a few of the best microwave
in fabricating portable electronic devices [186,187]. The need for con­ shielding materials as the addition of the dielectric material (RGO) in an
joining ferrite and polymer is important because it serves the purpose of appropriate amount modifies the EM wave interaction with the com­
absorbing both the magnetic and electric components of electromag­ posite material [198–202]. The increase in the dielectric property of the
netic radiation [188]. A high dielectric breakdown field of the polymers composite can be attributed to the elevation in conductivity with the
could be made used to develop and design highly efficient microwave incorporation of RGO in ferrite. The conductivity mechanism in RGO is
absorber materials [189]. For this purpose, conducting polymers such as scarce because of the very different band structure that it possesses,
polyaniline (PANi), polypyrrole (PPy) are chosen. Moreover, structural which permits the separation of electrons and holes. The defects and the
diversity is ensured in the ferrite-polymer nanocomposites, since it is a functional groups of the RGO structure contribute to the enhancement of
co-existence of organic and inorganic materials [190]. The association of the impedance matching property which is crucial for the microwave
non-magnetic material with a magnetic material primarily disrupts the absorption to take place in effect [93,203]. Ingrained defects of RGO
magnetic ordering of the material. The interaction at the interface be­ justifies the rise in electronic polarization and the incorporation of RGO
tween the polymer and the ferrite particles causes a diminishment in the in the ferrite lattice leads to the interfacial polarization (Maxwell-­
surface anisotropy of the ferrite material. The surface charge density of Wagner polarization). As a result, the accumulation of π-electrons in the
the ferrite particle is introduced with the addition of the polymer which RGO lattice acts as polarization centres and generates relaxation po­
weakens the domain wall movement resistance. Magnetic saturation is larization when the electromagnetic field is altered. Thus, there is an
dependent on the volume fraction of the ferrite content in the composite elevation in the dielectric properties of the heterogeneous nano­
material. This can be explained using equation (16), Ms = ϕms, where composite [112]. The effect of conductive material can be explained by
‘Ms’ denotes the magnetic saturation of the nanocomposite, ‘ϕ’ is the percolation theory which suggests that if the percolation threshold is
volume fraction of the ferrite particles and ‘ms’ represents the magnetic surpassed by the conducting part, the conductivity of the composite
saturation of the single moment. The increase in the percentage of increases to a great extent [204]. Consequently, the electrical resistivity
polymer would dilute the interactive forces that exist between the takes a dip [195].
magnetic grains [170,188,191]. The magneto-dielectric composite in­ Similar is the case with carbon nanotubes (CNTs). The addition of a
volves an interaction between the σ orbital of the Fe3+ of the ferrite part non-magnetic material tends to degrade the magnitude of the magnetic
and the π molecular orbital of the respective polymer [192]. When an parameters because there occurs a strain between the ferrite nano­
external magnetic field is applied, the amorphous polymer structure particles and the CNT surface. The cracks and surface defects are ‘cured’
rearranges itself to completely couple with the ferric ions (Fe3+) of the by the inclusion of CNTs which leads to homogeneity on the surface of

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S.A. Mathews and D.R. Babu Current Applied Physics 29 (2021) 39–53

the nanocomposite. Subsequently, the surface anisotropy drops, which silicon carbide nanowires, especially the cubic β-SiC (known as 3C–SiC)
causes a decrease in coercivity. Different studies suggest that only the named based on the stacking order sequences. The narrow bandgap of
ideal volume percent of the CNTs would result in high-quality micro­ the said material implies high conductivity and high dielectric loss are
wave absorption. In the case of excess of the CNTs (SWCNT, MWCNT), factors that assist in its excellence as an ideal high temperature
the material expresses weak reflection losses [205,206]. This can be seen absorbing material. Shen et al. has explained thoroughly in his recent
as a consequence of the weak chemical interaction between the ferrite study regarding the foresight of SiC nanowires as an efficient MAM. The
and CNT nanoparticles which guides to agglomeration of the particles in absence of magnetic loss makes the absorption capacity of the material
the composite material. The chemical bonding incompatibility can be chiefly depend upon the dielectric relaxation loss. Doping of nano­
redressed by the acid treatment of the CNTs which stabilizes the struc­ particles, introducing defects, structural modifications (core-shell)
ture of the nanocomposite [207–209]. Few hexaferrite material com­ would benefit the improvement in the utility of the SiC based MAMs
positions with their corresponding mode of synthesis, the thickness of [227]. Electrospun nanofibers could form a conductive network that
absorber, the frequency range in which the microwave study was con­ contributes to enhancing conduction loss. This technique in MAM is still
ducted, minimum reflection loss obtained at their matching frequency in its infant stage, research on this method can be extended to
along their references are tabulated in Table 1. compositing SiC and magnetic oxides; magnetic oxides, and polymer
and carbon-based materials. This can balance the impedance matching
6. Prospects of microwave absorption materials of the absorber [228]. It has been well established that graphite is an
excellent MAM. Structural modifications on this material could pave
The immense research on polymer and carbonaceous fillers and their way for an outstandingly economical and lightweight MAM. Batista
composites was the trend of the past decade. The development of the et al. [229] recently reported three different morphologies of the
two-dimensional material MXene (Ti3C2Tx) has achieved remarkable graphite material namely, graphite intercalation compound, expanded
shielding effectiveness of 92 dB as reported by Shahzad et al. [223]. The graphite, and exfoliated graphite flakes on silicon matrix. The ‘perco­
formula of MXene is Mn+1XnTx, where M represents the transition metal lation’ process that occurred in the network enabled the expanded
and X denotes whether it is carbon or nitrogen. MXenes are 2-D transi­ graphite flakes to perform better in comparison to other structures. This
tion metal carbides and or nitrides, obtained by the segregation of material can be extremely useful in aircraft and other military applica­
aluminium from the MAX phases (eg: Ti2AlC), where A is the main group tions because of its lightness in weight and cost-effectiveness. Meta­
element. This material is being widely researched for its potential as a materials are another possible influential material that may prove to be
microwave absorption material. The dielectric response of the nano­ efficacious in terms of their absorbing capacity. These are materials
sheets of MXene material was acclaimed to enhance the mechanism of whose absorbing property is attained from its state of the structure
microwave absorption and was studied in detail by Feng et al. [224]. rather than the composition of the material itself. Metamaterials are
The high electrical conductivity and permittivity of the MXenes will arranged in a periodic pattern in the form of rods, spheres, or rings.
contribute to the synergic effect when it is combined with a ferrite These are being studied in the recent past as a novel microwave absorber
material. This heightens the chances of procuring a maximum reflection and as a wave-guide structure. The bandwidth of the absorption peaks
loss as well as a wide absorption bandwidth [225,226]. The was reported to have increased by stacking the metamaterials into
sandwich-like structure and the multi-layered structures of MXenes are multi-layered structures [102,230,231]. Bio-compatible nano­
the promising structural adaptation of high-performing MAM [226]. composites are being widely researched for their admirable electro­
Another material that could be considered as a high functioning MAM is magnetic properties. ‘Green’ materials such as banana leaves, rice husk,

Table 1
Hexaferrite material compositions with their corresponding mode of synthesis, thickness of absorber, frequency range in which the microwave study was conducted,
minimum reflection loss obtained at their matching frequency along with their references.
Sl. Material composition Mode of synthesis Thickness Frequency Minimum Reflection Loss (dB)/Shielding References
No: (mm) range (GHz) effectiveness @ matching frequency
(GHz)

1. SrFe12O19/Ni0⋅6Zn0⋅4Fe2O4 One-pot solution combustion 3.5 X-band − 23 @ 9.9 [153]

2. SrFe12O19/Ni0⋅5Zn0⋅5Fe2O4 Sol-gel self-propagating 4.0 S, X, Ku-band − 45@ 6.2 [160]
combustion technique
3. Ag3PO4 nanorods/SrFe12O19 Hydrothermal 5.1 S, X, Ku-band − 63.1 @ 4.72 [163]
4. RGO/SrFe12O19 Hydrothermal 2.0 Ku-band − 49 @ 16.24 [210]
5. RGO/SrFe12O19/PVDF Facile one-pot chemical 3.0 X-band 33 [211]
reduction
6. RGO/SrFe12O19/PMMA In-situ polymerization process 3.2 X-band 37 [200]
followed by a gel casting
7. RGO/SrFe12O19/PANI Modified Hummer’s method, 1.5 Ku-band − 45@ 16.08 [212]
In-situ polymerization
8. SrFe12O19/Carbon black-nitrile rubber Ceramic technique 7 S, X-band − 28 @ 2.55 [55]
(50 wt% of CB)
9. PbCo0⋅5Sn0.5HoxFe11-xO19 Citrate combustion 1.8 Ku-band − 37 @ 16.2 [213]
10. SrMn0⋅4Cu0⋅4Zr0⋅8Fe10⋅4O19/MWCNT Co-precipitation 1.9 Ku-band − 56.47 @ 13.50 [208]
11. MWCNTs/Sr0⋅5Ba0⋅5Fe11Al0⋅5Cr0⋅5O19/ Sol-gel, In-situ polymerization 5.0 X, Ku-band − 26 @ 10 [214]
PANI
12. Ba0⋅69Sr0⋅17Cd0⋅07Zn0⋅07Fe12O19 Self-assembly re- flux method 2.1 X-band − 35 [215]
13. SrEr0⋅3Fe11⋅7O19/PANI (10 wt% ferrite) Sol-gel 3 S, X, Ku-band − 42@ 12 [216]
14. BaFe12O19/ZnFe2O4/CNTs Sol-gel 2 X-band − 43.22 @ 10.30 [217]
15. Ba0⋅3Sr0⋅4Pb0⋅3Fe12O19 Solid state reaction 2 S, X, Ku-band − 57.5 @ 15 [126]
16. BaMg0⋅5Co0⋅5Ti1⋅0Fe10O19 Traditional ceramic processing 2.3 Ku-band − 40 [218]
17. BaFe9(Mn0⋅5Cu0⋅5Zr)3/2O19 Sol-gel 1.8 Ku-band − 52.3 @ 16.75 [219]
18. Titania coated BaFe12O19 – 2.0 S, X-band − 19 @ 7.5 [220]
19. Ba(CoTi)0⋅25Fe11⋅5O19/PANI Solvothermal 2.5 − 45.2 @ 11.2 [221]
20. Ba0⋅25Sr0⋅75Ni0⋅5Mn0⋅5Fe11O19/PANI Sol-gel, In-situ polymerization 4.0 S, X-band − 21.68 @ 10.6 [222]
21. (Ba0⋅5Sr0⋅5Fe12O19)0⋅6/(NiFe2O4)0.4 Modified sol-gel technique 2.5 X-band − 38.74 @ 8.26 [159]

47
S.A. Mathews and D.R. Babu Current Applied Physics 29 (2021) 39–53

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Declaration of competing interest M. Eremina, E. Fadeev, E. Lähderanta, A.S.B. Sombra, D. Zhou, R.B. Jotania,
C. Singh, A.V. Trukhanov, Effect of titanium substitution and temperature
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interests or personal relationships that could have appeared to influence [23] J. Li, T. Xu, L. Liu, Y. Hong, Z. Song, H. Bai, Z. Zhou, Microstructure, magnetic
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