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Author's Accepted Manuscript: Journal of Magnetism and Magnetic Materials
Author's Accepted Manuscript: Journal of Magnetism and Magnetic Materials
www.elsevier.com/locate/jmmm
PII: S0304-8853(16)32216-8
DOI: http://dx.doi.org/10.1016/j.jmmm.2016.12.135
Reference: MAGMA62343
To appear in: Journal of Magnetism and Magnetic Materials
Received date: 15 September 2016
Revised date: 8 December 2016
Accepted date: 29 December 2016
Cite this article as: R. Vinaykumar, R. Mazumder and J. Bera, Characterization
of SrCo1.5Ti1.5Fe9O19 hexagonal ferrite synthesized by sol-gel combustion and
solid state route, Journal of Magnetism and Magnetic Materials,
http://dx.doi.org/10.1016/j.jmmm.2016.12.135
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Characterization of SrCo1.5Ti1.5Fe9O19 hexagonal ferrite synthesized by sol-gel combustion
and solid state route
_______________________________________________________
First author:
R. Vinaykumar,
E Mail: vinaykumar.r1984@gmail.com
*Corresponding author:
Japes Bera
E Mail: jbera@nitrkl.ac.in
Highlights:
SrCo1.5Ti1.5Fe9O19 ferrite was successfully prepared by sol–gel combustion process
using two types of raw materials for TiO2 namely titanium tetra-isopropoxide (TTIP)
TN based sol-gel synthesis has been reported first time for the synthesis of Co-Ti
Compare to solid state route, the density, saturation magnetization, permeability and
Abstract
combustion and solid state route. The effects of sources of TiO2 raw materials; titanium tetra-
isopropoxide (TTIP) and titanyl nitrate (TN) on the phase formation behaviour and properties of
the ferrite were studied. The thermal decomposition behavior of the gel was studied using TG-
DSC. The phase formation behavior of the ferrite was studied by using X-ray powder diffraction
and FTIR analysis. Phase formation was comparatively easier in the TN-based sol-gel process.
The morphology of powder and sintered ferrite was investigated using scanning electron
dielectric properties were investigated. The ferrite synthesized by sol-gel based chemical route
showed higher saturation magnetization, permeability and permittivity compared to the ferrite
Keywords: Sol-gel synthesis; SrM Hexagonal ferrite; Co-Ti substitutions; Magnetic properties
1. Introduction
In the recent decade, researchers pointed out that there is an increase industry requirement of M-
type hexagonal ferrites because of its excellent magnetic properties, high electrical resistivity,
high Curie temperature, and better chemical stability [1]. These ferrites have become massively
permanent magnets, magnetic recording and data storage materials, components for mobile and
for EM interference, radar absorbing material (RAM) and stealth technologies [1-3].
SrFe12O19 (SrM), BaFe12O19 (BaM), and PbFe12O19 (PbM) ferrites are belonging to the family of
M-type hexagonal ferrites. They have a magnetoplumbite-type crystal structure with space group
P63/mmc, where Fe3+ ions are in three octahedral (12k, 4f2, and 2a), one tetrahedral (4f1) and one
five-fold coordination bipyramidal (2b) site, respectively [1, 4, 5]. The structure of SrM ferrite
can be described as an alternate stacking of four building blocks, namely S (spinel: [Fe3+6O8]2+),
R (hexagonal: [Sr2+Fe3+6O11]2-), S* and R*, where asterisk (*) indicates the rotation of
Among M-type ferrites, the SrM ferrite has received a great deal of technological attention for
high-frequency application as it has higher values of magnetic properties than those of BaM or
PbM ferrites [1]. The pure SrM ferrite possesses large saturation magnetization (Ms: 74-92
emu/g), higher coercivity (Hc: 6.69 kOe) and high magnetocrystalline anisotropy constant (K1:
3.5 x106 erg/cm3) giving a large uniaxial crystalline anisotropy (Ha: 20 kOe) along the c-axis [4,
5]. Recently it has been reported that substituted hexagonal ferrites with planar anisotropy
exhibit excellent magnetic performance in the high-frequency region with higher ferromagnetic
resonance (FMR) frequencies compared to spinel ferrites. The FMR frequency of the ferrite can
also be varied by the substitution with different cations [6, 7]. The extensive investigation have
been carried out to modify the properties of SrM ferrites by substituting Fe3+ ions with trivalent
ions like Al3+, Ga3+, Cr3+, Mn3+ [8, 9] or with the pair substitution of divalent cations (Co2+, Zn2+,
Ni2+, Mg2+, etc) and tetravalent cations (Ti4+, Sn4+, Zr4+,Ir4+,etc) [10–13]. Among them,
substitution with Co2+Ti4+ pair is reported to alter the anisotropy and give rise to the noncollinear
magnetic structures [14-16]. Co2+cations prefer to occupy the 4f2 and 12k sites whereas,
nonmagnetic Ti4+cations prefer 12k site in M-type hexagonal structure [15, 16]. Ti4+ substitution
interrupts the magnetic interactions in a way that the two blocks SR and S*R* become more or
from uniaxial (along c axis) to planar (a-b plane) with increasing concentration of substitution.
Planar anisotropy in SrCoxTixFe12-2xO19 (SrCoTi-M) ferrite has been reported above a critical
Co-Ti concentration of x=1.1 to 1.3 and then the ferrite shows a typical soft magnetic behavior
[14,17,18]. Thompson et al. [17] reported that the FMR frequency of SrCoTi-M ferrite decreases
from ~50 GHz for x=0 (pure SrM) to below 1GHz for x=1.5 substitution concentration. This is
The conventional solid state route is the most extensively used method to produce SrCoTi-M
ferrite [19-22]. There are some deficiencies in this route such as the metal contamination from
the grinding media and necessary of high calcination temperatures more than 1200oC for a long
time, which lead to the formation of coarse and fused grains. However, the sol–gel combustion
synthesis has been demonstrated to be the optimal technique to synthesize ferrites with a
narrower grain-size distribution due to its atomic-level mixture of metal cations and low
crystallization temperature [23]. There are few reports available on sol–gel combustion synthesis
of BaM [24-28] and SrM [23, 29, 30] ferrite. However, there is only one report on the sol-gel
In this paper, we report the synthesis of SrCo1.5Ti1.5Fe9O19 ferrite by conventional solid state
method and sol–gel combustion method using two types of raw material for TiO2 namely
titanium tetra-isopropoxide and titanyl nitrate. The phase formation behavior, microstructure and
2. Experimental procedure
(C12H28O4Ti), titanyl nitrate (TiO(NO3)2), citric acid (C6H8O7) and ammonium hydroxide
(NH4OH) were used as starting raw materials for sol-gel combustion synthesis of
SrCo1.5Ti1.5Fe9O19 ferrite. Here two types of raw materials; titanium tetra-isopropoxide (TTIP)
and titanyl nitrate (TN) were used as TiO2 source in separate batches of experiments to study
the effect of the raw material on the phase formation and properties of the ferrite. The ferrite
synthesized using two respective TiO2 sources will be stated as TTIP and TN-based
powder/ferrite. The TN was prepared using the commercially available TiO2 through the process
described elsewhere [31]. The ferrite was also synthesized through conventional solid state
reaction route using SrCO3, Fe2O3, CoO, and TiO2 raw materials.
During sol-gel combustion synthesis of ferrite, the stoichiometric amount of all metal nitrates
were dissolved completely in distilled water to obtain solution-I. In the first experiment, required
molar ratio of TTIP was added dropwise to the solution-I and for the second experiment,
required amount of TN was added to the solution-I. The aqueous solution-II was prepared by
dissolving citric acid in distilled water. The solution I and II were then mixed with continuous
stirring for 30 min to form a transparent homogeneous solution. The molar ratio of citric acid to
total metal ions was maintained 1:1. Under this condition ammonium hydroxide was added
dropwise under the continuous stirring condition to adjust the pH of the solution to 7. The
produced sol was evaporated on a hot plate to transform into a gel. Further heating leads to a
self-propagating combustion of the gel with a violent exothermic reaction that propagated
through the entire gel in few seconds, and a foamy mass was swelled up. The foamy mass
yielded a loose agglomerated as burned powder when ground. The as burned powder was
calcined at a temperature ranging from 900 to 1200oC for 4h in an air atmosphere to study the
In conventional solid state reaction route, the raw materials were ball milled for 20 h in a
polyethylene vial using zirconia balls and isopropyl alcohol as the milling media. The mixed
powder was dried and then calcined at 1200oC for 4h in air. The ferrite powders prepared by two
routes were pressed into pellet and toroid shape (outer diameter 13.0 mm, inner diameter 3.0
mm, and thickness 2.0 mm) using PVA binder. Finally, pressed specimens were sintered at
2.2 Characterization
The thermal decomposition behavior of TTIP and the TN-based gel was evaluated by
using thermal analyzer (Model 449C; Netzsch, Germany) in the air atmosphere with the heating
rate of 10oC/min. The functional groups present in the dried gel, as burned and calcined powders
were identification by using Fourier Transformed Infrared (FTIR) spectroscopy (model 95277;
Perkin Elmer Spectrum) in the IR range 4000–400cm-1. The Phase formation behavior of the
ferrite was investigated by X-ray diffraction (XRD) analysis using the Rigaku diffractometer
(model; ULTIMA-IV/ Japan) with Cu Kα radiation. The Field Emission Scanning Electron
Microscope (FESEM Model; Nova NanoSEM/FEI) was used to analyze the morphology of
sintered ferrite. The magnetization behavior of the ferrite was measured using Vibrating Sample
The saturation magnetization (Ms) was deduced by a model described by R. Grossinger et al.
( ) (1)
crystalline anisotropy. Ms was calculated from the intercept of the straight line extrapolated in M
vs. 1/H2 plot for 1/H2 approaches zero and the slope was used to calculate b. The
magnetocrystalline anisotropy constant (K1) and the anisotropy field (Ha) were calculated using
( ) (2)
(3)
The frequency dependent inductance, resistance, magnetic loss factor (tan δµ) were measured on
toroid samples with six turn wound by copper wire and capacitance, dielectric loss factor (tan δε)
were measured on pellet samples using 16192A parallel electrode test fixture attached with an
LCR meter (Model; Agilent E4982A) in the frequency range 1MHz to 100MHz at room
temperature. Before each measurement the LCR meter was calibrated using the 16195B
calibration kit for Open, Short, Low-Loss Capacitor, and 50 Ω Load. The complex initial
permeability was calculated from the inductance data. The real component of initial permeability
N is the number of turns, Ht is the thickness, Do is the outer diameter and Din is the inner
diameter of the toroid sample. The imaginary component of initial permeability ( was
(5)
where R is the measured resistance of toroid, ω is angular frequency. The magnetic loss tangent
(6)
(7)
where ε0 is the permittivity of free space, the C is capacitance, t and A are the thickness and
cross-sectional area of the sample. The imaginary component of permittivity ( was calculated
(8)
Fig 1 (a) and (b) shows TG and DSC curves of TTIP and TN-based gel powders. For both the
gel, major weight loss was at 200oC. This weight loss corresponds to an enormous exothermic
peak in DSC curve. The exothermic peak at 200oC is due to the combustion reaction between
citric acid and nitrate ions in the gel [34]. The citric acid decomposes to CO2 and carbon
fragments, followed by the oxidation of carbon fragments with oxygen coming from NO-3 ion
In the case of TTIP based precursor the exothermic reaction almost complete at 200oC.
However, for TN based precursor there are two more exothermic peaks at 275 and 345oC
respectively. There was a weight loss under the sharp exothermic peak at 275oC, and there was
no weight loss under the broad exothermic peak at 345oC. The exothermic peak at 275oC
corresponds to the burning of residual carbon present in ash. The broad exothermic peak at
345oC may be due to the formation of crystalline phase from amorphous material [35]. The XRD
phase analysis showed the presence of two crystalline phases in TN-based as burned powder
(details of XRD phase analysis is presented in next section). There are some broad exothermic
peaks at 500oC and above in both TTIP and TN-based powder corresponding to the formation of
different crystalline phases. The crystalline phase formation is relatively slower process compare
to the oxidation- reduction reaction and the phase formation exotherms are broad in nature.
Fig 2 shows the XRD patterns of TTIP based as burned and calcined powders. The as burned
powder XRD pattern is almost amorphous. The XRD patterns of powder after calcined at 900oC
for 4h shows the phases; strontium titanate (SrTiO3, JCPDS file number 79-0175) and γ-Fe2O3
(JCPDS file number 86-0550). In addition to these phases, CoFe2O4 (JCPDS file number 22-
1086) phase was found in the powder calcined at 1100oC for 4h. However, after calcination at
1200oC for 4h, the single phase SrM ferrite was found, and all the diffraction peaks were
Fig 3 shows the XRD patterns of TN-based as burned and calcined powders. The as burned
powder XRD pattern shows the phases; SrFe0.5Ti0.5O2.85 (JCPDS file number 84-1004) and
CoFe2O4 (JCPDS file number 22-1086). The intermediate phase γ-Fe2O3 (JCPDS file number
86-0550) was found in the XRD patterns of powder calcined at 1000 oC for 4 h. However, after
calcination at 1100oC for 4h, a single SrM ferrite was found, and all the diffraction peaks were
Fig.4 shows the XRD patterns of solid state, TTIP, and TN-based SrFe9Co1.5Ti1.5O19 sintered
ferrite. All the three samples exhibited a single phase M-type hexagonal ferrite, and there was no
secondary phase found in the XRD patterns. The Co–Ti substitution does not affect the basic
crystal structure of M-type hexaferrite because Ti4+ and Co2+ ions have an almost similar ionic
ferrite, FTIR spectra of powders were recorded. Fig 5 and 6 shows FTIR spectra of gel, as
burned powder and calcined powder synthesized using TTIP and TN-based raw materials
respectively. In the spectra of both TTIP and TN-based dried gel, the broad bands in the range
3139 - 3149 cm-1 are attributed to the characteristics O-H stretching vibration of the hydroxyl
group of citric acid. The bands in the range 1616-1624 cm-1and 1455 cm-1 indicate asymmetrical
and symmetrical stretching vibrations respectively of –COO- carboxyl group of citric acid. The
bands in the range 1762-1767cm-1and 2396-2398 cm-1 correspond to the free carboxyl group of
citric acid. The bands located at 1384cm-1and 825- 832 cm-1 range are assigned to N-O stretching
and bending vibration respectively of NO3- [25,34]. So the result indicates that the gel contains
the –COO- ,–COOH functional group of citric acid and nitrate anions.
In the spectra of as burned powder, the O-H stretching vibration band at 3401cm-1 is very
prominent in the case of TTIP based powder. However, the band is absent in TN-based powder.
The result indicates that the burning temperature in the case of the TN-based experiment was
higher than TTIP-based one. In case of TTIP based synthesis, combustion temperature was not
so high for complete removal of crystalline water. The bands at 586 and 456cm-1 are attributed
to spinel ferrite [35]. The XRD analysis of as burned TTIP and TN-based powders stated above
also showed the formation of CoFe2O4 spinel ferrite. The band at 1384cm-1 found in both TTIP
and TN-based as burned powder are assign to the stretching vibration of NO3- group remaining
in the as burned powders. The same observation of the presence of NO3- group in as burned
powder was reported in the literature [25, 34]. In addition, there is some vibration band at 1624
and 1455cm-1 corresponding to the carboxylic group are found in TTIP based as burned powder.
This again indicates that burning temperature in the TTIP based experiment was not sufficiently
In the spectra of calcined powder, the bands at 586 cm-1 was identified as tetrahedral Fe-O
stretching and the bands in the range 432-430 cm-1were identified as tetrahedral Fe-O bending
and octahedral Fe-O stretching vibration of the M-type hexagonal ferrite [35-37]. These bands
are related to intrinsic stretching and bending vibration of the tetrahedral and octahedral Fe-O
bonds of hexagonal ferrite. Most of the –COO- , –COOH functional group and NO3- ion were
decomposed during calcination and no band related to these functional group are found in
Fig 7. (a) and (b) shows FESEM images of TTIP and TN-based as burned ferrite powder. The
micrograph indicates that the grains are in nanometer scale. An average grain size of about 100
and 200 nm was found in TTIP and TN-based as-burned powder respectively. The TN-based
specimen shows the formation of well-developed crystalline phases. The bigger grain size and
their crystalline shape again proved that the combustion temperature was comparatively higher
in the TN-based experiment. Fig 8 (a), (b) and (c) shows FESEM images of solid state route,
TTIP, and TN-based sintered ferrite samples. The micrograph indicates that the plate-like grains
are with hexagonal shape and grains are in 3 to 5-micron size range. The thickness of plate-like
grains was higher in solid state specimen and lower in the TTIP-based specimen. The densities
of three sintered ferrite measured by Archimedes’s method is shown in Table 1. The density of
solid state method pellet (4.7 g/cm3) was lower than the density of TN and TTIP based samples
(4.95 g/cm3).
Fig.9. The magnetic properties of ferrite such as coercive field (Hc) and remanence
magnetization (Mr) were determined directly from the hysteresis loops. The saturation
magnetization was obtained from the intercept of the straight line of the M vs. 1/H2 plot (Inset
Fig. 9) in the field region 6 kOe < H < 8 kOe for all the samples as per equation (1). While Ha
and K1 were calculated according to the equations (2) and (3). Table 1 summarizes the magnetic
properties of three different route ferrite samples. The Ms was in the range of 44 to 54.1emu/g,
and Hc was in the range 20 to 55.3 Oe. Both Ms and Hc were comparatively lower than the pure
SrM ferrite. The magnetization decreased to 54.12 emu/g (TN-based) from 72 emu/g for pure
SrM ferrite. The ion replacement process plays a primary role in the decrease of the net
magnetization. The decrease in Ms was attributed to the substitution of higher magnetic moment
Fe3+ ions (5µB) by Ti4+ ion with zero magnetic moment and Co2+ ions with 3 µB moments. The
substitution also dilutes the strength of the Fe3+–O2-–Fe3+ exchange interactions and reduces the
total magnetic moment [38]. The coercivity decreased dramatically to 55.3 Oe (TN-based) from
6.69 kOe (pure SrM ferrite). It is known that the Co2+ and Ti4+ cations preferentially occupy 2b,
4f2 and 12k sites of M-type hexagonal crystal structure [15,16]. The origin of large MCA in pure
SrM ferrite has been explained by the presence of Fe ions primary on the 2b site of the
hexagonal structure [15]. Occupancy of the Co and Ti ions on the 2b site leads to the decrease in
magnetocrystalline anisotropy. For that reason, there is the overall reduction in coercivity as the
coercivity is closely related to the anisotropy fields in hexaferrite. The magnetization
characteristic showed typical soft magnet behavior of SrCo1.5Ti1.5Fe9O19 ferrite. This soft
The magnetic moment (nB) in terms of μB was calculated by the relation; nB = (Molecular weight
of SrCo1.5Ti1.5Fe9O19 x Ms)/5585 as stated by the reference [9]. The values of nB and squareness
ratio (Mr/Ms) of the ferrite were about 9 μB and 0.1 respectively (shown in Table 1). As reported
in the literature, the pure SrM ferrite has nB of 20.6 μB and the squareness ratio (SR) of almost
0.5 [1]. The decreases in the values of nB to about 9 μB for the present ferrite samples is due to
the high-level of substitution of Fe3+ ions by non-magnetic Ti4+ and lower magnetic moment
Co2+ ions. Similarly, the decrease of SR to about 0.1 is due to the change of uniaxial anisotropy
to a planar anisotropy by the effect of Co-Ti substitution. The anisotropy constant (K1) and
anisotropy field (Ha) (shown in Table 1) were also found lower compared to pure SrM ferrite.
This was again due to the planar anisotropy in Co-Ti substituted SrM ferrite.
Fig. 10 shows the real (μ′) and imaginary (μ″) parts of the permeability respectively for different
ferrites in the frequency range from 1M to 100 MHz. The μ′, μ″ and tan δμ values at three
different frequencies are shown in Table 2. It can be seen from the Fig. 10 that the value of μ′
remains constant up to about 100 MHz frequency for all three samples. The permeability of solid
state, TTIP, and TN-based specimens were about 9, 15 and 16 respectively. The permeability is
closely correlated to the magnetization, densification and grain size of sintered ferrites [39]. The
TN and TTIP based sample shows higher μ′ compares to solid state sample due to its high Ms
and higher density. The imaginary (μ″) part of the permeability was about 0.4 for TN-based, 0.27
for TTIP-based and 0.1 for solid state based ferrite at 100 MHz frequency. The μ″ of TN-based
different ferrites in the frequency range from 1M to 100MHz. The ε′, ε and tan δε values at
three different frequencies are shown in Table 2. Both the ε′ and ε decreases with increasing
frequency. It is a typical behaviour of ferrites which can be explained with the help of Maxwell –
Wagener two layer model [40]. The decrease in permittivity with frequency might be originated
by the dielectric relaxation of the polarization which is generated by the space charges at the
grain boundary. The large value of permittivity at lower frequency is due to the predominance of
interfacial dislocation, oxygen vacancies, Fe2+ ions and grain boundary defect [41]. The ε′ was
comparatively higher in the ferrite synthesized by chemical route (TTIP and TN-based) compare
to solid state route. This may be due to the higher density and larger grain size of the ferrite
synthesized by chemical route. The ε values of all the samples are in the acceptable range.
The TN and TTIP based samples reveals the best performance compares to solid state sample
due to higher permeability and permittivity. The magneto-dielectric properties of the ferrite
4. Conclusions
SrCo1.5Ti1.5Fe9O19 was successfully prepared by sol–gel combustion method using two types of
raw material for TiO2 namely titanium tetra-isopropoxide (TTIP) and titanyl nitrate (TN). The
thermal decomposition behavior showed one stage and two stages weight losses respectively for
TTIP and TN-based gel. The pure SrCoTi-M ferrite phase was found after calcination of as
burned powder at 1100 and 1200oC respectively for TN and TTIP-based powder. This indicates
that the phase formation was easy in TN- based process. The FTIR functional group analysis
showed that the burning temperature in TTIP based combustion was not sufficiently high to
showed the formation of plate-like crystalline phase in TN-based powder. All these indicate that
combustion temperature of TN-based process was higher than TTIP-based one. The density,
saturation magnetization, permeability, coercivity and permittivity were comparatively higher in
the ferrite synthesized by chemical route (TTIP and TN-based) compare to solid state route. The
ferrite synthesized by chemical route showed high permittivity of in the range 36 to 41, low tan
δε of ~0.014, high permeability in the range 15 to 17, low tan δμ of ~0.02 at the frequency 100
MHz. All these properties of the ferrite suggest for its application as an inductor material and in
Acknowledgments
This work was supported by the SERB-DST (Grant No. SB/S3/ME/076/2013) of Government of
India. The authors would like to thank, Dr. Prasanta Chowdhury and Mr. Prabhanjan Kulkarni,
National Aerospace Laboratories, Bangalore, for the help on measuring the magnetic properties
of the samples.
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Fig.2 Room temperature XRD pattern of TTIP based ferrite powder (a) As burned and after
Fig.3 Room temperature XRD pattern of TN based ferrite powder (a) As burned and after
Fig.4 XRD pattern of (a) solid state (b) TTIP and (c) TN-based sintered ferrites obtained at
1300oC.
Fig.5 FTIR spectra of TTIP based (a) dried gel (b) as burned and (c) 1200oC calcined ferrite
powders.
Fig.6 FTIR spectra of TN-based (a) dried gel (b) as burned and (c) 1100oC calcined ferrite
powders.
Fig.7 FESEM images of (a) TTIP and (b) TN-based as burned powder.
Fig.8 FESEM images of (a) TN (b) TTIP and (c) solid state route synthesized sintered ferrite.
Fig.9 Magnetic hysteresis loops of ferrite samples synthesized by (a) solid state route and by sol-
gel route using (b) TTIP and (c) TN based raw materials. The inset figure shows the plot of Ms
ferrites synthesized by (a) solid state route and by sol-gel route using (b) TTIP and (c) TN based
raw materials.
ferrites synthesized by (a) solid state route and by sol-gel route using (b) TTIP and (c) TN based
raw materials.
Table 1 Density (D), saturation magnetization (Ms), remanence magnetization (Mr), coercivity
(Hc), squareness ratio (Mr/Ms), magnetic moment (nB), the anisotropy constant (K1) and
D Ms Mr Hc nB Mr/Ms K1 Ha
(gm/cm3) (emu/gm) (emu/gm) (Oe) (µB) (x104 (kOe)
Sample
erg/cm3)
ε″) and dielectric loss tangent (tan δε) at 1, 10, and 100 MHz for three SrCo1.5Ti1.5Fe9O19 ferrite
samples.