Journal of Electronic Materials

https://doi.org/10.1007/s11664-021-09019-y

ORIGINAL RESEARCH ARTICLE

Effects of Crystal Structure, Morphology and Ion Diffusion During

Annealing on Magnetic Properties of Hexagonal Barium Ferrite Films
Ke Zhou1 · Wei Chen1 · Hui Zheng1 · Peng Zheng1 · Liang Zheng1 · Qiong Wu2 · Yang Zhang1

Received: 10 January 2021 / Accepted: 14 May 2021

© The Minerals, Metals & Materials Society 2021

Abstract
In this work, the effect of the crystal structures, morphology and ion diffusion on magnetic properties of the hexagonal
barium ferrite films during the annealing process were studied. The structural characterization results demonstrated that the
orientation, crystallinity and morphology of the films can be controlled by the anneal temperature. Good crystallinity and
morphology of the film can be annealed at a temperature ≥ 1000°C, while the formation of ­BaFe12−xAlxO19 phase occurred
due to the ion diffusion when the annealing temperature reached 1200°C. Magnetic hysteresis loops showed that the satura-
tion magnetization, coercivity and remanence ratio of the films were all influenced by crystal structures, morphology and
ion diffusion. The platelet particle morphology and high crystallinity demonstrated a good magnetic film, but the ion diffu-
sion mutated the magnetic parameters. Additionally, the first-order reversal curve diagram further verified that the change
of crystallite sizes greatly influences the distribution of coercivity and interaction field. Consequently, the film annealed at
1000°C has a high out-of-plane c-axis orientation, high crystallinity with a full width at half maximum of 0.18° and high
saturation magnetization of 358 emu/cm3, which can be applied in the microwave device.

Keywords Hexagonal barium ferrite · annealing temperature · first-order reversal curve diagram · interaction field

Introduction use in microwave devices.12–15 Additionally, with the devel-

The M-type barium hexaferrite ­(BaFe12O19, BaM), a mag-
neto-plumbite crystal structure hexaferrite, has been widely
used in permanent magnets, catalysts, microwave devices
and absorbing material.1–5 This ferrite is composed of four
layers of structure, which consist of two spinel structures
with two oxygen layers and two hexagonal structures con-
sist of three oxygen layers.6 The unit cell of BaM contains
­38O2-, ­2Ba2+, ­24Fe3+, in which ­Fe3+ ions are distributed in
octahedral sites, tetrahedral sites and trigonal bipyramidal
sites.7 According to the crystal structure, the BaM has high
saturation magnetization and coercivity, large magneto-crys-
talline anisotropy (~17 kOe) and appropriate ferromagnetic
resonance linewidth.8–11 Therefore, BaM has encounter wide
* Hui Zheng
zhenghui0551@hdu.edu.cn
1
Laboratory for Nanoelectronics and NanoDevices,
Department of Electronics Science and Technology,
Hangzhou Dianzi University, Hangzhou 310018, China
2
Magnetism Key Laboratory of Zhejiang Province, China
Jiliang University, Hangzhou 310018, China
opment of miniaturization and integration of devices, the
traditional bulk materials cannot meet the requirements, and
the ferrite films are receiving more and more attention from
scientists. In the present day, the key work is focused on the
research and regulation of thin-film magnetic properties.16, 17
­ ai18 and Xu et al. 19 observed that the mag-
For instance, C
netic behavior varied in films as a result of the change of
the oxygen vacancies and valence state of ­Fen+ ion (n = 2,
3) were controlled by oxygen pressure during the growth of
films. Research shows that both F ­ e2+ formation and B ­ a2+
vacancy decrease the magnetic properties of films under
deficient oxygen and the excess oxygen environment, respec-
tively. ­Wei20 regulated the substrate temperature to change
the growth pattern of the films to prepare the BaM film with
high orientation and crystallinity, and mainly studied the
effect of orientation on the magnetic properties of films. The
result shows that the highly c-axis oriented films have higher
magnetic anisotropy and remanence ratio (0.53). In addition,
it has also been reported that the magnetic properties of the
BaM film are influenced by film-thickness,21 types of sub-
strate,22 and so on. It is well known that the lattice constant
and thermal expansion coefficient between substrate and film

13
Vol.:(0123456789)

is difficult to match perfectly, and the residual stress inside
the film leads to film cracking and delamination, which has
a great impact on the magnetic properties.23 To solve this
problem, ­Erickson24 and ­Chen25 et al. used MgO as a buffer
layer to reduce lattice mismatch. The film with several buffer
layers such as Au,26 ­Pt17, 27, 28 obtained a low ferromagnetic
resonance linewidth and high magnetic properties.
In addition to the above factors affecting the magnetic
properties of thin films, the microstructure, and crystal struc-
ture of the film, which can be adjusted by an annealing pro-
cess, also have a great influence on the magnetic properties
of the film. Therefore, in this paper, the microstructure and
crystal structure of the BaM film was changed by adjust-
ing the annealing temperature, and the effect on magnetic
properties was investigated. Meanwhile, the first-order rever-
sal curve diagram further verified that the crystal structure
gradually changed, which greatly influences the distribution
of the coercivity and interaction field.
Experimental
Pulsed laser deposition (PLD) has been widely used in the
preparation of films due to its unique characteristics. In
this work, the BaM films were deposited on ­Al2O3 (0001)
substrates by PLD with a KrF excimer laser (248 nm). The
BaM target with a 1-inch diameter, high-density (>95%),
and great microstructure (~1/11.8 of Ba/ Fe ratio) was home-
made, fabricated by solid-state reaction using precursors of
­BaCO3 (99%), and ­Fe2O3 (99.5%), and sintered by two-step
sintering at 1375°C -1325°C -20 h.29 The particular experi-
mental parameters are shown in Table I. The T–S distance
is the distance between the target and substrate. A 20 nm-Pt
buffer layer was first prepared on a substrate, the deposi-
tion conditions were shown in the first column of Table I.
Subsequently, the 0.5 μm-BaM film was deposited under the
conditions in the second column of Table I. When the depo-
sitions were finished, the as-deposited film was annealed at
different temperatures (800–1200°C) for 3 h in air.
Table I  The experimental parameters of depositing Pt and BaM films
by PLD
Parameters Values Values
Pt BaM
Deposition temperature 300°C 800°C
T-S distance 45 mm 45 mm
Laser energy 300 mJ 300 mJ
Laser frequency 5 Hz 5 Hz
Atmosphere Ar, 1 Pa O2, 8 × ­10−2 Pa
Annealing conditions – 800–1200°C, 3 h
Substrate material Al2O3 (0001) Pt/ ­Al2O3 (0001)
13
K. Zhou et al.
The crystal structures of the films were characterized
by x-ray diffraction (XRD, Ultima IV) theta-2theta scans
(20°–65° with a 0.02° step size). The surface microstructure
of the films was measured by field emission scanning elec-
tron microscopy (FESEM, JEOL JSM-7800F) and atomic
force microscopy (AFM, JPK) at tapping mode. The hyster-
esis loop of the membrane was measured using a vibrating
sample magnetometer (VSM, Lake Shore 7410). The local
magnetic properties of the BaM film were investigated by
using a first-order inversion curve (FORC). The detailed
measured illustration of the FORC has been reported in
other papers.30
Results and Discussion
In this work, the crystal structures and morphology of films
are controlled by the annealing temperature. An XRD pat-
tern of the crystal structures of BaM films annealed at dif-
ferent temperatures (800 ~1200°C) is displayed in Fig. 1a.
The diffraction peaks of BaM peaks, Pt peaks, ­Al2O3 peaks
are detected. The peaks at 2θ of ~36° is Kβ of Pt. As seen, the
Pt film with the orientation of face center cubic (111) grows
on ­Al2O3 (0001). Additionally, no matter the annealing tem-
perature, all peaks (except for Pt and ­Al2O3 peaks) belong
to (00l) BaM peaks, indicating that the film had an excel-
lent c-axis orientation perpendicular to the film plane. The
inset in Fig. 1a also shows the enlarged plot about 2θ from
30° to 32°. Obviously, the 2theta degree of the (008) peak
is gradually increased with the increase of the annealing
temperature. Other diffraction peaks of BaM also have the
same shift characteristic, the increase of angle for the (006),
(008) and (0014) peaks were 0.396°, 0.53° and 1.01° with
the increased annealing temperature from 800°C to 1200°C.
The peak at high 2theta has a higher increased value which
is consistent with the Bragg law, indicates the changing of
lattice value. The detected A ­ l2O3 peaks were all around at
39.9°, which excluded the instrumental zero shift.
The crystallite size has been calculated by Scherrer’s
formulae:31
K𝜆
D= (1)
𝛽cos𝜃
where the K is a constant of 0.89, λ is the wavelength of
radiation (Cu, = 0.154 nm), β is the full width at half maxi-
mum (FWHM), θ is Bragg’s diffraction angle. The calcula-
tion results are shown in Fig. 1b. The crystallite size increase
is attributed to the annealing process which further promoted
the crystal growth,32 and the higher the temperature, the
larger crystal growth, from 14 nm to 62 nm with the increase
of annealing temperature from 800°C to 1200°C.
Effects of Crystal Structure, Morphology and Ion Diffusion During Annealing on Magnetic…

70
Pt(111) Al O (0001)
(a) (b)
(006) (008) 2 3

(0014) 60
Intensity (arb.units)

kβ (0016) 1200 oC
50
1100 oC

Crystallite size
40
1000 oC
30
900 oC
20
800 oC
10
20 30 40 50 60 70 80 30 31 32 800 900 1000 1100 1200

2Theta (degree) Annealing temperature ( oC)

23.40 5.97
(c)
0.6
(d)
a
0.5 c
FWHM ( )
o

0.4 23.35
5.94
1000 oC
0.3
0.2
Lattice of c (Å)

Å
23.30
Counts (a.u.)

0.1
800 900 1000 1100 1200 5.91
0.18o

Lattice of a
Anneal temperature (oC)
23.25

5.88
23.20

23.15 5.85

14 15 16 17 18 800 900 1000 1100 1200

Theta (degree) Annealing temperature ( o C)

Fig. 1  (a) XRD patterns of the BaM film at different annealing tem- FWHM values of (008) peak varied with annealing temperature. (d)
peratures. right: diffraction peak at 2θ from 30° to 32°. (b) Changing Changing curve of the lattice parameter with the annealing tempera-
the curve of crystallite sizes with the annealing temperature. (c) The ture.
rocking curve of (008) peak of BaM film annealed at 1000°C. Inset:

To fully represent the change of crystal structure of the Table II  Parameters obtained from Rietveld analysis of XRD patterns
BaM films during annealing, the full width at half maxi- for the sample BaM film
mum (FWHM) of the rocking curves is given in Fig. 1c. Annealing Rwp χ2 a = b, Å c, Å Volume, Å3
The FWHM value of film under annealing temperature of temperature
1000°C is 0.18. Additionally, the FWHM value rapidly
800°C 1.697 1.215 5.940 23.78 726.63
decreased with the temperature increase from 800°C to
900°C 1.772 1.401 5.899 23.30 702.17
1000°C, while slowly decreasing when the temperature fur-
1000°C 2.639 2.289 5.891 23.29 699.97
ther increased to 1200°C. It is well known that the film’s
1100°C 4.404 4.098 5.890 23.28 699.43
crystallinity increases as the value of FWHM decreases.
1200°C 3.491 3.668 5.850 23.16 686.41
Thus, the high crystallinity of the film can be achieved by
post-annealing at high temperatures.
The results of the Rietveld analysis of XRD patterns of
the change of film crystal structure were shown in Table II constant (a = b = 5.94 Å and c = 23.78 Å), which is larger
The value of χ2 (goodness of fit) was between 1.2 and 4.1 than the theoretical value (a = b = 5.88 Å, c = 23.19 Å) due
for all the samples, which is a reasonable range.33 Firstly, the to the incomplete crystallization of the film. At 900–1100°C,
value of a and c decreases with the increase of the annealing the value of the lattice constant was slightly decreased
temperature, which can also be seen from Fig. 1d. The film because of the presence of biaxial stress in the film, which is
annealed at low temperature (800°C) has a higher lattice resulted from the difference of thermal expansion coefficient

13

between the film and substrate.34 In particular, there is a sig-
nificant drop at 1200°C, which could be accountable for the
formation of B­ aFe12−xAlxO19 phase. It has been reported that
the Pt film grows into discontinuous nanodots at high tem-
perature (>1100°C) and loses the isolated function between
the film and substrate.17 Therefore, the BaM film and the
­Al2O3 substrate diffuse and form the B­ aFe12−xAlxO19 phase.
FESEM and AFM measured the changes of surface
morphologies of the BaM films under different annealing
temperatures. Figure 2a, b and c shows the typical surface
morphologies of the BaM films under annealing tempera-
tures of 800°C, 1000°C and 1200°C. Nano-size particles
were formed on the ­Al2O3 substrate under an annealing
temperature of 800°C due to its incomplete crystallization.
When the annealing temperature increased to 1000°C, plate-
let particles were formed on the A
­ l2O3 substrate, indicating
a proper c-axis orientation of the film. Furthermore, some
particles grew abnormally large once the annealing tempera-
ture increased to 1200°C, and the dimensional uniformity
(a) (b)
1 µm
(e) (f)
0 1 µm 0 5 µm
2 3
Height (nm)
Height (nm)
1 2
0 1
-1 0
-2 -1
Fig. 2  SEM and AFM images of the BaM films surface under different annealing temperature, (a) 800°C -SEM, (b) 1000°C -SEM, (c)1200°C
-SEM, (d) 800°C -AFM, (e) 1000°C -AFM, (f) 1200°C -AFM.
13
K. Zhou et al.
deteriorated. AFM images in Fig. 2d, e, and f also display
the surface morphology of the films under different anneal-
ing temperatures. Naturally, blurred grains with small sizes
were obtained in the film for the incomplete crystalliza-
tion at 800°C. At 1000°C, the film grew into sheet grains
with a uniform size of 2 μm, which is consistent with the
SEM images. However, at 1200°C, the flatness of the film
becomes worse. The profile of the films at the black dotted
line is given below the corresponding AFM images. The
thickness of the sheet grains is around ~ 2 nm and ~ 4 nm at
800°C and 1200°C, respectively. The average roughness Ra
of the films was also calculated to be 0.29 ± 0.05 nm, 0.52 ±
0.05 nm and 1.22 ± 0.05 nm for annealed at 800°C, 1000°C,
1200°C, respectively, which gradually increased with the
annealing temperature.
Based on the above results, the crystal structure and
morphology of the BaM films can be controlled by
annealing temperature. Additionally, the formation of
­BaFe12−xAlxO19 phase at high annealing temperature also
(c)
1 µm 2 µm
(g)
10 µm
5
Height (nm)
3
1
-1
Effects of Crystal Structure, Morphology and Ion Diffusion During Annealing on Magnetic…

400
200
(a) (b) 400
(c)
300
150 300
100 200 900 oC-V
800 oC-V 200 1000 oC-V

M (emu/cm3)

M (emu/cm3)
900 oC-P 1000 oC-P
M (emu/cm3)

50 800 oC-P 100 100

0 0 0
-50 -100 -100
-100 -200
-200
-150 -300
-300
-200 -400
-400
-15000 -10000 -5000 0 5000 10000 15000 -15000 -10000 -5000 0 5000 10000 15000 -15000 -10000 -5000 0 5000 10000 15000
Field (Oe) Field (Oe) Field (Oe)
400 400 2000
(d) 150 (e) (f) 80
300
100 1600
200 o
1100 C-V
o
1200 C-P 300

)
60

3
M (emu/cm3)

M (emu/cm3)
1100 oC-P

Mr/Ms (%)
Ms (emu/cm
100 50 1200 oC-V
1200

Hc (Oe )
0 0 200
40
800
-100 -50

-200 100
-100 400 20

-300
-150
-400 0 0 0
-15000 -10000 -5000 0 5000 10000 15000 -15000 -10000 -5000 0 5000 10000 15000 800 900 1000 1100 1200
Field (Oe) Temperature (oC)
Field (Oe)

Fig. 3  Hysteresis loops for the prepared BaM film under different annealing temperatures, (a)800°C, (b) 900°C, (c) 1000°C, (d) 1100°C, (e)
1200°C, (f) change curves of Ms, HC, Mr/Ms ~ Temperature.

Table III  Measured magnetic properties of BaM film under different Table IV  Other reported values of the BaM films prepared by PLD
annealing temperatures
Substrate Anneal tem- Film thick- Ms, emu/cm3 References
3 3
Annealing Ms, emu/cm Mr, emu/cm Mr/Ms, % Hc, Oe perature, °C ness, μm
temperature
Pt/MgO 1000 0.13 315 17
800°C 190 124 65.5 1861 MgO/SiC 1050 – 318 25
900°C 326 162 49.8 1346 MgO 1000 ~ 0.3 239 35
1000°C 358 106 29.7 782 MgO 1000 1 334 36
1100°C 313 62 19.8 286 Al2O3 1100 0.85 335 37
1200°C 138 110 80 330 Al2O3 1050 0.65 374 38
Pt/Al2O3 1000 0.49 358 This work

influence the magnetic properties of the films. Therefore,

the magnetic hysteresis of the films along the vertical and dividing the magnetic moment by the volume of the film,
parallel directions at different annealing temperatures where the amount of the film was multiplied by the shal-
(800°C, 900°C, 1000°C, 1100°C, 1200°C) are shown in low area and thickness. It is obvious that the M s is less
Fig. 3a, b, c, d, and e. The high difference of the hysteresis than the theoretical value of the bulk (380 emu/cm 3). 39
loops along the vertical and parallel directions show aniso- The M s increases in the range of 800°C to 1000°C and
tropic behaviors of the films. The film at vertical direction then exhibits a decreasing trend; the maximum value of
is easier magnetized and owns higher saturation magneti- M s reaches 358 emu/cm 3. This value is almost higher
zation than the parallel directions. This natural magnetiza- than the reported BaM films deposited on Pt/MgO, MgO,
tion direction along the vertical direction indicates that the MgO/SiC, and ­Al2O3 substrate, as seen in Table IV. Sec-
c-axis is normal on the film surface which corresponds to ondly, for the HC perpendicular to the film direction, far
the XRD result. Table III lists the values of the saturation below the theoretical value (7.5 kOe) and monotonically
magnetization (Ms), coercivity (HC), and remanence ratio decreases with the increase of annealing temperature and
(M r/M s) in the vertical direction of the film at different keeps stabilization around 1100–1200°C. Lastly, the value
annealing temperatures. Ms of the film was calculated by of Mr/Ms decreases from 0.66 to 0.20 with the increase of

13

annealing temperature from 800°C to 1100°C; however, it
rapidly enlarges to 0.80 at 1200°C.
The following reasons can explain the above phenom-
enon. Firstly, it is known that Ms of BaM film associates with
the crystallinity of the film.40 Therefore, Ms increases in the
range of 800°C to 1000°C can be ascribed to its increasing
of crystallinity which the XRD results confirm. However,
Ms slightly decreases at the 1100°C and rapidly decreases at
1200°C mainly for the formation of B ­ aFe12−xAlxO19 phase,
which corresponds to the reported paper that Al-doped BaM
film has a lower Ms value.41 This is also the reason why Ms
is lower than the theoretical value.
Secondly, the value of HC is influenced by the magnetic
inversion in the film which is primarily related to domain
structure and defect in the film.42 It has been reported that a
multi-domain (MD) structure is more beneficial for the mag-
netic inversion which induces a low HC value.43 Addition-
ally, the defects in the film such as grain boundary defects
and point defects gradually disappear during the annealing
process, which is also one of the reasons for the decrease of
HC. In our prepared films, the decrease of HC might be due to
the increase of crystallite size and decreased defects with the
annealing temperature which can be confirmed from XRD
and SEM.44 However, the pinning effect caused by the incor-
poration of Al at 1200°C prevents the magnetic inversion
and causes an increase of HC,45, 46 which has been reported
by others.47 In addition, the HC decrease with the increasing
thickness of the film (<1 μm) has been reported.23, 48 This
trend is due to the interfacial strain between the film and the
substrate. This makes the HC of BaM film (500 nm) far lower
than the theoretical value and other reports.49
Thirdly, the value of Mr/Ms is determined by the film’s
integral demagnetizing field which is the vector sum of each
grains demagnetizing field. Furthermore, the direction and
value of each grain’s demagnetizing field are controlled by
the uniaxial anisotropic field and demagnetizing factor (ratio
of in-plane size and thickness). The uniaxial anisotropy field
(Hk) increases with the increase of crystallinity, which is
acquired from the parallel direction hysteresis loop.38 The
higher Hk of the film, the more consistent the direction of
Fig. 4  Schematic diagram of the effect mechanism of Mr/Ms at different annealing temperatures.
13
K. Zhou et al.
each grain’s demagnetizing field, which is along the normal
direction of the film.
On the other hand, the value of each grain demagneti-
zation field also gradually increases with the increase of
the demagnetization factor, which is proportional to the
grain size. Hence, the film’s integral demagnetizing field
increases, resulting in a decrease in Mr/Ms.
However, there is an interesting phenomenon that the
remanence ratio suddenly increases to 0.8 at the anneal-
ing temperature of 1200°C. Chen 42 explained that the
decrease in Ms when Al was doped into the BaM structure
causes a weakening of super-exchange interaction from the
­Fe3+-O-Fe3+ in octahedral and tetrahedral sites because the
­Fe3+ ions were substituted by non-magnetic A ­ l3+ ions. On
47
the other hand, Harward reported that the increase in Hk
with the increase of ­Al3+ concentration by the experimental
data and the formula ( Hk = 2KA ∕u0 Ms,KA is the anisotropy
constant), the decrease in Ms is mainly responsible for the
increase in Hk observed. The experiment data also indicated
that the 1200°C sample has high crystallinity and an increase
of thickness of grain size, which beneficial to reduce the
demagnetizing field of the film. Thence, there is a guess
that the influence mechanism of the Mr/Ms of the film is
divergent at different crystal structure and morphology of
the films during the annealing process, the schematic dia-
gram is shown in Fig. 4. At a low annealing temperature (<
1100°C), the Hk increased with the increase of crystallinity.
Simultaneously, Ms and the demagnetizing filed (Hd) also
increase, resulting in a decrease in Mr/Ms. When the anneal-
ing temperature reaches 1200°C, Al is doped into the BaM
structure and there is a decrease in Ms and an increase in Hk,
but the change of crystallizing size leads to a decrease of Hd.
Finally, the increase in Mr/Ms under the combined effect of
these factors. This mechanism also provided us with an idea
for preparing high Mr/Ms BaM films.
From the above mentioned, the crystal structure and
morphology of BaM film were adjusted by the annealing
process have a significant influence on the average mag-
netic properties. To further understand the effect of change
of structure on the local magnetic properties, especially the
Effects of Crystal Structure, Morphology and Ion Diffusion During Annealing on Magnetic…
3 3
10 ×10 (a) 10 ×10
5 5
Tails
Hu (Oe)
Hu (Oe)
0 0
-5 -5
Wishbone
-10 -10
0 5000 10000
Hc (Oe)
Fig. 5  The FORCs distribution diagrams for BaM films at different annealing temperatures, (a) 800°C, (b) 900°C, (c) 1000°C.
distribution of HC and Hu, the FORCs of the BaM films at
different annealing temperature are given in Fig. 5, which
is represented as a contour plot, ranging from purple (mini-
mum value) to red (maximum value). We ust illustrate three
features of the FORC diagram: (1) The “wishbone” struc-
ture appearing in the film annealed at 800°C, which is ~45°
with the negative axis of Hu. As the annealing temperature
increased, the “wishbone” structure gradually expands to the
positive and negative directions of the Hu axis, and the con-
centrated region is in the positive direction of the Hu axis.
It is an indication that the interaction gradually enhances
the different magnetic domains in the BaM film.50, 51 (2)
The high HC “tails” gradually disappear with the annealing
temperature (marked by the dotted box in Fig. 5a, further
indicating that the crystal structure of the film changes into
the MD structure. (3) Another essential feature that appeared
in the FORC diagrams is the non-null susceptibility at the
reversal field (As shown in the purple regions in Fig. 5,
indicating that the BaM film magnetization reversal occurs
utilizing reversible processes.52
Conclusions
In conclusion, the effect of the crystal structures, morphol-
ogy, and ion diffusion on the magnetic properties of the
hexagonal barium ferrite film during the annealing process
was studied. The structural characterization results demon-
strated high orientation, well crystallinity and morphology
of the films can be annealed at temperature ≥ 1000°C, while
there was the formation of ­BaFe12−xAlxO19 phase when the
annealing temperature reached 1200°C. Magnetic hyster-
esis loops show that (1) Ms increases in the range of 800-
1000°C, then exhibits a decreasing trend, and the maximum
value reaches 358 emu/cm3; (2) HC monotonically decreases
with the increase of annealing temperature, and stabilizes
3
(b) 10 ×10 (c)
5 300
200
Hu (Oe)
×10
0
100
-12
-5 0
-10
0 5000 10000 0 5000 10000
Hc (Oe) Hc (Oe)
around 1100–1200°C; (3) Mr/Ms decreases from 0.66 to 0.20
with the increase of annealing temperature from 800°C to
1100°C; however, it rapidly increases at 1200°C. Addition-
ally, the first-order reversal curve diagram further verified
that the crystal structure gradually changed which greatly
influences the distribution of the coercivity and interaction
field. The coercivity distribution concentrates toward the
low coercivity zone and increasing of the concentrated area
of the interaction field with an increase of annealing tem-
perature. Consequently, the film annealed at 1000°C has a
high out-of-plane c-axis orientation, high crystallinity with
FWHM of 0.18°, high Ms of 358 emu/cm3, which can be
applied in the microwave device.
Acknowledgments This work is funded by the National Natural Sci-
ence Foundation of China (Grant Nos. 51702075, 51771176), National
Key Research and Development Project (Grant No. 2019YFF0217205).
Conflict of interest The authors declare that they have no conflict of
interest.
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