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Vacuum 82 (2008) 12331237

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Vacuum
journal homepage: www.elsevier.com/locate/vacuum

Effect of external magnetic eld on the deposition of BaFe12O19


M.S. Raque a, M. Khaleeq-ur-Rahman a, Saif-ur-Rehman a, Saa Anjum a, *, M. Shahbaz Anwar a, K.A.
Bhatti a, Saba Saeed a, M.S. Awan b
a
Advanced Physics Laboratory, Department of Physics, University of Engineering and Technology, Lahore 54890, Pakistan
b
COMSATS Institute of Information Technology, Islamabad, Pakistan

a r t i c l e i n f o a b s t r a c t

Article history: The contribution of an external magnetic eld on the deposition of BaFe12O19 thin lm was investigated.
Received 10 October 2007 For this purpose, two (one with applied eld and another without eld) thin lms of BaFe12O19 were
Received in revised form 28 December 2007 deposited on the C-plane oriented sapphire (Al2O3) substrate employing pulsed laser deposition tech-
Accepted 17 January 2008
nique. Crystallographic orientation and texture were determined using an X-ray diffractometer. The
magnetic parameters were deduced from a vibrating sample magnetometer (VSM). A spectrometer was
used to study the optical properties of the lms. The structural results reveal the lm to be pre-
Keywords:
dominantly single phase with C-plane orientation in both the cases. The lm deposited with eld,
Barium hexaferrite
Pulsed laser deposition
however, has bigger grain size and more perfection in crystallinity. The magnetic parameters show that
X-ray diffraction (XRD) the lm deposited with the eld has more remanence magnetization and higher coercive eld. The
Vibrating sample magnetometer (VSM) diffuse reectance of the lm deposited with eld is much higher due to the increased grain size and
Optical spectra roughness.
2008 Elsevier Ltd. All rights reserved.

1. Introduction optic recording devices. It is used conventionally as a permanent


magnet. However, in recent years the development of radar elec-
Over the past few years, the pulsed laser deposition (PLD) tronics and wireless technologies requires planers and low loss
technique has emerged as one of the simplest and most versatile magnetic microwave devices (isolators, lters, phase shifters, cir-
methods for the deposition of thin lms of a wide variety of culators, etc.) [2], which can be realized by the integration of
materials [1]. The stoichiometric removals of constituent species a ferrite material with semiconductor platforms. Barium hex-
from the target during the ablation, as well as the relatively small aferrite has attracted much attention for microwave device appli-
no of control parameters, are two major advantages of PLD over cations because of its bulk properties of high permeability and low
some of the other physical deposition techniques. Various process conductive losses. Scientists all over the world are working on the
parameters including substrate temperature, pressure, ablation deposition of BaFeO [37]. In recent years emphasis has been given
yield and deposition rate inuence the chemical composition and on the improvement of the lm quality. Song et al [8] and Matsui
the crystal structure of the deposited lms. Epitaxial growth et al. [9] deposited barium ferrite lm on C-plane sapphire under
imposes a requirement that the lattice constant and the thermal the optimal conditions to get the pure single phase lm with the
expansion coefcient mismatch be minimal. Among these different narrowest possible ferromagnetic resonance line widths. Efforts
successful techniques, laser ablation appears to be one of the most were also made to look at the oxygen deciency effects on the
promising because of its ability to control lm thickness and magnetic properties of barium ferrite [10,11]. The improved mag-
composition, during deposition. netic and dielectric properties of BaFeO deposited by Pulsed laser
The deposition of multicomponent magnetic alloys by PLD is deposition were also reported [1214]. Geiler et al. [15] developed
motivated by the classic advantage of stoichiometric transfer for BaFe12O19 thin lm on Al2O3 at atomic scale with a controlled ionic
materials with complex composition. It has also been very distribution in the unit cell using an alternating target laser abla-
successful in the deposition of oxide materials. Barium hexaferrite tion deposition technique. Attempts were also made to improve the
(BaFe12O19) material is an oxide with hexagonal structure and texture and particle size of the barium hexaferrite thin lms [16,17].
seems to be a potential candidate for magnetic as well as magneto- Although the deposition of the ferrite material has gained a lot of
attraction and efforts are being made to improve the quality of the
thin lms, little work is found in the literature on the improvement
* Corresponding author. Tel.: 92 42 9029204. of the thin lm by the application of the external magnetic eld
E-mail address: saa_anjum@hotmail.com (S. Anjum). during the deposition process [18,19].

0042-207X/$ see front matter 2008 Elsevier Ltd. All rights reserved.
doi:10.1016/j.vacuum.2008.01.052
1234 M.S. Raque et al. / Vacuum 82 (2008) 12331237

This paper presents the growth of C-axis oriented barium hex- using the peak parameters such as position, intensity and FWHM of
aferrite (BaFe12O19) thin lm on Al2O3 substrate by the pulsed laser the intensity of the reected peaks. The Scherer formula was used
deposition technique. Initially the lm was developed in the oxygen to calculate the grain size [21]. The dislocation density (s) was
environment. Afterwards, a transverse external magnetic eld was evaluated from the grain size (D) by the following relation [22].
applied on the ablated material from the target to investigate the
1
contribution of the magnetic eld to the deposited thin lm. s (1)
D2

2. Experimental procedure For each lm, the magnetic characterization was done with
a vibrating sample magnetometer (VSM). The magnetization versus
The pulsed laser deposition system was developed following the eld was measured for perpendicular-to-plane eld.
a standard design [20]. An Nd:YAG (1064 nm, 1.1 MW) pulsed laser The optical analysis was done by a Perkin Elmer, Lambda 950,
was used to ablate the BaFe12O19 target material on to the Al2O3 UV/VIS Spectrometer with the probing wave length ranging from
substrate in a vacuum chamber with controlled atmosphere. The 200 nm to 1000 nm.
base pressure in the chamber was w10-6 Torr. Oxygen (99.9% pure)
was then lled into the chamber at 20 mTorr. The ablation was done 3. Results and discussion
by focusing the beam on the target (at an angle of 45 with respect
to the target surface) with the help of a focusing lens of 10 cm focal The results provide clear and conclusive evidence of good lm
length giving an intensity of w1012 W/cm2 at the ablation spot. The quality of BaFe12O19, especially in the case when deposited under
BaFe12O19 target was of 2.5 cm diameter with 0.5 cm thickness. The the inuence of the external magnetic eld of 3500 G. The crys-
target was rotated with a programmable motorized mount at tallographic, magnetic and the optical data are given below.
6 rpm. The C-oriented Al2O3 substrate was a 5 mm thick disk with
0.5 cm diameter. The substrate temperature was maintained at
300  C to allow the necessary adatom mobility for the near equi- 3.1. XRD analysis of thin lm
librium growth of the target material as a lm. The substrate was
also rotated at 600 rpm with the help of a controllable motor. An 3.1.1. Deposition without applied external magnetic eld
optimum 0.5 cm target to substrate distance was kept during the Fig. 2 shows the XRD pattern for BaFe12O19 deposited without
deposition process. applied eld. The lm was oriented such that the q rotation gave
Two lms were deposited: a scattered X-ray beam that matched the specular reection from
the surface. For this setup the detected diffraction peaks come
(i) with no external magnetic eld applied to the target; from the C-plane scattering. The (203) peak of BaFe12O19 at
(ii) with 3500 G transverse magnetic eld applied to the target. 2q 38 with intensity 31,014 cps is identied in Fig. 2. The
Dq 0.44 obtained from the FWHM of the only (203) peak pro-
In order to apply the external magnetic eld, two disk magnets vides a quantitative measure of the C-axis dispersion. The grain
with a uniform magnetic eld (at a separation distance of 3 cm size for the deposited thin was calculated to be 19.7 nm and the
between them) were mounted in the chamber with a specially dislocation line density was 25.58  1010 lines/cm2. At 2q 89 the
designed Perspex holder. A schematic of the experimental setup is single sapphire peak at (220) with reection intensity 70,632 cps is
shown in Fig. 1. identied.
For the crystallographic data the deposited lms were then
analyzed by a PANalytical X-ray diffractometer at room tempera- 3.1.2. Deposition of thin lm with external magnetic eld
ture with standard q/2q source and detector scan. Structural The XRD data in Fig. 3 presents the analysis of the BaFe12O19 lm
parameters, grain size and dislocation line density were calculated deposited under the inuence of 3500 G magnetic eld. The same
(203) peak of BaFe12O19 at 2q 38 with intensity 121,502 cps is
identied in Fig. 3. The strong (203) reection show that the lm is
single phase with much better C-plane orientation as compared to
the lm deposited with out the applied external magnetic eld
since the Dq 0.3 obtained from the FWHM of the (203) peak
provides a quantitative measure of the C-axis dispersion which is
fairly in agreement with the reported value [15]. The small orien-
tation dispersion in comparison with the lm deposited without
the application of the eld provides further evidence that better
epitaxial lm is deposited. The grain size for the deposited thin lm
was calculated to be 29.7 nm and the dislocation line density was
11.32  1010 lines/cm2. At 2q 89 there is a single sapphire peak at
(220) with reection intensity 1315 cps.
The increase in the grain size and the perfection in the crystal-
linity of thin lms grown with the applied external magnetic eld
has been reported earlier [18].
The comparison of the two lms reveals that the reection in-
tensity of (203) plane for the lm deposited under the inuence of
the magnetic eld has increased many fold, which is indicative of
the improved crystallinity at (203) plane. The lower reection in-
tensity of Al2O3 in the case of the lm deposited with magnetic eld
is a clear indication that the thickness of the lm has improved. The
reason for the improved thickness could be due the enhancement
in the forward peaking of Fe and Ba ions under the inuence of the
Fig. 1. A Schematic of the experimental setup. eld. The plume is more conned [23] with higher densities under
M.S. Raque et al. / Vacuum 82 (2008) 12331237 1235

Fig. 2. XRD pattern of lm without external magnetic eld.

the inuence of the magnetic eld. The higher density leads toward The X-ray data provide evidence that the lm grown with the
the setting up of a strong electric eld within the plume which applied magnetic eld is more epitaxial. The lm has low
causes the charge separation present in the plume. This charge crystallographic dispersion and bigger grain size, with improved
separation gives rise to strong and dense ion beams emitted in the crystallinity and more roughness.
forward direction (perpendicular to the target) [24]. These ion
beams are then deposited on the substrate. A large number of 3.2. Magnetization of thin lm
monometric units allow the formation of isolated clusters
impending in the nucleation of larger particles during the de- The data in this section is of magnetic properties of the lms
position process. The larger grain size of the lm also supports this obtained by using a vibrating sample magnetometer (VSM). The
explanation. With the increase in grain size the dislocation density magnetization M (emu/g) was measured as a function of externally
decreases, which also shows that epitaxy of the lm is improved. applied H (Oe) for both the lms deposited with and without
The grain size extracted from the XRD data gives indirect in- magnetic eld. The data were obtained perpendicular-to-plane
formation about the smoothness or roughness of the deposited thin applied eld conguration. Comparison of the data of two thin
lm. The increased grain size in our case indicates that the lms is shown in Fig. 4, deposited with and without applying
roughness of the lm has increased [25,26]. external magnetic eld.

Fig. 3. XRD pattern of lm with external magnetic eld.


1236 M.S. Raque et al. / Vacuum 82 (2008) 12331237

enhanced to increase the magnetization of the thin lm. It is evi-


4.0x10-3 dent from our VSM data that the magnetization of the thin lm
(with magnetic field)
deposited with the applied eld in comparison with that deposited
(without magnetic field)
3.0x10-3 without eld has increased.
2.0x10-3
3.3. Optical analysis of thin lm
1.0x10-3
M(emu/g)

0.0 The two deposited thin lms were also analyzed for optical re-
-3
ectance. Fig. 5 shows the diffuse reectance spectrum extracted
-1.0x10
from the KubelkaMunk (KM) theory. This is generally used for the
-2.0x10-3 analysis of diffuse reectance spectra obtained from weakly ab-
sorbing samples. It correlates the total diffused radiation from
-3.0x10-3 a material with its scattering or absorption as [30]
-4.0x10-3 1  R2 k Ac
F R (2)
-15000 -10000 -5000 0 5000 10000 15000
2R s s
H(Oe) where R is reectance; k, absorption coefcient; s, scattering co-
efcient; c, concentration of the absorbing species; A, absorbance.
Fig. 4. Magnetization hysteresis loops of BaFe12O19 thin lms measured perpendicular
to the lm plane. It is clear from the graph that the lm deposited with magnetic
eld has more diffuse reectance as compared to that without
magnetic eld. The distribution of the surface gradients plays a key
role in deciding the surface diffuse reectance. The surface of the
The data for the lm without applied magnetic eld gives lm without eld has a narrow distribution of the surface gradi-
a narrow hysteresis loop with a coercive force of about 925 Oe. ents. That is why it has a less diffuse reectance whereas the lm
Saturation at applied eld H is about 7500 Oe with the saturation deposited with eld has a wider distribution of the surface gradi-
value of M at 2.7  10-3 emu/g. The remanence magnetization is ents leading toward more diffuse reectance. This increased diffuse
found to be 0.25  10-3 emu/g. reectance is related to the increased grain size and hence the
The data for the lm deposited under the inuence of external roughness of the lm deposited with eld, as also supported by our
magnetic eld gives a wider loop with a coercive force of about XRD data. The spectral response based on KM theory determines
2800 Oe. The saturation at applied eld H is about 14,000 Oe with the opacity and transparency according to the internal absorption
the saturated M value about 3.7  10-3 emu/g. The hysteresis loop is and scattering properties of the lm. The diffuse reection spec-
in good agreement with the loop obtained by Chen et al. [14]. The trum of the lm without eld appears almost constant for the
remanence magnetization measured is 1.5  10-3 emu/g, much wavelengths ranging from 220 nm to 520 nm. The lm seems to
greater than remanence magnetization of the lm without apply- have less scattering coefcient for these wavelengths or more ab-
ing external eld. This drastic change in the magnetization sorption. For the wavelengths beyond 520 nm (up to 600 nm), the
parameters of the lm deposited under the inuence of the applied spectrum has a spike in the reectance, which indicates the lm has
external magnetic eld have also been reported earlier [27]. The a higher coefcient of scattering for this wavelength. The reason for
reason for the change could be explained by taking into consider- this might be related to the fact that the scattering coefcient
ation the following facts. depends upon the incident wavelength. If there are a large number
These measurements of the hysteresis loop were taken for out- of voids comparable to the incident wavelength, the coefcient of
of-plane magnetization. It seems that the easy axis was in the plane scattering increases, which in turn increases the diffuse reectance.
for the lm deposited with magnetic eld while the hard axis was Thus, the size of the voids in the deposited lm might be
out of the plane, so it was difcult to magnetize or demagnetize the
lm as compared to the lm deposited without external magnetic
eld for which the easy axis seems out of the plane and hard axis in 5.5x107
the plane. Therefore, the magnetization and demagnetization of the % (with out B Field)
5.0x107
lm deposited with magnetic eld was rather difcult. This also % (with B Field)
explains the higher value of the coercive eld. Another possible 4.5x107
Diffuse Reflectance (F(R))

explanation for the higher values of the coercive eld could be the 4.0x107
bigger grain size of the lm deposited under the inuence of 3.5x107
the external magnetic eld. The bigger grain size is a measure of
3.0x107
increased roughness. Our XRD data show that grain size of the lm
with magnetic eld has increased and hence its roughness. This 2.5x107
increased roughness is responsible for the higher value of the 2.0x107
coercive eld [28].
1.5x107
One property of barium hexaferrite (BaFe12O19) of particular
value in microwave device design is the strong uniaxial anisotropy 1.0x107
(HA w17,000 Oe) [29] with easy direction being along the C-axis. 5.0x106
This high magnetic anisotropy eld can be adjusted by appropriate 0.0
substitution for Fe and Ba ions [2]. The BaFe12O19 structure consists
-5.0x106
of seven ferric ions distributed onto ve interstitial sites. The
200 400 600 800 1000
magnetism arises from the super-exchange of Fe cations and is
Wavelength ()
mediated by the oxygen anion. The advantage of developing a thin
lm with applied magnetic eld is that the concentration of the Fe Fig. 5. KubelkaMunk method diffuse reectance spectra of BaFe12O19 deposited
ions can be controlled. Thus, the substitution of the Fe ions can be without and with the application of the external magnetic eld.
M.S. Raque et al. / Vacuum 82 (2008) 12331237 1237

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