Thin Solid Films 583 (2015) 16

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Thin Solid Films

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

Effect of sputtering parameters on the structure, microstructure and

magnetic properties of Tb-Fe lms
Himalay Basumatary a,b, J. Arout Chelvane a,, D.V. Sridhara Rao a, S.V. Kamat a, Rajeev Ranjan b
a
b

Defence Metallurgical Research Laboratory, Hyderabad, India

Department of Materials Engineering, Indian Institute of Science Bangalore, India

a r t i c l e

i n f o

Article history:
Received 30 August 2014
Received in revised form 8 March 2015
Accepted 13 March 2015
Available online 21 March 2015
Keywords:
Magnetic thin lms
Magnetization measurements
Microstructure

a b s t r a c t
The effect of sputtering parameters such as gas pressure and power on the structure, microstructure and magnetic
properties of sputtered Tb-Fe thin lms was investigated. X-ray diffraction and transmission electron microscopy
studies showed that all the lms were amorphous in nature irrespective of the sputtering parameters. A ne island
kind of morphology was observed at low sputtering power whereas large clusters were seen at higher sputtering
power. While the composition of Tb-Fe lms remained constant with increasing sputtering power, the magnetic
behaviour was found to change from superparamagnetic to ferromagnetic. On the other hand, the increase in
argon gas pressure was found to deplete the iron concentration in Tb-Fe thin lms, which in turn reduced the
anisotropy and Curie temperature. Annealing of the lms at 773 K did not result in any crystallization and the
magnetic properties were also found to remain unchanged.
2015 Elsevier B.V. All rights reserved.

1. Introduction
R-Fe (Rrare earth) alloys have fascinated experimentalists as well
as theoreticians for decades due to (i) the intrinsic magnetic properties
exhibited by them such as large anisotropy, giant magnetostriction,
compensation temperatures, spin reorientations and domain wall
pinning, etc., and (ii) their potential for technological applications
such as in transducers, sensors, energy harvesters both at micro and
macro level, etc. [110]. Of the several R-Fe alloys, Tb-Fe2 alloys exhibit
the highest cubic anisotropy, large Curie temperature and giant room
temperature magnetostriction [2]. The physics and metallurgical aspects of bulk Tb-Fe2 have been studied thoroughly and well understood
[36]. Numerous investigations on Tb-Fe alloys in thin lm form have
also been carried out and these studies have predominantly focused
on improving the magnetostriction for micro-actuator applications or
on achieving a strong perpendicular magnetic anisotropy (PMA) for
magneto-optical recording applications [1118]. It has been reported
in literature that amorphous Tb-Fe lms with Tb at. % less than 40% exhibit PMA, while lms with at. % of Tb greater than 40% display in-plane
anisotropy [19]. Amorphous Tb-Fe thin lms and Tb-Fe/Fe multilayers
exhibit large low eld magnetostriction and strong perpendicular
magnetic anisotropy when compared with its crystalline counterparts
[911]. It has also been reported that structure and microstructurerelated factors such as whether the lms are amorphous or crystalline,
fully dense, or contain voids and exhibit the presence of secondary
phases inuence the functional properties of Tb-Fe lms considerably
Corresponding author.
E-mail address: jac@dmrl.drdo.in (J. Arout Chelvane).

http://dx.doi.org/10.1016/j.tsf.2015.03.026
0040-6090/ 2015 Elsevier B.V. All rights reserved.

[20,21]. The processing of Tb-Fe thin lms poses several challenges

and efforts to overcome these challenges and improve the performance
of Tb-Fe thin lms constitute an important area of research. Of the
several thin lm processing techniques, sputtering has been widely
used to grow Tb-Fe lms to achieve the desired composition, thickness,
and surface roughness [1115]. Although there are several studies on
understanding of magnetic properties of sputter deposited Tb-Fe
lms, a comprehensive study on the effect of sputtering parameters
such as gas pressure and power on the magnetic properties and its correlation with structure and microstructure is still elusive. Further, the
studies on the low temperature magnetic behaviour of these lms are
limited. In this paper, we have systematically investigated the effect of
sputtering parameters on the structure and magnetic properties of
sputter deposited Tb-Fe lms grown on b100N oriented Si substrates.
2. Experimental details
Tb-Fe lms were deposited at room temperature on Si b100N substrate by dc magnetron sputtering (DC sputtering unit make: M/s LB
Equipments and Technologies, Singapore) employing an alloy target
having composition 50 at.% Tb and 50 at.% Fe. Prior to sputtering, the
base pressure of the sputtering chamber was kept at 1.33 10- 4 Pa.
Films were grown with varying argon gas pressure (viz., 0.67, 1.33,
2.0 Pa) keeping the sputtering power constant at 150 W) and sputtering
power (viz., 50, 100 and 150 W, keeping the Ar pressure constant at
0.67 Pa) at room temperature. The deposition time (60 min) and target
to substrate distance (0.15 m) were kept constant for all the experiments. Aluminium was used as a capping layer to prevent oxidation of
lms once they are removed from the vacuum chamber. The lms

H. Basumatary et al. / Thin Solid Films 583 (2015) 16

were subjected to post annealing under vacuum (1.33 10- 4 Pa) at

773 K for 30 min. The thickness and surface roughness of the lms
were measured using a stylus prolometer (Make : M/s. Tencor, USA)
. Structural studies were carried out using glancing incidence X-ray diffraction (GIXRD) technique (Diffractometer Make: M/s Rigaku smart lab
diffractometer, Japan) at room temperature using Cu-K radiation
keeping the incident angle constant at 2. Scan was performed by keeping the detector 2 angle from 20 to 90 and X- ray diffractogram was
recorded. Transmission electron microscope (TEM) (Make: M/s FEI,
Technai, 20T G2), Netherland) operating at 200 kV was used to study
the structure and microstructure of lm under bright eld mode along
the cross-sectional specimens. For the preparation of cross-sectional
samples for TEM, two thin lms were sandwiched using a fast setting
epoxy. This sandwich is then mechanically polished along the lms'
cross section using ne emery paper. The thin polished sample (~200
micron) is then mounted on a copper grid using a fast setting epoxy
and polished till the thickness reduces to ~50 m. This sample is further
thinned down further employing a precision ion polishing system
(Make: M/s Gatan, USA) till a ne hole is formed. The portion near the
hole is transparent for electrons. Along this electron transparent region,
the structure and microstructure of the lms were studied. Field emission gun scanning electron microscope (FEG-SEM) (Make: M/s Zeiss,
Germany) was also employed for investigating microstructure of the
thin lms under secondary electron mode at room temperature keeping
the working distance at ~ 6 mm and operating voltage at 5 kV. The
composition of the lms were analyzed using energy dispersive
spectrometer (Make: M/s Oxford, UK) attached to the FEG-SEM. The operating voltage of 20 kV and a working distance of 10 mm were used for
composition analysis. Magnetization measurements were carried out
employing a super conducting quantum interference device magnetometer (Make: M/s Quantum Design, USA) up to a magnetic eld of
4800 kA/m at different temperatures. Field cooled (FC) and Zero eld
cooled (ZFC) measurements were carried out in the temperature
range 4390 K with an applied magnetic eld of 4, 8, 80, 800 and
2400 kA/m.

3. Results and discussions

Table 1 shows the variation of lm thickness with Ar pressure. It is
evident from this table that with increasing Ar pressure, the thickness
of Tb-Fe lms decreases. The decrease in thickness can be attributed
to the increase in the collision between the dislodged atoms from the
target and the Ar ions in the plasma. On the other hand, the thickness
of the lms is found to increase with increasing sputtering power. The
increase in thickness is attributed to the increase in the sputtering
yield, i.e., the number of dislodged atoms from the target with increasing sputtering power.
Representative GIXRD patterns for Tb-Fe lm grown at different deposition conditions are shown in Fig.1a and b. Fig. 2 shows a typical
cross-sectional TEM image obtained from Tb-Fe lm deposited at
0.67 Pa Ar pressure and sputtering power of 150 W along with the selected area diffraction pattern (SADP). It can be observed from the
GIXRD pattern that Tb-Fe lms are amorphous in nature for all

deposition conditions. This was also corroborated from the SADP obtained from cross-sectional TEM studies.
Fig. 3a shows the FEG-SEM micrographs of Tb-Fe thin lms deposited for 60 min at various sputtering powers such as 50, 100 and 150 W
and with a constant gas pressure of 0.67 Pa. Films deposited at 50 W exhibit a very ne island like or globular morphology. The size of these
islands increases with increasing sputtering power. The number of
dislodged atoms from the target increases at higher sputtering power,
and they also have higher kinetic energy resulting in greater surface diffusion when they deposit on the substrate, and this results in coarser island sizes as well as higher surface roughness. The composition of the
lms is found to remain constant irrespective of the sputtering power
and was found to be ~Tb54Fe46. With increasing power, the sputtering
yield of Tb and Fe atoms from the target increase proportionately and
as a result, only the thickness of the lm increases without affecting
the composition.
The FEG-SEM micrographs for the lms deposited with different gas
pressures and with a constant sputtering power of 150 W are shown in
Fig. 3b. The increase in gas pressure is found to affect the morphology of
the lms. The size of the islands or globular features as well as surface
roughness decreases with increase in Ar pressure. This could be because
at higher Ar pressure, sputtered atoms experience larger scattering by
Ar atoms, thus resulting in lower kinetic energy of the deposited
atoms and hence reduced diffusion. It is also observed that the concentration of Fe in Tb-Fe lms decreases with increase in Ar pressure, indicating preferential scattering of sputtered Fe atoms by Ar ions which are
lighter than Tb atoms.
Fig. 4a shows the FC and ZFC thermo-magnetic curves of Tb-Fe thin
lms grown for 60 min at different sputtering powers and 0.67 Pa Ar
pressure. The FC and ZFC thermo-magnetic curves were also traced at
different magnetic elds such as 4, 8, 80, 800 and 2400 kA/m. The FC
and ZFC curves for 50 W (Fig. 4a) and 100 W (Fig. 4b) sputtering
power show a continuous increase in magnetization with decreasing
temperature. However, a small kink is observed in the ZFC magnetization curves at low elds viz., 4, 8 and 80 kA/m around 25 K. This kink
slowly decreases in magnitude with increasing magnetic elds and
eventually the FC and ZFC curves merge with each other at high magnetic elds. The observed thermo-magnetic behaviour for the lms
grown at 50 and 100 W sputtering power suggests that they exhibit
superparamagnetic behaviour. To conrm this superparamagnetic behaviour further, magnetization curves were traced at different temperatures up to a magnetic eld of 4800 kA/m for the 50 and 100 W power
sputtered samples (Fig. 5a, b). The magnetization curves from 300 to
50 K exhibit a typical paramagnetic behaviour. The magnetization
curves traced at 4 K shows superparamagnetic behaviour with near
zero remanence and coercivity. The origin of superparamagnetism for
the lms grown at low sputtering power (50 and 100 K) is most likely
due to the formation of nite size islands.
In contrast to the 50 and 100 W sputtering power, the Tb-Fe thin lm
deposited at 150 W show magnetic ordering at low temperatures
(Fig. 4c). The Curie temperature deduced from the magnetization
curves is found to be ~ 180 K. It is also observed that the temperature
at which the ZFC and FC curves diverge shifts to lower value with increase in applied magnetic eld strength, indicating ferromagnetic

Table 1
Sputtering parameters, composition, surface roughness, magnetic state and Curie temperature of sputtered Tb-Fe thin lms: bottom of form.
Sputtering parameters
Power (W)

Ar pressure (Pa)

50
100
150
150
150

0.67
0.67
0.67
1.33
2.0

Composition

Film thickness (nm)

Surface roughness
(RMS), nm

Magnetic state

Curie temperature (K)

Tb54Fe46
Tb54Fe46
Tb54Fe46
Tb56Fe44
Tb59Fe41

550
900
1300
1200
900

1.9
2.5
7.0
5.7
1.5

Superparamagnetic
Superparamagnetic
Ferromagnetic
Ferromagnetic
Ferromagnetic

180
160
100

H. Basumatary et al. / Thin Solid Films 583 (2015) 16

Fig. 1. GIXRD pattern of Tb-Fe lms deposited under different sputtering conditions (a) as deposited and (b) after annealing at 773 K for 30 min.

behaviour. The development of ferromagnetism in lms grown at

higher sputtering power is attributed to the formation of larger size
islands when compared with the lms deposited at lower sputtering
power. The Curie temperature of amorphous Tb-Fe thin lms
(~ 180 K) is found to be much lower when compared with the bulk
Tb-Fe alloy (705 K). A similar behaviour has also been reported by J.
Betz et al. [22]. This is attributed to the fact that the distribution of FeFe exchange interaction is not continuous in the amorphous state,
which frustrates the Fe sub-lattice, and as a result, the Curie temperature decreases. Fig. 5c shows the magnetization curves plotted at different temperatures for the Tb-Fe thin lm grown at 150 W and 0.67 Pa gas
pressure. While the room temperature magnetization curve shows a
typical paramagnetic behaviour, the magnetization curve measured at
200 K exhibits onset of ordering with a slope change. The magnetization
curves at low temperatures (b200 K) exhibit a ferromagnetic ordering

Fig. 2. Bright eld TEM micrograph of Tb-Fe lm deposited at 0.67 Pa Ar pressure and
150 W sputtering power along with the SADP as inset.

with the coercivities increasing with decrease in temperature. The magnetization curve measured at 4K does not seem to saturate even for an
applied magnetic eld of 4800 kA/m indicating the magnetization
curve is minor in nature. This is attributed to the large anisotropy arising
from the local short range ordering in the amorphous structure exhibited by the Tb-Fe system. Such short range ordering in amorphous Tb-Fe
thin lms has been reported by R. Malmhll and Tu Chen [11]. Ranchal
et al. has reported a similar magnetization behaviour in nano-crystalline
Tb-Fe thin lms deposited on Si with different buffer layers [23].
The ZFC and FC thermo-magnetic curves for the Tb-Fe thin lms
grown at 0.67, 1.33 and 2.0 Pa gas pressure and with constant sputtering
power of 150 W is shown in Fig. 6a. The thermo-magnetic plots show a
ferromagnetic behaviour for sputtering pressures of 1.33 and 2.0 Pa as
described earlier for the lms grown at 0.67 Pa / 150 W. It is also observed that the Curie temperature decreases with increasing argon gas
pressure. This can be attributed to the fact that with increasing argon
gas pressure, the lms are found to be depleted in iron concentration
(Table 1). The magnetization curve for lms grown at 1.33 Pa gas pressure and 150 W sputtering power at low temperature does not show
any sign of saturation, indicating that the anisotropy is very large for
this lm. However, the low temperature magnetization curve for the
lms grown with 2.0 Pa gas pressure is found to saturate indicating a decrease in anisotropy with increasing gas pressure.
In order to increase the Curie temperature of the lm by inducing
structural ordering, Tb-Fe lms were subjected to vacuum annealing
at 773 K for 30 min. The GIXRD patterns do not display any crystalline
peaks (Fig. 1b), indicating that the lms are amorphous in nature even
after heat treatment. Akin to the GIXRD the microstructures of the
lms as seen under FEG-SEM also do not show any remarkable change
after heat treatment. It is also observed that the ZFC & FC thermomagnetic plots do not show any signicant change after annealing.
The superparamagnetic behaviour is found to be retained for the 50
and 100 W sputtered power lms even after annealing (Fig. 7a, b).
The Curie temperature of the lm deposited at 0.67 Pa Ar pressure
and 150 W sputtering power is also found to remain unaltered after annealing (Fig. 8a, b). This clearly indicates that annealing did not aid in
the re-arrangement of Tb and Fe atoms among each other to form
crystalline phase owing to the large difference in their atomic sizes.
However, a slight decrease in coercivity for the lm deposited at 150
W sputtering power is observed after annealing as evidenced from the
M-H plot of the lm measured at 100 K (Fig. 8c) possibly due to reduction in residual stresses in the lm after annealing. Annealing at

H. Basumatary et al. / Thin Solid Films 583 (2015) 16

Fig. 3. FEG-SEM images of Tb-Fe thin lms deposited (a) under constant Ar pressure of 0.67 Pa and varying sputtering power and (b) under constant sputtering power of 150 W and
varying Ar pressure.

Fig. 4. FC and ZFC thermo-magnetic plots of Tb-Fe thin lms deposited at constant Ar pressure of 0.67 Pa and under varying sputtering power of (a) 50 W, (b) 100 W and (c) 150 W.

H. Basumatary et al. / Thin Solid Films 583 (2015) 16

Fig. 5. Magnetization plots of Tb-Fe thin lms deposited at constant Ar pressure and varying sputtering powers of (a) 50 W, (b) 100 W and (c) 150 W.

temperatures higher than 773 K resulted in delamination of the lms

from the substrate, hence were not attempted.
4. Summary
Structural and magnetic properties of Tb-Fe thin lms deposited on
Si b100N substrates under different sputtering conditions were investigated. GIXRD and TEM studies show that all the lms are amorphous in
nature. Increase in sputtering power does not seem to vary the composition of Tb-Fe lms, while the iron concentration is found to be depleted with increasing gas pressure. Magnetic properties changes from
superparamagnetic to ferromagnetic behaviour with increase in
sputtering power. Curie temperature of Tb-Fe lm is found to decrease
with increase in Ar pressure due to the depletion of iron in the lm. Annealing at 773 K for 30 min did not induce any structural or magnetic ordering in the lms owing to the huge difference in atomic sizes of Tb and
Fe atoms.
Acknowledgement
The authors acknowledge the nancial support obtained from the
DRDO and wish to thank the director of DMRL, Hyderabad, for his

Fig. 6. Thermo-magnetic and magnetization behaviour of Tb-Fe lms deposited at constant sputtering power of 150 W and different Ar pressure (a) ZFC and FC thermo-magnetic
plots, (b) magnetization plots measured at different temperatures for the lm deposited at
1.33 Pa Ar pressure and (c) magnetization plots measured at different temperatures for the
lm deposited at 2.0 Pa Ar pressure.

Fig. 7. Thermo-magnetic and magnetization behaviour of heat treated Tb-Fe lms

deposited at 100 W sputtering power and 0.67 Pa gas pressure: (a) FC and ZFC thermomagnetic plots and (b) magnetization measured at different temperatures.

H. Basumatary et al. / Thin Solid Films 583 (2015) 16

Fig. 8. Thermo-magnetic and magnetization curves of as grown and heat treated (HT) Tb-Fe Thin lms deposited at 150 W sputtering power and 0.67 Pa Ar pressure: (a) FC and
ZFC thermo-magnetic curve of the heat treated lm, (b) magnetization curves of the heat treated lm measured at different temperatures and (c) magnetization curves of as
grown and heat treated Tb-Fe lm measured at 100 K.

constant support and encouragement. The authors also thank the Electron microscopy group, DMRL, for providing the FEG-SEM facility.
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