ARTICLE IN PRESS

Journal of Magnetism and Magnetic Materials 322 (2010) 2585–2588

Contents lists available at ScienceDirect

Journal of Magnetism and Magnetic Materials

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

Fabrication of multilayered Co/Pd nano-dot array with an

areal density of 1 tera-dot/in2
Jung-Sub Wi a, Kipil Lim a, Tae Wan Kim b, Sang-Jun Choi c, Kyung-Ho Shin d, Ki-Bum Kim a,n
a
Department of Materials Science and Engineering, Seoul National University, 599 Gwanang-ro, Gwanak-gu, Seoul 151-742, Republic of Korea
b
Department of Advanced Materials Engineering, Sejong University, 98 Gunja-dogn, Gwangjin-gu, Seoul 143-747, Republic of Korea
c
Samsung Electonics Co. LTD, Young-in 446-711, Republic of Korea
d
Center for Spintronics Research, Korea Institute of Science and Technology, 5 Wolsong-Gil, Seongbuk-gu, Seoul 136-791, Republic of Korea

a r t i c l e in fo abstract

Article history: Multilayered Co/Pd nano-dot arrays with pitches varying from 100 to 25 nm were obtained using an
Received 7 December 2009 electron beam lithography and plasma etching process. The proximity effect in the lithography step and
Received in revised form redeposition phenomenon in the etching step was minimized by modifying the resist development
19 February 2010
method and plasma etching parameters. For the array with a pitch of 100 nm, the ferromagnetic single
Available online 3 April 2010
domain behavior of each Co/Pd nano-dot was confirmed by magnetic force microscopy at room
Keywords: temperature. In addition, its magnetization, coercivity, and switching field distribution were also
Pattened magnetic media evaluated quantitatively using an alternating gradient magnetometer.
Co/Pd multilayer & 2010 Elsevier B.V. All rights reserved.
Electron-beam lithography

The development of bit patterned magnetic media (BPM) has
become one of the necessary requirements to meet the ever growing
demand for higher information storage densities of up to 1 tera-bit/
in2 and beyond, by overcoming the superparamagnetic limitation
[1,2]. In order to accomplish this goal, a process which is capable of
defining an isolated dot array with a pitch size of 25 nm is essential.
In addition, each dot should behave as a single magnetic switching
volume with only two stable remanent states. In this regard, the Co/
Pd multilayer, which demonstrates high perpendicular magnetic
anisotropy with good squareness, is one of the most favorable
magnetic materials for BPM [3]. Thus, various methods have been
proposed for the fabrication of BPM using Co/Pd multilayer. For
instance, an array of mono-dispersed spherical polystyrene particles
ranging in size from about 50 to 300 nm was used as a template to
form a nanometer scale dot array of Co/Pd multilayer [4,5], and
nano-dots of Co/Pd multilayer with a pitch size of 50 nm were made
using a pre-patterned SiO2/Si substrate [6]. Moreover, the fabrication
of multilayered Co/Pd nano-dot arrays with pitches ranging from a
few micrometers down to 50 nm using advanced lithography
methods, such as extreme ultraviolet lithography, ion beam
lithography, and electron beam (e-beam) lithography, has been
reported [7–9]. However, most of the pitch sizes reported so far are
still far from the areal density of 1 tera-bit/in2. In this letter, we
report an e-beam lithography based patterning method for the
successful fabrication of multilayered Co/Pd nano-dot arrays with a
n
Corresponding author.
E-mail address: kibum@snu.ac.kr (K.-B. Kim).
diameter of 20 nm and pitch size of 25 nm. For the array with a pitch
of 100 nm, the ferromagnetic single domain behavior of each Co/Pd
nano-dot is demonstrated, including the quantitative analysis of its
magnetization, coercivity, and process damaged layer.
A multilayer with the structure of 40 Å Pd (top)/(3 Å Co/8 Å
Pd)10/50 Å Pd/40 Å Ta (bottom) was deposited on a 1000 Å
SiO2/Si(0 0 1) substrate by DC magnetron sputtering with a base
pressure of less than 10 9 Torr. Then, a 300 Å thick amorphous
silicon (a-Si) layer was deposited on top of this multilayer
structure. Afterwards, hydrogen silsesquioxane (HSQ) was spin-
coated with a thickness of 300 Å and baked at 90 1C for 1 min. The
e-beam exposures were conducted using a JEOL JBX9300FS with
an accelerating voltage of 100 KeV. Resist development was
carried out in a 25% aqueous solution of tetramethylammonium
hydroxide (TMAH) at 21 1C for 60 s. Dry etching was carried out in
the following sequence. At first, the remnant HSQ and a-Si
intermediate layer were etched by a Cl2 plasma in order to
transfer the resist pattern to the a-Si layer. Then, the remaining
a-Si and the metal layer were etched by an Ar plasma. Microscopic
images and diameters of the Co/Pd nano-dot patterns
were characterized by scanning electron microscopy (SEM, JEOL
JSM-7401F). The magnetic properties of the individual nano-dot
and magnetic hysteresis loops from the nano-dot array were
obtained at room temperature using magnetic force microscopy
(MFM, Digital instrument Dimension 3100) and an alternating
gradient magnetometer (AGM, Princeton MicroMag 3900),
respectively.
We reported in our previous publication a method of forming
nanostructures of Co/Pd multilayer using an e-beam lithography

0304-8853/$ - see front matter & 2010 Elsevier B.V. All rights reserved.
doi:10.1016/j.jmmm.2010.03.025
 ARTICLE IN PRESS
2586 J.-S. Wi et al. / Journal of Magnetism and Magnetic Materials 322 (2010) 2585–2588
and sequential etching process with an intermediate a-Si layer
[10]. Both the improvement in the adhesion of the resist afforded
by the insertion of a-Si between HSQ and the Co/Pd multilayer
and the large etch selectivity (  2) between a-Si and the Co/Pd
multilayer in the Ar plasma ensure the successful patterning of
the Co/Pd nanostructures. This patterning process was modified in
this study due to a close spacing between the nano-dots. In order
to mitigate the effect of the proximity of the e-beam during the
exposure of the high density patterns, we employed a two-step
resist development method: dipping in a TMAH solution, inter-
mediate dipping in a dilute hydrofluoric acid (HF) solution
(4000:1 D.I.water:HF), and a second dipping in a TMAH solution
[11,12]. Using this development method, the residual resist
between the neighboring dot patterns after the development step
(often referred to as a resist scum), which is the cause of
insufficient isolation of the resist pattern and caused by the e-
beam proximity effect, could be effectively removed and isolated
HSQ dot patterns with a pitch of 25 nm could be successfully
defined.
The other processing issue is the redeposition phenomenon
during Ar plasma etching. It has been reported that non-volatile
etch by-products from the Ar plasma are frequently redeposited
on the sidewall or surface of the pattern due to backscattering
from the plasma [13,14]. For instance, the plan-view SEM images
of the dot array with a pitch of 50 nm are presented in Fig. 1 after
the processing steps of resist development, Cl2 plasma etching,
and Ar plasma etching. As presented in Fig. 1a, the morphology of
the Co/Pd nano-dot array was significantly deteriorated during Ar
plasma etching. The inset of Fig. 1a shows that the redeposited
materials situated around the nano-dots grew with increasing
etching time and finally became interconnected. This issue could
be solved through the control of the backscattering events by
reducing the Ar pressure from 100 m Torr (Fig. 1a) to 10 m Torr
(Fig. 1b). By decreasing the operating pressure, the mean free path
of the particles in the etching chamber can be increased by 10
times to about 5 mm and, as a result, the redeposition problem is
eliminated, as shown in the insets of Fig. 1b.
Using the modified process conditions of two-step HSQ
development and low pressure Ar plasma etching, multilayered
Co/Pd nano-dot arrays with pitches in the range 50–25 nm were
Fig. 1. SEM images of the dot array pattern with a pitch of 50 nm from the
sequential process steps of resist development, Cl2 plasma etching, and Ar plasma
etching. The process pressures during Ar plasma etching are (a) 100 m Torr and
(b) 10 m Torr.
successfully fabricated, as shown in Fig. 2, in which a pitch of
25 nm corresponds to an areal density of 1 tera-dot/in2. The mean
diameter of the Co/Pd nano-dots is about 20 nm and is almost the
same irrespective of the pitch. Co/Pd nano-dot arrays with six fold
symmetry, which is due to the inaccurate e-beam deflection of the
lithography hardware, appear at pitches of less than 30 nm in a
local area, as presented in Fig. 2c and d. Contrast difference of
individual Co/Pd nano-dots in SEM image of Fig. 2 is originated
from the existence or absence of Pd2Si on the top surface of
pattern. Because the Pd2Si of a hemispherical shape with a radius
of about 4 nm is generated by the interfacial reaction between
a-Si and Pd capping layer during e-beam lithography step, the
height deviation of Co/Pd nano-dots is not so significant and the
microstructure of Co/Pd multilayer is not altered [15]. Bright
contrast of Pd2Si can be used as a useful marker for the
termination of Ar etching.
In order to confirm their 1 dot/1 bit operation, the MFM images
were obtained at room temperature using a laboratory made
scanning probe with a 50 nm thick CoFe coated multiwall carbon
nanotube tip [16]. MFM scanning was performed with a constant
lift height of 35 nm above the tapping mode of AFM operation.
Fig. 3 presents the (a) AFM image of a Co/Pd nano-dot array with a
diameter of 20 nm and pitch of 100 nm obtained from a scanning
area of 2  2 mm2 and (b) the corresponding MFM image of the AC
demagnetized state. The inset of Fig. 3(b) shows a higher
resolution MFM image obtained from a scanning area of
0.5  0.5 mm2. In contrast to the topographic data shown in
Fig. 3(a), image distortion caused by the probe apex is relatively
small in the MFM images. This means that the MFM data obtained
in this study are reliable from the interference with surface
topology. The randomly distributed bright and dark contrasts in
Fig. 2. SEM images of the fabricated Co/Pd nano-dot arrays with pitches of
(a) 50 nm, (b) 40 nm, (c) 30 nm with six (upper) and four (lower) fold symmetry,
and (d) 25 nm with six (upper) and four (lower) fold symmetry. Scale bars:
100 nm.
 ARTICLE IN PRESS
J.-S. Wi et al. / Journal of Magnetism and Magnetic Materials 322 (2010) 2585–2588
the MFM images demonstrate that each Co/Pd nano-dot behaves
as a ferromagnetic single domain with perpendicular anisotropy.
For more detailed analysis of the magnetic properties of the Co/
Pd nano-dots and comparison with the continuous film, their
magnetic hysteresis loops were measured by AGM at room
temperature. For the AGM analysis, a Co/Pd nano-dot array with a
pitch of 100 nm was generated with an area of 2.5  2.5 mm2. In
order to reduce the e-beam lithography time, an e-beam current of
5 nA was used, which is 50 times larger than that employed in the
other experiments described herein. Due to the e-beam proximity
effect resulting from the huge exposed area and the increase of the
e-beam spot size resulting from the large current, the diameter of
the Co/Pd nano-dots was enlarged from 20 to 35 nm. Fig. 4 presents
the hysteresis loops obtained from the Co/Pd nano-dot array (closed
black squares) and continuous film (open red circles). First of all, the
remanence (Mr) and coercivity (Hc) of the fabricated nano-dot array
clearly show that the nano-dots are ferromagnetic at room
temperature. The Hc was increased from 1.1 to 7.4 kOe through
the nanopatterning process. Moreover, the switching field
Fig. 3. (a) AFM and (b) MFM images of the AC demagnetized Co/Pd dot array with
a pitch of 100 nm from a scanning area of 2  2 mm2. The inset of (b) shows a
higher resolution MFM image from a scanning area of 0.5  0.5 mm2.
Fig. 4. Magnetic hysteresis loops from Co/Pd nano-dot arrays (closed black
squares) and continuous film (open red circles). The inset shows the derivative
(black colored line) of the hysteresis loop of the Co/Pd nano-dot array and its
Gaussian fitting (red colored line). (For interpretation of the references to color in
this figure legend, the reader is referred to the web version of this article.)
2587
distribution (SFD) of the nano-dots is much wider than that of the
continuous film. The estimated width of the SFD was evaluated as
860 Oe from the FWHM of the Gaussian fitting of the first derivative
of the hysteresis loop (inset of Fig. 4). The increase of Hc and the
broadening of the SFD are well consistent with the previous
references [4,6,8]. These trends can be explained by the change of
the magnetic reversal from the nucleation and domain wall
propagation of the continuous film to the coherent rotation of the
nano-dots in the single domain state [17,18]. In addition, the AGM
data directly show the magnetization value of the Co/Pd nano-dots.
The magnetic moment obtained from the overall array of Co/Pd
nano-dots was measured to be about 2.2 m emu. From this value, the
saturation magnetization of the Co/Pd nano-dots with a diameter of
35 nm and height of 11 nm can be calculated to be 330 emu/cc,
which is about 85% of that of the continuous film. If we assume that
this decrease of the magnetization resulted from the etch damage
during the nanopatterning process and that the damaged region is
locally generated at the sidewall of the Co/Pd nano-dots, the
thickness of the damaged layer can be estimated to be about 1.3 nm.
We expect the ferromagnetism of the Co/Pd nano-dots to be
maintained until the magnet size is reduced to a cube 10 nm on a
side, assuming the damaged layer thickness and the anisotropy
energy are not much changed.
Even though we did not obtain a magnetic signal from the Co/Pd
dot array with a pitch of 25 nm, due to the resolution limit of our
MFM analysis and the impractical lithography time that would be
required for the AGM analysis, the MFM data in Fig. 3 distinctly show
that the Co/Pd nano-dots with a diameter of 20 nm behave as a single
domain with only two stable remanent states. In addition, the AGM
analysis in Fig. 4 indicates that the etching damage is not significant.
Based on these results, we speculate that the Co/Pd nano-dot array
with a density of 1012 dot/in2 in Fig. 2d can function as a bit patterned
magnetic medium with an areal density of 1 tera-bit/in2.
In conclusion, we successfully fabricated a multilayered Co/Pd
nano-dot array with a pitch of 25 nm through the minimization of
the e-beam proximity effect and redeposition problem. From the
MFM and AGM analyses at room temperature, we showed that
the Co/Pd nano-dots with a diameter of 20 nm can function as
single bits in BPM. We believe the proposed process and
fabrication results in this paper demonstrate a solid experimental
route for exploiting the BPM. Further studies using focused moke
or high resolution MFM for the characterization of high density
BPM are desired.
The authors wish to thank Jehyuk Choi and Il Jae Shin for their
considerable efforts in the e-beam lithography and Co/Pd multi-
layer deposition experiments. This work was supported from the
National Program for Tera-level Nano Devices, one of the 21st
Century Frontier R&D Program funded by the Ministry of
Education, Science and Technology of Korea.
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