Nanotechnology

Nanotechnology 25 (2014) 165601 (6pp) doi:10.1088/0957-4484/25/16/165601

Intra-grain perpendicular percolated L11

CoPt thin films
Fu-Te Yuan1 , An-Cheng Sun2 , C F Huang2 and Jen-Hwa Hsu3
1
iSentek Ltd, Advanced Sensor Laboratory, New Taipei City 22101, Taiwan
2
Department of Chemical Engineering and Materials Science, Yuan Ze University, Taoyuan 320, Taiwan
3
Department of Physics, National Taiwan University, Taipei 106, Taiwan

E-mail: ftyuan@gmail.com and acsun@saturn.yzu.edu.tw

Received 30 September 2013, revised 16 January 2014

Accepted for publication 3 March 2014
Published 26 March 2014

Abstract
Ultrathin percolated high-K u magnetic films with thicknesses of 2 nm are realized simply by
using sputter deposition and post annealing. L11 CoPt:MgO, with K u on the order of
107 erg cm−3 , was deposited on a MgO(111) substrate at 350 ◦ C, followed by post annealing
to induce complete segregation of the added MgO dopants. The optimized film shows
significant enhancement of the out-of-plane coercivity, approximately an order of magnitude
greater than that of the CoPt binary film, a remanence ratio close to unity, considerably
reduced in-plane magnetization, sharp perpendicular magnetic reversal, and reduced surface
roughness in the range of a few angstroms. Microstructure results indicate that MgO
precipitates into grains within the interconnected L11 grains after appropriate post annealing.
The MgO grains, with sizes in the range 2–7 nm, form coherent interfaces to the CoPt matrix
and penetrate through the whole depth of the film. The development of ideal non-magnetic
domain wall pinning sites explains the optimization of the perpendicular magnetic properties.
The advantages of a simple fabrication process, a thin film layer structure, and remarkable
enhancement of the magnetic characteristics demanded by ultrahigh-density recording reveal
its potential for practical applications.

Keywords: CoPt thin film, percolated media, L11 ordering

(Some figures may appear in colour only in the online journal)

The areal storage density of hard drives has increased rapidly
with the development of magnetic recording technology. Ther-
mal stability of the magnetic media is an increasingly signifi-
cant issue due to downsizing of the magnetic grains, especially
for media with a conventional granular microstructure. The
reason for this is that isolation of the grains greatly reduces the
effective volume V in the term K u V /kB T , which represents
the energy barrier for thermal demagnetization [1, 2]. Bit-
patterned media, a well-known solution proposed more than a
decade ago, in which each patterned bit contains a number of
strongly exchange coupled grains and the bits form an ordered
array, solves the problem by increasing V and thus promises to
push the areal density beyond 1 Tbit in−2 [3–8]. Nevertheless,
an economic and efficient method to fabricate such a large
area array of nanostructures with good uniformity is still not
available. Recently, an innovative recording mechanism using
percolated perpendicular media (PPM) was proposed [9–11].
The media is composed of interconnected, strongly coupled
magnetic grains as a matrix dispersed uniformly with non-
magnetic domain wall pinning sites that penetrate through the
whole depth of the film. The pinning sites could be holes or
non-magnetic precipitates of oxides or metals. The thermal
stability of the bits recorded under this regime is no longer
determined by the factor K u V /kB T , which is greatly enhanced
by the strong exchange coupling of the matrix, but rather by
the pinning strength of non-magnetic defects to domain walls.
PPM is also expected to give reduced transition jitter noise,
because the width of the transition region between recording
bits, which is determined by the diameter and pitch of the
pinning sites, is narrower than in the case of conventional
granular media, where it is determined by the grain size.

0957-4484/14/165601+06$33.00 1 c 2014 IOP Publishing Ltd

Printed in the UK
Nanotechnology 25 (2014) 165601
Experimentally, different approaches have been proposed
to realize PPM. One is to use oxide columns precipitated at
the grain boundaries of interconnected hard magnetic grains
by alternating sputter deposition or post annealing segrega-
tion [12–14]. However, the alternating deposition process is
rather complex and difficult to control to obtain good unifor-
mity over a large area and the post segregation approach tends
to embed the spherical precipitants inside the films, failing
to form a percolated structure [13, 14]. Another method to
achieve a percolated microstructure is to use porous templates
such as anodized aluminum oxide (AAO) and ZrO2 [15–17]
or patterned defects [18]. The fabricated percolated films
show enhancement in their magnetic properties and the cor-
responding magnetic reversal behavior is consistent with the
theoretical predictions [19]. Nevertheless, due to the require-
ment for a low-temperature deposition process for the purpose
of optimizing the magnetic performance, the magnetic film
used to demonstrate the PPM with porous templates is a
Co/Pt multilayer [15–18]. The value of K u for the Co/Pt
multilayer is on the order of 106 erg cm−3 , which is an order
of magnitude smaller than the value required for recording
media with a density exceeding 1 Tbits in−2 . The challenges
in using high-K u materials such as Co–Cr–Pt, L10 FePt and
CoPt on porous templates will be texture control and a high-
temperature process. In addition, the high surface roughness
is another intrinsic problem in using porous templates for
practical applications.
In this study, we present a method of fabricating
nano-scale intra-grain perpendicular anisotropic percolated
films with the high-K u material L11 CoPt, a rhombohe-
dral metastable phase with a K u of approximately 2–4 ×
107 erg cm−3 [20–24]. Compared with other approaches
towards forming percolated microstructures, the method
presented is much simpler, giving the required high K u of
the order of 107 erg cm−3 , showing uniform dispersion of
fine precipitants on the scale of 2–7 nm in diameter, with
significant enhancement of the magnetic properties and ideal
magnetic reversal behavior, and achieving a reduced surface
roughness in the range of a few angstroms. The results confirm
the proposed route is a promising one for realizing PPM.
The L11 CoPt:MgO films were deposited by radio fre-
quency magnetron co-sputtering on MgO(111) substrates. The
background vacuum was better than 5 × 10−9 Torr and the
working pressure was fixed at 10 mTorr. High-purity tar-
gets of Co, Pt and MgO were used. The composition of
the samples was controlled by fine tuning the output power
of the individual sources. Before deposition, the MgO(111)
substrate was heated to 600 ◦ C for 1 h for surface cleaning
and structural reconstruction. The substrate temperature was
held at 350 ◦ C during deposition, after which a post annealing
was subsequently applied at temperatures (Ta ) in the range
350–650 ◦ C for 1 h for the purpose of MgO precipitation. The
thickness of the samples varied from 2 to 20 nm. The structure
of the samples was analyzed by x-ray diffractometry (XRD).
The microstructure was studied by field-emission transmis-
sion electron microscopy (FE-TEM). The surface roughness
was characterized by atomic force microscopy (AFM). Mag-
netic properties were characterized by an alternating gradient
2
F-T Yuan et al
Figure 1. XRD patterns of CoPt:MgO films with different MgO
volume fractions deposited at 350 ◦ C. The thickness of the films is
20 nm.
magnetometer (AGM) and a vibrating sample magnetometer
(VSM) at room temperature with maximum magnetic field
strengths of 1 T and 2 T, respectively.
To realize PPM in an L11 CoPt:MgO film, understanding
its basic structural and magnetic properties is necessary before
performing microstructure engineering. The effect of MgO
content on the structure is first studied in the as-deposited
state. The deposition temperature of the samples is set to
350 ◦ C, for which the L11 ordering is optimized [23]. Figure 1
shows the XRD patterns of as-deposited CoPt:MgO films of
20 nm in thickness containing different volumes of MgO.
The CoPt films grown on MgO(111) exhibit a strong texture
of close-packed planes. The binary CoPt sample forms an
L11 structure in the given conditions, as indicated by the
superlattice peak L11 (111) at an approximate 2θ of 21◦ . With
the addition of MgO, the integrated intensity of L11 (111)
increases and reaches a maximum at MgO = 23.1 vol.%.
The peak width increases with increasing intensity, indicating
that the doping of MgO broadens the distribution of the
L11 lattice parameter. Further increasing the MgO content
above 26.5 vol.% seems to compromise the order structure,
as indicated by the disappearance of the L11 (111) peak. The
results reveal that the addition of MgO with an appropriate
content facilitates the formation of the CoPt L11 phase.
Reflection fringes obtained around the fundamental peak for
most of the samples reveal that the surface of the films
is quite smooth. The result is consistent with the small
root-mean-square value of surface roughness, of only a few
angstroms (peak-to-peak value of ∼1 nm), measured by AFM.
Since the L11 ordering is optimized by the addition of
MgO at 23.1 vol.%, the magnetic properties and microstructure
on that sample are investigated to clarify the role of MgO in
the film. Figures 2(a) and (b) show in-plane and out-of-plane
hysteresis loops of 20-nm-thick CoPt and thin films deposited
at 350 ◦ C, respectively. Both films show perpendicular mag-
netic anisotropy (PMA). The anisotropy field Hk of the two
Nanotechnology 25 (2014) 165601
Figure 2. In-plane and out-of-plane hysteresis loops of the
20-nm-thick (a) L11 CoPt and (b) L11 CoPt–MgO 23.1 vol.% thin
films deposited at 350 ◦ C, as measured by VSM. Corresponding
cross-sectional TEM images of the two samples are shown in (c)
and (d).
films is around 2 T at RT; however, the CoPt:MgO film has
a smaller in-plane remanence and in-plane coercivity Hck ,
and a sharper magnetic reversal process, indicative of better
easy-axis alignment and a lower resistance to domain wall
motion. Corresponding cross-sectional TEM images showing
different microstructures are shown in figures 2(c) and (d).
The texture of close-packed planes is confirmed as induced
by the MgO(111) surface, although the interface is wavy,
with a roughness of a few monolayers. The lattice image
in figure 2(c) indicates that the binary film contains struc-
tural defects, including stacking faults, dislocations and lattice
distortions. In the CoPt:MgO film, segregation of MgO is
observed. The MgO precipitants form spherical clusters with
coherent interfaces to the L11 CoPt matrix with diameters in
the range from 1 to 2 nm. The coherent precipitation preserves
the texture but produces considerable lattice strain around the
precipitants due to the large difference in lattice parameters
between MgO and CoPt, as shown in figure 2(d). The variation
in lattice constants explains the broadened superlattice peak in
3
F-T Yuan et al
Figure 3. (a) In-plane and out-of-plane hysteresis loops measured
by VSM and (b) cross-sectional TEM images of the 2-nm-thick
single-layer L11 CoPt film. A local enlargement of (b) is shown
in (c).
figure 1. Since the segregated MgO did not penetrate through
the whole depth of the film, the domain wall pinning effect is
thus limited, leading to a small perpendicular coercivity Hc⊥
of 0.23 kOe.
In order to form a percolated structure, the film thickness
of the CoPt was decreased to 2 nm to match the size of the
MgO precipitants. In the CoPt L11 film deposited at 350 ◦ C,
the decrease of thickness down to 2 nm results in a higher
in-plane remanence and reduces Hk to about 13 kOe, as shown
in figure 3(a). As indicated by the cross-sectional TEM images
shown in figures 3(b) and (c), the PMA film has a continuous
layer structure, which is different from the (001)-textured L10
FePt or CoPt films with the same thickness, which exhibit an
island-like morphology [25–27]. The difference in microstruc-
ture results from the deposition temperature; the formation
temperature of L10 FePt or CoPt increases drastically with
decreasing film thickness [28–30] to over 600 ◦ C, leading to
island-growth, while the ordering temperature of L11 CoPt
seems independent of film thickness and thus preserves a
continuous structure even at 2 nm thickness. Prevention of
island-like structures is crucial for PPM because it decouples
magnetic grains, resulting in degraded thermal stability and
an independent magnetic reversal process similar to granular
films. The advantages of L11 CoPt include a low ordering
temperature, good PMA at very low thicknesses, and strong
exchange coupling between the interconnected grains, thus
manifesting itself as an ideal material for PPM.
The precipitation of MgO during the 350 ◦ C-deposition
is incomplete, leading to the formation of clusters in the
sub-nanoscale, which gives rise to considerable residual strain.
In order to facilitate the segregation as well as relax/decrease
the lattice distortion and structural defects to form the perco-
lated structure, post annealing was applied to the L11 CoPt–
MgO 23.1 vol.% films after deposition. Figure 4 shows the
Nanotechnology 25 (2014) 165601 F-T Yuan et al

Figure 4. In-plane and out-of-plane hysteresis loops measured by AGM of the 2-nm-thick single layer L11 CoPt–MgO 23.1 vol.% films
deposited at (a) 350 ◦ C, and subsequently followed by post annealing at (b) 350 ◦ C, (c) 400 ◦ C, (d) 450 ◦ C, (e) 500 ◦ C, (f) 550 ◦ C,
(g) 600 ◦ C and (h) 650 ◦ C for 1 h.

in-plane and out-of-plane hysteresis loops of the 2-nm-thick

L11 CoPt:MgO films post annealed at various temperature
(Ta ), as measured by AGM at RT. The magnetization values are
normalized to the saturation values in the out-of-plane direc-
tion. Compared to the CoPt sample shown in figure 3(a), the
as-deposited CoPt:MgO film demonstrates a remanence ratio
close to unity and a significantly reduced in-plane magnetic
component (figure 4(a)), which greatly enhances the effective
perpendicular magnetic anisotropy (the area enclosed by the
two magnetization curves). Hk obtained by extrapolation is
about 15 kOe. Nevertheless, the value of Hc⊥ is only about
0.2 kOe, due to the incomplete phase separation of MgO from
the CoPt matrix. Hc⊥ increases gradually with Ta in the sam-
ples subjected to post annealing. In the films with Ta = 350 and
400 ◦ C, an increased longitudinal magnetization and a reduced
perpendicular remanence ratio is observed, indicative of an
intermediate state of MgO phase separation. A square hystere-
sis loop and a remanence ratio of unity are obtained in the
film with Ta = 450 ◦ C. Hc⊥ rises to 4 kOe in the sample with
Ta = 500 ◦ C. The extrapolated value of Hk exceeds 20 kOe and
the estimated K u reaches 1.6–2.3 × 107 erg cm−3 , which are
sufficient for ultrahigh-density recording. The sharp magnetic
reversal signals the mechanism of domain wall motion and the
linear magnetization curve in the in-plane direction confirms
perfect alignment of the magnetic easy-axis. As Ta increases
to 550 ◦ C, Hc⊥ reaches a maximum of 4.4 kOe. Nevertheless,
the drop in magnetization at low field obtained in both in-plane
and out-of-plane hysteresis loops indicates the formation of a
soft magnetic phase, which is a disordered A1 phase. High-
temperature annealing triggers the phase transformation from
L11 to A1 that has been described previously [23]. On further Figure 5. (a) Plan-view and (b) cross-sectional TEM image of the
increasing Ta to 700 ◦ C, order–disorder transformation occurs 2-nm-thick L11 CoPt–MgO 23.1 vol.% film deposited at 350 ◦ C
again, forming a high-K u L10 structure with a strong (111) followed by post annealing at 550 ◦ C for 1 h.
texture, as evidenced by the increased coercivity and tilt of the
magnetic easy-axis. The in-plane and out-of-plane hysteresis The microstructure of the CoPt–MgO 23.1 vol.% film with
loops become similar in shape and coercivity (∼2.7 kOe) and Ta = 550 ◦ C exhibiting maximum Hc⊥ was studied to explain
magnetic reversal is broadened. the magnetic properties. The plan-view TEM image shown in

4
Nanotechnology 25 (2014) 165601
Figure 6. Dependence of out-of-plane coercivity Hc⊥ on post
annealing temperature for L11 CoPt–MgO 23.1 vol.% films with
different thicknesses.
figure 5(a) indicates the precipitation of MgO grains inside
the interconnected L11 CoPt grains. Most of the precipitants
are round, with diameters in the range 2–7 nm and mean
distances between the MgO particles similar to the diameter.
The size of the non-magnetic pinning sites is much smaller than
previously reported results [13–18]. The cross-sectional image
(figure 5(b)) shows the disconnected profile of the film, reveal-
ing that the non-magnetic precipitants penetrate through the
whole depth of the CoPt film. The microstructure results con-
firm that the observed coercivity enhancement originates from
the segregation of MgO, forming a percolated morphology
within a continuous matrix rather than a granular structure with
isolated grains. The intra-grain segregation facilitates sharp
magnetic reversal, as observed in figures 4(c)–(f), because the
propagation field of domain walls in a single-crystal region
is very small. Sharp reversal of PPM has been predicted
theoretically [9, 10]. Compared to the presented results, PPM
formed by inter-grain segregation of the non-magnetic phase
shows a rather broad magnetic reversal process [13, 14]. This
is due to the boundary precipitation somewhat decreasing
the exchange coupling of the magnetic grains, leading to
discontinuous propagation of the domain walls. The interface
between the L11 CoPt matrix and MgO particles proves to be
coherent, as presented in figure 5(c). This explains the high
remanence ratio and sharp magnetic reversal exhibited, the
combination of which is rarely achieved in reported results.
The coherent interface optimizes the alignment of the L10
magnetic easy-axis near the heterogeneous interfaces, which
greatly narrows the angular distribution of magnetization near
the pinning sites in the remanent state, leading to a high
out-of-plane remanence ratio, negligible in-plane remanence,
and a narrowed pinning field distribution. It also stabilizes the
hard magnetic phase of the matrix in the present case. In porous
PPM, in contrast, magnetic misalignment near pinning sites is
unavoidable due to the high surface roughness and structural
relaxation of the magnetic films near the pinholes, which tilts
the magnetization away from the direction normal to the plane.
The pinning mechanism of PPM has been investigated
theoretically by means of micromagnetic simulation [19]. In
5
F-T Yuan et al
that paper the pinning energy
√ of a domain wall in a PPM is
described as E pin ≈ 4N Dt AK u , where N is the number of
pinning defects, D is the diameter of the defects, t is the film
thickness, and A is the exchange constant (in the present case
A = 10−6 erg cm−1 [31]). A maximum E pin is shown at a
ratio δ0 /D = 1, where δ0 is the Bloch wall parameter,
√ which
is related to the domain wall width δ = π δ0 = π A/K u . The
value of δ in this study is between 6.5 and 7.5 nm and the
corresponding δ0 /D ratio is in the range 0.34–1.1, which
covers the plateau of pinning energy [19]; the strong pinning
effect of the presented microstructure is thereby confirmed.
Figure 6 shows the dependence of Hc⊥ on Ta of CoPt–
MgO 23.1 vol.% films with different thickness. Coercivity
enhancement does not occur in CoPt films with thicknesses
of 10 and 20 nm even after high-temperature post annealing.
Hc⊥ remains lower than 0.5 kOe, although a good PMA is
obtained in samples with Ta < 600 ◦ C. In the thicker films, the
MgO precipitants are embedded in the CoPt films rather than
forming pinning sites passing through the whole depth of the
film or developing a granular structure. Similar results have
been observed in the Co–Cr–Pt:SiO2 system [12, 14]. The
CoPt film remains continuous, therefore magnetic hardening
originating from domain wall pinning does not occur.
In summary, we have demonstrated a simple approach
to achieve very thin nano-scale intra-grain percolated films
using high-K u L11 CoPt:MgO on MgO(111) substrates with
thicknesses of 2 nm. Through an appropriate post annealing,
the MgO added via co-sputtering segregates into the nano-
grains with a coherent interface to the matrix of L11 CoPt.
The coherent segregation and the small size of the precipitants,
as well as their separation, yield a remarkable enhancement
in coercivity and a sharp magnetic reversal, both of which
are favorable to PPM. In addition to forming ideal pinning
sites for domain walls, the containment of MgO assists the
development of the L11 phase and optimizes the perpendicular
magnetic properties of the L11 phase by improving the easy-
axis alignment. From the processing aspects, the advantages
of the presented method are the avoidance of specialized
engineering of substrates, complex deposition processes for
the magnetic film, and multilayer structures, making it more
feasible for practical production. From the aspect of film
characteristics, the achievement of smooth surfaces, high K u ,
suitable coercivity, sharp magnetic reversal, and the ultrathin
nature of the film fulfills the requirements for a magnetic
medium with an extremely high recording density.
Acknowledgment
The authors would like to thank the National Science Council
of Taiwan (contract no. 101-2221-E-155-020-MY3).
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