Applied Surface Science 252 (2006) 3509–3513

www.elsevier.com/locate/apsusc

Direct observation of room temperature magnetism in

(In,Mn)As thin films by magnetic force microscopy
S.J. May, A.J. Blattner, D.P. Eam, B.W. Wessels *
Department of Materials Science and Engineering and Materials Research Center, Northwestern University,
2220 Campus Drive, Evanston, IL 60208, USA

Received 5 January 2005; accepted 13 May 2005

Available online 6 July 2005

Abstract

Variable-temperature magnetic force microscopy (MFM) has been performed over the temperature range of 298–348 K on
ferromagnetic (In,Mn)As thin films deposited by metal-organic vapor phase epitaxy (MOVPE). Ferromagnetic domains were
observed with submicron resolution in both single and two phase (In,Mn)As films, persisting up to 328 K. Isolated cylindrical
domains ranging from 100 to 350 nm in diameter with densities of 2–5  108 cm 2 were observed in phase pure films. Longer
range magnetic order, in the form of ribbon-like domains up to 1 mm in length, are present in the regions between the cylindrical
domains. Two phase (In,Mn)As films produced a well-resolved complex domain structure consisting of 1808 parallel and
antiparallel domains. Excellent agreement between the temperature dependence of the relative magnetization obtained by MFM
and superconducting quantum interference device measurements was observed.
# 2005 Elsevier B.V. All rights reserved.

PACS: 68.37.Rt; 75.50.Pp; 75.70.Kw

Keywords: Ferromagnetic semiconductors; Magnetic domains; Magnetic force microscopy

1. Introduction effect transistor, requires magnetic semiconductors

Ferromagnetic semiconductors, obtained by alloy-
ing III–V compounds with magnetic elements such as
Mn, have generated much interest for their possible
use in all semiconductor spintronic devices [1–3]. The
realization of practical devices, including the spin field
* Corresponding author. Tel.: +1 847 491 3219;
fax: +1 847 491 7820.
E-mail address: b-wessels@northwestern.edu (B.W. Wessels).
that maintain their ferromagnetic properties above
room temperature [4]. Recently, ferromagnetism has
been observed at temperatures up to 330 K in
(In,Mn)As grown by metal-organic vapor phase
epitaxy (MOVPE) [5]. The high Curie temperature
(TC), which is independent of Mn concentration, has
been attributed to short-range order involving Mn–Mn
near neighbor pairs [6]. The nature of the ferromag-
netic domain structures of these thin films is not
known. However, there have been several recent

0169-4332/$ – see front matter # 2005 Elsevier B.V. All rights reserved.
doi:10.1016/j.apsusc.2005.05.036
3510 S.J. May et al. / Applied Surface Science 252 (2006) 3509–3513
reports on magnetic domain structures in other
ferromagnetic semiconductors [7–9]. In low tempera-
ture measurements of (Ga,Mn)As films, both stripe
domains and isolated, randomly oriented cylindrical
domains have been observed [10–12].
In this report, the magnetic domain structure of
MOVPE grown (In,Mn)As thin films is determined
using variable temperature magnetic force microscopy
(MFM). Cylindrical domains and larger ribbon-like
domains have been observed in the (In,Mn)As films
persisting up to 328 K. A well-defined interconnected
rod-like domain structure was observed in two phase
films consisting of (In,Mn)As and hexagonal MnAs.
For both single and two-phase films, the temperature
dependence of the relative magnetization as deter-
mined by MFM is in agreement with SQUID
magnetization measurements.
2. Experimental
(In,Mn)As films were grown using atmospheric
pressure MOVPE on semi-insulating GaAs (0 0 1) and
undoped n-InAs (0 0 1) substrates under conditions
previously described [13]. All films grown on GaAs
were p-type as determined by Hall effect measure-
ments with hole concentrations between 1  1018 and
3  1018 cm 3. Carrier concentrations of the films
grown on InAs are unknown as the substrate resistance
is less than that of the film. Film thickness ranged from
350 to 740 nm as determined by profilometry. Double
crystal X-ray diffraction (XRD) with Cu Ka1 radiation
was used to determine phase composition. Mn
concentration of the films was determined by energy
dispersive X-ray spectroscopy. Magnetic force micro-
scopy was performed using a Digital Instruments
NanoScope IIIa atomic force microscope. A cobalt
coated magnetic tip with a resonant frequency of
70 kHz was used in all scans. To obtain a topogra-
phical image of the surface, the microscope first scans
along the surface in the tapping mode. The same area
is then rescanned at a programmed tip lift height to
obtain the magnetic image. Magnetic interactions
between the oscillating magnetic tip and sample
produce a change in the resonant frequency of the
cantilever. These frequency changes are detected
optically and converted into an image of the local
magnetic structure [14]. Domains with magnetization
perpendicular to the plane of the film, and parallel to
the magnetization of the tip, appear as regions of light
and dark contrast [15]. Domains in films with in-plane
magnetization appear as gray regions between domain
walls, which are observed as light and dark lines [16].
Since the change in resonant frequency is proportional
to the strength of the magnetic interaction between the
film and the magnetic tip, the RMS contrast of the
MFM images scales with the magnetization of the film
[17]. Thus, relative magnetization of the samples is
obtained by measuring the RMS contrast of each
MFM image. A lift height of 60 nm was used for the
In0.92Mn0.08As and In0.8Mn0.2As films, while a lift
height of 30 nm was used for the In0.96Mn0.04As film.
Two different scanners were used, one for fixed
temperature measurements and one for variable
temperature measurements. An applied magnetic field
of 500 Oe normal to the film is used to hold the
samples fixed to the variable temperature scanner. No
magnetic field is applied to the sample by the fixed
temperature scanner.
3. Results and discussion
The room temperature domain structure of a
400 nm thick In0.96Mn0.04As film grown on an InAs
(0 0 1) substrate was investigated using the fixed
temperature scanner. The obtained MFM image is
shown in Fig. 1(a). In order to ensure that the MFM
image contrast is caused by the film magnetization and
not due to topographical artefacts, the tip magnetiza-
tion was reversed by 1808 and a MFM scan was
obtained of the same area. In the resulting scan, shown
in Fig. 1(b), the magnetization of all the domains
appears to be reversed, proving that the contrast is
caused by the film magnetization.
A complex domain structure is observed, consist-
ing of local cylindrical domains with regions of
longer-range magnetic order between the cylindrical
domains. The cylindrical domains are attributed to
single domains with magnetization perpendicular to
the plane of the film [9]. The diameters of these
domains range from approximately 100–350 nm. The
density of the cylindrical domains is approximately
5  108 cm 2. The local cylindrical domains are often
accompanied by surface pits ranging from 5 to 25 nm
in depth. The areas between the pits, for instance along
 S.J. May et al. / Applied Surface Science 252 (2006) 3509–3513
Fig. 1. MFM images of an In0.96Mn0.04As film at 295 K measured
before (a) and after (b) reversing the tip magnetization by 1808. The
images are 4.7 mm  1.5 mm. The contrast data measured along the
white lines in (a) and (b) is shown in (c).
the line scans in Fig. 1(a) and (b), are atomically
smooth. It is likely that the cylindrical domains are
caused by higher Mn concentrations in these areas,
which in turn cause the defects responsible for the
surface pitting. Magnetic contrast is also present in the
regions between the cylindrical domains. This is
clearly shown in Fig. 1(c), in which the MFM data
obtained from the line scans of the white lines in
Fig. 1(a) and (b) is plotted. Even though the line scan
does not pass through any bright cylindrical domains,
a clear and consistent magnetic signal is obtained.
These longer-range domains vary in length from 500
to 1000 nm and in width from 200 to 500 nm. The
magnetic signal from the cylindrical domains is 5–7
times stronger than the signal from the long-range
domains.
Fig. 2 shows the MFM images obtained at
temperatures between 298 and 348 K from an
3511
Fig. 2. MFM images of an In0.92Mn0.08As film at (a) 298 K, (b)
308 K, (c) 318 K, (d) 328 K, and (e) 348 K. The images in (a–e) are
5 mm  5 mm. A 1.5 mm  1.5 mm MFM image of a domain
structure between dark cylindrical domains at 308 K is shown in
(f). The light, horizontal streaks near the top of the images (a) and (b)
are scan artifacts and not magnetic domains.
epitaxial In0.92Mn0.08As film grown on GaAs. The
observed domain structure, consisting of both cylind-
rical and larger ribbon-like domains, is similar to that
of the In0.96Mn0.04As film shown in Fig. 2. In contrast
to Fig. 1, the cylindrical domains all appear dark
indicating that the applied magnetic field of 500 Oe
has aligned these domains. SQUID measurements
show that a 500 Oe field is 33% of the saturation field
for this film. The measured cylindrical domain density
at room temperature is approximately 2  108 cm 2.
A few domains with their magnetization axis in the
plane of the film are also visible, which manifest
themselves as neighboring bright and dark regions
[9,17]. An example of an in-plane domain can be seen
in Fig. 2(c) indicated by the arrow. An example of the
ribbon domains found can be seen in Fig. 2(f), which is
an enlargement of the bottom region of Fig. 2(b)
indicated by the arrow. The persistence of the domains
up to 328 K is in agreement with the measured
TC = 330 K obtained from SQUID measurements. A
similar cylindrical domain structure, persisting up to
330 K, was also observed in an epitaxial
In0.97Mn0.03As film. The RMS contrast values of
the MFM images were obtained and are shown in
Fig. 3 for the In0.92Mn0.08As film. SQUID magnetiza-
3512 S.J. May et al. / Applied Surface Science 252 (2006) 3509–3513
Fig. 3. Magnetization, M, and RMS magnetization image contrast
as a function of temperature for the In0.92Mn0.08As film. Magnetiza-
tion data obtained from SQUID measurement with a 10 kOe field
applied perpendicular to the plane of the film.
tion data, obtained with a magnetic field of 10 kOe
applied perpendicular to the same film, is also plotted
in Fig. 3. Excellent agreement between the tempera-
ture dependent MFM and SQUID magnetization data
is observed.
Two phase epitaxial films, consisting of zinc blende
(In,Mn)As and second phase hexagonal MnAs as
determined by XRD, were also investigated. Fig. 4(a)
and (b) show the topographic and magnetic contrast
images obtained from a two phase In0.80Mn0.20As film
at room temperature, respectively. The MnAs pre-
cipitates are clearly visible in the topographic image
and range from 50 to 100 nm in diameter. The
magnetic contrast image shows a well-resolved
domain structure that is significantly different from
that of single-phase films. The magnetic domains
appear as interconnected bright and dark regions,
indicative of a 1808-domain structure with their
Fig. 4. Topographic tapping mode image of In0.80Mn0.20As two
phase film (a), MFM image at 298 K (b), MFM image at 348 K (c).
All images are 5 mm  5 mm.
Fig. 5. Magnetization, M, and RMS magnetization image contrast
as a function of temperature for the In0.80Mn0.20As film.
magnetization perpendicular to the plane of the film.
These domains average approximately 520 nm in
width with a standard of deviation of 130 nm. The
applied field is only 10% of the saturation field for the
two-phase film and as a result rod-like domains with
magnetization parallel and antiparallel to the applied
field are observed. MFM images of the In0.80Mn0.20As
film were obtained for temperatures up to 348 K. The
MFM image at 348 K is shown in Fig. 4(c). No
contrast is noted. The MFM relative magnetization
decreases with increasing temperature and is found to
agree with temperature dependent SQUID magnetiza-
tion data, as shown in Fig. 5.
4. Conclusions
In summary, variable temperature magnetic force
microscopy has been performed on both single and
two-phase (In,Mn)As films grown by MOVPE. MFM
relative magnetization measurements indicate that
both the single phase and multiphase films are
ferromagnetic up to 330 K. A complex domain
structure consisting of local cylindrical domains and
longer range ribbon-like domains were observed in
single phase (In,Mn)As films. A distinctly different
domain structure was observed in the two-phase
In0.80Mn0.20As film, consisting of interconnected
cylindrical domains with magnetization perpendicular
to the plane of the film. The temperature dependence
of the magnetization measured using MFM and
SQUID magnetometry was in excellent agreement.
 S.J. May et al. / Applied Surface Science 252 (2006) 3509–3513
Acknowledgements
The authors are grateful to Prof. L.J. Lauhon for
discussions on scanning probe microscopy. This work
is supported by the NSF under the Spin Electronics
Program ECS-0224210. D.P. Eam was supported by
the NSF MRSEC REU program at Northwestern
University under contract DMR-0076097. Extensive
use of the MRSEC Surface Science Facility at
Northwestern University is acknowledged.
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