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

that maintain their ferromagnetic properties above
Ferromagnetic semiconductors, obtained by alloy- room temperature [4]. Recently, ferromagnetism has
ing III–V compounds with magnetic elements such as been observed at temperatures up to 330 K in
Mn, have generated much interest for their possible (In,Mn)As grown by metal-organic vapor phase
use in all semiconductor spintronic devices [1–3]. The epitaxy (MOVPE) [5]. The high Curie temperature
realization of practical devices, including the spin field (TC), which is independent of Mn concentration, has
been attributed to short-range order involving Mn–Mn
* Corresponding author. Tel.: +1 847 491 3219;
near neighbor pairs [6]. The nature of the ferromag-
fax: +1 847 491 7820. netic domain structures of these thin films is not
E-mail address: [email protected] (B.W. Wessels). 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 perpendicular to the plane of the film, and parallel to
ferromagnetic semiconductors [7–9]. In low tempera- the magnetization of the tip, appear as regions of light
ture measurements of (Ga,Mn)As films, both stripe and dark contrast [15]. Domains in films with in-plane
domains and isolated, randomly oriented cylindrical magnetization appear as gray regions between domain
domains have been observed [10–12]. walls, which are observed as light and dark lines [16].
In this report, the magnetic domain structure of Since the change in resonant frequency is proportional
MOVPE grown (In,Mn)As thin films is determined to the strength of the magnetic interaction between the
using variable temperature magnetic force microscopy film and the magnetic tip, the RMS contrast of the
(MFM). Cylindrical domains and larger ribbon-like MFM images scales with the magnetization of the film
domains have been observed in the (In,Mn)As films [17]. Thus, relative magnetization of the samples is
persisting up to 328 K. A well-defined interconnected obtained by measuring the RMS contrast of each
rod-like domain structure was observed in two phase MFM image. A lift height of 60 nm was used for the
films consisting of (In,Mn)As and hexagonal MnAs. In0.92Mn0.08As and In0.8Mn0.2As films, while a lift
For both single and two-phase films, the temperature height of 30 nm was used for the In0.96Mn0.04As film.
dependence of the relative magnetization as deter- Two different scanners were used, one for fixed
mined by MFM is in agreement with SQUID temperature measurements and one for variable
magnetization measurements. 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
2. Experimental magnetic field is applied to the sample by the fixed
temperature scanner.
(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 3. Results and discussion
previously described [13]. All films grown on GaAs
were p-type as determined by Hall effect measure- The room temperature domain structure of a
ments with hole concentrations between 1  1018 and 400 nm thick In0.96Mn0.04As film grown on an InAs
3  1018 cm 3. Carrier concentrations of the films (0 0 1) substrate was investigated using the fixed
grown on InAs are unknown as the substrate resistance temperature scanner. The obtained MFM image is
is less than that of the film. Film thickness ranged from shown in Fig. 1(a). In order to ensure that the MFM
350 to 740 nm as determined by profilometry. Double image contrast is caused by the film magnetization and
crystal X-ray diffraction (XRD) with Cu Ka1 radiation not due to topographical artefacts, the tip magnetiza-
was used to determine phase composition. Mn tion was reversed by 1808 and a MFM scan was
concentration of the films was determined by energy obtained of the same area. In the resulting scan, shown
dispersive X-ray spectroscopy. Magnetic force micro- in Fig. 1(b), the magnetization of all the domains
scopy was performed using a Digital Instruments appears to be reversed, proving that the contrast is
NanoScope IIIa atomic force microscope. A cobalt caused by the film magnetization.
coated magnetic tip with a resonant frequency of A complex domain structure is observed, consist-
70 kHz was used in all scans. To obtain a topogra- ing of local cylindrical domains with regions of
phical image of the surface, the microscope first scans longer-range magnetic order between the cylindrical
along the surface in the tapping mode. The same area domains. The cylindrical domains are attributed to
is then rescanned at a programmed tip lift height to single domains with magnetization perpendicular to
obtain the magnetic image. Magnetic interactions the plane of the film [9]. The diameters of these
between the oscillating magnetic tip and sample domains range from approximately 100–350 nm. The
produce a change in the resonant frequency of the density of the cylindrical domains is approximately
cantilever. These frequency changes are detected 5  108 cm 2. The local cylindrical domains are often
optically and converted into an image of the local accompanied by surface pits ranging from 5 to 25 nm
magnetic structure [14]. Domains with magnetization in depth. The areas between the pits, for instance along
 S.J. May et al. / Applied Surface Science 252 (2006) 3509–3513 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-
Fig. 1. MFM images of an In0.96Mn0.04As film at 295 K measured rical and larger ribbon-like domains, is similar to that
before (a) and after (b) reversing the tip magnetization by 1808. The of the In0.96Mn0.04As film shown in Fig. 2. In contrast
images are 4.7 mm  1.5 mm. The contrast data measured along the to Fig. 1, the cylindrical domains all appear dark
white lines in (a) and (b) is shown in (c).
indicating that the applied magnetic field of 500 Oe
has aligned these domains. SQUID measurements
the line scans in Fig. 1(a) and (b), are atomically show that a 500 Oe field is 33% of the saturation field
smooth. It is likely that the cylindrical domains are for this film. The measured cylindrical domain density
caused by higher Mn concentrations in these areas, at room temperature is approximately 2  108 cm 2.
which in turn cause the defects responsible for the A few domains with their magnetization axis in the
surface pitting. Magnetic contrast is also present in the plane of the film are also visible, which manifest
regions between the cylindrical domains. This is themselves as neighboring bright and dark regions
clearly shown in Fig. 1(c), in which the MFM data [9,17]. An example of an in-plane domain can be seen
obtained from the line scans of the white lines in in Fig. 2(c) indicated by the arrow. An example of the
Fig. 1(a) and (b) is plotted. Even though the line scan ribbon domains found can be seen in Fig. 2(f), which is
does not pass through any bright cylindrical domains, an enlargement of the bottom region of Fig. 2(b)
a clear and consistent magnetic signal is obtained. indicated by the arrow. The persistence of the domains
These longer-range domains vary in length from 500 up to 328 K is in agreement with the measured
to 1000 nm and in width from 200 to 500 nm. The TC = 330 K obtained from SQUID measurements. A
magnetic signal from the cylindrical domains is 5–7 similar cylindrical domain structure, persisting up to
times stronger than the signal from the long-range 330 K, was also observed in an epitaxial
domains. In0.97Mn0.03As film. The RMS contrast values of
Fig. 2 shows the MFM images obtained at the MFM images were obtained and are shown in
temperatures between 298 and 348 K from an 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 Fig. 5. Magnetization, M, and RMS magnetization image contrast
as a function of temperature for the In0.92Mn0.08As film. Magnetiza- as a function of temperature for the In0.80Mn0.20As film.
tion data obtained from SQUID measurement with a 10 kOe field
applied perpendicular to the plane of the film. magnetization perpendicular to the plane of the film.
These domains average approximately 520 nm in
tion data, obtained with a magnetic field of 10 kOe width with a standard of deviation of 130 nm. The
applied perpendicular to the same film, is also plotted applied field is only 10% of the saturation field for the
in Fig. 3. Excellent agreement between the tempera- two-phase film and as a result rod-like domains with
ture dependent MFM and SQUID magnetization data magnetization parallel and antiparallel to the applied
is observed. field are observed. MFM images of the In0.80Mn0.20As
Two phase epitaxial films, consisting of zinc blende film were obtained for temperatures up to 348 K. The
(In,Mn)As and second phase hexagonal MnAs as MFM image at 348 K is shown in Fig. 4(c). No
determined by XRD, were also investigated. Fig. 4(a) contrast is noted. The MFM relative magnetization
and (b) show the topographic and magnetic contrast decreases with increasing temperature and is found to
images obtained from a two phase In0.80Mn0.20As film agree with temperature dependent SQUID magnetiza-
at room temperature, respectively. The MnAs pre- tion data, as shown in Fig. 5.
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 4. Conclusions
domain structure that is significantly different from
that of single-phase films. The magnetic domains In summary, variable temperature magnetic force
appear as interconnected bright and dark regions, microscopy has been performed on both single and
indicative of a 1808-domain structure with their 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
Fig. 4. Topographic tapping mode image of In0.80Mn0.20As two
to the plane of the film. The temperature dependence
phase film (a), MFM image at 298 K (b), MFM image at 348 K (c). of the magnetization measured using MFM and
All images are 5 mm  5 mm. SQUID magnetometry was in excellent agreement.
 S.J. May et al. / Applied Surface Science 252 (2006) 3509–3513 3513

Acknowledgements [7] T. Dietl, J. König, A.H. MacDonald, Phys. Rev. B 64 (2001)

241201.
[8] U. Welp, V.K. Vlasko-Vlasov, X. Liu, J.K. Furdyna, T. Woj-
The authors are grateful to Prof. L.J. Lauhon for towicz, Phys. Rev. Lett. 90 (2003) 167206.
discussions on scanning probe microscopy. This work [9] F. Zhang, N. Chen, Z. Liu, C. Chai, S. Yang, J. Yang, J. Wu, L.
is supported by the NSF under the Spin Electronics Lin, F.D. Callaghan, T. Li, C.T. Foxon, C.A. Bates, Jpn. J.
Program ECS-0224210. D.P. Eam was supported by Appl. Phys. 42 (2003) 3389.
the NSF MRSEC REU program at Northwestern [10] T. Shono, T. Hasegawa, T. Fukumura, F. Matsukura, H. Ohno,
Appl. Phys. Lett. 77 (2000) 1363.
University under contract DMR-0076097. Extensive [11] T. Fukumura, T. Shono, K. Inaba, T. Hasegawa, H. Koinuma, F.
use of the MRSEC Surface Science Facility at Matsukura, H. Ohno, Physica E 10 (2001) 135.
Northwestern University is acknowledged. [12] A. Pross, S. Bending, K. Edmonds, R.P. Campion, C.T. Foxon,
B. Gallagher, J. Appl. Phys. 95 (2004) 3225.
[13] A.J. Blattner, J. Lensch, B.W. Wessels, J. Electron. Mater. 30
(2001) 1408.
References [14] Y. Martin, H.K. Wickramasinghe, Appl. Phys. Lett. 50 (1987)
1455.
[1] H. Ohno, H. Munekata, S. von Molnár, L.L. Chang, J. Appl. [15] H.J. Hug, B. Stiefel, P.J.A. van Schendel, A. Moser, R. Hofer,
Phys. 69 (1991) 6103. S. Martin, H.-J. Güntherodt, S. Porthun, L. Abelmann, J.C.
[2] H. Ohno, Science 281 (1998) 951. Lodder, G. Bochi, R.C. O’Handley, J. Appl. Phys. 83 (1998)
[3] S.A. Wolf, D.D. Awschalom, R.A. Buhrman, J.M. Daughton, 5609.
S. von Molnár, M.L. Roukes, A.Y. Chtchelkanova, D.M. [16] F. Schippan, G. Behme, L. Daweritz, K.H. Ploog, B. Dennis,
Treger, Science 294 (2001) 1488. K.-U. Neumann, K.R.A. Ziebeck, J. Appl. Phys. 88 (2000)
[4] S. Datta, B. Das, Appl. Phys. Lett. 56 (1990) 665. 2766.
[5] A.J. Blattner, B.W. Wessels, J. Vac. Sci. Technol. B 20 (2002) [17] S.H. Chung, S.R. Shinde, S.B. Ogale, T. Venkatesan, R.L.
1582. Greene, M. Dreyer, J.B. Dottellis, A. Millis, R.D. Gomez,
[6] A.J. Blattner, B.W. Wessels, Appl. Surf. Sci. 221 (2004) 155. IEEE Trans. Magn. 38 (2002) 2886.