Journal of Magnetism and Magnetic Materials 240 (2002) 546–549

Structural, magnetic and magnetotransport properties

of thin films of the Heusler alloys Cu2MnAl,
Co2MnSi, Co2MnGe and Co2MnSn
U. Geiersbach, A. Bergmann, K. Westerholt*
. Experimentalphysik IV, Ruhr-Universitat,
Institut fur . D 44780 Bochum, Germany

Abstract

We report structural, magnetic and transport properties of thin films of the Heusler compounds Cu2MnAl, Co2MnSi,
Co2MnGe and Co2MnSn prepared by RF-sputtering. Cu2MnAl grows epitaxially on MgO (1 0 0), for the Co-based
Heusler compounds it is possible to induce (1 1 0)-growth on Al2O3 a-plane by the use of metallic seed layers. The Co-
based alloy thin films grow in the ordered L21 structure and essentially preserve the full ferromagnetic magnetization of
the bulk. The electrical conductivity is rather low indicating substantial magnetic or structural disorder. r 2002
Elsevier Science B.V. All rights reserved.

Keywords: Half-metallic ferromagnets; Spin electronics; Heusler compounds

Mainly motivated by the new, rapidly evolving field of
magnetoelectronics [1] there is an upsurge of interest in
ferromagnetic metals with full spin polarization at the
Fermi level. These so-called half-metallic ferromagnets
are favourable candidates for applications in tunnelling
magnetoresistance (TMR) or giant magnetoresistance
(GMR) elements and as electrodes for spin polarized
current injection into semiconductors. There are an
increasing number of metallic ferromagnetic oxides like
CrO2 [2] and La1
xSrxMnO3 [1] with full spin polariza-
tion at the Fermi level which are presently under intense
investigation.
Half-metallic ferromagnetic alloys are scarce, since
usually the s- and p-type valence electrons contribute
both spin directions at the Fermi level. Until now there
are only a few intermetallic compounds known to have
this unique property, all belonging to the Heusler group
with the general formula A2BX (A=Cu, Co, Niy,
B=Mn, Fey, X=Al, Ge, Siy) [3]. The basic Heusler
structure is a cubic lattice (space group Fm3m) with four
*Corresponding author. Fax: +49-234-1721-4173.
E-mail address: kurt.westerholt@ruhr-uni-bochum.de
(K. Westerholt).
interpenetrating FCC sublattices occupied by A-, B- or
X-atom, respectively. The ferromagnetic half metals
known from theoretical band structure calculations are
the compounds PtMnSb and NiMnSb [4] (so-called half-
Heusler compounds since one A-sublattice is empty) and
the compounds Co2MnSi, Co2MnGe [5]. Following
band structure calculations, Co2MnSn and Co2MnSb in
a strict sense do not belong to this group, since they
possess only about 90% of spin polarization, but they
can be made half-metallic ferromagnets by alloying [6].
In recent years, the properties of thin films of the half-
Heusler compounds PtMnSb and NiMnSb have been
studied by several groups [7] and these compounds have
already been tested in TMR- and GMR-thin film
heterostuctures [8]. The other group Co2MnSi,
Co2MnGe, Co2MnSn and Co2MnSb found little atten-
tion in the experimental literature until now. To the best
of our knowledge, we present the first systematic
experimental study of the basic properties of thin films
of these compounds in order to elucidate their potential
for future applications in the field of spin electronics.
Thin films of Cu2MnAl, Co2MnSi, Co2MnGe and
Co2MnSn were prepared on sapphire a-plane and
MgO(1 0 0)-substrates by RF sputtering in Ar. The base

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 U. Geiersbach et al. / Journal of Magnetism and Magnetic Materials 240 (2002) 546–549
pressure of the sputtering system was 10–7 mbar during
the sputter deposition process. The targets were made
from single-phase, stoichiometric ingots of the Heusler
compounds prepared by high-frequency melting in
carbon crucibles.
We varied the growth rate, the Ar pressure and the
substrate temperature for optimizing the structural
quality of the films. The optimized parameters we used
for the film preparation combined an Ar pressure of
5  10
3 mbar, a growth rate of 0.06 nm/s and a
substrate temperature of 4701C.
Using these preparation conditions, the Cu2MnAl-
phase can be grown with a perfect (1 1 0)-texture on
sapphire a-plane. On MgO (1 0 0) we achieved an
epitaxial (1 0 0)-growth with a rocking width of the
out-of-plane (2 0 0)-Bragg peak of 0.161 (Fig. 1) and a
fourfold symmetry of the (1 0 0)-in-plane Bragg peak (
see in-plane rocking scan in the inset of Fig. 1).
Fig. 1. Out-of-plane X-ray Bragg scan of a Cu2MnAl film on
MgO(1 0 0) (Cu-Ka -radiation, film thickness 100 nm). The inset
shows the in-plane rocking scan of the Heusler (2 0 0)-peak.
(220)
Al2O3
3
10
Au Al 2O3
counts
(111)
Au
(440)
102 (220)
20 40 60 80 100
2Θ (deg.)
Fig. 2. Out-of-plane Bragg scan of a Co2MnGe-film grown on
sapphire a-plane with an Au-seedlayer (thickness of the Heusler
film 95 nm, of the Au-seedlayer 5 nm).
547
In contrast, for the Co-based half-metallic Heusler
ferromagnets we find polycrystalline growth when
sputtering directly on sapphire a-plane or MgO. Only
with suitable metallic seed layers it is possible to achieve
textured growth of good quality. For the Co2MnSn-
phase, the optimum seed layer is Au, with a nearly
perfect lattice matching of the (1 1 1)-Au and the (1 1 0)-
Heusler layers. For the Co2MnSi-phase, we obtained
the best structural results using V-seed layers, for the
Co2MnGe-phase V, Au and Cr-seed layers give com-
parably good structural quality. In Fig. 2, we show as a
representative example the out-of-plane Bragg scan of
a film Co2MnGe grown on an Au-seed layer. One
observes only the (2 2 0)- and the (4 4 0)-Heusler Bragg
peak, evidencing pure (1 1 0)-texture. Systematic inves-
tigations of the low angle X-ray reflectivity revealed flat
surfaces and interfaces with a rms roughness below
1 nm. The lattice parameters determined from the Bragg
peaks and other parameters characterizing the thin film
structure are summarized in Table 1.
A quantitative electron microprobe analysis of the
thin film composition showed that for the Cu2MnAl-
phase there is some excess Cu in the films (53 at%), for
the Co2MnSi-phase we find a Si deficiency (23 at%). For
the other two phases in Table 1 the thin films preserve
the stoichiometric composition of the targets.
The ferromagnetic magnetization of the films was
analysed by a Quantum Design SQUID magnetometer.
Fig. 3 shows representative ferromagnetic hysteresis
loops measured at 5 K. The saturation magnetization
decreases up to room temperature by about 5%
for the Co2MnSi- and the Co2MnGe-phase and by
about 7% for the Co2MnSn-phase, consistent with their
high ferromagnetic Curie temperatures of 985, 905 and
829 K, respectively [3]. The coercive force, depending on
the microstructure and the magnetic anisotropy of
the thin films, is lowest for the Co2MnGe-phase
(Hc ¼ 70 Oe).
The ferromagnetic saturation magnetization mea-
sured at 5 K has been included in Table 1. When
comparing the thin film and the bulk values for the
saturation magnetization in Table 1, one notes that for
the Cu2MnAl-phase the magnetization value of the thin
film is only about 40% of the bulk value. This reduction
of the magnetization is caused by incomplete metallur-
gical order in the unit cell, mainly of the B2-type [3], i.e.
site disorder with some Mn atoms on the A-positions
and vice versa.
For the Co-based Heusler alloy thin films in Table 1,
the saturation magnetization is much closer to the bulk
values and for the Co2MnSn- and the Co2MnGe-phase
nearly coincides with them. This indicates the absence of
sizable B2-type site disorder, consistent with the fact
that for these phases the ordered L21-type phase is very
stable. Only for the Co2MnSi thin film we observe a
definitely lower value of the magnetization than in the
548 U. Geiersbach et al. / Journal of Magnetism and Magnetic Materials 240 (2002) 546–549

Table 1
Structural parameters and saturation magnetization measured at 5 K for the Heusler films on Al2O3 a-plane used for the present study.
The values for the bulk have been taken from Ref. [3]

Phase Seed layer Texture Rocking width Lattice parameter (nm) Magnetization (emu/g)
(2 2 0)-peak (deg)
Bulk Film Bulk Film

Cu2MnAl No (1 1 0) 1 0.5962 0.5905 97 40

Co2MnSi V (1 1 0) 3 0.5654 0.5688 138 97
Co2MnGe Cr (1 1 0) 4 0.5743 0.5766 111 103
Co2MnSn Au (1 1 0) 3 0.6000 0.6003 91 87

Fig. 3. Magnetic hysteresis loops of measured at 5 K for the

Heusler-phase Co2MnSi (dotted line) Co2MnGe (dash-dotted)
and Co2MnSn (full line). Fig. 4. Electrical resistivity versus temperature for the Heusler
thin films from Table 1.

bulk, which we would attribute to the deviation from the 105.856

ideal stoichiometry for this film. 105.85
The temperature dependence of the electrical resistiv-
ity for the samples from Table 1 measured by a standard
four-point DC-method is plotted in Fig. 4. We observe a 105.80

rather high value for the resistivity of the Co-based 105.848

ρ(µΩcm)

compounds with a residual resistivity ratio reaching only

105.75
about 1.3 for the Co2MnGe- and the Co2MnSn-phase 0 500
and an even lower value for the Co2MnSi-phase, H(Oe)

indicating a strong scattering on magnetic or non- 105.70

magnetic defects. Interestingly, all Co-based Heusler
phases exhibit a shallow minimum in the rðTÞ-curve
with a minimum temperature at about 40 K reminiscent 105.65
0 10000 20000 30000 40000
of a Kondo-type of low temperature anomaly. The H(Oe)
origin of this behaviour is not clear yet, we tentatively
attribute it to a thermal excitation of charge carriers Fig. 5. Resistivity versus magnetic field measured at 4.2 K for a
across the gap in the minority spin band [6]. thin film Co2MnSn. The inset shows the low field magneto-
One example of a magnetoresistivity curve for the Co- resistance.
based Heusler compounds measured with the magnetic
field applied in the film plane and parallel to the current negative magnetoresistance up to magnetic fields of 5 T.
is shown in Fig. 5. The anisotropic magnetoresistance in The most plausible interpretation of the isotropic
the range of the hysteresis loop is very small (see inset in magnetoresistance is the assumption of some spin
Fig. 5) and as a characteristic feature of all Co-based disorder in the Heusler compounds even at 4 K, indicat-
Heusler thin films we find a rather large isotropic ing that the ferromagnetic ground state is not perfect.
 U. Geiersbach et al. / Journal of Magnetism and Magnetic Materials 240 (2002) 546–549
In summary, we have shown that for the Co-based
half-metallic Heusler compounds single-phase thin films
with the ordered L21structure, very flat surfaces and a
strong (1 1 0)-texture can be prepared by RF-sputtering
on sapphire a-plane. The preparation of the (1 0 0)-
textured films on MgO (1 0 0) with similar quality is also
possible. Thus, it seems promising to use these
compounds in spin transport applications. The thin film
quality still needs some improvement, especially with
respect to the still rather low electrical conductivity.
However, the Co-based Heusler half-metallic ferro-
magnets share these difficulties with all other fully spin
polarized metallic compounds including the half Heus-
lers [8] and the oxides [1]. The optimization of the thin
film preparation is just in the beginning and we think
that essential progress can be achieved by using an
UHV-based deposition technique and developing the
preparation conditions for perfect epitaxial growth.
The authors thank the DFG for financial support of
this work within the SFB 491, P. Stauche for the
549
.
preparation of the alloy targets and S. Erd-Bohm for
running the sputtering equipment.
References
[1] J.H. Park, E. Vescovo, E. Kim, C. Kwon, R. Ramesh,
T. Venkatesan, Nature 392 (1998) 794.
[2] K. Schwarz, J. Phys. F 16 (1986) 794.
[3] P.J. Ziebeck, K.R.A.Webster, Landolt-Bornstein. New
Series III/19c, 1986.
[4] R.A. de Groot, F.M. Muller, P.G. van Engen, K.H.J.
Bushow, Phys. Rev. Lett. 50 (1983) 2024.
[5] S. Ishida, T. Masaki, S. Fujii, S. Asano, Physica B 145
(1998) 1.
[6] S. Ishida, T. Masaki, S. Fujii, S. Asano, J. Phys. Soc. Jpn.
64 (1995) 2152.
[7] R. Kabani, M. Terada, A. Roshko, J.S. Moodera, J. Appl.
Phys. 67 (1990) 4898.
[8] J.A. Caballero, A.C. Reilly, Y. Hao, J. Bass, W.P. Pratt Jr.,
F. Petroff, J.R. Childress, J. Magn. Magn. Mater. 198–199
(1999) 55.