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Scripta Materialia 83 (2014) 2932
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High-temperature magnetic shape memory actuation

in a NiMnGa single crystal
E. Pagounis,a, R. Chulist,b M.J. Szczerbab and M. Laufenberga
a
ETO MAGNETIC GmbH, Hardtring 8, 78333 Stockach, Germany
b
Institute of Metallurgy and Materials Science, Polish Academy of Sciences, 30-05 Krakow, Poland
Received 13 March 2014; revised 3 April 2014; accepted 3 April 2014
Available online 13 April 2014

We report a NiMnGa single crystal that demonstrates giant magnetic eld-induced strain of 7.3% at room temperature and of
4.5% at 80 C. This is the highest temperature at which strain caused by twin boundary motion induced by an external magnetic eld
has been reported. A dedicated testing bench was constructed for the high-temperature experiments. X-ray diraction reveals that at
room temperature the material possesses a mixture of 5M and of 7M martensites, while at 80 C the 5M structure predominates.
2014 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Keywords: Ferromagnetic shape memory; Magnetic properties; Crystal structure; Twinning; Actuators

Magnetic shape memory (MSM) materials elon-
gate and contract in a controlled way in the presence of
a moderate (<0.5 T) magnetic eld [1]. They oer the
advantage that, depending on the crystal structure, a
large strain (>6%) and stress (>2 MPa) can be produced
at an extremely short reaction time (of the order of
microseconds). They are typically single-crystalline
materials, but polycrystals [2,3], thin lms [4,5] and com-
posite structures [6] have also been produced. The rst
report on a giant magnetic eld-induced strain (MFIS),
attributed to structural re-orientation due to twinning
dates back in 1970s, when a 3.4% strain was measured in
a dysprosium single crystal at cryogenic temperatures
[7]. However, this novel approach to inducing motion
and force gained considerable attention only after engi-
neering materials based on NiMnGa were developed
[812]. In these materials magnetically favorably ori-
ented twin variants are aligned to the direction of the
external eld, inducing twin boundary motion and a
large shape change. The eect takes place in the mar-
tensitic phase, and is driven by the dierence in the mag-
netocrystalline anisotropy energy between variants
possessing dierent crystallographic orientations with
respect to the magnetic eld.
Corresponding author. Tel.: +49 7771809468; e-mail: e.pagounis@
etogroup.com
Initially, NiMnGa MSM materials demonstrated
0.2% MFIS at 8 C [13]. The MFIS has since been
increased [14,15], the twinning stress decreased [16,17],
and the work output and eciency have reached their
maximum theoretical values [18,19]. The mechanical sta-
bility and brittleness of NiMnGa have also been
improved [20]. Furthermore, advancements in the sin-
gle-crystal production and in the manufacturing of
MSM elements for actuator and sensor applications
have been achieved [2123]. On the other hand, little
progress has been reported in increasing the operating
temperature of MSM materials, which todayas dem-
onstrated by published measurement curvesis slightly
above room temperature, and in some cases, involving
addition of a fourth element, at temperatures of up to
60 C [24]. Extending the high-temperature operational
limit constitutes a major challenge in MSM materials
research, because it will lead to the wider utilization of
these materials in actuator applications. Alloying the
NiMnGa material with fourth or fth elements to
obtain high-temperature structures has therefore also
been studied [25]. The absence of MFIS at temperatures
P80 C was attributed to the large twinning stress of
martensitic structures typically observed at these tem-
peratures [26].
Glavatskyy et al., using magnetic dilatometry,
reported a MFIS of 4.2% at 60 C in a NiMnGa alloy
containing 2.7 at.% Cu [24]. So far this is the highest

http://dx.doi.org/10.1016/j.scriptamat.2014.04.001
1359-6462/ 2014 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.
30 E. Pagounis et al. / Scripta Materialia 83 (2014) 2932
temperature at which MFIS is reported; however, no
information was given as to whether MFIS was also
measured at room temperature in the same material.
In most cases MFIS is measured at room temperature
and then it is assumed that the strain is maintained up
to the austenite transformation. This is not always the
case, however, because intermartensitic transformations,
change in lattice parameters and other eects may result
in a considerably dierent strain output, or no strain at
all, as the temperature increases or decreases [24,27].
Herein, we report a NiMnGa single crystal
demonstrating MFIS both at room and at elevated tem-
peratures. The crystal, with the composition Ni50.8
Mn28.4Ga20.8 (0.6 at.%), was produced at ETO
MAGNETIC GmbH using Bridgman-type crystal
growth. The present alloy has a higher Ni/Ga at.% ratio
than in standard MSM alloys, giving a ratio of valence
electrons per atom e/a = 7.692, which contributes to
increasing the phase transition temperatures [26]. Utiliz-
ing the Bridgman technique yields homogeneous single
crystals [22]. After the crystal growth process the mate-
rial was heat treated at temperatures close to 1000 C for
homogenization and ordering. The crystallographic ori-
entation was determined using electron backscattering
diraction techniques. Rectangular elements with the
dimensions of 2  3  15 mm3 were cut along the
{1 0 0} planes of the parent L21 cubic phase, using elec-
trical discharge machining. The sample for magnetome-
chanical measurements was electropolished and trained,
by repeated compressions along the three surfaces, to
achieve a single variant state with the short (001) crystal-
lographic axis along the samples long axis. The austen-
ite (TA) and martensite (TM) transformation
temperatures and the Curie point (Tc) were measured
using dierential scanning calorimetry (DSC) with a
Netzsch Phoenix DSC 204 analyzer operating at a heat-
ing/cooling rate of 5 K min1.
High-temperature MFIS measurements are rarely
reported in the literature, which is a paradox considering
the emerging research target of developing MSM mate-
rials operating at elevated temperatures. Besides the lim-
ited data on high-temperature MSM alloys, the main
reason for this may also be that accurate measurements
are not easy to perform, and a carefully designed test
bench needs to be established. We therefore constructed
a dedicated test bench for room- and high-temperature
MFIS measurements. Here, the MSM sample is intro-
duced in a copper holder, which is heated and cooled
using a Julabo F32-EH thermostat. The copper holder
is designed to surround the sample in order to achieve
a homogeneous temperature distribution. The tempera-
ture of the test sample was constantly monitored with a
deviation of 2 C using a thermocouple placed just
below the sample. Compression stressstrain measure-
ments, without eld, along the [1 0 0] direction of the
sample were carried out in order to determine the
mechanically induced strain and the twinning stress.
The mechanical compression tests were performed using
a ZwickRoell testing machine with a load cell of
2.5 kN. Strain vs. eld measurements were performed
in the magnetic eld generated by a water-cooled
GMW 5403 electromagnet (GMW, San Carlos, CA).
The strain was recorded with a laser triangulation sensor
(Micro-Epsilon, LD1627-20) operating at a sampling
rate of 37 kHz. The magnetic eld in the air gap of the
electromagnet was monitored with a Magnet-Physik
FH 55 eld strength meter and a Hall sensor. The mag-
netic eld was applied along the [1 0 0] direction of the
sample and the strain was measured perpendicular to
this direction.
The crystal structure and lattice parameters were
studied with a Bruker D8 Advance X-ray diractometer
equipped with a Co tube. The diraction information
was recorded using a linear detector with a 2h range of
2.5, which allowed a simultaneous collection of (2 0 2}
reections of both 5M and 7M phases. The (} notation
means that the rst index is xed, whereas the two last
indices may be changed. In order to detect the crystal
structure rst a texture type scan for {2 2 0} and {4 0 0}
was performed. Subsequently, using these reections, a
ne scan for the u and v angles was performed
(Fig. 3a, b). Additionally, to ensure the correct distinc-
tion between the 5M and 7M phases, the rst-order
satellite reections for the 7M and 5M structures were
detected. The lattice parameters were established by
measuring {2 2 0} and {4 0 0} reections combined with
an accurate 2h scan. Using both measurements, the best
t was found. For high-temperature X-ray diraction
(XRD) studies the sample was heated up to 73 2 C,
to ensure that it remains in the martensite state. Upon
heating, the same experimental parameters (position,
exposure time) were used, which enables a direct com-
parison of structural changes.
Figure 1 shows the DSC measurement of the heat-
treated NiMnGa single crystal, with the phase trans-
formation temperatures and the Curie point on heating
(T hc 98 C) and on cooling (T cc 94 C). The hysteresis
in magnetic transitions has been reported also in other
high-temperature NiMnGa materials [26]. At 66 C
a transformation peak is observed during heating, indi-
cating the intermartensitic 7M to 5M transformation
[26]. The relatively broad phase transformation intervals
are attributed to internal stresses in the single crystal
[28]. The residual stresses mainly come from the crystal
growth process, and the subsequent annealing did not
relieve them completely. Large internal stresses generally
contribute to the brittleness of MSM single crystals,
and, in this respect, should be avoided. For the material
studied in the present work, however, brittleness has not
Figure 1. Plot of the DSC curve showing the austenite (TA) and
martensite (TM) transformation temperatures, the intermartensitic
7M ! 5M transformation, and the Curie point on heating (T hc ) and on
cooling (T cc ).
 E. Pagounis et al. / Scripta Materialia 83 (2014) 2932
been an issue. Guo et al. [29] reported that internal stres-
ses in NiMnGa ribbons are benecial in obtaining
large phase transition-induced strain and MFIS. The
eect of these stresses on the magnetomechanical prop-
erties of single-crystalline MSM materials is not clear
yet, and is therefore an interesting topic for further
research.
The MFIS measurements of the NiMnGa sample
are summarized in Figure 2a. It can be seen that a
7.3% strain is obtained at room temperature and a
4.5% strain at 80 C. This result indicates that a 7M
martensite structure is expected at room temperature
and a 5M structure at 80 C [1]. In both cases the activa-
tion eld is below 250 kA m1, i.e. similar to standard
NiMnGa MSM materials reported in the literature
[1,30]. The slightly higher eld needed to produce the
maximum strain at the high-temperature measurement
can be attributed to the dierent martensitic structures
predominating at the two temperatures with corre-
spondingly dierent twinning stress values. At both tem-
peratures, however, the maximum strain is achieved at a
eld strength well below 600 kA m1, which is compat-
ible with commercially available electromagnetic
devices.
The mechanical stressstrain curves of the NiMn
Ga sample at the two temperatures are shown in Fig-
ure 2b. The twinning stress, dened as the stress
required to produce half of the samples maximum
22 C
strain [30], measured rtw 1:13 MPa at room temper-

80 C
ature and rtw 1:53 MPa at high temperature. The
stress increases slowly with strain until a maximum is
reached, and then it decreases rapidly. This is a sign of
a possible stress-induced intermartensitic transforma-
tion at a critical stress. This stress is measured as
2.1 MPa, both at 22 C and at 80 C. The maximum
Figure 2. Magnetomechanical measurements for the NiMnGa single
crystal showing (a) MFIS at room and at high temperature, and (b)
mechanical stressstrain curves at the two temperatures.
31
mechanically induced strain was 10.9% at 22 C and
5.8% at 80 C. These values are close to the theoretical
ones based on the crystallographic lattice distortions
for 7M and 5M martensitic structures, respectively.
The MFIS in both measurements is 70% of the respec-
tive mechanically induced strain. The reason for this dif-
ference may lie in the maximum available magnetic
stress rM Ku =e0 , where Ku is the magnetocrystalline
anisotropy energy and e0 the maximum strain due to lat-
tice distortion [30].
For a 7M martensite, Straka [31] reported that the
maximum available magnetic stress at room tempera-
22 C
ture is rM 1:5 MPa. In the present material this
stress produces a strain of 7.3%, as shown in the
stressstrain curve in Figure 2b. Accordingly, the mea-
sured 7.3% MFIS at room temperature indicates good
agreement with the MSM model [30,31]. In a typical
5M structure the maximum available magnetic stress
at 40 C is of the order of 2.8 MPa [30]. When the tem-
perature increases, this stress decreases, because the
magnetocrystalline anisotropy decreases [30]. At 80 C
the obtained MFIS is 4.5%, which, as seen in the
stressstrain curve, corresponds to a magnetic stress of
C
r80
M 2:1 MPa. Further work is planned by the
authors on this topic, and particularly on investigating
the magnetocrystalline anisotropy energy of the studied
alloy. In any case, the criterion rtw < rM is fullled, and
therefore the observation of the giant MFIS is justied
at both temperatures. The subsequent dip in the
stressstrain curve with the correspondingly lower
mechanical stress values does not aect the MFIS values
obtained.
The XRD experiments shown in Figure 3 indicate
that the sample exhibits a mixture of 7M and 5M mar-
tensite at room temperature (estimated ratio from all
Figure 3. (a) XRD pattern over the 2h scan at u = 267 and v = 50,
showing only the (2 0 2} and (2 2 0) reections for 5M and 7M phases,
respectively. (b) The analogous scan for the (2 0 2) reection of 7M
phase performed at u = 267 and v = 42.
32 E. Pagounis et al. / Scripta Materialia 83 (2014) 2932
recorded reections 40:60). The lattice parameters for
the 7M monoclinic crystal structure measured
a7M = 0.6242 nm, b7M = 0.5802 nm, c7M = 0.5525 nm
and b7M = 93.04. This yields the theoretical maximum
strain of 11.5% (emax = 1  c/a). For the tetragonal
5M structure the lattice parameters at 73 C are
a5M = 0.5946 nm, b5M = 0.5937 nm and
c5M = 0.5573 nm, resulting in a maximum theoretical
strain of 6.2%. The XRD measurements conrm that
above 70 C no 7M structure exists (Fig. 3b), because
only the reections belonging to the 5M structure are
detected (Fig. 3a). When cooling back to room temper-
ature (marked as after heating in Fig. 3), however, the
7M structure does not reappear. This suggests that the
intermartensitic 5M ! 7M transformation starts below
room temperature during cooling. Large temperature
hysteresis in the intermartensitic transformation is com-
mon in NiMnGa materials [26]. Theoretical strain val-
ues, calculated from the lattice parameters, are in good
agreement with the experimental results. At room tem-
perature a mechanical strain of 10.9% has been mea-
sured, indicating an intermartensitic 5M ! 7M
transformation, which is stress induced. It should be
noted that the lattice parameters of the 5M structure
at high temperature slightly dier from those at room
temperature. After the heating cycle the lattice parame-
ters of the 5M structure change again depending on
whether the 5M structure coexists with 7M or occurs
separately. This indicates that the lattice parameters of
5M are strongly adaptive, which constitutes an interest-
ing topic for further research.
Similar to Ref. [27]the stability of NiMnGa
martensites as a function of temperature on cooling
follows the well-known sequence: austenite ! 5M !
7M ! NM. The stress level needed to activate the inter-
martensitic phase transformation is signicantly lower
here, 2.1 MPa, i.e. within the range of the shear stress
induced by the magnetic eld in several MSM materials
[1]. However, as deduced above, in the present material
the stress of 1.5 MPa at 22 C and of 2.1 MPa at 80 C is
the maximum that can be induced by the magnetic eld.
Consequently, no eld-induced intermartensitic trans-
formation takes place.
In conclusion, a NiMnGa MSM material demon-
strating a giant MFIS of 4.5% at 80 C is reported in
the present work. The extension of the high-temperature
limit of MSM materials is a major breakthrough,
achieved after almost two decades of research, which
considerably broadens their application potential.
Detailed XRD investigation revealed that a 5M mar-
tensitic structure predominates in the material at tem-
peratures above 70 C, while at room temperature a
mixture of 7M and 5M martensites coexists. The mag-
netomechanical properties correlate well with the respec-
tive martensitic structures. The required magnetic elds
for MSM actuation are of the order typically used in
electromagnetic actuators.
The authors would like to thank M. Helmer and
M. Maier of ETO MAGNETIC GmbH for sample
preparation and testing. Part of the work (R.C.) was
carried out within the Homing Plus Program (project
2013-8/3) of Foundation for Polish Science, co-nanced
by the European Union Regional Development Fund.
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