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APPLIED PHYSICS LETTERS

VOLUME 80, NUMBER 10

11 MARCH 2002

Giant magnetic-field-induced strain in NiMnGa seven-layered


martensitic phase
A. Sozinov,a) A. A. Likhachev, N. Lanska, and K. Ullakko
Helsinki University of Technology, P.O. Box 6200, FIN-02015 HUT, Finland

Received 13 November 2001; accepted for publication 4 January 2002


Giant magnetic-field-induced strain of about 9.5% was observed at ambient temperature in a
magnetic field of less than 1 T in NiMnGa orthorhombic seven-layered martensitic phase. The strain
proved to be caused by magnetic-field-controlled twin boundary motion. According to an analysis
of x-ray diffraction data, the crystal structure of this phase is nearly orthorhombic, having lattice
parameters a0.619 nm, b0.580 nm, and c0.553 nm in cubic parent phase coordinates at
0 p system was
ambient temperature. Seven-layer shuffling-type modulation along the (110) 11
recorded. The results of mechanical tests and magnetic anisotropy property measurements are also
reported. 2002 American Institute of Physics. DOI: 10.1063/1.1458075

In 1996 Ullakko1,2 suggested the mechanism of


magnetic-field-induced strain in magnetic shape memory alloys with large magnetic anisotropy. The mechanism is based
on the magnetic-field-induced rearrangement of the crystallographic domains twin variants that lower magnetization
energy. It can provide large strain similar to a stress-induced
one. Magnetic shape memory materials are expected to have
a high potential in the design of a different kind of actuating
devices and sensors.1,2 During the few past years, significant
progress based on this general idea of designing a new class
of magnetic shape memory alloys MSMAs and a detailed
investigation of them has been achieved.317
As of now, the largest magnetostrain effects were attained in NiMnGa ferromagnetic shape memory alloys.
Several research groups have succeeded in the observation
and investigation of a superlarge up to 6% magnetostrain
effect in some nonstoichiometric Ni2 MnGa-based alloys.
The crystal structure of the martensitic phase of these alloys
was identified as a tetragonal one that also has five-layer
shuffling type modulation and a tetragonality aspect ratio
c/a1.16,18
Depending on the chemical composition and temperature
there are also two other kinds of martensitic phase in Ni
MnGa that have orthorhombic seven-layered and tetragonal
nonlayered crystal structures with c/a1.18,19 The possibility of observing large magnetic field-induced strain in any
other martensitic phase was the main purpose of our last
study. Here we first briefly report on the observation of superlarge 9.5% strain effect in orthorhombic martensitic phase
in NiMnGa. It greatly exceeds the best result of 6% obtained earlier in the tetragonal five-layered phase of this alloy.
The alloy Ni48.8Mn29.7Ga21.5 was prepared by melting in
an induction furnace in argon atmosphere. A single crystal
specimen was cast in an alumina crucible and solidified at a
rate of 0.5 mm/min in the Bridgman crystal growth furnace
at AdaptaMat Ltd. After homogenization at 1253 K for 20 h
and aging at 1073 K for 30 h the alloy was cooled in air to
a

Electronic mail: asozinov@cc.hut.fi

room temperature. Single-crystal samples were then cut by a


spark cutting machine with dimensions of 446 mm3 .
The faces of the prismatic single-crystal samples were nearly
parallel to the 100, 010, and 001 directions of the hightemperature cubic phase. The samples were also wet polished and electropolished.
Figure 1 shows the temperature dependence of the lowfield ac magnetic susceptibility of the alloy during heating
and cooling. The abrupt change in the value of the susceptibility at 367369 K is attributed to paramagnetic
ferromagnetic transformation of the L2 1 cubic phase. The
Curie temperature is about T C 368 K.
During the coolingheating cycle we also observed a
sequence of martensitic and intermartensitic transformations.
The martensitic transformation starts at 337 K (M s ) and is
completed at 333 K (M f ) during cooling. At lower temperatures, starting at 245 K, the value of the magnetic susceptibility increased, indicating the intermartensitic transforma-

FIG. 1. Temperature dependence of low-field ac magnetic susceptibility


measured during cooling solid line and heating dashed line of the
Ni48.8Mn29.7Ga21.5 alloy. Arrows mark phase transformations. C: ferromagnetic cubic phase, Or: orthorhombic seven-layered phase, T: tetragonal nonmodulated phase. The inset shows the scattering intensity distribution in
reciprocal space between 400 and 620 nodes in the orthorhombic phase
of the Ni48.8Mn29.7Ga21.5 alloy. Arrows mark additional peaks connected
with seven-layered modulation of the lattice.

0003-6951/2002/80(10)/1746/3/$19.00
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2002 American Institute of Physics
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Sozinov et al.

Appl. Phys. Lett., Vol. 80, No. 10, 11 March 2002

FIG. 2. Magnetization curves measured along different axes of orthorhombic seven-layered phase the single-variant constrained state in the
Ni48.8Mn29.7Ga21.5 alloy at 300 K.

tion. During heating both structure transformations occur in


reverse order and show some temperature hysteresis. In particular, the reverse intermartensitic transformation takes
place during heating at 306 316 K. So reverse martensitic
transformation from the orthorhombic to the cubic parent
phase upon heating takes place between A s 338 K and A f
342 K.
By x-ray studies made with the Philips XPert diffractometer it was found that the crystal structure of the first high
temperature martensitic phase is nearly orthorhombic and
has lattice parameters of a0.619 nm, b0.580 nm, and c
0.553 nm in coordinates related to the high temperature
parent cubic phase at ambient temperature. Seven-layer
0 p system was observed.
modulation along the (110) 11
The insert in Fig. 1 shows the scattering intensity distribution
in reciprocal space between 400 and 620 nodes recorded
by a Q-type scan. There are six approximately equally
spaced additional peaks. This kind of martensitic phase is
known for nonstoichiometric Ni2 MnGa alloys.18,19 We also
found that the crystal structure of the second martensite is
tetragonal with lattice parameters of ab0.547 nm, and
c0.660 nm (c/a1.207) at 200 K and ab0.551 nm
and c0.654 nm (c/a1.187) at ambient temperature.
Since the magnetic and the mechanical properties of nonmodulated tetragonal martensite phase have recently been
studied,16 our attention was attracted to the orthorhombic
seven-layered martensite.
Usually, after a martensitic phase transition the multiple
variants of martensite form within a single crystal of the
parent high-temperature phase. Afterwards, that multivariant
state can be transformed into a nearly single variant of martensitic phase by appropriate mechanical treatment. In this
way nearly single-variant samples of orthorhombic phase
were prepared.
The magnetic properties were determined for singlevariant samples from the magnetization curves M (H) recorded along the 100, 010, and 001 directions. The
samples were constrained by epoxy to prevent a magnetically field-induced redistribution of martensite variants during the measurements. The results of the magnetic measurements are shown in Fig. 2. The magnetization curves indicate

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FIG. 3. Stressstrain curve for compression of a single-variant sample of


the Ni48.8Mn29.7Ga21.5 alloy along the 100 direction at 300 K. The change
in microstructure is shown schematically in the inset.

that the shortest axis c axis is the axis of easiest magnetization, the longest a axis is the axis of hard magnetization,
and the b axis is the intermediate one. Unlike for a single
uniaxial magnetic anisotropy constant of tetragonal phase
one needs two magnetic anisotropy parameters to characterize the orthorhombic crystal structure. The values of magnetic anisotropy constants K b 0.7105 J/m3 and K a 1.6
105 J/m3 were calculated from the magnetization data
Fig. 2 as the area cross section between the easiest curve c
axis and the two others b and a directions.
Figure 3 shows the stressstrain curve obtained during
compression along the 100 direction parallel to the longest
a axis of the orthorhombic single crystal. The maximal
twinning strain obtained is consistent with the crystal lattice
aspect ratio estimate of 0 (1c/a)10.66% found from
x-ray diffraction studies. It was confirmed that the final crystallographic structure of the sample is the same orthorhombic
system from
one but transformed by twinning (101) 101
one single crystalline variant to another with the shortest c
axis parallel to the direction of compression instead of to the
longest a axis before the testing.
The mechanical test reveals that the uniaxial compressive stress tw is approximately as low tw2 MPa as was
found before10,12,13,16 for the five-layered tetragonal phase.
This is very important because the low twinning stress and
high energy of magnetic anisotropy are key to obtaining a
large magnetic field controlled strain response MSM the
MSM effect through the mechanism of twin boundary
motion.12,13 More exactly, it is only possible in ferromagnetic
shape memory alloys that satisfy the simple criterion,17
K 0 tw .
The magnetic anisotropy energy density K which is exactly
equal to the magnetic driving force applied to the twin
boundary13,17 must always exceed or be the same order as the
mechanical driving force 0 tw needed to produce twinning.
Strain response MSM for similar systems is expected to be
practically equal to the maximal strain 0 (1c/a) allowed by twinning crystallography. In the case of the orthorhombic phase studied the K a value of 1.6105 J/m3 is of
the same order but a little less compared to 0 tw2.0

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Sozinov et al.

Appl. Phys. Lett., Vol. 80, No. 10, 11 March 2002

National Technology Agency of Finland Tekes as well as


by their industrial research partners Nokia Research Centre,
Outokumpu Research Oy, Metso Oyj, and AdaptaMat Ltd..
The authors are grateful to Tor Meinander of the Technical
Research Centre of Finland VTT for his help with magnetic
measurements, to Sanni Mustala for energy-dispersive analysis measurements, and to Olavi Mattila of AdaptaMat Ltd.
for single-crystal preparation.

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1
2

FIG. 4. Field-induced strain of a single-variant sample of orthorhombic


seven-layered phase in the Ni48.8Mn29.7Ga21.5 alloy at 300 K measured perpendicular to the magnetic field applied along the 100 direction.

105 J/m3 . So, the large MSM value, which is a little lower
than 0 10.66%, is expected for the orthorhombic phase.
Figure 4 confirms this prediction and shows the results
of the field-induced strain measurements of the alloy at ambient temperature. The magnetic field was applied parallel to
the a axis. The maximal strain achieved in the first cycle at
the field of 1.05 T is MSM9.5%. In agreement with our
earlier explanation this value is lower than the crystallographic limit 0 (1c/a)10.66% expected for complete
transformation between two single variants. As confirmed by
optical observation and x-ray diffraction studies, the transformation to the second variant with favorable c-axis orientation along the field is not complete. There are residual twin
bands in the sample.
The authors would like to acknowledge funding by the

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