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A. Sozinov, A. A. Likhachev, N. Lanska, and K. Ullakko
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APPLIED PHYSICS LETTERS VOLUME 80, NUMBER 10 11 MARCH 2002
In 1996 Ullakko1,2 suggested the mechanism of room temperature. Single-crystal samples were then cut by a
magnetic-field-induced strain in magnetic shape memory al- spark cutting machine with dimensions of 446 mm3 .
loys with large magnetic anisotropy. The mechanism is based The faces of the prismatic single-crystal samples were nearly
on the magnetic-field-induced rearrangement of the crystal- parallel to the 100, 010, and 001 directions of the high-
lographic domains twin variants that lower magnetization temperature cubic phase. The samples were also wet pol-
energy. It can provide large strain similar to a stress-induced ished and electropolished.
one. Magnetic shape memory materials are expected to have Figure 1 shows the temperature dependence of the low-
a high potential in the design of a different kind of actuating field ac magnetic susceptibility of the alloy during heating
devices and sensors.1,2 During the few past years, significant and cooling. The abrupt change in the value of the suscepti-
progress based on this general idea of designing a new class bility at 367369 K is attributed to paramagnetic
of magnetic shape memory alloys MSMAs and a detailed ferromagnetic transformation of the L2 1 cubic phase. The
investigation of them has been achieved.317 Curie temperature is about T C 368 K.
As of now, the largest magnetostrain effects were at- During the coolingheating cycle we also observed a
tained in NiMnGa ferromagnetic shape memory alloys. sequence of martensitic and intermartensitic transformations.
Several research groups have succeeded in the observation The martensitic transformation starts at 337 K (M s ) and is
and investigation of a superlarge up to 6% magnetostrain completed at 333 K (M f ) during cooling. At lower tempera-
effect in some nonstoichiometric Ni2 MnGa-based alloys. tures, starting at 245 K, the value of the magnetic suscepti-
bility increased, indicating the intermartensitic transforma-
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 possibil-
ity 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 su-
perlarge 9.5% strain effect in orthorhombic martensitic phase
in NiMnGa. It greatly exceeds the best result of 6% ob-
tained earlier in the tetragonal five-layered phase of this al-
loy.
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 FIG. 1. Temperature dependence of low-field ac magnetic susceptibility
measured during cooling solid line and heating dashed line of the
rate of 0.5 mm/min in the Bridgman crystal growth furnace
Ni48.8Mn29.7Ga21.5 alloy. Arrows mark phase transformations. C: ferromag-
at AdaptaMat Ltd. After homogenization at 1253 K for 20 h netic cubic phase, Or: orthorhombic seven-layered phase, T: tetragonal non-
and aging at 1073 K for 30 h the alloy was cooled in air to modulated 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
a
Electronic mail: asozinov@cc.hut.fi with seven-layered modulation of the lattice.
tion. During heating both structure transformations occur in that the shortest axis c axis is the axis of easiest magneti-
reverse order and show some temperature hysteresis. In par- zation, the longest a axis is the axis of hard magnetization,
ticular, the reverse intermartensitic transformation takes and the b axis is the intermediate one. Unlike for a single
place during heating at 306 316 K. So reverse martensitic uniaxial magnetic anisotropy constant of tetragonal phase
transformation from the orthorhombic to the cubic parent one needs two magnetic anisotropy parameters to character-
phase upon heating takes place between A s 338 K and A f ize the orthorhombic crystal structure. The values of mag-
342 K. netic anisotropy constants K b 0.7105 J/m3 and K a 1.6
By x-ray studies made with the Philips XPert diffracto- 105 J/m3 were calculated from the magnetization data
meter it was found that the crystal structure of the first high Fig. 2 as the area cross section between the easiest curve c
temperature martensitic phase is nearly orthorhombic and axis and the two others b and a directions.
has lattice parameters of a0.619 nm, b0.580 nm, and c Figure 3 shows the stressstrain curve obtained during
0.553 nm in coordinates related to the high temperature compression along the 100 direction parallel to the longest
parent cubic phase at ambient temperature. Seven-layer a axis of the orthorhombic single crystal. The maximal
modulation along the (110) 110 p system was observed. twinning strain obtained is consistent with the crystal lattice
The insert in Fig. 1 shows the scattering intensity distribution aspect ratio estimate of 0 (1c/a)10.66% found from
in reciprocal space between 400 and 620 nodes recorded x-ray diffraction studies. It was confirmed that the final crys-
by a Q-type scan. There are six approximately equally tallographic structure of the sample is the same orthorhombic
spaced additional peaks. This kind of martensitic phase is one but transformed by twinning (101) 101 system from
known for nonstoichiometric Ni2 MnGa alloys.18,19 We also one single crystalline variant to another with the shortest c
found that the crystal structure of the second martensite is axis parallel to the direction of compression instead of to the
tetragonal with lattice parameters of ab0.547 nm, and longest a axis before the testing.
c0.660 nm (c/a1.207) at 200 K and ab0.551 nm The mechanical test reveals that the uniaxial compres-
and c0.654 nm (c/a1.187) at ambient temperature. sive stress tw is approximately as low tw2 MPa as was
Since the magnetic and the mechanical properties of non- found before10,12,13,16 for the five-layered tetragonal phase.
modulated tetragonal martensite phase have recently been This is very important because the low twinning stress and
studied,16 our attention was attracted to the orthorhombic high energy of magnetic anisotropy are key to obtaining a
seven-layered martensite. large magnetic field controlled strain response MSM the
Usually, after a martensitic phase transition the multiple MSM effect through the mechanism of twin boundary
variants of martensite form within a single crystal of the motion.12,13 More exactly, it is only possible in ferromagnetic
parent high-temperature phase. Afterwards, that multivariant shape memory alloys that satisfy the simple criterion,17
state can be transformed into a nearly single variant of mar-
K 0 tw .
tensitic phase by appropriate mechanical treatment. In this
way nearly single-variant samples of orthorhombic phase The magnetic anisotropy energy density K which is exactly
were prepared. equal to the magnetic driving force applied to the twin
The magnetic properties were determined for single- boundary13,17 must always exceed or be the same order as the
variant samples from the magnetization curves M (H) re- mechanical driving force 0 tw needed to produce twinning.
corded along the 100, 010, and 001 directions. The Strain response MSM for similar systems is expected to be
samples were constrained by epoxy to prevent a magneti- practically equal to the maximal strain 0 (1c/a) al-
cally field-induced redistribution of martensite variants dur- lowed by twinning crystallography. In the case of the ortho-
ing the measurements. The results of the magnetic measure- rhombic phase studied the K a value of 1.6105 J/m3 is of
ments are shown in Fig. 2. The magnetization curves indicate the same order but a little less compared to 0 tw2.0
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1748 Appl. Phys. Lett., Vol. 80, No. 10, 11 March 2002 Sozinov et al.
1
K. Ullakko, J. Mater. Eng. Perform. 5, 405 1996.
2
K. Ullakko, Proc. SPIE 2779, 505 1996.
3
K. Ullakko, J. K. Huang, C. Kantner, R. C. OHandley, and V. V. Kokorin,
Appl. Phys. Lett. 69, 1966 1996.
4
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36, 1133 1997.
5
R. D. James and M. Wuttig, Philos. Mag. A 77, 1273 1998.
FIG. 4. Field-induced strain of a single-variant sample of orthorhombic 6
R. C. OHandley, J. Appl. Phys. 83, 3263 1998.
seven-layered phase in the Ni48.8Mn29.7Ga21.5 alloy at 300 K measured per- 7
R. Tickle, R. D. James, T. Shield, M. Wuttig, and V. V. Kokorin, IEEE
pendicular to the magnetic field applied along the 100 direction.
Trans. Magn. 35, 4301 1998.
8
R. D. James, R. Tickle, and M. Wuttig, Mater. Sci. Eng., A 273275, 320
1999.
105 J/m3 . So, the large MSM value, which is a little lower 9
R. C. OHandley, S. J. Murrey, M. Marioni, H. Nembach, and S. M. Allen,
than 0 10.66%, is expected for the orthorhombic phase. J. Appl. Phys. 87, 4712 2000.
10
Figure 4 confirms this prediction and shows the results S. J. Murrey, M. Marioni, S. M. Allen, and R. C. OHandley, Appl. Phys.
of the field-induced strain measurements of the alloy at am- Lett. 77, 886 2000.
11
T. Kakeshita, T. Takeuchi, T. Fukuda, M. Tsujiguchi, T. Saburi, R. Oshima,
bient temperature. The magnetic field was applied parallel to and S. Muto, Appl. Phys. Lett. 77, 1502 2000.
the a axis. The maximal strain achieved in the first cycle at 12
A. A. Likhachev and K. Ullakko, Eur. Phys. J. B 14, 263 2000.
the field of 1.05 T is MSM9.5%. In agreement with our 13
A. A. Likhachev and K. Ullakko, Phys. Lett. A 275, 142 2000.
14
earlier explanation this value is lower than the crystallo- A. Sozinov, P. Yakovenko, and K. Ullakko, Mater. Sci. Forum 373376,
35 2001.
graphic limit 0 (1c/a)10.66% expected for complete 15
O. Heczko, A. Sozinov, and K. Ullakko, IEEE Trans. Magn. 36, 3266
transformation between two single variants. As confirmed by 2001.
16
optical observation and x-ray diffraction studies, the transfor- A. Sozinov, A. A. Likhachev, and K. Ullakko, Proc. SPIE 4333, 189
mation to the second variant with favorable c-axis orienta- 2001.
17
A. A. Likhachev, A. Sozinov, and K. Ullakko, Proc. SPIE 4333, 197
tion along the field is not complete. There are residual twin 2001.
bands in the sample. 18
V. V. Martynov and V. V. Kokorin, J. Phys. III 2, 739 1992.
19
J. Pons, V. A. Chernenko, R. Santamarta, and E. Cesari, Acta Mater. 48,
The authors would like to acknowledge funding by the 3027 2000.
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