Tailoring magnetostriction sign of ferromagnetic composite by increasing magnetic

field strength
,
Junming Gou, Xiaolian Liu, Kaiyun Wu, Yue Wang, Shanshan Hu, Hui Zhao, Andong Xiao, Tianyu Ma , and Mi
,
Yan

Citation: Appl. Phys. Lett. 109, 082404 (2016); doi: 10.1063/1.4961668

View online: http://dx.doi.org/10.1063/1.4961668
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Published by the American Institute of Physics
 APPLIED PHYSICS LETTERS 109, 082404 (2016)

Tailoring magnetostriction sign of ferromagnetic composite by increasing

magnetic field strength
Junming Gou,1 Xiaolian Liu,1 Kaiyun Wu,1 Yue Wang,1 Shanshan Hu,1 Hui Zhao,2
Andong Xiao,2 Tianyu Ma,1,a) and Mi Yan1,b)
1
State Key Laboratory of Silicon Materials, School of Materials Science and Engineering, Key Laboratory
of Novel Materials for Information Technology of Zhejiang Province, Cyrus Tang Center for Sensor Materials
and Applications, Zhejiang University, Hangzhou 310027, China
2
Multi-disciplinary Materials Research Center, Frontier Institute of Science and Technology,
Xi’an Jiaotong University, Xi’an 710049, China
(Received 14 June 2016; accepted 13 August 2016; published online 25 August 2016)
The unitary deformation of single-phase ferromagnets by a magnetic field, i.e., either positive or
negative linear magnetostriction, allows only monotonous control. Here we report a proof-of-prin-
ciple ferromagnetic composite Fe73Ga27, for which the magnetostriction sign changes from positive
to negative by increasing the magnetic field strength. Based on the transformation from body-cen-
tered-cubic (BCC) to face-centered-cubic (FCC) phases in this binary system, Fe73Ga27 composite
is prepared by aging the BCC averaged precursor for 3 days at 803 K. Magnetic measurements indi-
cate that the BCC phase exhibits smaller magnetocrystalline anisotropy constant than the FCC
phase. The offset effect between BCC and FCC phases produces positive net magnetostriction at
low magnetic fields but negative net magnetostriction at high magnetic fields. By tuning the field
strength, such composites can mediate compressive and tensile strains to other functional materials,
e.g., piezoelectric material or optic-fibers, which is beneficial to design multifunctional devices.
Published by AIP Publishing. [http://dx.doi.org/10.1063/1.4961668]

Magnetostrictive materials that generate linear mechani- anisotropy) and the crystallographic/magnetic textures deter-
cal deformation under uniaxial magnetic field are widely mine the magnetostriction sign, magnitude as well as the sat-
used in actuators, sensors, and transducers.1,2 The magnetic uration field, as one can see from the typical examples of
field induced strain mediated to other functional materials, Ni with negative magnetostriction and Fe with positive
such as piezoelectric materials,3 optical fibers,4 and negative magnetostriction.1 The basic idea of this letter is that if a fer-
thermal expansion polymers,5 facilities the design of multi- romagnetic composite contains both negative and positive
functional devices. For instance, magnetoelectric coupling magnetostriction phases with different magnetocrystalline
effect of magnetostrictive/piezoelectric heterostructures can anisotropies, tensile or compressive strain control can then
be utilized to manipulate the polarization (or magnetization) be achieved by increasing the DC magnetic field strength.
with applied magnetic (or electric) field, known as a direct Herein, we report a proof-of-principle Fe-Ga composite with
(or converse) magnetoelectric effect.6,7 Technologically, if such promising function.
the interface strain state could be tuned from compressive Solid solution type Fe-Ga alloys (Galfenol)15 are superior
into tensile (or vice versa) by changing the magnetic field in ductility and mechanical strength to Terfenol-D as the well-
strength, it would be highly desirable that the electric signals known giant magnetostrictive material. Previous studies15–17
(polarization) could be alternated through a DC magnetic of Fe100-xGax alloys have shown two anomalous peaks in the
field. It then allows the generation of an AC electrical signal magnetostriction at x  19 at. % and 27 at. %, respectively.
by a DC magnetic field, instead of using the conventional Magnetostriction (3/2k100) exceeding 400 ppm at room temper-
vibrated mechanical stress on the brittle piezoelectric com- ature has been reported for both Fe81Ga1915,16 and Fe73Ga2717
ponent.8,9 Unfortunately, the magnetostrictive materials, single crystals (as opposed to 30–130 ppm for bulk Fe-, Co-, or
including pure metal Ni,10 alloy Fe-Ga,11 and intermetallic Ni-based alloys18). Both structure and magnetostrictive proper-
compound Tb0.3Dy0.7Fe2 (Terfenol-D),12 usually output uni- ties of Fe-Ga alloys are very sensitive to the thermal his-
tary elastic strain (either compressive or tensile) and allow tory.19–26 When Ga content is within 26–29 at. %, disordered
monotonous control only. If the magnetostriction sign of a body-centered-cubic (BCC) A2, ordered DO3, ordered face-
ferromagnet changes at different magnetic field strengths, centered-cubic (FCC) L12, and ordered hexagonal DO19 struc-
i.e., contraction or elongation, it then facilitates biconditional tures can be obtained by heat-treatments, as shown by two
control by a DC magnetic field. early studies of Fe72.5Ga27.5 alloy.22,23 For this alloy, A2 and
The linear magnetostriction in single-phase ferromagnets DO3 structured samples possess positive magnetostriction,
is resulted from the motion of non-180 domain walls (DWs) whereas the L12 and DO19 structured ones exhibit negative
and rotation of magnetization under magnetic fields.1,13,14 The magnetostriction. Compared to the BCC and HCP phases, the
intrinsic spin-orbit interaction (the origin of magnetocrystalline L12 phase has much larger magnetization. Following such
structure-property relation, one could achieve a Fe-Ga compos-
a)
maty@zju.edu.cn; ite containing both the positive-magnetostriction BCC phase
b)
mse_yanmi@zju.edu.cn and the negative-magnetostriction FCC phase. Early work by

0003-6951/2016/109(8)/082404/5/$30.00 109, 082404-1 Published by AIP Publishing.

082404-2 Gou et al. Appl. Phys. Lett. 109, 082404 (2016)

Kawamiya et al. has shown that the L12 phase forms after
long-term aging (3 days annealing at 773 K followed by 1
month annealing at 623 K (Ref. 21)) due to the slow transfor-
mation kinetics from a BCC precursor. Our recent work27
also shows that aging at 803 K produces a composite, where
the volume fraction of FCC L12 phase is closely relied on
the aging time. In this letter, a Fe73Ga27 composite contain-
ing both BCC and FCC phases was prepared by aging for 3
days at 803 K. Magnetic and magnetostriction measurements
reveal that the BCC phase exhibits smaller magnetocrystal-
line anisotropy and smaller saturation field than those of the
FCC phase, and that the preferable DW motion and magneti-
zation rotation in the Fe73Ga27 composite give rise to sign-
changed-magnetostrictions.
Fe73Ga27 alloy was prepared by arc melting, copper-
mold casting, and subsequent Bridgeman solidification. The
cylindered rod sample (U7  40 mm3) was quenched into ice
water after solution-treating for 3 h at 1373 K, which exhibits
a BCC average structure.27 Further aging for 3 days at 803 K
promotes the formation of L12 phase. For comparison,
another sample was prepared by aging for 30 days at 803 K,
which mainly consists of L12 phase. The axial magnetostric-
tions were measured by the output of a 1 mm-long  1 mm-
wide electrical resistance strain gauge attached to the speci-
men surface. Initial magnetization curves and magnetization
hysteresis loops were measured by SQUID magnetometer.
Sample for transmission electronic microscopy (TEM) char-
acterization was prepared by twin-jet electropolishing below
243 K, followed by ion-milling for 15 min (beam glancing
angle ¼ 6 , beam voltage ¼ 2 keV, and beam current ¼ 5 mA) FIG. 1. (a) Magnetostriction of Fe73Ga27 composite formed by aging at
to remove surface contaminations. TEM examination was 803 K for 3 days. XRD profiles; schematically elongation and subsequent
performed with a JEOL JEM-2100F microscope. In-situ DW contraction are shown in the insets. (b) Magnetostrictions of Fe73Ga27 sam-
ples after solution-treating and aging at 803 K for 30 days, respectively. The
motions were observed using the Lorentz mode with the corresponding XRD profiles are shown in the inset. Average BCC structure
magnetic field up to 300 Oe. The magnetic field was applied is identified for the as-solution-treated sample. The longer the aging time,
parallel to the sample surface. the larger the volume fraction of L12 phase.
Figure 1(a) illustrates the room temperature magneto-
striction curves of the Fe73Ga27 sample aged at 803 K for 3 demagnetized state, which thus enable biconditional strain
days. The inset XRD profiles reveal that it contains both control by changing the magnetic field strength.
BCC and FCC phases. Both the magnetic field and strain To understand the mechanism of the sign-changed-mag-
measurement direction are parallel to the rod axis. The mag- netostrictions, we first distinguish the intrinsic magnetic
netostriction in this letter refers to the strain measured along property difference between the BCC and the L12 phase. Fig. 2
the field direction. Butterfly-type strain output behavior is shows the magnetization loops for the as-solution-treated,
observed. Upon increasing field strength, the axial magneto- the 3-day-aged, and the 30-day-aged samples, respectively.
striction changes from positive under lower fields into nega- Using the initial magnetization curves, the saturation magne-
tive under higher fields. It means that the sample first expands tization MS and the magnetocrystalline anisotropy constant
and then contracts along the field direction. However, the K1 are calculated by the law of approach to saturation and
saturation magnetostriction is positive (145 ppm) for the as- summarized in the upper-right inset of Fig. 2. The coercivity
solution-treated state with an average BCC structure (Fig. HC, derived from the enlarged M-H loops (bottom-right inset
1(b)). Meanwhile, it is negative (76 ppm) for the Fe73Ga27 of Fig. 2), is also summarized. K1, MS, and HC increase from
sample after aging at 803 K for 1 month which mainly con- 1.23  104 J/m3, 143.68 emu/g, and 0.035 kOe for the as-
tains the L12 phase. Difference in the magnetostriction sign solution-treated sample to 1.41  104 J/m3, 147.12 emu/g,
between the BCC and the L12 phases is consistent with pre- and 0.149 kOe for the one aged for 3 days, and further
vious work.22,23 It also shows that the sample aged for 1 increase to 1.66  104 J/m3, 151.50 emu/g, and 0.151 kOe for
month exhibits a larger saturation magnetic field than the as- the one aged for 30 days. The longer the aging time is, the
solution-treated one. In any case, during magnetization, these larger the K1, MS, and HC are. It also reflects that the volume
two samples show only unitary elongation or contraction fraction of FCC phase increases with aging time, being con-
without changing the magnetostriction sign. Besides, the sistent with the XRD results in Fig. 1. It demonstrates that
abnormal sign-changed-magnetostrictions have never been FCC phase possesses stronger magnetocrystalline anisotropy
observed in other single-phase ferromagnets at the thermally than the BCC phase. Consequently, magnetostriction for the
082404-3 Gou et al. Appl. Phys. Lett. 109, 082404 (2016)

FIG. 2. Magnetization hysteresis loops of the as-solution-treated sample

with average BCC structure, the one aged for 3 days at 803 K with both
BCC and FCC phases, and the one aged for 30 days at 803 K with mainly of
FCC phase. The upper-left inset illustrates the coercivity HC, anisotropy
constant K1, and saturation magnetization MS of these two samples. The
bottom-right inset illustrates the enlarged magnetization loops at low mag-
netic fields.

FIG. 3. TEM characterizations of Fe73Ga27 composite. (a) Bright field image

sample with mainly of the FCC phase saturates under a taken with [010]BCC incidence. (b), (c), and (d) SAED patterns of blue, red,
much higher magnetic field than that of the one with aver- and yellow regions in (a), respectively. The blue index below each diffrac-
aged BCC structure (Fig. 1(b)). tion spot for BCC phase in (b) and (d) takes the DO3 structure as reference;
the red index above each diffraction spot for FCC phase in (c) and (d) takes
In fact, magnetization and magnetostriction for the the L12 structure as reference.
Fe73Ga27 composite are the net effects contributed from both
the BCC and the FCC phases. The magnetization at low using the superlattice reflections). The bright contrast is the
magnetic fields (i.e., below 1 kOe, positive magnetostric- FCC phase, as revealed by the SAED pattern in Fig. 3(c),
tion occurs) for the composite is lower than that of the as- which is obtained by tilting the grain to [110]FCC zone axis.
solution-treated sample due mainly to the enhanced magne- The ordered L12 structure is verified by the superlattice
tocrystalline anisotropy. The positive magnetostriction for reflections at {001}* and {110}* positions. Their grain size is
the former (Fig. 1(a)) is also lower than that of the latter from several hundreds of nanometers to several microns.
(blue curve Fig. 1(b)). Again, within the field range where The lattice parameter is aFCC  0.37(1) nm calculated using
negative magnetostriction takes place, the magnetization for the superlattice reflections, being close to that determined by
the composite is still lower than that of the BCC structured XRD measurement. The crystallographic relationship
sample. Meanwhile, the absolute magnetostriction is much between these two phases, as revealed by the SAED pattern
lower than that of the sample containing mainly of FCC in Fig. 3(d), is [010]BCC//[110]FCC and (202)BCC//(11 1)FCC.
phase. These indicate that the sign-changed-magnetostric- Such relationship follows the Bain relation between BCC
tions are due to net effect of DW motions and magnetization and FCC structures. We estimate the Bain strain for the DO3
rotations for both BCC and FCC phases. Under lower mag- (BCC) ! L12 (FCC) transformation as e[001]BCC ¼ p2a
ffiffiffi FCC/
netic fields, the positive magnetostriction of the BCC phase aBCC – 1  0.277(1) and e[100]BCC ¼ e[010]BCC ¼ 2aFCC/
is not completely compensated by the negative magnetostric- aBCC – 1  0.096(9). Such large lattice distortion indicates
tion of the FCC phase. When the magnetic field is increased high energy barrier between DO3 and L12. On the other
to a critical level, the contributions of two phases reach a hand, the DO3 ! L12 transformation requires atomic posi-
complete compensation. With further increased magnetic tion exchanges (Fe or Ga change sites, for instance, in the
field, the DW motions and magnetization rotations of FCC (001)DO3 plane).20 The low kinetics for DO3 ! L12 transfor-
phase with stronger magnetocrystalline anisotropy dominate, mation can then be understood. Consequently, both trans-
giving rise to a net negative magnetostriction. formed FCC phase and untransformed BCC phase coexist
The constituting phases are identified by TEM (Fig. 3). after aging for 3 days at 803 K, forming a composite before
The bright field image (Fig. 3(a)) taken with [010]BCC inci- reaching complete transformation. In addition, there is still
dence clearly reveals the bi-phase structure. The dark con- some untransformed BCC phase even after aging at 803 K
trast is the BCC phase, as demonstrated by the selected area for 30 days (XRD profile in the inset of Fig. 1(b)) for such a
electron diffraction (SAED) pattern in Fig. 3(b). The weak diffusion-type transformation.
{002} superlattice reflections indicate that the BCC phase is Finally, direct evidence for preferable DW motion is
partially ordered. SAED pattern taken with [110]BCC zone provided by the in-situ Lorentz TEM observations. Fig. 4(a)
axis reveals the existence of superlattice reflections at shows the in-focus image and the corresponding SAED pat-
{111}* positions, which belong to the DO3 structure only. If terns. Similar to those illustrated in Figs. 2(b) and 2(d), the
we take DO3 structure to index the SAED pattern of BCC selected area 1 only contains BCC phase, while the selected
phase, the lattice parameter is aBCC  0.58(1) nm (calculated area 2 contains both BCC and FCC phases, respectively. The
082404-4 Gou et al. Appl. Phys. Lett. 109, 082404 (2016)

magnetostrictive/functional hybrids can be controlled by the

magnetic field strength, which may facilitate numerous appli-
cations. For the magnetostrictive/piezoelectric composites
with magnetoelectric coupling effect, change of strain state at
the interface could alternate the electric signals from positive
to negative or vice versa. In addition, for the hybrid magneto-
optical sensors,4 change of strain state at the interface may
tune the central wavelength from right-shifting to left-shifting
of the optic-fibers attached with magnetostrictive materials,
increasing the sensitivity to both low and high magnetic fields.
Besides, the sign-changed-magnetostrictions may also be
potentially unitized in multi-channel micro-flow liquid valves
and multi-position detectors. Second, the different intrinsic
properties between two ferromagnetic phases can be used to
achieve zero magnetostriction at a certain magnetic field,
which is always the goal of soft magnets. In order to minimize
the noise as well as magnetic loss, zero magnetostriction is
usually achieved by precise control of the material composi-
FIG. 4. In-focus Lorentz-TEM image and the corresponding SAED patterns. tion,29 for instance, in Fe-Si-Al30 and Fe-Ni alloys.31 As
(a) In-situ over-focus Lorentz-TEM images at (b) 0 Oe, (c) 100 Oe, and (d)
shown in Fig. 1, the zero magnetostriction can also be
300 Oe, where the domain wall motion of the BCC phase (highlighted by
blue square) is easier than the FCC phase (highlighted by red rectangle). obtained at a certain field once the elongation of the BCC
phase is compensated completely by the contraction of the
zero field over-focus image in Fig. 4(b) reveals bright con- FCC phase. This certain magnetic field can be tuned through
trasts of the DWs at different regions. Under 100 Oe changing the relative volume fractional between the two ferro-
(Fig. 4(c)), a DW in the blue-highlighted BCC phase region magnetic phases, for example, through alternating the aging
moves, whereas the one in the red-highlighted FCC phase time for the present Fe73Ga27 alloy.
region keeps unchanged. When further increasing the field to In summary, sign-changed-magnetostrictions are obtained
300 Oe (Fig. 4(d)), the DW of BCC phase gradually moves, in a ferromagnetic composite with both negative- and positive-
tending to be parallel to the external field direction. magnetostriction phases, as demonstrated in the Fe73Ga27 com-
Meanwhile, the FCC DW is still stable. The favorable DW posite. This effect stems from the preferable domain wall
motion of the BCC phase then generates positive magneto- motion and magnetization rotation of the magnetostrictive
striction at lower magnetic fields. The DW for FCC phase components with different magnetocrystalline anisotropies.
could be moved at stronger magnetic fields once its higher Such materials are appealing for biconditional strain control by
magnetocrystalline anisotropy is overcome. Although the DC magnetic field, which may lead to numerous applications
DW motion and magnetization rotation within a thin film when hybrided with other functional materials. It also suggests
and a bulk material could be different, the DW motion of the a potential route to obtain zero-magnetostriction in addition to
BCC phase is prior to the FCC phase in Fig. 4 when the mag- composition control, which is essential for the design of soft
netic field is applied in plane, being consistent with the sign- magnets.
changed-magnetostrictions.
The above results demonstrate sign-changed-magneto- This work was supported by the 973 Program (No.
strictions for the Fe-Ga composite, which allows bicondi- 2012CB619401), and National Natural Science Foundation of
tional strain control by increasing the field strength. The key China (Nos. 51331001, 51431007, 51571176, 51622104, and
peculiarity is the phase mixture of a positive and a negative 51590881). Professor Chengbao Jiang of Beihang University
magnetostriction components with different magnetocrystal- and Professor Xiaobing Ren of Xi’an Jiaotong University are
line anisotropies. The preferable DW motions and magneti- acknowledged for helpful discussions. Professor Weixing Xia
zation rotations of the positive magnetostriction component of Ningbo Institute of Industrial Technology, CAS, is
at lower magnetic fields result in elongation, meanwhile the acknowledged for the assistance of Lorentz TEM
contribution from the negative magnetostriction component characterizations.
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