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Magnetoelectric Composites
G. Srinivasan
Department of Physics, Oakland University, Rochester, Michigan 49309;
email: Srinivas@oakland.edu
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INTRODUCTION
The magnetoelectric (ME) effect is defined as the dielectric polarization of a material in an applied
magnetic field or as an induced magnetization in an external electric field (1). There are very few
single-phase ME materials, and most of them show very weak ME coupling at room temperature
(2–6). Composites are of interest for the engineering of materials with either desired or new char-
acteristics that are absent in single-phase materials. In a composite consisting of magnetostrictive
and piezoelectric phases, the ME effect is the result of a product property, i.e., mechanical de-
formation because of magnetostriction results in a dielectric polarization due to the piezoelectric
effect. The early works on ME composites were primarily on sintered bulk samples of ferrites
and piezoelectrics (7–10). Such composites showed weak ME effects due to poor mechanical cou-
pling caused by microcracks and loss of magnetic-field-induced polarization due to high leakage
currents. This review is on ME phenomena in magnetostrictive-piezoelectric composites, with
a specific focus on layered composites (laminates) that show the strongest coupling. We discuss
Annu. Rev. Mater. Res. 2010.40. Downloaded from arjournals.annualreviews.org
key developments and significant findings during the past decade as well as recent reviews on
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multiferroics and magnetoelectrics (4–6) and on ME phenomena and device applications (11–14).
This review is organized as follows. We first briefly discuss ME phenomena, historic devel-
opments, and early works on bulk ME composites. This discussion is followed by a section on
the theory of ME interactions in layered samples, including low-frequency coupling, resonance
enhancement at frequencies corresponding to bending modes and electromechanical resonance
(EMR), coupling when the magnetic subsystem shows resonance [i.e., ferromagnetic resonance
(FMR)], and coupling at magnetoacoustic resonance (MAR), corresponding to the coincidence of
EMR and FMR. The theory section is followed by discussion on experimental works on the above
phenomena in a series of layered composites and nanocomposites. The use of ME composites
for sensors of magnetic fields, dual electric-field- and magnetic-field-tunable devices operating at
1–110 GHz, and antenna miniaturization is also discussed here. We conclude with remarks on
avenues for potential enhancement of the strength of ME interactions in layered composites and
new directions for research on ME composites.
MAGNETOELECTRIC MATERIALS
In ME materials, the induced polarization P is related to the applied magnetic field H by the
expression P = αH, where α is the second-rank ME-susceptibility tensor and is expressed in
s m−1 in SI units (in Gaussian units, α = 4π P/H is dimensionless). One generally determines α
= δP/δH by subjecting the sample to a bias field H and an AC field δH and by measuring δP or
the electric field δE. Another parameter of importance is the ME voltage coefficient α E = δE/δH,
which is related to α by α = εo εr α E , where εr is the relative permittivity of the material. One can
also determine the inverse ME coefficient α H = δH/δE by measuring the magnetic response of
the sample to an applied electric field. There are few such studies, and they are not part of this
review.
In a single-phase material, the symmetry of the crystal is a key factor that determines the exis-
tence of ME effects. Such effects were first observed in antiferromagnetic Cr2 O3 (2). Several other
single-phase materials that are either antiferromagnetic, weak ferromagnetic, or ferrimagnetic,
such as TbFeO3 and Fex Ga2−x O3 , show weak ME effects (reviewed in References 3–6). The only
known single-phase multiferroic with a large α at room temperature is BiFeO3 (15).
For the engineering of materials with the desired properties, Van Suchtelen (7) proposed
two types of composites, those with sum properties and those with product properties. A product-
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the ME susceptibility α = δP/δH is the product of the piezomagnetic deformation δz/δH and the
piezoelectric charge generation δQ/δz. The system of primary interest in the past was bulk samples
of ferrites and BaTiO3 . Although ferrites are not piezomagnetic, magnetostriction in a combined
AC and DC magnetic field results in a pseudopiezomagnetic effect. For such composites, Van
Den Boomgaard et al. (8) estimated a ME voltage coefficient α E = E/H = 5 V cm−1 Oe−1 .
[Note: The SI unit for α E is V A−1 . Most works in recent years provide α E in V cm−1 Oe−1 . For
conversion purposes, 1 V cm−1 Oe−1 = 1.257 V m−1 .] But most attempts in the past to realize
strong ME effects in bulk composites of ferrites and piezoelectrics prepared by several techniques,
including traditional sintering, microwave sintering, and hot pressing, were unsuccessful (14, 16–
19). Possible causes include microcracks, defects, impurity phases, and high-leakage currents.
Harshe and colleagues (20, 21) in their pioneering works proposed a model for ME coupling
in a bilayer of magnetostrictive and piezoelectric phases (as in Figure 1) and fabricated such
structures. A bilayer or multilayer configuration for ME composites has several advantages over
bulk composites. In particular, the loss of polarization in bulk composites due to leakage currents
can be overcome in layered structures. The piezoelectric phase can be poled to enhance the ME
coupling. It is also possible to vary the poling and applied field directions to achieve maximum ME
coupling. The strain-mediated ME phenomena of importance in layered and nanocomposites are
giant low-frequency coupling and resonance enhancement of ME effects anticipated for bending
modes, EMR, FMR, and MAR (20–38). Next we consider theories for these phenomena.
E, δE
Piezoelectric phase
E, δH Magnetostrictive phase
2
1
Figure 1
A bilayer of magnetostrictive and piezoelectric phases in the (1, 2) plane with its thickness along axis 3. The
bilayer is assumed to be poled with an electric field along axis 3. A bias magnetic field H and an AC magnetic
field δH result in an AC electric field δE across the piezoelectric layer. From Reference 23. V I E
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magnetic field (T-T) (14)] and (b) α E31 for electric fields along direction 3 and magnetic fields in
the plane of the sample [referred to as transverse field (23) or longitudinal magnetic and transverse
electric field (L-T) (14)]. The ME voltage coefficient α E33 is given by (23)
δ E3 μ0 t(1 − t) p d 31 m q 31
α E33 = =2 p 2
δH3 {2 d 31 (1 − t) + ε33 [( p s 11 + p s 12 )(t − 1) − t(m s 11 + m s 12 )]}
p
[( p s 11 + p s 12 )(t − 1) − t(m s 11 +m s 12 )]
× . 1.
{[μ0 (t − 1) − μ33 t][t(m s 12 + m s 11 ) − ( p s 11 + p s 12 )(t − 1)] + 2m q 31
m 2 2
t }
For the magnetic fields H and δH along direction 1, one obtains (23)
δ E3 −t(1 − t)(m q 11 + m q 21 ) p d 31
α E31 = = . 2.
δH1 p ε33 ( s 12 + s 11 )t + p ε33 ( p s 11 + p s 12 )(1 − t) − 2 p d 31 2 (1 − t)
m m
Here m and p refer to the magnetostrictive and the piezoelectric phases, respectively; d and q
are the piezoelectric and the piezomagnetic coupling coefficients, respectively; s is the compliance
Annu. Rev. Mater. Res. 2010.40. Downloaded from arjournals.annualreviews.org
coefficient; ε is permittivity at constant stress; μ is the tensor permeability; p t and m t are the
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thicknesses of the magnetostrictive and the piezoelectric layers, respectively; and t = p t/(p t + m t)
is the fractional thickness for the piezoelectric layer. The model was applied to several systems,
including ferrites, transition metals and alloys, and rare-earth alloys for the magnetic phase and
lead zirconate titanate (PZT), lead magnesium niobate–lead titanate (PMN-PT), barium titanate
(BTO), and polyvinylidenedifluoride (PVDF) for the piezoelectric phase (22–26). Figure 2 shows
estimates of α E versus t for the specific case of nickel ferrite (NFO)-PZT from Reference 23. The
ME coefficient is 0 for t = 0 or 1, as expected, and a maximum in α E occurs for t = 0.4–0.6.
250
NFO-PZT αE31
200
ME voltage coefficient (mV cm–1 Oe–1)
150
100
αE33
50
0
0.0 0.2 0.4 0.6 0.8 1.0
Thickness fraction for PZT
Figure 2
Estimates of low-frequency magnetoelectric (ME) voltage coefficient α E31 = δE3 /δH1 and α E33 = δE3 /δH3
as a function of thickness fraction for lead zirconate titanate (PZT) in a bilayer consisting of nickel ferrite
(NFO) and PZT. The poling field E is along the sample thickness (direction 3). For α E31 , the bias field H
and the AC magnetic field δH1 are assumed to be parallel to each other and to the sample plane, and the
induced electric field δE3 is measured perpendicular to the sample plane. For α E33 , all the fields are along
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The parameter α E33 is quite small compared with α E31 due to demagnetizing fields and weak
q13 . The maximum value of α E31 for in-plane magnetic fields is a factor of five higher than for
out-of-plane magnetic fields, and the model predicts a giant ME coupling in NFO-PZT. Data on
low-frequency coupling for several systems are discussed in the sections below.
was obtained by solving the electrostatic, magnetostatic, and elastodynamic equations. Bilayers
free to vibrate at both ends, or simply supported at both ends or fixed at one end, were considered.
This model showed that the bending resonance and consequent enhancement in ME coupling
occur at the lowest frequency for a bilayer that is fixed at one end and free at the other end.
Figure 3 shows estimates of the frequency dependence of α E31 and α E33 for a bilayer of perme-
ndur, a transition-metal alloy with high magnetostriction, and PZT. Peaks in α E occur at the
frequency of bending oscillations, and the peak values are two orders of magnitude higher than
low-frequency ME coefficients.
8
αE31
Permendur-PZT
ME voltage coefficient (V cm–1 Oe–1)
2 αE33
0
26 28 30 32 34
Frequency (kHz)
Figure 3
Theoretical frequency f dependence of magnetoelectric (ME) voltage coefficient for a bilayer of permendur
and lead zirconate titanate (PZT) showing the resonance enhancement of ME interactions at the bending-
mode frequency. The bias field H and AC field δH( f ) are either parallel or perpendicular to the sample
plane. PZT is poled along its thickness. The bilayer is free to bend at both ends so that the wavelength of the
bending mode corresponds to the length L. The sample dimensions are L = 9.2 mm and thickness 0.7 mm,
and the PZT thickness fraction t = 0.6. From Reference 28. V I E
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1400
NFO-PZT
1200
800
600
400
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200
fr
0
0 100 200 300 400 500
Frequency (kHz)
Figure 4
Theoretical magnetoelectric (ME) voltage coefficient α E33 as a function of the frequency of the AC field δH
for a 10-mm-diameter bilayer of nickel ferrite (NFO)–lead zirconate titanate (PZT). PZT is poled along its
thickness, and H and δH are perpendicular to the sample plane. Estimates are for a sample thickness much
smaller than the radius. Notice the resonance in α E33 versus f due to the radial acoustic mode
(electromechanical resonance). From Reference 29.
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2
E = 300 kV cm–1 E = 0 kV cm–1
0
–2
9.3 GHz
–4
–6
5000 6000 7000 8000
Magnetic field, H (Oe)
Figure 5
Theoretical magnetic-field H dependence of microwave magnetic susceptibility at 9.3 GHz showing
Annu. Rev. Mater. Res. 2010.40. Downloaded from arjournals.annualreviews.org
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ferromagnetic resonance (FMR) in a nickel ferrite (NFO)–lead zirconate titanate (PZT) bilayer. The static
magnetic field H and a DC electric field E are perpendicular to the sample plane. The microwave magnetic
field is parallel to the sample plane. Notice the shift in the FMR profile with the application of E =
300 kV cm−1 across PZT. From Reference 31.
with static fields H and E perpendicular to the sample plane and an in-plane microwave magnetic
field at a frequency of 9.3 GHz (31). The magnetic susceptibility χ is estimated as a function of H
and for a series of E. Figure 5 shows results for NFO-PZT for E = 0 and 300 kV cm−1 . For E =
0, one observes the expected FMR in the χ profile. With the application of E = 300 kV cm−1 , a
downshift in the FMR profile occurs because E-induced mechanical strain manifests as an internal
magnetic field in NFO. The shift δHE is strongly influenced by, among other factors, the sample
magnetization, the magnetostriction λ, and the piezoelectric coupling d (30). Results on studies
of the ME coupling at FMR and composite-based microwave devices based on this effect are
discussed in this review.
Magnetoacoustic Resonance
A significant enhancement in the strength of ME interactions is expected in a ferrite-piezoelectric
bilayer when FMR and EMR frequencies overlap, i.e., at MAR (32, 33). Because FMR in general
occurs at gigahertz or higher frequencies, the phenomenon can be observed only in nanocompos-
ites with EMR in the same frequency range. In our theory discussed in Reference 32, we considered
ME interactions under MAR in NFO-PZT bilayers. Figure 6 shows the theoretical α E31 versus
f for (a) a bias field H that is much smaller than the FMR field Hr and for (b and c) H = Hr . For
H < Hr , Figure 6a shows peaks in the ME voltage coefficient at the fundamental-harmonic and
higher-harmonic thickness modes of EMR. Figure 6b shows the estimated α E31 versus f for FMR
at H = Hr coinciding with the fundamental EMR. One anticipates a 40-fold increase in α E31
for H = Hr . Coincidence of FMR and EMR allows energy transfer between phonons and spin
waves. This transfer is very efficient in ferrite-PZT, leading to ME coefficients on the order of
several hundred volts per centimeter Oersted. Figure 6c corresponds to the condition when the
second harmonic of EMR coincides with FMR. The observation of MAR is yet to be reported
in any system. A nano-ME composite with defect-free ferrite with narrow FMR line width, such
as NFO (35), is essential for the observation of MAR. A similar phenomenon may be observed
in exotic systems such as piezoelectric and magnetic antiperovskites (34). The ME effect at MAR
can be utilized for the realization of nanosensors and transducers operating at microwave and
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a H0 = 1800 Oe NFO-PZT
10
4
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b H0 = 4950 Oe
ME voltage coefficient, αE31 (V cm–1 Oe–1)
400
300
200
100
c H0 = 6850 Oe
300
200
100
0
0 2 4 6 8 10 12
Frequency (GHz)
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to the sample plane is estimated from the voltage δV measured with a lock-in amplifier or similar
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techniques (14). Data are obtained as a function of H, the frequency of the AC field, and the
temperature. Alternatively, a pulsed magnetic-field technique can be used for studies on frequency
dependence of ME voltage coefficients (40). The method is based on the excitation of the composite
with magnetic-field pulses, followed by the measurement and Fourier analysis of the ME response
signal. The technique is ideal for studies on resonant ME coupling. Other innovative measurement
techniques include ME measurements through piezoelectric coupling (42), use of a scanning
microwave microscope (43), and a magnetic cantilever for measurements on nanocomposite films
(44).
←−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−−
Figure 6
Estimated variation of magnetoelectric (ME) voltage coefficient α E31 with the frequency of AC magnetic
field δH for a bilayer of nickel ferrite (NFO)–lead zirconate titanate (PZT). The thicknesses of the NFO and
the PZT layers are 100 nm and 200 nm, respectively. (a) The bias field H is smaller than the field Hr for
ferromagnetic resonance (FMR) in NFO. The peaks in α E31 occur at the fundamental harmonic and the
second harmonic of thickness electromechanical resonance (EMR) modes. (b) The ME coupling at the
coincidence of fundamental EMR mode and FMR: the magnetoacoustic resonance (MAR). H is selected so
that FMR in NFO coincides with the fundamental EMR mode. (c) Similar results as in panel b, but for the
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coincidence of FMR and the second harmonic of EMR. From Reference 32. E W
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400
NFO-PZT
200
αE33
0
800
NCFO-PZT-NCFO
600
αE31
400
–200
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200
αE33
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0
0 2000 3000 4000
H (Oe)
–400
–2000 –1000 0 1000 2000
Static magnetic field, H (Oe)
Figure 7
Data on static-field H dependence of α E31 and α E33 measured at 1 kHz for a multilayer composite with 15
layers of nickel ferrite (NFO), 14 layers of lead zirconate titanate (PZT), and a layer thickness of 14 μm. The
open circles and filled circles are data points for increasing H and decreasing H, respectively. The lines are
guides to the eye. The inset shows similar data for a trilayer of NFO with 5% Co substitution (NCFO) and
PZT. From Reference 46.
magnetostriction attains saturation. Although the overall features for variations with H are similar
for both α E31 and α E33 , one notices the following differences. (a) The initial rate of increase in
α E with H is much higher for α E31 than for α E33 . (b) The peak α E31 is a factor of 10 higher than
α E33 . (c) The peak value in α E33 occurs for a higher bias field H than for α E31 . These observa-
tions can be understood in terms of H variation of piezomagnetic coupling q. Equations 1 and
2 show that α E31 and α E33 arise due to (q11 + q12 ) and q13 , respectively. Estimates of q reveal an
order-of-magnitude difference for the two orientations due to demagnetization associated with
out-of-plane H. Consequently, α E33 is expected to be weaker than α E31 , as is the case in the data
of Figure 7. The ME coefficients in Figure 7 are more than an order of magnitude higher than
those for the best single-phase material, i.e., α E = 20 mV cm−1 Oe−1 for single-crystal Cr2 O3
(2). Other studies on ferrite-PZT composites of interest are the dependence of ME couplings on
the ferrite composition, volume/thickness fraction for the two phases, temperature, and frequency
(46–48). It is possible to accomplish high q values for the ferrite by tailoring of the composition or
by substitutions. An example is the substitution of Co in NFO. Figure 7 shows measured α E for
a trilayer of NFO with 5% Co substitution and PZT. The data reveal doubling of α E31 compared
with NFO-PZT multilayers.
A giant ME effect is evident only for NFO-PZT and is not observed for systems such as cobalt
ferrite (CFO)-PZT (47). The critical ferrite parameter that controls the ME coupling, i.e., q, arises
primarily due to the Joule magnetostriction caused by domain wall motion and domain rotation.
The key requirements for strong ME coupling are unimpeded domain motion and a large λ. A
soft, high initial permeability and a high-λ ferrite, such as NFO, is the key ingredient for giant
V I E ME effects. In magnetically hard CFO, however, one has the disadvantage of a large anisotropy
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150
LSMO-PZT 298 K
αE31
ME coefficient (mV cm–1 Oe–1)
100
238 K
199 K
50
86 K
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0
0 100 200 300
Bias magnetic field (Oe)
Figure 8
Magnetoelectric (ME) voltage coefficient α E31 measured at 100 Hz as a function of H for a series of
temperatures for a single-crystal La0.7 Sr0.3 MnO3 (LSMO)–lead zirconate titanate (PZT) bilayer. From
Reference 56.
and coercive field that limits domain rotation (47). An observation of importance in this regard is
the higher ME coefficient in samples with single-crystal ferrites than in sintered polycrystalline
composites (49). The highest α E31 reported for ferrite-piezoelectrics is for nickel copper ferrite
with a trilayer stack of PZT and PZN-PT (51).
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Terfenol and PZT. A ME coupling that is not strain mediated is predicted in Fe-BTO multilayers
(79). According to the theory, when the polarization in BTO is reversed, changes in the chemical
bonding at the interface lead to a variation in the interface magnetization (79).
tangentially magnetized Ni-PZT with 57-μm-thick Ni on 25-mm-diameter PZT. The data are
for H = 110 Oe and δH = 2.5 Oe. The ME voltage V is approximately 1–2 mV in the whole-
frequency band with resonance enhancements at specific frequencies. The frequencies f1 and f2
correspond to bending-oscillation modes of the disk, whereas the frequency f3 corresponds to the
radial acoustic mode. The frequency response also contains a set of weak resonances that arise
probably because of the nonuniformity of the structure. The quality factor for resonances was
Q1 ∼ 30–120 and increased linearly with Ni layer thickness. For magnetic fields perpendicular
to the disk plane, V versus f had a similar shape as in Figure 9, but the maximum in V occurred
at a higher bias field H, on the order of 400 Oe, due to demagnetization. The mode frequency
associated with bending can be controlled with proper choice for the bilayer dimensions. Xing
f1 Ni-PZT
60
ME voltage (mV)
40
f3
20
f2
0
0 50 100
Frequency (kHz)
Figure 9
Measured frequency dependence of magnetoelectric (ME) voltage generated by a bilayer of 57-μm Ni on a
25-mm-diameter lead zirconate titanate (PZT) disc and for a tangential bias field H = 110 Oe and an AC
modulation field δH = 2.5 Oe. The frequencies f1 and f2 correspond to bending-oscillation modes of the
V I E disk, whereas the frequency f3 corresponds to the radial acoustic mode. From Reference 78.
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et al. (76) reported ME coefficients of 16 V cm−1 Oe−1 and 250 V cm−1 Oe−1 , respectively, for
off-resonance and at 60-Hz bending modes in a PZT bimorph mounted onto a NdFeB magnet.
Figure 9 also shows an enhancement in ME interactions at EMR, for which the theory is
discussed above (78, 80–85). The peak in α E at f3 ∼ 100 kHz is attributed to radial acoustic
modes in Ni-PZT (78). One observes a substantial increase in the ME coefficient compared with
low-frequency values, although the coefficient is somewhat smaller than for the bending modes.
Dong et al. (82) reported on the utility of EMR in enhancing the sensitivity of a PZT–Terfenol-D
laminate for the detection of fields as low as 10 nT. Shi et al. (84) studied EMR in a PZT rod
array in a Terfenol-D–epoxy matrix.
A related effect of importance is the influence of bias field H on EMR frequency fr . A shift
in fr is expected in a bias magnetic field due to changes in the Young’s modulus, termed the E
effect. Srinivasan et al. (85) provide a theory for the effect. The model was used to account for the
dependence of fr on H in a ME multilayer capacitor (86).
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0
YIG-PZT
Transducer
8 kV cm–1
–20 –8 kV cm–1 E=0 Pin(f) Pref(f)
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in nanocomposites, and the sample must have a very narrow FMR profile for the observation of
enhancement in ME coupling predicted by the theory (32, 33).
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a b
0 4 μm 0 4 μm
Figure 11
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(a) A nanopillar and (b) a nanobelt of barium titanate–cobalt ferrite (BTO-CFO) composite thin films. After
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Reference 99.
Similar efforts since 2004 have focused mainly on ferrite-ferroelectric bilayers, multilayers,
nanopillars, nanobelts, and core-shell nanowires (104–114). Samples have been synthesized by
a variety of techniques, including wet-chemical methods, MBE, laser deposition, and sol gel.
Figure 11 shows images for representative cases of CFO-BTO nanopillars and nanobelts (99).
The ME coupling in such nanosystems has been demonstrated through polarization in H and the
magnetodielectric response (110, 111). Zhang et al. (107) reported ME coupling in a CFO-BTO
bilayer grown on strontium titanate substrates. The middle BTO layer essentially reduced any
substrate clamping on CFO, leading to ME coefficients as high as 100 mV cm−1 Oe−1 , which is
comparable to thick-film values. Finally, Chung et al. (115) fabricated Ni nanobars on PZT thin
films and studied ME coupling through electric-field effects on magnetic domains.
MAGNETOELECTRIC DEVICES
The coupling between the electric and the magnetic subsystems in a ME material opens up the
possibility of novel sensors and devices. Wood & Austin (116) examined the possibility of devices
based on single-phase multiferroics and concluded that the effects were too weak for practical
devices. Because composites show very strong ME interactions, several research groups in recent
years focused on the possibility of low-frequency ME devices such as wireless powering systems
(117, 118), energy harvesting (119), tunable inductors (120), magnetic-field sensors (121–128), gy-
rators and transformers (129, 130), dual electric-field- and magnetic-field-tunable microwave and
micrometer-wave devices (131–135), and miniature antennas (136–139). Magnetic-field sensing
is based on measurements of the charge or voltage produced by a composite. Ultrasensitive AC
and DC magnetic-field sensors and current sensors have been demonstrated using highly magne-
tostrictive and piezoelectric phases and innovative designs for the sensor (121–123). Zhao et al.
(128) fabricated a thin-film magnetic-field sensor of PZT-(Fe,Ga) on Si that operates at EMR. ME
transformers or gyrators are useful for voltage-gain and power-conversion applications (129, 130).
Very high voltage-gain effect under resonance drive has been reported in laminates consisting of
Terfenol-D and PZT layers (129).
Studies discussed above (87–97) on microwave ME effects in YIG-PZT, YIG–PMN-PT, and
YIG-BST led to the design, fabrication, and characterization of a new family of signal-processing
devices that are tunable by both magnetic and electric fields. The devices studied include res-
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a
Metal electrodes
YIG film
PZT plate U H
GGG substrate
Microstrip line
Pout(f)
Substrate
Pin(f)
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–5
E=0 1 2 3 kV cm–1
–10
Insertion loss (dB)
–15
–20
are ideal for use in microwave devices due to low losses. The novel feature in all the above-discussed
ME devices is the electric field or voltage tunability. Magnetic-field tuning of ferrite devices is
often slow and noisy and requires watt or kilowatt power for operation. Such devices cannot be
miniaturized or integrated with semiconductor devices. But electric-field tuning is rapid and less
noisy and requires minimal power, and the devices can be miniaturized. A specific example is
a YIG-PZT band-pass filter shown in Figure 12 (133). The ME filter consists of a dielectric
ground plane, input and output microstrips, and a YIG-PZT bilayer. Power is coupled from input
to output under FMR in the ME element. The frequency dependence of the insertion loss is
shown in Figure 12. An upshift in the pass band is observed with increasing voltage across PZT.
The frequency shift of 120 MHz for E = 3 kV cm−1 corresponds to 2% of the central frequency
of the filter and is a factor of 40 higher than the line width for pure YIG. Another example is
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E W the microwave resonator and data shown in Figure 10. The E tuning of FMR in YIG-PZT in
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Figure 10 is on the order of 0.1% of the resonator operating frequency over E = ± 8 kV cm−1 ,
which is sufficient for many applications. The resonator Q ranged from 1000 to 2000 (132). With
proper choice of the ferrite and piezoelectric phases and E value, a tuning range of 0.5 GHz to 1
GHz is quite possible (30, 31). Similar layered composites with high and equal values of perme-
ability and permittivity could be used as substrates for impedance-matched miniature antennas
(136–139). Several of the devices, microwave devices in particular, have been demonstrated with
the use of bonded ferrite and piezoelectrics. It is critically important to develop processes for the
growth of epitaxial ferrite films on ferroelectric substrates for use in such devices.
cause the ME interactions are strain mediated, one needs to understand the relationship between
ME coefficients and functionally grading the key parameters for ferromagnetic and piezoelectric
phases, such as the piezomagnetic coupling q and the piezoelectric coupling d. Such grading could
potentially be obtained with compositional grading of the two phases.
Recent studies on compositionally graded ferroelectrics and ferrites reveal grading of order
parameters ( P or M) and piezoelectric and piezomagnetic couplings, resulting in an internal po-
tential, induced anisotropies, and spontaneous strain (138–147). A compositionally graded NZFO,
for example, is expected to show a near-linear variation in the saturation magnetization and q over
x = 0–0.4 (146). A similar d variation can be achieved for PZT or PMN-PT (138, 142). A bilayer
with graded q and d will result in additional bending moment. The main point here is that the
bending moments will give rise to strain that will affect the strength of ME interactions.
Next we consider modeling of grading effects on low-frequency ME coupling (148–150). A
bilayer of NZFO and PZT with grading of q and d is assumed along an axis perpendicular to
its plane. Positive grading and negative grading represent increasing and decreasing material
parameters relative to the poling direction in PZT, respectively. Figure 13 shows the estimated
ME coefficient α E31 for homogeneous and graded bilayers. α E31 is determined by the sum of
longitudinal strain due to the applied magnetic field and to bending strains. There are two types
of bending strains that are of opposite sign: The first is due to asymmetry of the bilayer, and the
second is due to grading. These two bending strains will combine to either decrease or increase
the overall ME coefficient relative to a homogeneous bilayer. Notice the difference in α E31 versus
t for homogeneous bilayers in Figure 13 and in Figure 2. Results in Figure 2 are for the case
when bending strain due to asymmetry is ignored. In Figure 13 there is overall reduction in α E31
for homogeneous bilayers due to bending. But a combination of negative grading of NZFO and
positive grading of PZT will increase α E31 by as much as 60% compared with the homogeneous
case. Negative grading of NZFO, for example, leads to a decrease in the overall bending moment
of the ferrite and therefore increases the in-plane strain of PZT and α E31 . Similar arguments apply
for the effects of grading d.
Results of preliminary studies on graded systems are in agreement with the theory. Effects of
compositional grading of ferrites in a composite are illustrated in the data of Figure 14, which
shows α E33 versus H for two cases. In the first case, data are for a trilayer of two identical but
oppositely poled PZT and a homogeneous NZFO. Because of the symmetry associated with the
trilayer and because the ferrite is homogeneous, there is no bending moment. The ME voltages
across the PZT discs are of equal magnitude but with a phase difference of 180◦ so that the
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net voltage is near zero, as seen in the data. In the second case, the NZFO is compositionally E W
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NZFO-PZT
(3)
(1)
0.08
(2)
0.04
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0.00
0.0 0.2 0.4 0.6 0.8 1.0
Thickness fraction for PZT
Figure 13
Theoretical lead zirconate titanate (PZT) thickness fraction dependence of low-frequency magnetoelectric
(ME) voltage coefficient α E31 for bilayers of Ni1−x Znx Fe2 O4 (nickel zinc ferrite, or NZFO) and PZT.
Estimates are for samples with homogeneous or functionally graded ferrites and PZT to obtain a linear
variation in piezomagnetic and piezoelectric coefficients. Results are shown for (1) homogeneous
NZFO-PZT, (2) positively graded NZFO and negatively graded PZT, and (3) negative grading of NZFO
and positive grading of PZT. From Reference 149.
CONCLUDING REMARKS
Layered composites of magnetostrictive and piezoelectric phases are of importance for studies on
the physics of ME interactions and for useful technologies. Theories for low-frequency coupling
predict a giant ME voltage coefficient in these composites for in-plane magnetic fields. Resonance
enhancement of the ME interactions is expected for bending modes, for acoustic modes, and
at MAR. Studies on composites of ferrites, manganites, transition metals and alloys, and rare-
earth alloys for the magnetic phase and PZT, BTO, PMN-PT, and PVDF for the piezoelectric
phase show the anticipated strong coupling. Studies on nanocomposites have thus far focused
on CFO-ferroelectric nanopillars, nanobelts, and multilayers. Studies on device applications of
ME composites reveal their potential for use as magnetic-field sensors, energy harvesters, trans-
formers, gyrators, and miniature antennas. Low-loss ME microwave and micrometer-wave signal
processors that are tunable with magnetic and electric fields have been demonstrated. Recent
theories predict the potential for further enhancement of ME interactions in functionally graded
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80
60 PZT
NZFO
αE33 (mV cm–1 Oe–1)
PZT
40
Graded ferrite
20
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Homogeneous
0
0 1 2 3 4
H (k Oe)
Figure 14
Measured magnetoelectric (ME) coefficient α E33 versus H for a trilayer of lead zirconate titanate (PZT) with
homogeneous or compositionally graded Ni1−x Znx Fe2 O4 (nickel zinc ferrite, or NZFO). The
compositional grading of NZFO over x = 0–0.4 leads to grading of the piezomagnetic coupling coefficient
q. The PZT discs are poled in the opposite directions, as indicated.
SUMMARY POINTS
1. Bilayer or multilayer ME composites with magnetostrictive and piezoelectric phases are
ideal for realizing strong strain-mediated coupling. Ferromagnets with high piezomag-
netic coupling (q = dλ/dH), such as ferrites (e.g., Ni-Zn ferrites), transition metals or
alloys (e.g., Ni, permendur, and Metglas), rare-earth alloys (e.g., Terfenol-D), and piezo-
electrics (e.g., PZT and PMN-PT), are candidate materials for use in these composites.
2. Theoretical models for ME effects at low frequency, bending resonance, electromechan-
ical resonance (EMR), ferromagnetic resonance (FMR), and magnetoacoustic resonance
(MAR) predict strong coupling in the layered structures. The coupling strength, in gen-
eral, is the strongest for in-plane applied magnetic fields. With proper choice for com-
posite dimensions, bending resonance–related enhancement could be accomplished at
frequencies as low as 10 Hz.
3. Studies on several composites show the anticipated strong ME coupling over 1 mHz–
110 GHz. The highest ME coefficients are reported for ferromagnetic alloys-
piezoelectrics at low frequencies, bending resonance and EMR and in ferrites or alloys-
PZT at FMR.
4. ME nanostructures have attracted considerable attention in recent years. Most studies
have focused on cobalt ferrite (CFO)-piezoelectric nanopillars. Many questions regarding
the ME coupling in nanostructures remain unanswered.
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5. Composites are candidate materials for sensors of magnetic field and currents, energy
harvesters, transformers, gyrators, read heads for memory applications, miniature anten-
nas, and high-performance microwave and micrometer-wave resonators, filters, phase
shifters, and delay lines.
FUTURE ISSUES
1. Several studies discussed in this review were on bonded bilayers. Growth of thick-film,
epitaxial heterostructures and studies on ME interactions are critically important in par-
ticular for sensors and high-frequency device applications.
2. Nanocomposites will be a current and future topic of interest for studies on the physics
Annu. Rev. Mater. Res. 2010.40. Downloaded from arjournals.annualreviews.org
yet to be developed for measurements of direct and converse ME effects in such systems.
3. A potential unexplored topic of importance in ME composites is functionally graded
bilayers of magnetic and piezoelectric phases. The synthesis of compositionally graded
ferromagnetic and ferroelectric materials and studies on order parameters and the nature
of ME interactions are essential.
DISCLOSURE STATEMENT
The author is not aware of any affiliations, memberships, funding, or financial holdings that might
be perceived as affecting the objectivity of this review.
ACKNOWLEDGMENTS
There have been very significant works on bulk composites and other ME materials and phenom-
ena since 2000. I sincerely apologize for not covering all of them in this review due to constraints
on the length of the manuscript and the number of references. The research at Oakland University
was supported by grants from the National Science Foundation, Army Research Office, Office of
Naval Research, and Defense Advanced Research Project Agency and by a Congressional Grant
administered by the U.S. Department of Education. I gratefully acknowledge contributions by
collaborators Professors Mirza Bichurin and Vladimir Petrov (Novgorod State University), Boris
Kalinikos and Alexey Ustinov (St. Petersburg Electrotechnical University), Yuri Fetisov (MIREA,
Moscow), and Igor Zavislyak and Maksym Popov (University of Kiev) and by several research
associates and graduate students.
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