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Review Article
Current Status of Magnetoelectric Composite Thin/Thick Films
Rahul C. Kambale,1 Dae-Yong Jeong,2 and Jungho Ryu1
1 Functional
2 School
Ceramics Group, Korea Institute of Materials Science (KIMS), Gyeongnam, Changwon 641-831, Republic of Korea
of Materials Engineering, Inha University, Incheon 402-751, Republic of Korea
Correspondence should be addressed to Dae-Yong Jeong, dyjeong@inha.ac.kr and Jungho Ryu, jhryu@kims.re.kr
Received 19 September 2011; Accepted 2 December 2011
Academic Editor: Vladimir Petrov
Copyright 2012 Rahul C. Kambale et al. This is an open access article distributed under the Creative Commons Attribution
License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly
cited.
Here we review the current status of magnetoelectric (ME) multiferroics and ME composite thin/thick films. The magnitude
of ME coupling in the composite systems is dependent upon the elastic coupling occurring at the interface of piezoelectric and
magnetostrictive phases. The multiferroic ME films in comparison with bulk ME composites have some unique advantages and
show higher magnitude of ME response. In ME composite films, thickness of the films is one of the important factors to have
enough signal. However, most of all reported ME nanocomposite structured films in literature are limited in overall thickness
which might be related to interface strain resulting from dierence in thermal expansion mismatch between individual phases
and the substrate. We introduced noble ME composite film fabrication technique, aerosol deposition (AD) to overcome these
problems. The success in AD fabrication and characterization of ME composite films with various microstructure such as 3-2, 2-2
connectivity are discussed.
1. Introduction
The progress of human civilization has been strongly
influenced by the progress in the field of materials science.
Materials science is an extremely interdisciplinary subject
involving branches such as Physics, Chemistry, Engineering,
Biology, and so forth. Understanding the basic aspects of a
variety of materials such as their structure and properties is
the key issue in materials science. Based upon the fundamental understanding of structure-property relationship, new
materials with enhanced performance are currently being
developed. A material is generally said to be functional if it
possesses a physical property that is utilizable in applications.
Among the various classes of materials, functional materials,
which interest lies in their physical properties, occupy a
particularly important place in our lives, as they allow, for
example, for the design of many electronic devices we use
them on a daily basis. Especially, the rapid improvement
of mobile devices requires smaller components, which can
be obtained by designing multifunctional materials which
possess several properties as ferromagnetism, ferroelectricity.
Magnetic and ferroelectric materials are present in the
wide range of modern science and technology. Ferromag-
(1)
3
10 m
Figure 1: Microstructure of 1st ME composite by Suchtelen. Samples were fabricated by unidirectional solidification of a eutectic
composition of the quinary system FeCoTiBaO, [28].
Year
Researcher
1888
Rontgen
1894
Curie
1905
Wilson
1922
Perrier
1926
Debye
1959
Dzyaloshinskii
1960
Landau
1961
Astrov
1961
1972
Suchtelen
1978
Boomgaard
1973
Freeman
1994
M. I. Bichurin
1997
M. I. Bichurin
2001
J. Ryu
2001
C. W. Nan
2002
M. I. Bichurin
2003
M. I. Bichurin
2003
S. Dong
2003
C. W. Nan
2004
C. W. Nan
1st report on the calculation of giant ME by using the finite element method
2004
S. Dong
2004
S. Dong
2005
M. Fiebig
2005
N. A. Spaldin
2005
S. Dong
2006
S. Dong
2006
G. Srinivasan
2006
G. Srinivasan
2006
J. F. Scott
2007
S. Priya
2007
R. Ramesh
2008
C. W. Nan
2008
R. Grossinger
2008
D. Viehland
2009
M. Fiebig
2009
L. Yan
2009
J. P. Rivera
2009
V. Bedekar
Magnetoelectric gradiometer
2010
C. W. Nan
2010
R. Ramesh
2010
C. W. Nan
2010
M. I. Bichurin
2011
F. Fang
400
350
Number of papers
300
250
200
150
100
50
0
1970 1975 1980 1985 1990 1995 2000 2005 2010 2015
Year
Figure 2: The year wise number of articles published in the literature on the magnetoelectric composite materials.
100
Scopus keyword: magnetoelectric AND composite AND film
Total 221 papers (as of Sep. 2011)
Number of papers
75
50
25
0
1995
2000
2005
Year
2010
2015
Figure 3: The year wise number of articles published in the literature on the magnetoelectric composite thin/thick films.
3-0/Particulate
3-0/Particulate
3-0/Particulate
PZT
-20 wt%NiCo0.02 Cu0.02 Mn0.1 Fe1.8 O4
Muzumder and
Bhattacharyya 2004 [53]
2-2/Laminate
3-0/Particulate
3-0/Particulate
3-0/Particulate
NiFe2 O4 + PMN-PT
3-0/Particulate
Priya and Islam 2006 [61] NiFe1.9 Mn0.1 O4 -Pb(Zr0.52 Ti0.48 )O3
3-0/Particulate
Srinivasan et al. 2004 [52] Ni0.8 Zn0.2 Fe2 O4 -0.75 vol% PZT
Single phase
3-0/Particulate
3-0/Particulate
3-0/Particulate
Srinivasan et al. 2004 [52] Ni0.8 Zn0.2 Fe2 O4 -0.41 vol% PZT
3-0/Particulate
Epoxy-glued
composites
5.150 (peak)
140
0.0956
10.43
Static ME
measurement
Solid-state reaction
sintered at 1250 C
Sintered at 1,100 C/
24 h
Controlled
precipitation route
1,570 Oe/DC
0.78
Solid-state reaction
2.34
115
0.35
4,500 (f=?)
1,250 Oe/1 kHz
5.58
3300
45
110
421
80
50
Low-temperature sintering
Homogeneous dispersion
ME
Remark
(mV/cmOe)
250 Oe/100 Hz
0.80.9 kOe at RT
Solid-state reaction
sintered at 1250 C
4 kOe/50 Hz
for 10 h with heating
rate 5 C/min
Sintered at 1,250 C
Sintering
Sintered at
1,300 C/24 h
Sintered at
950 C/2 h
Standard ceramic
method
Standard ceramic
method
Hot pressed at
1,000 C/7 Mpa
Hot pressed at
1,000 C/7 Mpa
Sintered in @
1,0001,200 C/3 h
3-0/Particulate
Fabrication method
Bridgman/1 atm
O2 /50 cm h1
Connectivity
3-3/Unidirection
0.62BaTiO3 -.0.38CoFe2 O4 (eutectic
composition with 1.5 wt% excess TiO2 ) solidification
Composition
Author/year
6
Advances in Condensed Matter Physics
Terfenol-D/PMN-PT
CoFe2 O4 -PZT
FeBSiC/piezofiber laminates
(Metglas/PZT)
Metglas/PVDF
FeBSiC/PZNPT-fiber laminate
Metglas/Terfenol-D/
PMN-PZT/Terfenol-D/Metglas
Layered laminate
Fabrication method
Layered laminate
2-2/Multilayer
Aerosol deposition
Sol-gel-processing
and spin-coating
technique
Sol-gel process and
spin-coating
technique
Aerosol-deposition
Epoxy-glued
composites
Epoxy-glued
composites
Electrodeposition
0.4
273
68
50 kHz/dynamic
Hac = 1 Oe
f = 1 kHz
150
530
45000
8500
1800
7200 and
238 V/cmOe
Thin and flexible ME composites
@ resonance
50 kHz
10500@ low
frequency Long-type FeBSiC/ PZNPT-fiber
with low dc laminates
bias 2 Oe
22000
430
220
1.200
ME
Remark
(mV/cmOe)
10 kOe/50 Hz
Hac = 1 Oe
f = 1 kHz
L-T mode
Hac = 1 Oe
f = 1 kHz
Hac = 1 Oe
f = 1 kHz
Hac = 1 Oe
f = 1 kHz
150 kHz/1.2 kOe
Hac = 1 Oe.
Epoxy-glued
composites
Epoxy-glued
composites
Hac = 1 Oe and f =
1 kHz
Epoxy-glued
composites
11 layers of 13 m
1,050 Oe/350 kHz@
NiFe2 O4 1 and 10
resonance
layers of 26 m PZT
PLD; single-crystal
1-3/Vertically
SrTiO3 (001)
aligned structure.
substrates
550 < Hdc < 800 Oe. f
2-2/Laminate
L-L laminates
= 1 kHz
Sol-gel process and
1 kHz/6 kOe (10 Oe
0-3/Nanostructure spin-coating
ac)
technique
Epoxy-glued
L-L mode @ 5 Oe dc
2-1/Laminate
composites
bias and f = 1 Hz
NiFe2 O4 -PZT
Connectivity
Composition
Author/year
Table 2: Continued.
Substrate
Substrate
Substrate
(a)
(b)
(c)
Figure 4: Schematic illustration of three ME composite films with the three common connectivity schemes: (a) 0-3 particulate composite,
(b) 2-2 laminate composite, and (c) 1-3 fiber/rod composite films, [2].
Table 3: Summary of advantages/disadvantages of ME composite films with dierent connectivity.
Connectivity
Advantage
Disadvantage
0-3
Easy processing.
Weak ME eect.
2-2
1-3
Remarks
Sintering with ceramic power
mixture. Ceramic/polymer
composite.
Cofiring at high temperature.
All ceramic materials. Tape
casting.
Thin film process layer by layer.
Integrated ME devices.
Epoxy bonding at room
temperature. Ceramic/magnetic
metal alloy.
Large in-plane strain. Thin film
process.
Nozzle
PZNT matrix
NCZF
Scan direction
PZNT/NCZF
particle beam
As-deposited
film
Platinized Si substrate
Platinized Si substrate
(a)
(b)
Figure 5: Schematic illustration of (a) ME composite film fabrication and (b) microstructure of nanocomposite ME films by AD, [75].
13 m
7 m
ME Comp As Dep
SE
Mag: 5000 x HV: 20 kV WD: 10 mm
(a)
ME Comp 700
SE
Mag: 5000 x HV: 20 kV WD: 10 mm
7 m
(b)
Pb-L
Fe-K
100 nm
(c)
100 nm
(d)
Figure 6: Microstructural analysis of 3-2 nanocomposite thick films by AD cross-sectional SEM image of (a) as-deposited and (b) annealed
film. STEM micrographs and SAED of (c) as-deposited and (d) annealed film and EDX mapping.
10
150
100
50
0
50
100
150
200
3000 2000 1000
0
1000
DC magnetic field (Oe)
2000
3000
Figure 7: ME coecient of 3-2 nanocomposite ME thick films by AD as a function of magnetic DC bias. The maximum ME coecient was
measured to be 150 mV/cmOe. This magnitude is about 3 times higher than the previously reported nanocomposite films by other thin film
processes, [75].
11
1
0.8
600
0.6
400
0.4
200
Dielectric constant
800
0.2
0
1
0
1000
10
100
Frequency (kHz)
15% NZF
20% NZF
25% NZF
30% NZF
Figure 8: Dielectric constants and losses according to the frequency of PZT-PMnN + NZF nanocomposite films by AD as a function of NZF
content, [72].
250
Magnetization (emu/cm3 )
200
150
100
50
0
50
100
150
200
250
6000
4000
2000
2000
4000
6000
25% NZF
30% NZF
Figure 9: M-H hysteresis loops PZT-PMnN + NZF thick films by AD with dierent NZF content, [72].
ME coecient (mV/cmOe)
100
80
60
40
20
0
15
20
25
NZF content (%)
30
Figure 10: Maximum ME coecient of PZT-PMnN + NZF nanocomposite films by AD as a function of NZF content, [72].
12
PZT
Ag
CFO
20 m
SE Pb Fe Ag
(a)
(b)
Figure 11: (a) cross-sectional SEM micrographs and (b) EDX mapping of 2-2 ME composite thick films by AD.
The composite films showed coexistence of perovskite (PZTPMnN), and spinel (NZF) phases and peak intensities from
NZF phase were changed with changing NZF content in
the composite films; this means that AD can control the
composition ratio of composite films by controlling raw
power mixture. This is confirmed by electrical and magnetic
properties as shown in Figures 8 and 9. The magnetization of
composite films was measured and reflecting the ferromagnetic characteristics of all the composite films. With increasing NZF content, the remnant and saturated magnetizations
were gradually increased, and coercive magnetic fields were
keeping the almost the same value. This indicates that NZF
content variation did not severely aect its own magnetic
characteristics in the composite films. The ME coecients
were not changed severely in that NZF content range of
1525%, but there was drop when 30% NZF was added
(Figure 10). The maximum ME output voltage was reported
to be 68 mV/cmOe from 20% NZF-added composite film.
This magnitude is lower than that of their previous PZTPZN + NZCF system, but still higher than that of the
nanocomposite films made by other thin film process which
had maximum ME output voltages under 40 mV/cmOe [34,
83, 89]. In addition to the ME characteristics, the deposition
rate of ME films was exceptionally higher (over 1 m/min)
than other conventional thin film process. By using this
fabrication technique, 2-2-type laminate thick films (over
10 m-thick) is possible as depicted in Figure 11, and the
evaluation results will be published in elsewhere.
5. Conclusion
Nowadays, many researchers are getting attracted towards
the investigations of magnetoelectric phenomenon in ME
multiferroics composites due to their cross-coupling eect
which lead them to be useful for many potential applications on device level. We presented the review on ME
composite thin/thick films in this paper. A brief discussion
was presented on ME multiferroics, ME composites, and
ME composite films by historically and microstructurally. It
seems that there is an increasing scientific interest in magnetoelectric phenomenon which is evidenced by the rising
number of publications in the last 10 years. Therefore, there
Acknowledgment
This work was supported by the National Research Foundation of Korea (NRF) Grant funded by the Korea government
(MEST) no. 2009-0086909.
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