Materials Science and Engineering B 171 (2010) 7985

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Materials Science and Engineering B

journal homepage: www.elsevier.com/locate/mseb

Enhancement of the piezoelectric properties of sodium lanthanum bismuth

titanate (Na0.5 La0.5 Bi4 Ti4 O15 ) through modication with cobalt
Chun-Ming Wang , Jin-Feng Wang, Li-Mei Zheng, Ming-Lei Zhao, Chun-Lei Wang
School of Physics, State Key Laboratory of Crystal Materials, Shandong University, Jinan 250100, Peoples Republic of China

a r t i c l e i n f o a b s t r a c t

Article history: The dielectric, piezoelectric, and electromechanical properties of B-site cobalt-modied sodium lan-
Received 26 August 2009 thanum bismuth titanate (Na0.5 La0.5 Bi4 Ti4 O15 , NLBT) piezoelectric ceramics were investigated. The
Received in revised form 19 March 2010 piezoelectric properties of NLBT ceramics can be enhanced by cobalt modications. The NLBT ceramics
Accepted 31 March 2010
modied with 0.2 wt.% cobalt trioxide (NLBT-C4) possess good piezoelectric properties, with piezoelectric
coefcient d33 of 27 pC/N, electromechanical coupling factors (kp and kt ) of 6.5% and 28.5%, and mechan-
PACS:
ical quality factor Qm (kp mode) of 3400. The Curie temperature Tc of cobalt-modied NLBT ceramics
77.84.s
was found to slightly higher than that of pure NLBT ceramics. A large dielectric abnormity in dielectric
77.84.Dy
77.65.Bn
loss tan was observed in NLBT ceramics, which can be signicantly suppressed by cobalt modication.
77.80.Bh Thermal annealing studies presented the cobalt-modied NLBT ceramics possess stable piezoelectric
77.80.Dj properties.
2010 Elsevier B.V. All rights reserved.
Keywords:
Piezoelectric materials
Ferroelectrics
Dielectric properties
Sodium bismuth titanate

1. Introduction
High temperature technology is of major importance to
the automotive, aerospace, and power generation industries
[14]. Piezoelectric single crystals such as LiNbO3 , La3 Ga5 SiO14 ,
Sr2 Nb2 O7 , and La2 Ti2 O7 , and GaPO4 are generally used as high
temperature sensing components, however, the crystal growth of
these materials needs expensive equipment and has low yield. The
important advantage of polycrystalline piezoelectric ceramics over
single crystals is the ease with which composition and properties
may be tailored.
Aurivillius-type bismuth layer-structured ferroelectrics (BLSFs)
are widely known to possess a structure expressed by the gen-
eral formula of (Bi2 O2 )2+ (Am1 Bm O3m+1 )2 , where A is a mono-,
di-, and tri-valent ion or combination of them allowing dodec-
ahedral coordination, B is a transition element or combination
of cations well suited to octahedral coordination, and m is
an integer which represents the number of BO6 octahedra in
(Am1 Bm O3m+1 )2 between the (Bi2 O2 )2+ layers, usually in the
range of 15. The pseudo-perovskite (Am1 Bm O3m+1 )2 layers inter-
leave with (Bi2 O2 )2+ layers along the c-axis of the BLSFs. Fig. 1
shows the crystal structure of four-layer BLSFs, for the NLBT, A-
site ions are Na, La, Bi ions, and B-site ions are Ti ions. The grain
growth rate in the direction perpendicular to the c-axis of the BLSFs
crystal is much higher than that in the direction parallel to the c-
axis, so the grain growth is structurally highly anisotropic, and the
grains are plate-like shape. The BLSF ceramics, due to their rela-
tively high Curie temperature Tc , have received signicant attention
for their potential use in high-temperature piezoelectric devices,
such as high-temperature piezoelectric owmeter, actuator, and
accelerometer [24]. However, the piezoelectric activities in pure
and modied BLSF ceramics were found to be very low, and it is
difcult to achieve high piezoelectric activities in ordinary sintered
BLSF ceramics with randomly oriented grain structure, because of
the two-dimensional orientation restriction of the rotation of their
spontaneous polarization (Ps ) and their high coercive elds (Ec ).
Generally, among the material properties determining device
performance, the piezoelectric activities of piezoelectric materials
are very important. For example, for a charge mode accelerometer,
this can be demonstrated by the charge sensitivity which is a vital
parameter used to scale the device sensitivity:
Sq = d m (1)

where d is the piezoelectric coefcient (for a ceramic, generally it is

Corresponding author. Tel.: +86 138 6914 4988; fax: +86 531 8837 7031. d33 or d15 ), m is the preinstalled mass. In designing an accelerom-
E-mail address: wangcm@sdu.edu.cn (C.-M. Wang). eter, the piezoelectric coefcient should be as high as possible.

0921-5107/$ see front matter 2010 Elsevier B.V. All rights reserved.
doi:10.1016/j.mseb.2010.03.076
80 C.-M. Wang et al. / Materials Science and Engineering B 171 (2010) 7985

ics [1116]. However, B-site cations locate at the center of oxygen

octahedra, therefore, the slight change in B-site cationic radius may
also play a major structural role in the polarization process. There-
fore, in the present work, B-site modied layer-structured sodium
lanthanum bismuth titanate (Na0.5 La0.5 Bi4 Ti4 O15 , NLBT) ceramics
were fabricated by a conventional solid state processing, and the
dielectric, and piezoelectric properties of B-site cobalt-modied
NLBT ceramics were investigated. The layer-structured NLBT was
selected herein due to its high Curie temperature (600 C) [17],
and the B-site modication of cobalt cations were chosen because
of cobalt oxide often used as an effective additive in enhancing the
piezoelectric properties of perovskite-structure materials [1820].

2. Experimental

Sodium lanthanum bismuth titanate piezoelectric ceramics

were produced using a conventional mixed oxide processing route
procedure. Analytical grades Na2 CO3 (99.8%), La2 O3 (99.9%), Bi2 O3
(99.8%), and TiO2 (99.9%) (Sinopharm Chemical Reagent Co., Ltd.)
were selected as starting materials. The QM series planetary ball
mill (Nanjing University Instrument Plant) was used to mix the raw
material. The weighed chemicals were wet-milled in polyethylene
bottles (the inner diameter is about 8 cm) with ZrO2 balls for 12 h in
ethanol. The milled powders were dried, and the size of the milled
powder was examined. It is found that the particle size distributes
from 100 to 500 nm. And then the milled powders were calcined at
800 C for 2 h. After calcinations, the mixture was milled again in
the same conditions. The milled powders were dried, grinded, and
granulated with 5 wt.% polyvinyl alcohol (PVA) binder. The granu-
lated powder was pressed into disks 15 mm in diameter by 2.0 mm
in thickness at a pressure of 150 MPa. After burning out the PVA at
650 C, the green compacts were put into the sealed Al2 O3 crucibles
and fully surrounded with the powder of matching compositions,
so as to prevent the volatilization of the samples. The samples were
sintered by ordinary ring (OF) for 3 h at 11301150 C, and then
cooled to room temperature freely. Cobalt at different amounts up
to 1 wt.% was added in the form of Co2 O3 (99%) to the raw materials
Fig. 1. Crystal structure of BLSF (m = 4). One-half of the pseudo-tetragonal unit cell. after calcinations, according to the nominal compositions: NLBT + x
For the NLBT, A-site ions are Na, La, Bi ions, and B-site ions are Ti ions. wt.% Co2 O3 (x = 0.1, 0.2, 0.3, and 0.4, abbreviated as NLBT-C2, NLBT-
C4, NLBT-C6, and NLBT-C8, respectively). The cobalt-modied NLBT
However, the piezoelectric activities in pure and modied BLSF piezoelectric ceramics were also produced under the same proce-
ceramics were found to be very low, and it is difcult to achieve high dure.
piezoelectric activities in ordinary sintered BLSF ceramics with ran-
domly oriented grain structure, due to their plate-like grains and
spontaneous polarization restricted to lying in the ab plane.
As a consequence of the anisotropy of the microstructures and
properties, grain orientation techniques, such as hot-forging (HF),
templated grain growth (TGG), and spark plasma sintering (SPS),
could signicantly enhance their piezoelectric properties in direc-
tions parallel to the ab plane [59]. However, the conductivity in
the plane of the maximum piezoelectric activity is higher than that
in the perpendicular axis, which makes the poling process dif-
cult, and also limits the integration in devices at high temperature
in which conductivity increases [10]. Moreover, it is desirable to
obtain high d33 BLSF piezoelectric ceramics by conventional sinter-
ing method, from the point of view of commercial applications.
Therefore, A-site rare-earth elements modication, B-site modi-
cation, and A-site vacancy modication have been proposed. In
these works, it is found that the introduction of A-site modication
is more obvious than that of B-site modication in enhancing the
piezoelectric properties of BLSF ceramics, since the cations in B-
site, such as Ti4+ , Nb5+ , Ta5+ , W6+ , are similar in size and do not play
a major structural role in the polarization process. As a result, only
few reports are focused on B-site modication when engaging in Fig. 2. X-ray diffraction patterns of the cobalt-modied NLBT piezoelectric ceramics
enhancing ferroelectric and piezoelectric properties of BLSF ceram- (a) NLBT-C2, (b) NLBT-C4, (c) NLBT-C6, and (d) NLBT-C8.
 C.-M. Wang et al. / Materials Science and Engineering B 171 (2010) 7985 81

The density of the sintered samples was determined by apply- For electrical and dielectric properties measurements, silver elec-
ing the Archimedes method. The X-ray diffraction (XRD) patterns trodes (1 cm2 ) were screen-printed on both surfaces of the polished
for the polished surface were obtained with an X-ray diffrac- pellets and red at 570 C for 20 min. The electrical resistivity
tometer (D8 Advance, Bruker AXS GmbH) using Cu K1 radiation. was calculated from the resistance, which was measured using

Fig. 3. Temperature dependence of dielectric permittivity and dielectric loss tan of the control and cobalt-modied NLBT piezoelectric ceramics (a) NLBT, (b) NLBT-C2, (b)
NLBT-C4, and (d) NLBT-C8.
82 C.-M. Wang et al. / Materials Science and Engineering B 171 (2010) 7985

a 2410 High-Voltage SourceMeter (Keithley) by applying 100 V

on the samples. Samples were pooled in silicone oil at 180 C
for 20 min under a dc electric eld. The piezoelectric coefcient
d33 was measured using a quasi-static d33 meter (Institute of
Acoustics, Academia Sinica, ZJ-2). The dielectric spectra measure-
ments were performed with 4294A impedance analyzer (Agilent)
as a function of temperature. The electromechanical coupling fac-
tors for the planar and thickness modes were determined by
the resonanceantiresonance frequency method using HP 4294A
impedance analyzer (Agilent) according to IEEE standards [21]. The
mechanical quality factor Qm , planar mode electromechanical cou-
pling factor kp , and thickness mode coupling kt were calculated
according to the following equations:
1
Qm = , (2)
2fr Ca R
1 fr
= 0.398 + 0.579, (3)
kp2 fa fr
 f  f 
r r
kt2 = cot , (4)
2 fa 2 fa
where fa is the antiresonant frequency, fr is the resonant frequency,
and R and Ca are the resistance and capacitance, respectively.

3. Results and discussion

The XRD analyses of the cobalt-modied NLBT piezoelectric

ceramic powder diffraction patterns reveal the presence of only
a bismuth oxide layer-type structure with m = 4 within the compo-
sition studied herein, as shown in Fig. 2. All the diffraction patterns
are in agreement with the diffraction data for the pure NLBT [17].
The highest intensity of diffraction peak was found to be the (1 1 9)
orientation, which is consistent with the fact that the most intense
reection of BLSFs is all of the type of (112m + 1 ). The patterns
of the cobalt-modied NLBT ceramics are almost the same and the
peak position shifts slightly, so the theoretical density of the cobalt-
modied NLBT ceramics does not change signicantly. Related to
theoretical density, the relative density of BLSFs was obtained and
was found to be very high, and higher than 97% of theoretical,
indicating acceptable densication during the sintering process.
The density of the samples increases slightly with cobalt contents
increasing. It is also found that the introduction of cobalt into NLBT
ceramics can decrease the sintering temperature. As known, the
diffusion-controlled processes of oxides depend strongly on the
defect chemistry and on the nature of foreign atoms. For diffusion-
controlled processes like sintering, the slowest diffusion species
should determine the overall rate of the sintering. Cobalt ions,
substituting for B-site Ti ions, are accepter dopants for the NLBT
ceramics, and are usually ionically compensated by the formation
of oxygen vacancies. Since the NLBT ceramics show the n-type con-
ductivity, and the oxygen is the rate-controlling diffusion species,
increasing the oxygen vacancies would increase the sintering rate.
Therefore, the enhanced sinterability associated with the cobalt
addition is owed in fact to the creation of oxygen vacancies, which
allow ease of diffusion. The above-mentioned processes may be
described by the following KrgerVink equations [21]:
950 C 1
Co2 O3 2CoO + O2
2
Ti 2x
CoOCoTi + VO + xO
O + O2 , x = 0 to 1
2 modication [17], while, in the present work, the dielectric abnor-
From equations, it is found that the introduction of cobalt into
the NLBT crystal lattices leads to the formation of oxygen vacancies
by substituting the titanium ions (because the ionic radius of cobalt
ions is similar to that of titanium ions, the cobalt ions will enter the
B-site of NLBT). The enhanced sinterability can also attributed to
Fig. 4. Temperature dependence of dielectric permittivity and dielectric loss tan
at 1 MHz of the control and cobalt-modied NLBT ceramics.
the low melting point of cobalt oxide, which accelerates sintering
process and make the ceramics densify.
Fig. 3 shows the relative dielectric permittivity r and dielectric
loss tan measured at 10 kHz, 100 kHz and 1 MHz as a function of
temperature for the pure and cobalt-modied NLBT piezoelectric
ceramics. The Curie temperature of the cobalt-modied NLBT-
based piezoelectric ceramics was found to be higher than that
of the pure NLBT ceramics, and Tc gradually increased from 575
to 595 C with cobalt contents increasing up to 0.8 wt.%, showing
that the modication of cobalt increased the Curie temperature Tc .
Fig. 4 shows the comparative relative permittivity and dielectric
loss tan measured at 1 MHz as a function of temperature. The
inset of Fig. 4 clearly shows the Tc gradually increased with cobalt
contents increasing, where dielectric peaks slightly shift to higher
temperature. The peak value of the dielectric permittivity is about
six times higher than the value of room temperature permittivity.
Fig. 4 also presents that the dielectric loss is very low, especially
the temperature is lower than 400 C. For the pure NLBT ceram-
ics, there is a large dielectric abnormity in dielectric loss tan at
450 C. In most BLSFs, the dielectric abnormity can be observed
in the temperature range 300500 C, and it is attributed to the
jumps of oxygen vacancies during sintering process [22]. However,
(5) the dielectric abnormity was found to be signicantly suppressed
in cobalt-doped NLBT ceramics. It has been reported that this
(6) dielectric abnormity can be suppressed by A-site donor cerium
mity can also be suppressed by B-site accepter cobalt modication.
It seems that the dielectric suppression behavior by cobalt modi-
cation is contradiction to the KrgerVink equation (6), because
the modication of accepter cobalt will produce oxygen vacancies.
However, from KrgerVink equations, the cobalt trioxide may pro-
 C.-M. Wang et al. / Materials Science and Engineering B 171 (2010) 7985
Fig. 5. Scanning electron microscopy images for the surface of the pure and cobalt-modied NLBT piezoelectric ceramics (a) NLBT, (b) NLBT-C2, (c) NLBT-C4, (d) NLBT-C6,
and (e) NLBT-C8.
duce oxygen at elevated temperature, so the oxygen vacancies can
be compensated by oxygen, and then the dielectric abnormity may
also be suppressed. Further work must be conducted to determine
the exact mechanism on the dielectric abnormity. The dielectric
loss tan was found to increase with the temperature increasing,
but with the temperature further increasing, the loss tan sharply
drops at a specic temperature, which is corresponding to the Curie
temperature Tc . That is, this dielectric loss valley is corresponding
to the dielectric permittivity peak. From Fig. 4, it is also found that
the cobalt-modied NLBT ceramics, especially NLBT-C2 and NLBT-
C4, presented reduced loss tan in the temperature range from RT
to 500 C, compared to the pure NLBT ceramics.
Fig. 5 shows the scanning electron microscopy images for the
surface of the pure and cobalt-modied NLBT piezoelectric ceram-
ics. Due to the high grain growth rate in the direction perpendicular
to the c-axis of the BLSFs crystal, the grain growth is structurally
highly anisotropic and the length l of the plate-like grain is much
83
bigger than the thickness t. It also can be seen, the cobalt-modied
NLBT ceramics exhibited the larger grain size compared to the pure
NLBT ceramics, indicating that the introduction of cobalt enhanced
the grain growth of the ceramics. The increase in grain size resulted
in both the density and the shrinkage increasing, which are bene-
cial to the piezoelectric properties of the ceramics.
The detailed room temperature (RT) electrical properties of the
pure and cobalt-modied NLBT ceramics are characterized and
listed in Table 1. The RT relative dielectric permittivity of the
NLBT ceramics does not change signicantly with cobalt modi-
cation, varying between 180 and 210. The RT dielectric loss tan
for the pure and cobalt-modied NLBT was found to be very low,
less than 0.5%. The loss tan of the cobalt-modied NLBT ceram-
ics was found to be lower than that of the pure NLBT ceramics,
and the dielectric loss for the NLBT-C4 ceramics was found to be
only 0.2%. The piezoelectric properties of the cobalt-modied NLBT
ceramics were obviously enhanced compared to that of the pure
84 C.-M. Wang et al. / Materials Science and Engineering B 171 (2010) 7985

Table 1
Electrical properties of cobalt-modied sodium lanthanum bismuth titanate ceramics.

Samples r tan (%) d33 (pC/N) Qm kp (%) kt (%) Np (Hz m) Nt (Hz m) Tc ( C)

NLBT 182 0.5 16 2600 3.5 10.2 2280 2050 575

NLBT-C2 199 0.4 25 3040 5.8 26.2 2370 2240 583
NLBT-C4 210 0.2 27 3400 6.5 28.5 2330 2220 589
NLBT-C6 202 0.2 24 3350 5.4 27.7 2340 2260 -
NLBT-C8 210 0.4 22 3210 5.3 25.8 2360 2210 595

NLBT ceramics. The d33 of the NLBT-C4 was found to be 27 pC/N,

the highest value among the cobalt-modied NLBT piezoelectric
ceramics. The enhancement of the piezoelectric activities can be
attributed to the substitution of B-site Ti4+ ions by Co2+ ions. The
B-site cations locate at the center of oxygen octahedra, so the slight
change in B-site cationic radius (Ti4+ and Co2+ ions have different
ionic radius) may play a major structural role in the polarization
process, which is benecial to the domain wall movements and
improves the piezoelectric properties. Fig. 6 shows the frequency
dependence of the impedance |Z| and phase angle  measured at
room temperature in the piezoelectric radialextensional vibration
mode (kp mode) for the NLBT-C4 ceramics, which possess the high-
est piezoelectric activities. If the ideal poling state is obtained, the
impedance phase angle  approaches 90 in the frequency range
between the resonance and antiresonance frequencies. The phase
angle of impedance was limited to approximately 83 , which was
similar to those of other BLSFs. The resonanceantiresonance char-
acteristics of the thickness-extensional (kt ) vibration mode of the
NLBT-C4 ceramics were also measured. According to Eqs. (2)(4), Fig. 7. Temperature dependence of electrical resistivity of the NLBT and NLBT-C4
the electromechanical coupling factors and mechanical quality fac- ceramics.
tors were calculated and listed in Table 1. The electromechanical
coupling factors, kp and kt , and mechanical quality factor Qm (kp
mode) for the NLBT-C4 ceramics were found to be 6.5%, 28.5% and charge leakage. Fig. 7 gives the Arrhenius relationship of electrical
3400, respectively. Compared to that of the pure NLBT ceramics, the resistivity with temperature for the NLBT and NLBT-C4 ceram-
electromechanical properties of the cobalt-modied NLBT ceram- ics. It is also found that both the NLBT and NLBT-50 ceramics
ics were signicantly enhanced. In general, the samples with high still showed high resistivity up to 500 C, higher than 106  cm at
piezoelectric activities have high electromechanical coupling fac- 500 C. The activation energy (Ea ), calculated according to Arrhe-
tors and low dielectric loss, though this need not always holds good. nius law:  = 0 exp(Ea /kT), of the NLBT and NLBT-C4 ceramics was
From Table 1, it is also found that the kt is almost ve times of the found to be 1.47 and 1.31 eV, respectively. The resistivity of NLBT-
kp , indicating that the layer-structured NLBT ceramics presented C4 ceramics was found to be lower than that of NLBT ceramics in
strong anisotropic electromechanical properties. The planar fre- the temperature range from 300 to 500 C. The decrease in the
quency constant Np and thickness frequency constant Nt for the resistivity related to the defects is probably one of the reasons
pure and cobalt-modied NLBT ceramics were found to be higher of the enhancement of piezoelectric activities. In the lattice hav-
than 2200 and 2000 Hz m, respectively. ing defects, the atoms transport is easier than in perfect lattice,
High electrical resistivity is important so that a large electric and then the domain wall movements can be caused by a smaller
eld can be applied during poling without breakdown or excessive mechanical stress. Therefore, the piezoelectric activities of cobalt-
modied NLBT ceramics can be enhanced.

Fig. 6. Frequency dependence of impedance |Z| and phase angle  of the NLBT-C4 Fig. 8. Effect of annealing temperature for 1 h on the piezoelectric coefcient d33 of
piezoelectric ceramics in a planar mode. the NLBT-C4 piezoelectric ceramics.
 C.-M. Wang et al. / Materials Science and Engineering B 171 (2010) 7985
The thermal annealing behaviors of the NLBT-C4 ceramics are
shown in Fig. 8, where the piezoelectric coefcient d33 is plot-
ted against the annealing temperature. The value of piezoelectric
coefcient d33 shows no obvious drop, when the annealing tem-
perature is lower than 500 C, and it retains 25 pC/N, even if the
annealing temperature reaches 500 C. This reveals that the four-
layer NLBT layer-structured materials are very stable to thermal
annealing, and can potentially be used in high-temperature piezo-
electric applications. When the annealing temperature approaches
the Curie temperature, the d33 decreases sharply.
4. Conclusions
The cobalt-modied Aurivillius-type sodium lanthanum bis-
muth titanate Na0.5 La0.5 Bi4 Ti4 O15 polycrystalline ceramics were
synthesized using conventional solid state processing. The dielec-
tric and piezoelectric properties were investigated in detail. The
piezoelectric activities of NLBT ceramics were improved by cobalt
modication. The piezoelectric coefcient d33 and Curie temper-
ature Tc of the 0.2 wt.% cobalt-modied NLBT were found to be
27 pC/N and 589 C, respectively. A large dielectric abnormity in
dielectric loss tan was observed in NLBT ceramics, which can be
signicantly suppressed by cobalt modication. High Curie temper-
ature and enhanced piezoelectric activities make cobalt-modied
NLBT ceramics promising materials for high-temperature piezo-
electric applications.
Acknowledgments
This research was supported by the National Natural Science
Foundation of China under the Grant Nos. 50902087 and 50702030,
the Natural Science Foundation of Shandong Province of China
under the Grant No. ZR2009FQ009, the Outstanding Youth Sci-
85
entist Research Foundation of Shandong Province of China under
Grant No. 2008BS04002, the Specialized Research Fund for the
Doctoral Program of Higher Education of China under Grant Nos.
20070422059 and 20080422003.
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