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Electromechanical Properties of Mn-Doped PB (In1/2Nb1/2) O3-Pb (Mg1/3Nb2/3) O3-Pbtio3 Piezoelectric Ceramics

This document summarizes research on the electromechanical properties of manganese (Mn)-doped lead indium niobate-lead magnesium niobate-lead titanate (PIN-PMN-PT) piezoelectric ceramics. The study finds that doping with 2% Mn increases the mechanical quality factor (Qm) to as high as 2000 while maintaining an electromechanical coupling factor (kp) of 57%, comparable to undoped PIN-PMN-PT. Mn doping also results in ferroelectric hysteresis loop deviations that can be interpreted as an internal bias field formation due to defect dipoles. The relatively high Curie temperature, very high Qm, and low dielectric
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0% found this document useful (0 votes)
131 views7 pages

Electromechanical Properties of Mn-Doped PB (In1/2Nb1/2) O3-Pb (Mg1/3Nb2/3) O3-Pbtio3 Piezoelectric Ceramics

This document summarizes research on the electromechanical properties of manganese (Mn)-doped lead indium niobate-lead magnesium niobate-lead titanate (PIN-PMN-PT) piezoelectric ceramics. The study finds that doping with 2% Mn increases the mechanical quality factor (Qm) to as high as 2000 while maintaining an electromechanical coupling factor (kp) of 57%, comparable to undoped PIN-PMN-PT. Mn doping also results in ferroelectric hysteresis loop deviations that can be interpreted as an internal bias field formation due to defect dipoles. The relatively high Curie temperature, very high Qm, and low dielectric
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Electromechanical properties of Mn-doped Pb(In1/2Nb1/2)O3-


Pb(Mg1/3Nb2/3)O3-PbTiO3 piezoelectric ceramics

Article  in  Ceramics International · June 2016


DOI: 10.1016/j.ceramint.2016.06.175

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Ceramics International 42 (2016) 15332–15337

Contents lists available at ScienceDirect

Ceramics International
journal homepage: www.elsevier.com/locate/ceramint

Electromechanical properties of Mn-doped


Pb(In1/2Nb1/2)O3-Pb(Mg1/3Nb2/3)O3-PbTiO3 piezoelectric ceramics
Xudong Qi a, Enwei Sun a,n, Junjun Wang a, Rui Zhang a,n, Bin Yang a, Wenwu Cao a,b
a
Condensed Matter Science and Technology Institute, Harbin Institute of Technology, Harbin 150080, China
b
Department of Mathematics and Materials Research Institute, The Pennsylvania State University, University Park, PA 16802, USA

art ic l e i nf o a b s t r a c t

Article history: The dielectric, piezoelectric, and ferroelectric properties of Mn-doped and undoped yPb(In1/2Nb1/2)O3-
Received 20 March 2016 (1  x  y)Pb(Mg1/3Nb2/3)O3-xPbTiO3 (PIN-PMN-PT) ternary ceramics with morphotropic phase boundary
Received in revised form composition have been investigated. Mn-doped PIN-PMN-PT ceramics show obvious hardening char-
18 June 2016
acteristics. With 2 mol% Mn doping the mechanical quality factor Qm can be increased to as high as 2000,
Accepted 26 June 2016
while the electromechanical coupling factor (kp ¼57%) is still comparable to that of the undoped coun-
Available online 27 June 2016
terpart. The internal bias field Ei was analyzed and calculated based on the P-E hysteresis loops for the
Keywords: Mn-doped PIN-PMN-PT ceramic. The relatively high Curie temperature, very high Qm, and low dielectric
PIN-PMN-PT ceramic loss make the Mn-doped PIN-PMN-PT ceramics good candidates for high power and high temperature
Piezoelectric
electromechanical device applications.
Mechanical quality factor
& 2016 Elsevier Ltd and Techna Group S.r.l. All rights reserved.
Internal bias field

1. Introduction Recently, the development of ternary yPb(In1/2Nb1/2)O3-


(1  x  y)Pb(Mg1/3Nb2/3)O3-xPbTiO3 (PIN-PMN-PT) solid solution
Relaxor-based ferroelectric (1  x)Pb(Mg1/3Nb2/3)O3-xPbTiO3 provided a better candidate for piezoelectric applications at higher
(PMN-xPT) single crystals have attracted extensive attention in the temperatures. The ternary PIN-PMN-PT ceramics near MPB region
past two decades due to their superior piezoelectric and electro- show comparable electromechanical properties (d33  500 pC/N,
mechanical coupling properties [1]. The piezoelectric coefficient kp  61%) and higher Curie temperature (TC 210 °C) [13–15]. There
d33 and electromechanical coupling factor k33 of [001]c poled have been a lot of work done to harden relaxor-PT ceramics
PMN-0.33PT single crystal have super large values of 2820 pC/N through the doping of acceptor dopants in order to increase the
and 94% [2–4], respectively, which make it good candidate for mechanical quality factor Qm and decrease the dielectric loss [16–
applications in medical ultrasonic imaging, sonar transducers, and 19]. A higher Qm and lower dielectric loss are essential for high
solid-state actuators [5–7]. Compared to single crystals, piezo- power piezoelectric transformer application. This could be
electric ceramics are more economic for industrial applications for achieved by Mn doping. For example, the Qm of Mn-doped PIN-
their low-cost. The d33 and kp of PMN-xPT ceramics with mor- PMN-PT single crystal can be increased by a factor of 4 or even
photropic phase boundary (MPB) composition are 500–600 pC/N more compared to undoped PIN-PMN-PT single crystals [20]. Al-
and 55–60%, respectively, with the Curie temperature in the range though some studies on the electromechanical properties of Mn
of 130–160 °C [8–10]. Although PMN-xPT systems have excellent doped relaxor-PT single crystals have been done [21,22], there is
electromechanical properties, a low Curie temperature TC and little reports in the literature on Mn-doped PIN-PMN-PT ceramics
lower depoling temperature TR-T limited their application in the [23], which are more uniform in composition and much more cost
high-temperature range [11]. Another drawback of PMN-xPT sys- effective for high-power device applications.
tem is the low coercive field (2–3 kV/cm), which also limits their In this work, PIN-PMN-PT and Mn-doped PIN-PMN-PT ceramics
specific applications due to depolarization and degradation of were synthesized and their dielectric, ferroelectric, and electro-
piezoelectric properties under high-power operations [12]. mechanical properties were investigated. The PIN-PMN-PT cera-
mics show much improved mechanical quality factor Qm but
n slightly decreased dielectric and piezoelectric properties after Mn
Corresponding authors.
E-mail addresses: [email protected] (E. Sun), doping. The deviation of ferroelectric hysteresis loops after Mn-
[email protected] (R. Zhang). doping may be interpreted by the formation of internal bias field

http://dx.doi.org/10.1016/j.ceramint.2016.06.175
0272-8842/& 2016 Elsevier Ltd and Techna Group S.r.l. All rights reserved.
X. Qi et al. / Ceramics International 42 (2016) 15332–15337 15333

due to detect dipoles. The Raman spectroscopy of PIN-PMN-PT


ceramics was analyzed by using the principle of deconvolution.

2. Experimental procedure

The 24PIN-42PMN-34PT ternary ceramics with MPB composi-


tion and Mn-doped 24PIN-42PMN-34PT with different doping
ratio (0–5 mol%) were synthesized using two-step columbite pre-
cursor method [13,24]. The raw materials (In2O3 and Nb2O5) (MgO
and Nb2O5) with purities better than 99.9% were heat-treated at
1100 °C and 1000 °C for 7 h to prepare the precursor of InNbO4 and
MgNb2O6, respectively. In the preparation of MgNb2O6, fast heat-
ing rate (5 °C/min) was adopted to avoid the pyrochlore phase.
Then, the PbO, InNbO4, MgNb2O6, TiO2 and MnO2 powders with
different doping ratio (0–5 mol%) were wet mixed by ball milling
for 24 h and the mixed powders were calcined at 850 °C for 4 h.
After a second ball-milling, the powders were pressed using PVA
binder to form 13 mm diameter discs with the thickness of 1 mm.
Fig. 2. Deconvolution of the depolarized Raman spectrum of undoped 24PIN-
After burning out the PVA binder at 550 °C for 2 h, the samples 42PMN-34PT ceramic at room temperature. The inset is the depolarized Raman
were sintered at 1200–1300 °C for 6 h. To compensate for PbO spectra of Mn-doped 24PIN-42PMN-34PT ceramics (0–5 mol%).
evaporation during sintering, a PbO-rich atmosphere was main-
tained. Silver electrodes was printed on both sides of the disc
samples and then fired at 550 °C for 30 min. Poling was carried out
in silicon oil at 130 °C for 10 min with an electric field of 40 kV/cm.
The P-E hysteresis loops and the piezoelectric strain were
measured by the Precision Premier II system (Radiant Technolo-
gies). The temperature dependence of the dielectric constant was
computed from the capacitance at 1 kHz measured by Agilent
E4980A precision LCR meter based on the parallel capacitance
approximation. The mechanical quality factor Qm and electro-
mechanical coupling factor kp were calculated from impedance
spectra measured by Agilent 4294A Precision Impedance Analyzer
according to the IEEE standard on piezoelectricity. The piezo-
electric constant d33 was measured by the ZJ-2 piezo d33 meter.
The Raman spectra were taken by a Jobin Yvon HR800 micro-Ra-
man spectrometer using the 514.5 nm excitation line from an Ar
ion laser.

3. Results and discussion Fig. 3. Ferroelectric hysteresis loops of Mn-doped 24PIN-42PMN-34PT ceramics (0–
5 mol%).
Fig. 1 shows the XRD patterns of 24PIN-42PMN-34PT ceramics
with different Mn-doped contents. In these patterns, only pure (R) phases can be identified by an analysis of the peaks (002) and
perovskite phase exists without detectable trace of pyrochlore (111). The splitting of (002) peak indicates the T phase, while the
structure. It is noted that tetragonal (T) and rhombohedral single (111) peak shows the R phase. In these patterns, there is no
observable split in both (111) and (200) peaks. In addition, the
broadened (200) peak indicates the coexistence of rhombohedral
and tetragonal phases [13,15].
Unlike the XRD, which investigates the average crystal struc-
ture of materials, Raman spectroscopy is a convenient method to
study lattice dynamics, micro-symmetry and phase transitions.
Combined with an optical microscope, a Raman spectrum can be
collected in micron scale by focusing the laser on the sample with
the spot size about 1–2 mm. In the past decade, micro-Raman
scattering technique has been used to study relaxor ferroelectrics
extensively, such as PMN, PMN-PT and PIN-PMN-PT [25]. Fig. 2
shows the depolarized Raman spectra of Mn-doped PIN-PMN-PT
ceramics. It can be seen that all Raman spectra with different Mn
doping exhibited analogous bands and all bands are relatively
broad due to peak overlapping, which is a typical feature of re-
laxor-based ferroelectrics. According to lattice dynamics calcula-
tions and the mode assignment of PMN and PMN-PT, the region of
500–900 cm  1 was related to B-O-B′ and B-O-B stretching modes,
Fig. 1. XRD patterns of Mn-doped 24PIN-42PMN-34PT ceramics (0–5 mol%). the modes from 150 to 500 cm  1 were attributed to B-O-B
15334 X. Qi et al. / Ceramics International 42 (2016) 15332–15337

Table 1
Dielectric, piezoelectric, and ferroelectric properties of Mn-doped 24PIN-42PMN-34PT ceramics.

Mn (mol%) TC (°C) TR-T (°C) T


ε33/ε0 (1 kHz) tanδ (%) d33 pC/N Qm kp Pr (μC/cm2) Ei (kV/cm)

0 205 103 2388 1.6 516 85 0.67 32.3 0.04


1 206 114 1382 0.3 430 1296 0.57 27.2 0.48
2 209 116 1214 0.6 347 2381 0.57 14.4 1.05
3 205 109 1106 1.1 313 1812 0.56 15.9 0.90
4 197 105 1106 1.5 302 1508 0.55 16.8 1.00
5 189 96 1104 2.0 297 1295 0.52 16.9 1.08

Fig. 6. Piezoelectric strain as a function of electric field in Mn-doped 24PIN-


42PMN-34PT ceramics (0–5 mol%).
Fig. 4. (a) Remanent polarization Pr and internal bias field Ei, and (b) piezoelectric
coefficient d33 and electromechanical coupling factor kp of 24PIN-42PMN-34PT 34PT ceramics, similar to what had been observed in PIN-PMN-PT
ceramics as a function of Mn content.
single crystals [25–27]. In addition, there are no obvious traces
indicating that Mn doping obviously affects the phase structure at
room temperature because both the XRD and Raman spectroscopy
show no obvious changes after the Mn doping.
The polarization hysteresis loops of PIN-PMN-PT ceramics with
different Mn-doped contents are shown in Fig. 3. The hysteresis
loops became asymmetrical after Mn doping with respect to the
point of E ¼0 kV/cm. This is because that an internal bias field was
induced from the development of acceptor-oxygen vacancy defect
dipoles [28–30]. The Mn ions doped in the ferroelectric crystal are
Mn2 þ or Mn3 þ , which substitute high valent cations of B sites,
such as Mg2 þ , Nb5 þ or Ti4 þ according to the crystal chemistry
principle [31]. In order to compensate the charges, oxygen va-
cancies were created, which formed defect dipoles with charge
defects to produce an internal bias field after poling [32].
Ei ¼(Ec þ þ Ec  )/2 was used to describe the internal bias field,
where Ec þ and Ec  are the intersections of polarization loops with
positive and negative field axis, respectively [33]. The calculated Ei
were given in Table 1. With increasing the Mn content from
0 mol% to 2 mol%, internal bias field increases gradually, but Ei
Fig. 5. Temperature dependence of dielectric constants in Mn-doped 24PIN- becomes saturated beyond 2 mol% Mn doping, as shown in Fig. 4
42PMN-34PT ceramics (0–5 mol%).
(a). Hence, the amplitude of Ei or deviation degree of ferroelectric
hysteresis loop is related to the amount of Mn doping. The cor-
bending and O-B-O stretching modes, while the region below responding remnant polarization Pr as a function of Mn doping
150 cm  1 was classified as the Pb vibrating modes with respect to amount is also shown in Fig. 4(a). With the increase of Mn content,
the octahedron [25,26]. the remnant polarization Pr decreases first, then increases slightly
The deconvolution of Raman spectrum for undoped 24PIN- beyond 2 mol% Mn-content. The dropping amplitude is fast (from
42PMN-34PT ceramic was obtained by using Lorenz curve fitting, 32.3 μC/cm2 at 0 mol% to 10.4 μC/cm2 at 2 mol%), then the change
as shown in Fig. 2. At room temperature, the spectrum was de- becomes much slower beyond 2 mol% Mn doping.
composed into 15 Raman active modes. According to group theory, The temperature dependence of the dielectric constant for Mn-
rhombohedral and tetragonal ferroelectric phases give rise to doped 24PIN-42PMN-34PT ceramics at 1 kHz is shown in Fig. 5.
7 and 8 Raman active phonon modes, respectively. Based on the One can see that a broad dielectric peak centered at the tem-
XRD pattern and Raman spectrum fitting, we can conclude that perature of the maximum dielectric constant. Such diffuse phase
the rhombohedral and tetragonal phases coexist in 24PIN-42PMN- transition is typical for relaxor ferroelectrics due to the presence of
X. Qi et al. / Ceramics International 42 (2016) 15332–15337 15335

Fig. 7. SEM microstructures of 24PIN-42PMN-34PT ceramics doped with Mn of (a) 0 mol%, (b) 1 mol%, (c) 2 mol%, (d) 3 mol%, (e) 4 mol%, and (f) 5 mol%.

polar nanoregions (PNRs). The dielectric constant and dielectric addition, the Curie temperature TC has slightly increased from
loss tanδ (at 1 kHz) at room temperature are listed in Table 1. The 205 °C at 0 mol% to 209 °C at 2 mol%, and decreased by 16 °C from
Curie temperature TC basically keeps similar values for different 3 mol% to 5 mol% Mn doping. Similar phenomena were also re-
mount of Mn additions. However, the dielectric peaks were sup- ported in the Mn-doped PZT system [34]. In addition, the dielectric
pressed by the Mn doping due to the domain pinning effect. In loss (tanδ) was significantly decreased to 3  10  3 after 1 mol%
15336 X. Qi et al. / Ceramics International 42 (2016) 15332–15337

doping, but increased again when the Mn addition is larger than charge carrier, so that the dielectric loss will be increased. On the
2 mol%. other hand, the mechanical quality factor is affected by both the
The piezoelectric strain as a function of electric field is illu- domain pinning and grain size effects, and shows the largest value
strated in Fig. 6. The piezoelectric strain (S%) is a relative bipolar at 2 mol% due to the solubility limit.
strain, which was obtained using the true strain dividing the
sample thickness along the vibration direction. From Fig. 6, it can
be seen that the strain had an obvious decrease from 0 mol% to 4. Conclusion
2 mol% Mn content. Further increasing the amount of Mn beyond
2 mol%, the strain gradually reached a saturated level. The S% can The Mn-doped PIN-PMN-PT ceramics exhibited representative
reach 0.14% without doping and the lowest level was only around hardening character with greatly improved mechanical quality
0.025% after doping under a field of 20 kV/cm. factor Qm and dielectric loss tanδ. At the same time, there is a
The piezoelectric coefficient d33 and electromechanical cou- slight decrease of the electromechanical coupling factor kp and
pling factor kp are very important properties for ferroelectric piezoelectric constant d33. The internal bias field was induced by
ceramics. They reflect the ability of electromechanical energy dipolar defects, and piezoelectric and dielectric activities were
conversion and electromechanical coupling. As shown in Fig. 4(b), suppressed due to the pinning of domain wall motions. Our results
d33 shows similar trend as that of the strain. With the increase of also indicated that the 2 mol% Mn-doping is the solubility limit for
doping ratio, the d33 has a significant decrease from 516 pC/N at the PIN-PMN-PT ceramics and the dielectric, piezoelectric, and
0 mol% to 347 pC/N at 2 mol%, and slightly decrease from 313 pC/N electromechanical properties of Mn-doped PIN-PMN-PT ceramics
at 3 mol% to 297 pC/N at 5 mol% Mn doping. It is well known that begin to decrease beyond 2 mol% Mn doping.
the d33 value could also be deduced from the slope of strain vs
electric field, consequently the d33 and the strain show the same
varying trend in this work. The kp is about 57% with 2 mol% Mn Acknowledgements
doping, which is lower than that of undoped PIN-PMN-PT ceramic
(kp ¼ 67%). Through the above description, one can see that partial This research was supported in part by the National Key Basic
piezoelectric properties of the PIN-PMN-PT ceramics were sup- Research Program of China (973 Program) under Grant No.
pressed by Mn additions. 2013CB632900, the NSFC under Grant No. 11304061 and
The mechanical quality factor Qm is a crucial property for high 51575344, the China Postdoctoral Science Foundation under Grant
power piezoelectric devices, such as ultrasonic motors, ultrasonic No. 2013M531029, the Heilongjiang Postdoctoral Fund under
cleaners and ultrasonic welding machines. The formula of Qm ¼fr/ Grant No. LBH-Z13072, and the Fundamental Research Funds for
(f1  f2) was applied to calculate the Qm, where fr is the resonance the Central Universities under Grant No. HIT. NSRIF. 2014083.
frequency, f1 and f2 are frequencies at 3 dB down the maximum
admittance. The calculated values of Qm are given in Table 1. The
results show that the mechanical quality factor Qm of PIN-PMN-PT References
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