Zuo-Guang. Ye Advanced Dielectric Piezoelectric and Ferroelectric Materials: Synthesis, Characterisation and Applications
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Handbook of dielectric, piezoelectric and ferroelectric materials150
The preliminary results show that A-site or B-site modifications on PMNT
single crystals obtain only modest increase (~10–20 °C) in the ferroelectric
phase transition. The modification level is controlled at lower than 5 mol%
in order to obtain pure perovskite phase. The growth of various relaxor–PT
systems were explained by several research groups, but with little success
due to the following reasons: either no significant improvement (only up to
30 °C when compared with PMNT crystals) of the ferroelectric phase transition
temperature (such as PIN–PMN–PT and PSN–PMN–PT systems), which is
the major factor limiting the application temperature range; or it is very hard
to grow large crystals and no successful Brigman growth was achieved due
to the inferior perovskite stability (like PYNT system, which will form
pyrochlore phase or decomposed to PbO at high temperature). Bismuth-
based perovskite system, BSPT, was found to have excellent temperature
stability, comparable piezoelectric performance, and significantly enhanced
usage temperature range when compared to other lead-based perovskite single
crystals. But it is difficult to obtain large crystals and hard to control the
crystal quality because there are two volatile compositions, PbO and Bi
2
O
3
,
in the material.
Compared with the perovskite MPB single crystals, non-perovskite
piezoelectric crystals were found to possess very low piezoelectric and
dielectric properties, but their much better temperature-independent properties
and much wider usage temperature range make this kind of crystals employable
where stable piezoelectric responses at ultra-high temperatures are required.
Large piezoelectric voltage coefficients are expected in these crystals because
of the ultra-low dielectric constant. Usually these piezoelectric crystals have
very low symmetry – for example, the langasite family and GaPO
3
belong to
32 group, and the oxyborate family belongs to m group – which make it very
hard to find suitable orientations for the practical applications. The high
resistivity should also be considered in the ultra-high-temperature sensor or
actuator applications because of the length of time that a charge can be
maintained within a sensor or actuator is proportional to the RC time constant.
5.8 Future trends
The future trend for high-temperature piezoelectric single crystals may be
focused on two issues, first, how to raise the Curie temperature and/or the
usage temperature range of the ferroelectric single crystals? Three approaches
are discussed in this chapter, in which the bismuth-based solid solution is
very promising owing to the lower tolerance factor, when compared with
their lead-based counterparts, and supposed to have higher Curie temperature
in the MPB composition based on the tolerance factor. Second, how to
commercialize the crystals, which includes how to get large, high-quality
crystals and how to reduce the production cost? Owing to perovskite unstable
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High-performance, high-T
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piezoelectric crystals 151
and/or high-temperature decomposition for many of the lead-based and
bismuth-based solid solution, it is difficult to grow the crystal from melt
directly. So it is important to select suitable flux compositions in the high-
temperature solution or flux Bridgman growth methods. Also, the solid-state
conversion crystal growth method has the advantage of low-cost and
composition control (homogeneous composition), which is also a feasible
solution to obtain large size single crystals.
5.9 Acknowledgment
The work was supported by ONR and NIH under #P41-RR11795.
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158
6.1 Introduction
Some piezoelectric single crystals such as Pb(Mg
1/3
Nb
2/3
)O
3
–PbTiO
3
(PMN–
PT), Pb(Zn
1/3
Nb
2/3
)O
3
–PbTiO
3
(PZN–PT), and Ba(Ti,Zr)O
3
(BZT) are known
to exhibit remarkable piezoelectric properties.
1–3
Lead-based piezoelectric
PMN–PT and PZN–PT single crystals were reported to have piezoelectric
coefficients (d
33
) higher than 2000 pC/N and electromechanical coupling
factors (k
33
) higher than 0.9.
1,2
It was also demonstrated that the lead-free
Ba(Ti,Zr)O
3
single crystals with appropriate amounts of Zr also have a k
33
of
about 0.9 and a d
33
higher than 1000 pC/N. Because of their extraordinary
piezoelectric properties, it is expected that a breakthrough in piezoelectric
applications will be possible in the near future.
PMN–PT and PZN–PT single crystals have usually been fabricated by the
flux method and the Bridgman technique.
4–10
The flux method is a simple
and low-cost technique, but is limited because of crystal quality and quantity.
The Bridgman technique has a good reproducibility, but requires sophisticated
and expensive equipment and may have a problem providing composition
homogeneity. These methods are suitable for growing bulk single crystals,
but are not easily transferable to large-scale manufacturing. The solid-state
single crystal growth (SSCG) technique has been developed as an alternative
crystal growth method that offers advantages over the conventional melt
methods such as the flux method and the Bridgman technique.
11,12
In the SSCG process, a small single crystal seed is diffusion-bonded to a
polycrystalline body and grows by consuming fine matrix grains to become
a large single crystal after long annealing of crystal growth step. This process
was referred to as solid-state single crystal growth because it does not involve
complete melting of major components. Since this process is basically the
same as a normal sintering process, it is not only cost-effective but also
suitable to mass production of single crystals. Especially, the SSCG method
is useful for single crystal growth of materials with high melting temperature,
destructive phase transitions, volatile components, and incongruent melting.
6
Development of high-performance
piezoelectric single crystals by using
solid-state single crystal growth
(SSCG) method
H Y L E E, Sunmoon University and Ceracomp Co. Ltd, Korea
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Development of high-performance piezoelectric single crystals 159
As an alternative crystal growth method, several research groups have already
studied and developed the SSCG method, e.g. NGK in Japan developed the
SSCG method to produce ferrite single crystals.
13,14
The SSCG method was
also proved to be feasible for BaTiO
3
single crystals.
15–18
As an alternative
to the Bridgman method, the SSCG technique has been intensively studied
for growth of PMN–PT single crystals.
19,20
In this chapter 1 report that piezoelectric single crystals of Ba(Ti,Zr)O
3
,
PMN–PT (undoped, Fe-doped, and Mn-doped), and PMN–PZT have been
successfully fabricated by the SSCG method. The dielectric and piezoelectric
properties of the grown crystals have also been characterized. These results
shows that the SSCG technique can be applied to the growth of Ba(Ti,Zr)O
3
,
PMN–PT, and relaxor–PZT single crystals and can also be used for development
of new high-performance piezoelectric single crystals which are difficult to
fabricate by conventional single crystal growth techniques.
6.2 Solid-state crystal growth (SSCG) process
The abnormal grain growth (AGG, also referred to as discontinuous grain
growth or exaggerated grain growth) during sintering of polycrystalline
ceramics has been extensively studied. During AGG, a few grains grow much
faster than surrounding fine matrix grains so that the microstructure exhibits
a bimodal distribution of grain size. Abnormal grains usually grow until they
impinge each other. This suggests the possibility of single crystal growth by
controlling AGG. If it is possible to control the nucleation of abnormal grains
in a polycrystalline material, AGG can be used to grow a single crystal in a
polycrystalline material. In the SSCG process a small single crystal seed can
be used to control the nucleation of abnormal grains effectively. By using a
seed crystal with known crystallographic orientation, the crystallographic
orientation of the growing single crystal can be easily predetermined.
Figure 6.1 shows the solid-state growth of a (100) Ba(Zr
0.1
Ti
0.9
)O
3
(BZT)
seed crystal in a Ba(Zr
0.1
Ti
0.9
)O
3
ceramic. Before the annealing of crystal
growth, a small (100) BZT single crystal was placed on the top of the BZT
ceramic. During the heat treatment, the small (100) BZT seed crystal grew
from the top to the bottom of the Ba(Zr
0.1
Ti
0.9
)O
3
ceramic and thus a
Ba(Zr
0.1
Ti
0.9
)O
3
single crystal of ~40 × 40 × 8mm
3
formed in the BZT
ceramics. The grown single crystal, i.e. the region swept by the seed crystal
during the heat treatment, is clearly discerned from the appearance of the
specimen compared with the remaining polycrystalline region. During the
growth of the (100) seed crystal, the {100} planes of the grown single crystal
were always well developed. Figure 6.2 shows a polished surface of a (100)
BZT single crystal larger than 50 × 50 × 10 mm
3
, which was grown in a BZT
ceramic. The seed crystal on the grown Ba(Zr
0.1
Ti
0.9
)O
3
crystal was ground
off after the SSCG process.
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