Recent Developments on High Curie Temperature PIN-PMN-PT Ferroelectric Crystals.

Pb(In(0.5)Nb(0.5))O(3)-Pb(Mg(1/3)Nb(2/3))O(3)-PbTiO(3) (PIN-PMN-PT) ferroelectric crystals attracted extensive attentions in last couple years, due to their higher usage temperatures range (> 30°C) and coercive fields (~5kV/cm), meanwhile maintaining similar electromechanical couplings (k(33)> 90%) and piezoelectric coefficients (d(33)~1500pC/N), when compared to their binary counterpart Pb(Mg(1/3)Nb(2/3))O(3)-PbTiO(3). In this article, we reviewed recent developments on the PIN-PMN-PT single crystals, including the Bridgman crystal growth, dielectric, electromechanical, piezoelectric and ferroelectric behaviors as function of temperature and dc bias. Mechanical quality factor Q was studied as function of orientation and phase. Of particular interest is the dynamic strain, which related to the Q and d(33), was found to be improved when compared to binary system, exhibiting the potential usage of PIN-PMN-PT in high power application. Furthermore, PIN-PMN-PT crystals exhibit improved thickness dependent properties, due to their small domain size, being on the order of 1µm. Finally, the manganese acceptor dopant in the ternary crystals was investigated and discussed briefly in this paper.

Polarization Fatigue in Pb(In(0.5)Nb(0.5))O(3)-Pb(Mg(1/3)Nb(2/3))O(3)-PbTiO(3) Single Crystals.

Electric fatigue tests have been conducted on pure and manganese modified Pb(In(0.5)Nb(0.5))O(3)-Pb(Mg(1/3)Nb(2/3))O(3)-PbTiO(3) (PIN-PMN-PT) single crystals along different crystallographic directions. Polarization degradation was observed to suddenly occur above 50-100 bipolar cycles in <110> oriented samples, while <001> oriented samples exhibited almost fatigue free characteristics. The fatigue behavior was investigated as a function of orientation, magnitude of the electric field and manganese dopant. It was found that <001> oriented PIN-PMN-PT crystals were fatigue free, due to its small domain size, being on the order of 1µm. The <110> direction exhibited a strong electrical fatigue behavior due to mechanical degradation. Micro/macro cracks were developed in fatigued <110> oriented single crystals. Fatigue and cracks were the results of strong anisotropic piezoelectric stress and non-180° domain switching, which completely locked the non-180° domains. Furthermore, manganese modified PIN-PMN-PT crystals were found to show improved fatigue behavior due to its enhanced coercive field.

Giant piezoelectricity of Sm-doped Pb(Mg1/3Nb2/3)O3-PbTiO3 single crystals.

High-performance piezoelectrics benefit transducers and sensors in a variety of electromechanical applications. The materials with the highest piezoelectric charge coefficients (d 33) are relaxor-PbTiO3 crystals, which were discovered two decades ago. We successfully grew Sm-doped Pb(Mg1/3Nb2/3)O3-PbTiO3 (Sm-PMN-PT) single crystals with even higher d 33 values ranging from 3400 to 4100 picocoulombs per newton, with variation below 20% over the as-grown crystal boule, exhibiting good property uniformity. We characterized the Sm-PMN-PT on the atomic scale with scanning transmission electron microscopy and made first-principles calculations to determine that the giant piezoelectric properties arise from the enhanced local structural heterogeneity introduced by Sm3+ dopants. Rare-earth doping is thus identified as a general strategy for introducing local structural heterogeneity in order to enhance the piezoelectricity of relaxor ferroelectric crystals.

Ultrahigh energy density harvested from domain-engineered relaxor ferroelectric single crystals under high strain rate loading.

Relaxor ferroelectric single crystals have triggered revolution in electromechanical systems due to their superior piezoelectric properties. Here the results are reported on experimental studies of energy harvested from (1-y-x)Pb(In1/2Nb1/2)O3-(y)Pb(Mg1/3Nb2/3)O3-(x)PbTiO3 (PIN-PMN-PT) crystals under high strain rate loading. Precise control of ferroelectric properties through composition, size and crystallographic orientation of domains made it possible to identify single crystals that release up to three times more electric charge density than that produced by PbZr0.52Ti0.48O3 (PZT 52/48) and PbZr0.95Ti0.05O3 (PZT 95/5) ferroelectric ceramics under identical loading conditions. The obtained results indicate that PIN-PMN-PT crystals became completely depolarized under 3.9 GPa compression. It was found that the energy density generated in the crystals during depolarization in the high voltage mode is four times higher than that for PZT 52/48 and 95/5. The obtained results promise new single crystal applications in ultrahigh-power transducers that are capable of producing hundreds kilovolt pulses and gigawatt-peak power microwave radiation.

Field stability of piezoelectric shear properties in PIN-PMN-PT crystals under large drive field.

The coercive fields (E(C)) of Pb(In0.5Nb0.5)O3-Pb(Mg(¹/3)Nb(²/3)O3-PbTiO3 (PIN-PMN-PT) ternary single crystals were found to be 5 kV/cm, double the value of binary Pb(Mg(¹/3)Nb(²/3)O3-PbTiO3 (PMNT) crystals, further increased to 6 to 9 kV/cm using Mn modifications. In addition to an increased EC, the acceptor modification resulted in the developed internal bias (E(int)), on the order of ~1 kV/cm. The piezoelectric shear properties of unmodified and Mn-modified PIN-PMN-PT crystals with various domain configurations were investigated. The shear piezoelectric coefficients and electromechanical coupling factors for different domain configurations were found to be >2000 pC/N and >0.85, respectively, with slightly reduced properties observed in Mn-modified tetragonal crystals. Fatigue/cycling tests performed on shearmode samples as a function of ac drive field level demonstrated that the allowable ac field levels (the maximum applied ac field before the occurrence of depolarization) were only ~2 kV/cm for unmodified crystals, less than half of their coercive field. Allowable ac drive levels were on the order of 4 to 6 kV/cm for Mn-modified crystals with rhombohedral/orthorhombic phase, further increased to 5 to 8 kV/cm in tetragonal crystals, because of their higher coercive fields. It is of particular interest that the allowable ac drive field level for Mn-modified crystals was found to be ≥ 60% of their coercive fields, because of the developed E(int), induced by the acceptor-oxygen vacancy defect dipoles.

Investigation of single and multidomain Pb(In(0.5)Nb(0.5))O(3)-Pb(Mg(1∕3)Nb(2∕3))O(3)-PbTiO(3) crystals with mm2 symmetry.

The piezoelectric properties of Pb(In(0.5)Nb(0.5))O(3)-Pb(Mg(1∕3)Nb(2∕3))O(3)-PbTiO(3) crystals with various engineered domain configurations were investigated. Rhombohedral and monoclinic∕orthorhombic crystals poled along their crystallographic [011] directions were found to possess macroscopic mm2 symmetry, with "2R" and "1O" domain, respectively. Crystals with the "2R" domain configuration were found to exhibit high extensional piezoelectric coefficients d(33) (∼1300 pC∕N) and d(32) (∼-1680 pC∕N), while crystals with the "1O" configuration possessed high shear coefficients d(15) (∼3500 pC∕N) and d(24) (∼2070 pC∕N), with relatively low extensional piezoelectric coefficients d(33) (∼340 pC∕N) and d(32) (∼-260 pC∕N). The observed results were explained by "polarization rotation" model, as related to their respective domain configurations.

Electromechanical characterization of [Formula: see text] crystals as a function of crystallographic orientation and temperature.

Relaxor based [Formula: see text] ternary single crystals (PIN-PMN-PT) were reported to have broader temperature usage range [Formula: see text] and comparable piezoelectric properties to [Formula: see text] (PMNT) crystals. In this work, the orientation dependent dielectric, piezoelectric and electromechanical properties for PIN-PMN-PT crystals were investigated along [Formula: see text] and [Formula: see text] directions. The electromechanical couplings [Formula: see text] and [Formula: see text] for [Formula: see text] poled crystals were found to be 0.91 and 0.91, respectively, with piezoelectric coefficients [Formula: see text] and [Formula: see text] on the order of 925 and -1420 pC/N. Of particular significance was the mechanical quality factor [Formula: see text] for [Formula: see text] oriented crystals, which was found to be [Formula: see text], much higher than the [Formula: see text] values of [Formula: see text] oriented relaxor-PT crystals [Formula: see text]. The temperature dependence of the piezoelectric properties exhibited good temperature stability up to their ferroelectric phase transition [Formula: see text], indicating [Formula: see text] and [Formula: see text] oriented PIN-PMN-PT are promising materials for transducer applications, with the latter for high power resonant devices where low loss (high [Formula: see text]) was required.

Characterization of Pb(In(12)Nb(12))O(3)-Pb(Mg(13)Nb(23))O(3)-PbTiO(3) ferroelectric crystal with enhanced phase transition temperatures.

The full set of material constants for relaxor-based ternary single crystals Pb(In(12)Nb(12))O(3)-Pb(Mg(13)Nb(23))O(3)-PbTiO(3) (PIN-PMN-PT) were determined and compared to binary Pb(Mg(13)Nb(23))O(3)-PbTiO(3) (PMNT) crystals. The Curie temperature for rhombohedral compositions of PIN-PMN-PT was found to be in the range of 160-200 degrees C with ferroelectric rhombohedral to tetragonal phase transition on the order of 120-130 degrees C, more than 30 degrees C higher than that found for PMNT. The piezoelectric coefficients (d(33)) were in the range of 1100-1500 pCN, with electromechanical coupling factors (k(33)) about 89%-92% comparable to PMNT crystals. The coercive field of the ternary crystal was found to be 5.5 kVcm, double the value of the binary counterparts. The dielectric behavior under varying dc bias exhibited a similar trend as observed in PMNT with a much broader usage temperature range. Together with its enhanced field induced phase transition level, the ternary PIN-PMN-PT crystals are promising candidates for high temperature and high drive transducer applications.