Increasing Performances of 1-3 Piezocomposite Ultrasonic Transducer by Alternating Current Poling Method.

Ultrasonic transducers are the basic core component of diagnostic imaging devices, wherein the piezoelectric materials are the active element of transducers. Recent studies showed that the alternating current poling (ACP) method could develop the properties of piezocomposites, which had great potential to improve transducer performance. Herein, transducers (fc = 3 MHz) made of DCP and ACP 1-3 piezocomposites (prepared by PZT-5H ceramics and PMN-PT single crystals) were fabricated. The effect of the ACP method on the bandwidth and insertion loss (sensitivity) was explored. The results indicate that the ACP method can significantly enhance the bandwidth and slightly increase the insertion loss of transducers. Particularly, a superhigh bandwidth of 142.8% was achieved in the transducer of ACP 1-3 PMN-PT single crystal combined with suitable matching and backing layers. This bandwidth is higher than that of all reported transducers with similar center frequency. Moreover, the optimization mechanism of transducer performance by the ACP method was discussed. The obtained results suggested that the ACP is an effective and convenient technology to improve transducer performances, especially for the bandwidth.

Enhancement of Ultrasonic Transducer Bandwidth by Acoustic Impedance Gradient Matching Layer.

High-performance broadband ultrasound transducers provide superior imaging quality in biomedical ultrasound imaging. However, a matching design that perfectly transmits the acoustic energy between the active piezoelectric element and the target medium over the operating spectrum is still lacking. In this work, an anisotropic gradient acoustic impedance composite material as the matching layer of an ultrasonic transducer was designed and fabricated; it is a non-uniform material with the continuous decline of acoustic impedance along the direction of ultrasonic propagation in a sub-wavelength range. This material provides a broadband window for ultrasonic propagation in a wide frequency range and achieves almost perfect sound energy transfer efficiency from the piezoelectric material to the target medium. Nano tungsten particles and epoxy resin were selected as filling and basic materials, respectively. Along the direction of ultrasonic propagation, the proportion of tungsten powder was carefully controlled to decrease gradually, following the natural exponential form in a very narrow thickness range. Using this new material as a matching layer with high-performance single crystals, the -6 dB bandwidth of the PMN-PT ultrasonic transducer could reach over 170%, and the insertion loss was only -20.3 dB. The transducer achieved a temporal signal close to a single wavelength, thus there is the potential to dramatically improve the resolution and imaging quality of the biomedical ultrasound imaging system.

Phase-field simulation on the interaction of oxygen vacancies with charged and neutral domain walls in hexagonal YMnO3.

A three-dimensional model of the interaction between the charged or neutral domain walls and oxygen vacancies in the hexagonal manganite YMnO3was proposed, and simulated using Landau-Ginzburg-Devonshire (LGD) theory, dynamic diffusion equation and Maxwell's equation. The calculation proves that stiffness anisotropic factors can adjust the domain wall state and ultimately affect the distribution of oxygen vacancies. The head-to-head domain wall corresponds to low oxygen vacancy density, and the tail-to-tail domain wall corresponds to high oxygen vacancy density. The electrostatic field generated by the bound charge is the key factor leading to the change of oxygen vacancy distribution. Finally,e-index lawNd=aeb*dP/dzcan fit the relationship between the oxygen vacancy concentration and the polarization gradient alongzdirection. Our theory provides a new way to modulate the distribution of oxygen vacancies through domain wall morphology in hexagonal YMnO3.

Grain-Oriented Ferroelectric Ceramics with Single-Crystal-like Piezoelectric Properties and Low Texture Temperature.

High-performance piezoelectrics are pivotal to various electronic applications including multilayer actuators, sensors, and energy harvesters. Despite the presence of high Lotgering factor F001, two key limitations to today's relaxor-PbTiO3 textured ceramics are low piezoelectric properties relative to single crystals and high texture temperature. In this work, Pb(Yb1/2Nb1/2)O3-Pb(Mg1/3Nb2/3)O3-PbTiO3 (PYN-PMN-PT) textured ceramics with F001 ∼ 99% were synthesized at only 975 °C through liquid-phase-assisted templated grain growth, where of particular significance is that single-crystal properties, i.e., very large electrostrain Smax/Emax ∼ 1830 pm V-1, giant piezoelectric figure of merit d33 × g33 ∼ 61.3 × 10-12 m2 N-1, high electromechanical coupling k33 ∼ 0.90, and Curie temperature Tc ∼ 205 °C, were simultaneously achieved. Especially, the Smax/Emax and d33 × g33 values correspond to ∼180% enhancement as compared to the regularly 1200 °C-textured ceramics with F001 ∼ 96%, representing the highest values ever reported on piezoceramics. Phase-field simulation revealed that grain misorientation has a stronger influence on piezoelectricity than texture fraction. The ultrahigh piezoelectric response achieved here is mainly attributed to effective control of grain orientation features and domain miniaturization. This work provides important guidelines for developing novel ceramics with significantly enhanced functional properties and low synthesis temperature in the future and can also greatly expand application fields of piezoceramics to high-performance, miniaturized electronic devices with multilayer structures.

Enhanced Piezoelectric Effect Derived from Grain Boundary in MoS2 Monolayers.

Recent discovery of piezoelectricity that existed in two-dimensional (2D) layered materials represents a key milestone for flexible electronics and miniaturized and wearable devices. However, so far the reported piezoelectricity in these 2D layered materials is too weak to be used for any practical applications. In this work, we discovered that grain boundaries (GBs) in monolayer MoS2 can significantly enhance its piezoelectric property. The output power of piezoelectric devices made of the butterfly-shaped monolayer MoS2 was improved about 50% by the GB-induced piezoelectric effect. The enhanced piezoelectricity is attributed to the additional piezoelectric effect induced by the existence of deformable GBs which can promote polarization and generates spontaneous polarization with different piezoelectric coefficients along various directions. We further made a flexible piezoelectric device based on the 2D MoS2 with the GBs and demonstrated its potential application in self-powered precision sensors for in situ detecting pressure changes in human blood for health monitoring.

Significantly Enhanced Energy-Harvesting Performance and Superior Fatigue-Resistant Behavior in [001]c-Textured BaTiO3-Based Lead-Free Piezoceramics.

Energy-harvesting utilizing piezoelectric materials has recently attracted extensive attention due to the strong demand of self-powered electronics. Unfortunately, low power density and poor long-term stability seriously hinder the implementation of lead-free piezoelectrics as high-efficiency energy harvesters. For the first time, we demonstrate that tailoring grain orientations of lead-free ceramics via templated grain growth can effectively produce ultrahigh power generation performance and excellent endurance against electrical/mechanical fatigues. Significantly improved fatigue resistance was observed in (Ba0.94Ca0.06)(Ti0.95Zr0.05)O3 grain-oriented piezoceramics (with ∼99% [001]c texture) up to 106 bipolar cycles, attributed to the enhanced domain mobility, less defect accumulation, and thus suppressed crack generation/propagation. Interestingly, the novel energy harvesters, which were developed based on the textured ceramics with high electromechanical properties, possessed ∼9.8 times enhancement in output power density compared to the nontextured counterpart while maintaining stable output features up to 106 vibration cycles. The power densities, which increased from 6.4 to 93.6 µW/mm3 with increasing acceleration excitation from 10 to 50 m/s2, are much higher than those reported previously on lead-free energy harvesters. This work represents a significant advancement in piezoelectric energy-harvesting field and can provide guidelines for future efforts in this direction.

Temporal and spatial variations in sand and dust storm events in East Asia from 2007 to 2016: Relationships with surface conditions and climate change.

We analyzed the frequency and intensity of sand and dust storms (SDSs) in East Asia from 2007 to 2016 using observational data from ground stations, numerical modeling, and vegetation indices obtained from both satellite and reanalysis data. The relationships of SDSs with surface conditions and the synoptic circulation pattern were also analyzed. The statistical analyses demonstrated that the number and intensity of SDS events recorded in spring during 2007 to 2016 showed a decreasing trend. The total number of spring SDSs decreased from at least ten events per year before 2011 to less than ten events per year after 2011. The overall average annual variation of the surface dust concentration in the main dust source regions decreased 33.24µg/m3 (-1.75%) annually. The variation in the temperatures near and below the ground surface and the amount of precipitation and soil moisture all favored an improvement in vegetation coverage, which reduced the intensity and frequency of SDSs. The strong winds accompanying the influx of cold air from high latitudes showed a decreasing trend, leading to a decrease in the number of SDSs and playing a key role in the decadal decrease of SDSs. The decrease in the intensity of the polar vortex during study period was closely related to the decrease in the intensity and frequency of SDSs.

Influence of phase transitions on green fluorescence intensity ratio in Er3+ doped K0.5Na0.5NbO3 ceramic.

The fluorescence intensity ratio (FIR) method is a non-contact temperature (T) measurement technique based on thermally coupled levels of rare earth ions in a doped host. Green fluorescence originating from 2H11/2 and 4S3/2 states of Er3+ doped K0.5Na0.5NbO3 (KNN) ceramic are studied in the temperature range of 300 K to 720 K. The fluorescence intensities change dramatically around phase transition points where the crystal symmetry changes, inducing deviation of the FIR from Boltzmann's law. The temperature determined by the FIR method deviates from thermocouple measurements by 7 K at the orthorhombic to tetragonal phase transition (TO-T) point and 13 K at the Curie point (TC). This finding gives guidance for developing fluorescent T sensors with ferroelectrics and may also provide a fluorescent method to detect phase transitions in ferroelectric materials.

Optimization of electrooptic and pieozoelectric coupling effects in tetragonal relaxor-PT ferroelectric single crystals.

The electrooptic and piezoelectric coupling effects in tetragonal relaxor-based ferroelectric 0.62Pb(Mg1/3Nb2/3)O3-0.38PbTiO3 (PMN-0.38PT) and 0.88Pb(Zn1/3Nb2/3)O3-0.12PbTiO3 (PZN-0.12PT) single-domain crystals have been analyzed by the coordinate transformation. The orientation dependence of the electrooptic and half-wave voltage was calculated based on the full sets of refractive indices, electrooptic and piezoelectric coefficients. The optimum orientation cuts for achieving the best electrooptic coefficient and half-wave voltage were found. The lowset half-wave voltage is only 76 V for the PMN-0.38PT single-domain crystal. Compared to commonly used electrooptic crystal LiNbO3, tetragonal relaxor-PT ferroelectric single-domain crystals are much superior for optical modulation applications because of their much higher linear electrooptic coefficients and substantially lower half-wave voltages when the piezoelectric strain influence is considered.

Electromechanical properties of orthorhombic 0.24Pb(In1/2Nb1/2)O3-0.43Pb(Mg1/3Nb2/3)O3-0.33PbTiO3 single-domain crystal.

Single-domain structure with orthorhombic symmetry has been achieved in morphotropic phase boundary composition 0.24Pb(In1/2Nb1/2)O3 -0.43Pb(Mg1/3Nb2/3)O3-0.33PbTiO3 ternary single crystal by applying a large field along the pseudo-cubic direction [011]c. Complete set of elastic, piezoelectric, and dielectric constants has been determined with self-consistency. This crystal shows very large thickness shear piezoelectric coefficient d15=4324 pC/N and extremely high shear electromechanical coupling factor k15=96%. Three-dimensional orientation dependence of the longitudinal piezoelectric constant d33 was calculated and compared with experimental values, which revealed nearly 20% extrinsic contributions in domain engineered [001]c and [111]c poled conditions.

Relaxor-based ferroelectric single crystals: growth, domain engineering, characterization and applications.

In the past decade, domain engineered relaxor-PT ferroelectric single crystals, including (1-x)Pb(Mg1/3Nb2/3)O3-xPbTiO3 (PMN-PT), (1-x)Pb(Zn1/3Nb2/3)O3-xPbTiO3 (PZN-PT) and (1-x-y)Pb(In1/2Nb1/2)O3-yPb(Mg1/3Nb2/3)O3-xPbTiO3 (PIN-PMN-PT), with compositions near the morphotropic phase boundary (MPB) have triggered a revolution in electromechanical devices owing to their giant piezoelectric properties and ultra-high electromechanical coupling factors. Compared to traditional PbZr1-x Ti x O3 (PZT) ceramics, the piezoelectric coefficient d33 is increased by a factor of 5 and the electromechanical coupling factor k33 is increased from < 70% to > 90%. Many emerging rich physical phenomena, such as charged domain walls, multi-phase coexistence, domain pattern symmetries, etc., have posed challenging fundamental questions for scientists. The superior electromechanical properties of these domain engineered single crystals have prompted the design of a new generation electromechanical devices, including sensors, transducers, actuators and other electromechanical devices, with greatly improved performance. It took less than 7 years from the discovery of larger size PMN-PT single crystals to the commercial production of the high-end ultrasonic imaging probe "PureWave". The speed of development is unprecedented, and the research collaboration between academia and industrial engineers on this topic is truly intriguing. It is also exciting to see that these relaxor-PT single crystals are being used to replace traditional PZT piezoceramics in many new fields outside of medical imaging. The new ternary PIN-PMN-PT single crystals, particularly the ones with Mn-doping, have laid a solid foundation for innovations in high power acoustic projectors and ultrasonic motors, hinting another revolution in underwater SONARs and miniature actuation devices. This article intends to provide a comprehensive review on the development of relaxor-PT single crystals, spanning material discovery, crystal growth techniques, domain engineering concept, and full-matrix property characterization all the way to device innovations. It outlines a truly encouraging story in materials science in the modern era. All key references are provided and 30 complete sets of material parameters for different types of relaxor-PT single crystals are listed in the Appendix. It is the intension of this review article to serve as a resource for those who are interested in basic research and practical applications of these relaxor-PT single crystals. In addition, possible mechanisms of giant piezoelectric properties in these domain-engineered relaxor-PT systems will be discussed based on contributions from polarization rotation and charged domain walls.

Linear electro-optic properties of relaxor-based ferroelectric 0.24Pb(In1/2Nb1/2)O3-(0.76 - x)Pb(Mg1/3Nb2/3)O3-xPbTiO3 single crystals.

Linear electro-optic properties of 0.24Pb(In1/2Nb1/2)O3-(0.76 - x)Pb(Mg1/3Nb2/3)O3-xPbTiO3 single crystals, with compositions in the rhombohedral, morphotropic phase boundary (MPB) and tetragonal phases, have been investigated. Very large effective electro-optic coefficient [Formula: see text] (204 pm/V) was observed in a crystal with the MPB composition when it is poled along [001]. The rhombohedral phase (x = 0.27 and 0.30) single crystals poled along [111] direction and tetragonal phase (x = 0.39) single crystal poled along [001] direction are in single domain, and their electro-optic coefficients ([Formula: see text] = 76, 94, and 43 pm/V for the crystals with x = 0.27, 0.30, and 0.39, respectively) were found to be much higher than that of traditional electro-optic single crystal LiNbO3 ([Formula: see text] = 19.9 pm/V). The electro-optic coefficients of the single crystal in the rhombohedral phase have excellent temperature stability in the experimental temperature range of 10-40 °C. The half-wave voltage [Formula: see text] was calculated to be much lower (less than 1000 V) than that of LiNbO3 single crystal (2800 V). These superior properties make the ternary relaxor-PT single crystals very promising for electro-optic modulation applications.

Influence of manganese doping to the full tensor properties of 0.24Pb(In1/2Nb1/2)O3-0.47Pb(Mg1/3Nb2/3)O3-0.29PbTiO3 single crystals.

Complete sets of elastic, piezoelectric, dielectric, and electromechanical properties of [001]c and [011]c poled pure and 0.5 wt. % manganese-doped 0.24Pb(In1/2Nb1/2)O3-0.47Pb(Mg1/3Nb2/3)O3-0.29PbTiO3 single crystals have been characterized at room temperature. The results indicate that manganese ion substitution in the B-site of perovskite 0.24PIN-0.47PMN-0.29PT single crystals makes the material harder with much higher mechanical quality factor Qm and slight decrease in piezoelectric and dielectric constants. The much improved Qm value (200-900) makes Mn-doped single crystals more suitable for high-power transducer applications than pure single crystals.

Complete matrix properties of [001](c) and [011](c) poled 0.33Pb(In(1/2)Nb(1/2))O(3)-0.38Pb(Mg(1/3)Nb(2/3))O(3)-0.29PbTiO(3) single crystals.

The elastic, piezoelectric, and dielectric properties of [001](c) and [011](c) poled 0.33Pb(In(1/2)Nb(1/2))O(3)-0.38Pb(Mg(1/3)Nb(2/3))O(3)-0.29PbTiO(3) single crystals have been fully characterized at room temperature, and the temperature and frequency dependence of the dielectric susceptibility ε(33) were also measured. The depoling temperature of this crystal is more than 20 °C higher than that of the corresponding binary 0.71Pb(Mg(1/3)Nb(2/3))O(3)-0.29PbTiO(3) system. From the measured P-E hysteresis loops, the coercive fields along [001](c) and [011](c) directions have been determined to be 6.0 kV/cm and 6.6 kV/cm, respectively, which indicate that these domain engineered ternary relaxor-based ferroelectric single crystals are excellent candidates for high-power applications.

Polarized Raman study on phase transitions in 0.24Pb(In1/2Nb1/2)O3-0.43Pb(Mg1/3Nb2/3)O3-0.33PbTiO3 single crystal.

Polarized Raman spectroscopy was performed to investigate the local lattice structure and phase transitions of unpoled 0.24Pb(In1/2Nb1/2)O3-0.43Pb(Mg1/3Nb2/3)O3-0.33PbTiO3 (0.24PIN-0.43PMN-0.33PT) single crystal in the temperature range from 30 °C to 260 °C. MA- and MC-type monoclinic phases were detected by micro-Raman spectra measured in different micro areas. Temperature dependence of Raman intensities, frequency shifts, mode merge and intensity ratios in the VV and VH geometries were investigated. Our results indicated that the monoclinic-tetragonal (M-T) phase transition of the ternary relaxorbased ferroelectric single crystal 0.24PIN-0.43PMN-0.33PT occurs at 85 °C, which is verified by the mode merging from 520 cm-1 and 580 cm-1 to 500 cm-1, and the tetragonal-cubic (T-C) phase transition happens at 200 °C based on the vanishing mode at 780 cm-1 measured in the VH polarization.

Optical interband transitions in [111] poled relaxor-based ferroelectric 0.24Pb(In1/2Nb1/2)O3-(0.76 - x)Pb(Mg1/3Nb2/3)O3-xPbTiO3 single crystal.

Optical transmission spectra of single crystal 0.24Pb(In1/2Nb1/2)O3-(0.76 - x)Pb(Mg1/3Nb2/3)O3-xPbTiO3 (x = 0.27, 0.33) were measured in the pseudo-cubic crystallographic directions [111] and [112̄]. Ferroelectric domain structures were observed in order to explain the difference of transmittance for the two composition crystals. Wavelength dependence of the absorption coefficients was measured and the optical energy band gaps were calculated for both direct and indirect transitions, which are Egd = 3.09-3.18 eV and Egi = 2.89-2.96 eV, respectively, and the phonon energy is Ep = 0.07-0.08 eV. The transmission spectra were explained by the refractive indices and extinction coefficients measured by spectroscopic ellipsometry.

Temperature dependence of electric-field-induced domain switching in 0.7Pb(Mg1/3Nb2/3)O3-0.3PbTiO3 single crystal.

The influence of temperature on electric-field-induced domain switching of [0 0 1]c oriented 0.7Pb(Mg1/3Nb2/3)O3-0.3PbTiO3 (PMN-0.3PT) single crystal has been studied. The piezoelectric properties of PMN-0.3PT single crystal change drastically at one critical field at 30 °C and two critical fields at 90 °C corresponding to electric-field-induced domain switching. The domain structures were studied by polarizing light microscopy on the [100]c surface under the electric field applied along [001]c direction. The PMN-0.3PT single crystal exhibits a rapid increase in piezoresponse at 100 V/mm, which is related to R-MA phase transformation. At 90°C, the M and T0 0 1 phases coexist at 100 V/mm, while T001 mono-domain appears at 300 V/mm. The domain switching process here can be identified as (T100 or T010) → M → T001. The experimental results show that the phase state and domain structures of the crystal are closely related to the piezoelectric behaviors.

Frequency dispersion of longitudinal ultrasonic velocity and attenuation in [001]c-poled 0.24Pb(In1/2Nb1/2O3- 0.45Pb(Mg1/3Nb2/3)O3-0.31PbTiO3 single crystal.

The frequency dispersion of ultrasonic velocity and attenuation in [001](c)-poled 0.24Pb(in(1/2)Nb(1/2))O(3)-0.45Pb(Mg(1/3)Nb(2/3))o(3)-0.31PbTio(3) (PIN-0.45PMN-0.31PT) ternary single crystal were measured by ultrasonic spectroscopy from 25 to 100 MHz for the longitudinal wave. It was found that the velocity has a linear relationship with the frequency f, but the attenuation has a quadratic relation with f. The attenuation and frequency dispersion of the ternary system are lower than that of the (1-x)Pb(Mg(1/3)Nb(2/3))O(3)-xPbTiO(3) (PMN-PT) binary system and the coercive field also increased by a factor of 2.5, hence, the ternary single system is superior to the corresponding binary single-crystal system for high-frequency and high-power transducer applications.

Complete set of material properties of single domain 0.24Pb(In(1∕2)Nb(1∕2))O(3)-0.49Pb(Mg(1∕3)Nb(2∕3))O(3)-0.27PbTiO(3) single crystal and the orientation effects.

Multidomain relaxor-based single crystals have intrigued the enthusiasm of many researchers due to their superior electromechanical properties. In order to understand the physical origin of multidomain properties, one must know the complete set of material coefficients in single domain state. Previous published single domain data were all measured under bias because single domain state is unstable. Here, we report a set of single domain data without bias for rhombohedral 0.24Pb(In(1∕2)Nb(1∕2))O(3)-0.49Pb(Mg(1∕3)Nb(2∕3))O(3)-0.27PbTiO(3) single crystal. Comparing rotated coefficients from single domain data with measured multidomain material coefficients, we concluded that the orientation effects account for more than 90% of the observed multidomain properties.

Complete set of material properties of [011](c) poled 0.24Pb(In(1/2)Nb(1/2))O(3)-0.46Pb(Mg(1/3)Nb(2/3))O(3)-0.30PbTiO(3) single crystal.

A complete set of elastic, piezoelectric, and dielectric constants of [011](c) poled multidomain 0.24Pb(In(1/2)Nb(1/2))O(3)-0.46Pb(Mg(1/3)Nb(2/3))O(3)-0.30PbTiO(3) ternary single crystal has been determined using resonance and ultrasonic methods and the temperature dependence of the dielectric permittivity has been measured at 3 different frequencies. The experimental results revealed that this [011](c) poled ternary single crystal has very large transverse piezoelectric coefficient d(32) = -1693 pC/N, transverse dielectric constant ε(11)/ε(0) ~ 7400 and a high electromechanical coupling factor k(32) ~ 90%. In addition, its coercive field is 2 times of that of the corresponding binary 0.7Pb(Mg(1/3)Nb(2/3))O(3)-0.30PbTiO(3) single system with much better temperature stability. Therefore, the crystal is an excellent candidate for transverse mode electromechanical devices.