Dezhen Xue

Elastic, piezoelectric, and dielectric properties of Ba(Zr0.2Ti0.8)O3- 50(Ba0.7Ca0.3)TiO3 Pb-free ceramic at the morphotropic phase boundary

There is an urgent demand for high performance Pb-free piezoelectrics to substitute for the current workhorse, the lead zirconate titanate (PZT) family. Recently, a triple point (also tricritical point) type morphotropic phase boundary (MPB) in Pb-free Ba(Zr0.2Ti0.8)O3-x(Ba0.7Ca0.3)TiO3 system has been reported that shows equally as excellent piezoelectricity as soft PZT at room temperature (Liu and Ren6). In the present study, we measured a full set of elastic, piezoelectric, and dielectric properties for the MPB composition, Ba(Zr0.2Ti0.8)O3-50(Ba0.7Ca0.3)TiO3 (BZT-50BCT), by using a resonance method. The resonant method gives piezoelectric properties d33 = 546 pC/N, g33 = 15.3 × 10−3 Vm/N, electromechanical coupling factor k33 = 65%, and the elastic constant s33E = 19.7 × 10−12 m2/N, c33E = 11.3 × 1010 N/m2, which are close to the properties of soft PZT (PZT-5A). Furthermore, the piezoelectric coefficients (k33, d33), the ferroelectric properties (coercive field, remnant polarization), and the elastic ...

Microstructure basis for strong piezoelectricity in Pb-free Ba(Zr0.2Ti0.8)O3-(Ba0.7Ca0.3)TiO3 ceramics

In this letter, we use transmission electron microscopy to study the microstructure feature of recently reported Pb-free piezoceramic Ba(Zr0.2Ti0.8)O3-x(Ba0.7Ca0.3)TiO3 across its piezoelectricity-optimal morphotropic phase boundary (MPB) by varying composition and temperature, respectively. The domain structure evolutions during such processes show that in MPB regime, the domains become miniaturized down to nanometer size with a domain hierarchy, which coincides with the d33-maximum region. Further convergent beam electron diffraction measurement shows that rhombohedral and tetragonal crystal symmetries coexist among the miniaturized domains. Strong piezoelectricity reported in such a system is due to easy polarization rotation between the coexisting nano-scale tetragonal and rhombohedral domains.

Large piezoelectric effect in Pb-free Ba(Ti,Sn)O3-x(Ba,Ca)TiO3 ceramics

We designed a Pb-free pseudo-binary system, Ba(Sn0.12Ti0.88)O3-x(Ba0.7Ca0.3)O3 (BTS-xBCT), characterized by a phase boundary starting from a tricritical triple point of a paraelectric cubic phase, ferroelectric rhombohedral, and tetragonal phases. The optimal composition BTS-30BCT exhibits a high piezoelectric coefficient d33 � 530 pC/N at room temperature. In view of the recent report of high piezoelectricity in another Pb-free system BZT-BCT (Liu and Ren, Phys. Rev. Lett. 103, 257602 (2009)), which possesses a similar tricritical triple point in the phase diagram, it seems that forming a suitable phase boundary starting from a tricritical triple point could be an effective way to develop high-performance Pb-free piezoelectrics. V C 2011 American Institute of Physics.

Triple-point-type morphotropic phase boundary based large piezoelectric Pb-free material—Ba(Ti0.8Hf0.2)O3-(Ba0.7Ca0.3)TiO3

We report a large piezoelectric Pb-free system—Ba(Ti0.8Hf0.2)O3-(Ba0.7Ca0.3)TiO3, designed upon a triple-point morphotropic phase boundary (TMPB) idea. The system shows anomalies of both ac (dielectric and piezoelectric) and dc (P-E hysteresis) properties around TMPB, especially the d33 achieving � 550 pC/N at room temperature. Moreover, the detected non-zero thermal hysteresis around triple point shows a first order transition nature and non-isotropic polarization state, as well as verified by our theoretical Landau-type deduction, thus being considered as an important factor to influence the piezoelectricity along TMPB. Our work may stimulate the study on triple-pointrelated critical phenomena in other ferroic systems. V C 2012 American Institute of Physics.

Accelerated search for materials with targeted properties by adaptive design

Finding new materials with targeted properties has traditionally been guided by intuition, and trial and error. With increasing chemical complexity, the combinatorial possibilities are too large for an Edisonian approach to be practical. Here we show how an adaptive design strategy, tightly coupled with experiments, can accelerate the discovery process by sequentially identifying the next experiments or calculations, to effectively navigate the complex search space. Our strategy uses inference and global optimization to balance the trade-off between exploitation and exploration of the search space. We demonstrate this by finding very low thermal hysteresis (ΔT) NiTi-based shape memory alloys, with Ti50.0Ni46.7Cu0.8Fe2.3Pd0.2 possessing the smallest ΔT (1.84 K). We synthesize and characterize 36 predicted compositions (9 feedback loops) from a potential space of ∼800,000 compositions. Of these, 14 had smaller ΔT than any of the 22 in the original data set.

Phase transitions and the piezoelectricity around morphotropic phase boundary in Ba(Zr0.2Ti0.8)O3-x(Ba0.7Ca0.3)TiO3 lead-free solid solution

In this paper, two displacive phase transitions around the morphotropic phase boundary (MPB) in Ba(Zr0.2Ti0.8)O3-x(Ba0.7Ca0.3)TiO3 (BZT-xBCT) ceramics were detected by inspecting two anomalies of the Raman Ti4+-O2− longitudinal optical mode (∼725 cm−1). Further, permittivity and X-ray diffraction results demonstrated these two phase transitions originate from tetragonal (T) to rhombohedral (R) through an intermediate orthorhombic (O) phase. Importantly, we found that the maximum piezoelectric response (d33 = 545pC/N) was achieved at the boundary between the T and O phase, indicating that the giant piezoelectricity of BZT-xBCT may mainly stem from the T-O phase boundary due to easier polarization rotation and larger lattice softening.

Symmetry determination on Pb-free piezoceramic 0.5Ba(Zr0.2Ti0.8)O3-0.5(Ba0.7Ca0.3)TiO3 using convergent beam electron diffraction method

(1−x)(Ba(Zr0.2Ti0.8)O3-x(Ba0.7Ca0.3)TiO3 (BZT-xBCT) Pb-free piezoceramic has been reported showing ultrahigh piezoelectric performance in its morphotropic phase boundary (MPB) region. However, the crystal structure characteristic for the MPB composition of BZT-xBCT is still under debate—between single orthorhombic phase and tetragonal + rhombohedral two phase mixture. In the present study, we perform the local symmetry determination on the MPB composition x = 0.5 using convergent beam electron diffraction analysis (CBED). Our CBED results from multiple zone axes suggest that there are two coexisting phases with the point group symmetries of 4 mm (tetragonal) and 3 m (rhombohedral) respectively, which agree with two phase mixture model. The strong piezoelectricity can thus be understood by considering the polarization rotation between tetragonal and rhombohedral phases by external field.

High temperature strain glass in Ti50(Pd50−xCrx) alloy and the associated shape memory effect and superelasticity

Strain glass has recently been reported in Ti50−xNi50+x (x≥1.5 at %) alloys and caused by the existence of point defects. This strain glass alloy, being nonmartensitic, exhibits shape memory effect (SME) and superelasticity (SE) around the freezing temperature T0. However, the T0 of Ti50−xNi50+x (x≥1.5 at %) strain glass alloy is very low (∼160 K), thus restricting its potential applications. In the present letter, we report a strain glass system, Ti50(Pd50−xCrx) (x≥9 at %), which has a significantly higher freezing temperature. It is based on a high-temperature martensitic system TiPd (with Ms∼810 K) and dopant Cr (as point defect). For Ti50(Pd40Cr10) strain glass, the freezing transition occurs at T0∼250 K, being close to the room temperature. Correspondingly, it exhibits SME and SE around its high T0. We further clarified that T0 of strain glass alloy is controlled by the martensitic transformation temperature Ms (i.e., martensite stability) of its corresponding host alloy without point defect. Our wor...

Adaptive Strategies for Materials Design using Uncertainties

We compare several adaptive design strategies using a data set of 223 M2AX family of compounds for which the elastic properties [bulk (B), shear (G), and Young’s (E) modulus] have been computed using density functional theory. The design strategies are decomposed into an iterative loop with two main steps: machine learning is used to train a regressor that predicts elastic properties in terms of elementary orbital radii of the individual components of the materials; and a selector uses these predictions and their uncertainties to choose the next material to investigate. The ultimate goal is to obtain a material with desired elastic properties in as few iterations as possible. We examine how the choice of data set size, regressor and selector impact the design. We find that selectors that use information about the prediction uncertainty outperform those that don’t. Our work is a step in illustrating how adaptive design tools can guide the search for new materials with desired properties.

Microstructure at morphotropic phase boundary in Pb(Mg1/3Nb2/3)O3-PbTiO3 ceramic: Coexistence of nano-scaled {110}-type rhombohedral twin and {110}-type tetragonal twin

For more than half a century, the morphotropic phase boundary (MPB) has drawn constant interest in developing piezoelectric materials, as the phase instability at the region significantly enhances piezoelectricity. However, the local structure/symmetry at the MPB region is still under controversy. The investigation on morphology and origin of the local structure at MPB is of considerable importance to provide a microstructure basis for high piezoelectricity. In the present study, we thus use high resolution transmission electron microscopy to investigate the microstructure feature of MPB at PMN-PT ceramics. The local structure is shown to be the coexistence of nano-scaled {110}-type rhombohedral (R) twin and {110}-type tetragonal (T) twin. Such nano-scaled coexistence can be due to a nearly vanishing polarization anisotropy and low domain wall energy at MPB, which thus facilitates polarization rotation between 〈001〉T and 〈111〉R states and leads to high properties of MPB compositions.