118 research outputs found

    Macroscopic constitutive model for ergodic and non-ergodic lead-free relaxors

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    A fully electromechanically coupled, three dimensional phenomenological constitutive model for relaxor ferroelectric materials was developed for the use in a finite-element-method (FEM) solution procedure. This macroscopic model was used to simulate the macroscopic electromechanical response of lead-free ergodic 0.94Na1/2Bi1/2TiO3−0.06BaTiO3 and non-ergodic 0.90Na1/2Bi1/2TiO3−0.06BaTiO3−0.04K0.5Na0.5NbO3 relaxor materials. The presented constitutive model is capable of accounting for the observed pinched hysteretic response as well as non-deviatoric polarization induced strain and internal order transitions. Time integration of the history dependent internal variables is done with a predictor-corrector integration scheme. The adaptability of the constitutive model regarding the pinching of the hystereses is shown. Simulations are compared to experimental observations

    Tailoring of unipolar strain in lead-free piezoelectrics using the ceramic/ceramic composite approach

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    The electric-field-induced strain response mechanism in a polycrystalline ceramic/ceramic composite of relaxor and ferroelectric materials has been studied using in situ high-energy x-ray diffraction. The addition of ferroelectric phase material in the relaxor matrix has produced a system where a small volume fraction behaves independently of the bulk under an applied electric field. Inter- and intra-grain models of the strain mechanism in the composite material consistent with the diffraction data have been proposed. The results show that such ceramic/ceramic composite microstructure has the potential for tailoring properties of future piezoelectric materials over a wider range than is possible in uniform compositions.open1

    Local structure change evidenced by temperature-dependent elastic measurements: Case study on Bi1/2Na1/2TiO3-based lead-free relaxor piezoceramics

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    The temperature-dependent Young's modulus Y(T) of the lead-free piezoceramics of 0.8Bi(1/2)Na(1/2)TiO(3)-0.2Bi(1/2)K(1/2)TiO(3) (20BKT) and 0.96(0.8Bi(1/2)Na(1/2)TiO(3)-0.2Bi(1/2)K(1/2)TiO(3))-0.04 BiZn1/2Ti1/2O3 (4BZT) is measured with the impulse excitation technique and contrasted with corresponding dielectric and structural data. While the dielectric properties suggest a phase transition, the high resolution XRD patterns remain virtually unchanged from room temperature up to high temperatures, confirming no change in their long-range order. In contrast, the elastic properties indicate a broad and diffuse ferroelastic transition denoted by a minimum in Y(T). By analogy to the elastic and dielectric data of PbZrxTi1-xO3 and PLZT, it is concluded that 20BKT and 4BZT are relaxors with polar nanoregions embedded in a metrically cubic matrix. Interestingly, no indication for the freezing temperature was reflected in any of the employed measurement techniques. From the saturation of Y(T), it is suggested that the Burns temperature may be approximated as 700 degrees C. Moreover, it is found that the modification with the ternary end-member BiZn1/2Ti1/2O3 results in an increase in Young's modulus. A comparison with the Bi1/2Na1/2TiO3-BaTiO3-K0.5Na0.5NbO3 yields the same results.open0

    Stress-modulated relaxor-to-ferroelectric transition in lead-free (Na1/2Bi1/2)TiO3-BaTiO3 ferroelectrics

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    The effect of external mechanical fields on relaxor 0.94 (Na1/2Bi1/2)TiO3−0.06 BaTiO3 was investigated by means of temperature- and stress-dependent dielectric constant measurements between 223 and 673 K. Analogous to previous investigations that showed an electric-field-induced ferroelectric long-range order in relaxor ferroelectrics, we show that compressive stress can also result in the transition to the long-range ferroelectric order, marked by the formation of an anomaly in the permittivity-temperature curves and a nonlinear, remanent change in permittivity during mechanical loading. In situ stress-dependent high-energy x-ray diffraction experiments were performed at room temperature and reveal an apparent phase transition during mechanical loading, consistent with previous macroscopic electrical measurements. The transition lines between the relaxor states and the stress-induced ferroelectric state were determined at constant temperatures with stress-dependent dielectric constant measurements, providing a stress-temperature phase diagram

    Electric-field-induced paraelectric to ferroelectric phase transformation in prototypical polycrystalline BaTiO₃

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    An electric-field-induced paraelectric cubic to ferroelectric tetragonal phase transformation has been directly observed in prototypical polycrystalline BaTiO3 at temperatures above the Curie point (TC) using in situ high-energy synchrotron X-ray diffraction. The transformation persisted to a maximum temperature of 4-°C above TC. The nature of the observed field-induced transformation and the resulting development of domain texture within the induced phase were dependent on the proximity to the transition temperature, corresponding well to previous macroscopic measurements. The transition electric field increased with increasing temperature above TC, while the magnitude of the resultant tetragonal domain texture at the maximum electric field (4-kV mm-1) decreased at higher temperatures. These results provide insights into the phase transformation behavior of a prototypical ferroelectric and have important implications for the development of future large-strain phase-change actuator materials

    Requirements for the transfer of lead-free piezoceramics into application

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    The recent review for the Restriction of Hazardous Substances Directive (RoHS) by the expert committee, appointed by the European Union, stated that the replacement of PZT “… may be scientifically and technologically practical to a certain degree …”, although replacement “… is scientifically and technically still impractical in the majority of applications.” Thus, two decades of sustained research and development may be approaching fruition, at first limited to a minority of applications. Therefore, it is of paramount importance to assess the viability of lead-free piezoceramics over a broad range of application-relevant properties. These are identified and discussed in turn: 1. Cost, 2. Reproducibility, 3. Mechanical and Thermal Properties, 4. Electrical Conductivity, and 5. Lifetime. It is suggested that the worldwide efforts into the development of lead-free piezoceramics now require a broader perspective to bring the work to the next stage of development by supporting implementation into real devices. Guidelines about pertinent research requirements into a wide range of secondary properties, measurement techniques, and salient literature are provided

    Designing properties of (Na1/2Bix) TiO3-based materials through A-site non-stoichiometry

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    Point defects largely determine the properties of functional oxides. So far, limited knowledge exists on the impact of cation vacancies on electroceramics, especially in (Na1/2Bi1/2)TiO3 (NBT)-based materials. Here, we report on the drastic effect of A-site non-stoichiometry on the cation diffusion and functional properties in the representative ferroelectric (Na1/2Bi1/2)TiO3–SrTiO3 (NBT–ST). Experiments on NBT/ST bilayers and NBT–ST with Bi non-stoichiometry reveal that Sr2+-diffusion is enhanced by up to six orders of magnitude along the grain boundaries in Bi-deficient material as compared to Bi-excess material with values of grain boundary diffusion B108 cm2 s 1 and B1013 cm2 s 1 in the bulk. This also means a nine orders of magnitude higher diffusion coefficient compared to reports from other Sr-diffusion coefficients in ceramics. Bi-excess leads to the formation of a material with a core–shell microstructure. This results in 38% higher strain and one order of magnitude lower remanent polarization. In contrast, Bi-deficiency leads to a ceramic with a grain size six times larger than in the Bi-excess material and homogeneous distribution of compounds. Thus, the work sheds light on the rich opportunities that A-site stoichiometry offers to tailor NBT-based materials microstructure, transport properties, and electromechanical properties.T. F., A. A., and K. G. W. gratefully acknowledge financial support by the Deutsche Forschungsgemeinschaft under WE 4972/2 and FR 3718/1-1. T. F. thanks Dr Edvinas Navickas for his help with the ToF-SIMS measurements. M. A. acknowledges the support of the Feodor Lynen Research Fellowship Program of the Alexander von Humboldt Foundation. M. D. and L. M.-L. acknowledge financial support from the Hessen State Ministry of Higher Education, Research and the Arts via LOEWE RESPONSE. L. M.-L. acknowledges financial support from DFG Grant MO 3010/3-1
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