Journal

J. Am. Ceram. Soc., 90 [8] 2297–2314 (2007) DOI: 10.1111/j.1551-2916.2007.01820.x r 2007 The American Ceramic Society

Texture and Anisotropy of Polycrystalline Piezoelectrics
Jacob L. Jones
Materials Science and Engineering, University of Florida, Gainesville, Florida 32611

Benjamin J. Iverson and Keith J. Bowmanw
Materials Engineering, Purdue University, West Lafayette, Indiana 47907

Piezoelectricity is manifested in ferroelectric ceramics by inducing a preferred volume fraction of one ferroelectric domain variant orientation at the expense of degenerate orientations. The piezoelectric effect is therefore largely controlled by the effectiveness of the electrical poling in producing a bias in ferroelectric (1801) and ferroelastic (non-1801) domain orientations. Further enhancement of the piezoelectric effect in bulk ceramics can be accomplished by inducing preferred orientation through grain-orientation processes such as hot forging or tape casting that precede the electrical-poling process. Coupled crystal orientation and domain orientation processing yields ceramics with an even greater piezoelectric response. In this paper, preferred orientations of domains and grains in polycrystalline piezoelectric ceramics generated through both domain- and grain-orientation processing are characterized through pole figures and orientation distribution functions obtained using data from a variety of diffraction techniques. The processing methods used to produce these materials and the methods used to evaluate preferred orientation and texture are described and discussed in the context of prior research. Different sample and crystal symmetries are explored across a range of commercial and laboratory-prepared materials. Some of the variables presented in this work include the effects of in situ thermal depoling and the detailed processing parameters used in tape casting of materials with preferred crystallite orientations. Preferred orientation is also correlated with anisotropic properties, demonstrating a clear influence of both grain and domain orientations on piezoelectricity.

I. Introduction
MATERIAL with a crystallographic texture is best described as a polycrystal with a nonrandom distribution of crystal orientations or a preferred crystallographic orientation. This is unique from a polycrystal with a morphological texture, or preferred grain shape orientation, although they are frequently correlated. Because most crystalline properties are a function of crystallographic direction (anisotropic), the distribution of crystals and the intrinsic crystalline anisotropy is coupled to the macroscopic anisotropy of textured polycrystalline materials. This is illustrated in Fig. 1. Fundamental to these texture–anisotropy relationships is the requirement of a quantitative description of the orientation of crystals. Preferred orientation is most completely described by an orientation distribution function (ODF), which gives the relative presence of each possible crystal orientation relative to that in a random distribution of orientations. Panel A describes this further. Researchers in the metallurgy and geology communities produced the first publications on crystallographic textures tied to directional deformation in the first half of the 20th century.5,6 The Laue diffraction experiments by Wever5 tied forming to the subsequent concentration of orientations in polycrystal aluminum and iron through the first use of X-rays to describe the development of preferred orientations. Because these first examples of crystallographic texture arose from large-scale plasticity in ductile metals, quantitative measures of texture development in polycrystalline ceramics were at first limited and tied to textures arising from green body processing of materials with nonequiaxed particles (e.g., Pentecost and Wright7 and Bowman8) until hot working of ceramics was used to evaluate the orientation effects on the optical properties of aluminum oxide9,10 and the potential for improved performance in structural applications.11 The motivation in most engineering applications for inducing crystallographic texture is the desire to optimize a particular property, its anisotropy, or both.1 Crystallographic texture may be correlated or uncorrelated with the directional morphology of crystals or defects that may otherwise result from the directionality of processing. In the last two decades, research on crystallographic texture in ceramics related to high-temperature forming operations has been broadened to include a wide range of processes for introducing texture, including templating

A

D. Green—contributing editor

Manuscript No. 22750. Received January 30, 2007; approved April 17, 2007. This research was supported by the U.S. National Science Foundation under award numbers DMR-0224991 and OISE-0402066 and the Indiana 21st Century Research and Technology Fund No. 092200-0076. This work has benefited from the use of the Los Alamos Neutron Science Center at the Los Alamos National Laboratory, funded by the U.S. Department of Energy under Contract W-7405-ENG-36 and the NSLS at Brookhaven National Laboratory, supported by the U.S. Department of Energy, Division of Materials Sciences and Division of Chemical Sciences, under Contract No. DE-AC02-98CH10886. w Author to whom correspondence should be addressed. e-mail: kbowman@ecn. purdue.edu

Feature

of preferred orientation. . (1). and property evaluations. and j2. after Bunge and Schwarzer. j1. j2). j1. most of these processes take advantage of the intrinsic surface energy anisotropy of the crystal structure to synthesize textured materials. 8 Fig. of all orientations j1. wherein the first angle. our recent research has shown that the behavior of domains inherent to most ceramic piezoelectrics couples with crystallographic texture and concurrent changes in other property tensors. is a tilting of the crystallite z-axis from the specimen Z-axis about the crystallite x-axis. we describe the context and characteristics of these coupled textures and show new examples of how this coupling can be explored through tailored processing. The third angle.18 shape-memory properties. and j2. Other attributes of anisotropy have also been explored that can occur within the crystals of a polycrystalline material. 1.21 Without an external mechanical or electrical field biasing the formation of these domain orientations. which. f. (b) macro-anisotropy of the material Vol. F. is a rotation about the new specimen z-axis. The noncubic materials that exhibit piezoelectricity typically have a domain structure that is inherited during a phase transformation from a higher temperature phase of a higher symmetry. A1. thermoelectricity. in effect. Pole figures are usually plotted on an equal area projection. Angles describing a coordinate transformation. f(j1. conductivity. three angles are required to transform the specimen coordinate axis to the grain coordinate axis or vice versa. In other words. The second angle. In this paper. two definitions are required: (1) a description of the individual crystallite orientation relative to the specimen coordinate axes and (2) a measure of the frequency at which a particular orientation is preferred relative to that in a random distribution of crystallites. from Bowman. A1. while inverse pole figures are typically plotted on a stereographic projection. Influence of micro-anisotropy of the crystals on the macroanisotropy of the material. Until a macroscopic electric dipole is formed. a piezoelectric material will not demonstrate piezoelectricity. fracture toughness.17 magnetic properties. For example. For the former. The ODF is difficult to represent linearly in two dimensions and pole figures or inverse pole figures are typically sufficient for describing textures in real materials.96 processes for bulk. The three-dimensional (3D) ODF. is a rotation about the specimen Z-axis. This value can also be described as the density. We adopt here the Bunge notation.12 and thin-film materials.97 For a definition of frequency.12. Piezoelectricity in polycrystalline ceramics depends on the orientation achieved from poling of non-centrosymmetric materials that are also ferroelectric.2298 (a) micro-anisotropy of the crystals Journal of the American Ceramic Society—Jones et al.19 and piezoelectricity. a crystallite orientation that is twice as probable in a textured material as in a randomly oriented material is described as having a density of 2 mrd. rigorous quantitative texture assessments. F. or amplitude. Phase transformations within crystals or the development of biased domains or twins have recognized contributions to anisotropy in noncubic ceramics. Many reference texts have been written on texture and the ODF1–4 and the description provided in this panel is intended only to be a brief introduction. On cooling through the temperature at which the phase transformation occurs (Curie temperature).20 In this last category. Pole figures and inverse pole figures are integrations of the ODF in two dimensions and represent either the densities of a single crystallographic direction in sample orientation directions (pole figure) or the densities of all crystallographic directions in a single sample direction (inverse pole figure).13 Incidentally. the degree of preferred orientation can be described as a multiple of a random distribution (mrd). F. No. therefore consists of the densities. (2). F. optical properties. the breaking of symmetry results in a multiplicity of orientations consistent with the change in symmetry. To describe the probability of certain crystallite orientations in a polycrystalline material quantitatively. is used to generate anisotropy in macroscopic properties. Fig. strength.2 These angles are illustrated in Fig. it is expected that they will form with nearly equal fractions within each crystal. j2. The orientation variants can Panel A: The Orientation Distribution Function The ODF is a means of describing the probability of every possible crystal orientation relative to the probability in a randomly oriented material.14–16 superconductivity. There are various definitions of these three angles based on the sequence of rotations. These efforts have resulted in an ever increasing range of anisotropic proper- ties including elasticity. 90. the density of each crystallite orientation is described relative to its density in a randomly oriented ceramic.

The software package MAUD41. atomic coordinates. the property changes resulting from domain textures can be modulated with only slight changes in defect content. Gold electrodes were sputtered onto two opposing sides. recrystallization. a sample of the same composition and from the same manufacturing lot as those used for the diffraction measurements was received from the manufacturer in the shape of a disk of 10-mm diameter and 1-mm thickness. 2. The sample dimension through which the electric field was applied was measured before and after poling. Indianapolis.45. Sections III and IV are devoted to describing property and texture measurements in ceramics with an initial texture in the unpoled state. Fig. For the strain and polarization hysteresis measurements. Because the domain textures and the resulting properties are coupled to the initial grain orientation. grain size. The d33 was measured on a Berlincourt d33 meter (APC International. 2. E. In Section V. resulting from the application of an electric field. lattice constants and texture were refined. y 6). After electrical poling through the application of electric field.August 2007 (a) (b) Texture and Anisotropy of Polycrystalline Piezoelectrics 2299 E E tallographic texture.12. and electric fields in the system. Mackeyville. a fourth-order SH was determined to be sufficient for describing the small degrees of preferred orientation and wide distributions in non-1801 domain textures. . piezoelectric ceramics can demonstrate the piezoelectric effect. fiber symmetry was enforced about the maximum of the 002 peak. and grain boundary chemistry. and elastic anisotropy become very complex once a polarization has been introduced. orientation is conventionally induced by applying an electric field to an initially untextured ceramic at temperatures near the Curie temperature to increase the size of domains aligned with the applied electric field. Our limited understanding of how domain walls move and overcome obstacles to their motion has not changed significantly despite their wide range of applications. termed poling. The poling process provides a method for tuning the domain orientation distribution to optimize the coefficients of dij. corresponding to the so-called 1801 and non-1801 domains. grain boundary structure. dij is the piezoelectric modulus. other texture– anisotropy relationships are explored with a focus on polarization in materials exhibiting monoclinicity.20.5–1. and sj is the applied stress (i 5 1. Details of the dielectric properties. This process. Texture was modeled using a fourth-order SH (Panel B). grain shape. The remainder of the paper is divided as follows: Section II describes the evolution of domain structure and piezoelectric properties through the poling and thermal depoling process in initially randomly oriented lead zirconate titanate (PZT) ceramics. Figure 2(a) illustrates the reorientation of non-1801 domains.3 mHz triangular waveform. certain domain orientations increase in directions relative to the electric field. in turn producing piezoelectric stresses. particularly at the morphotropic phase boundary where both a monoclinic structure and nanodomains of a high-symmetry phase are argued to exist. followed by refinement of individual spectra intensities and polynomial background coefficients. With piezoelectric ceramics. the orientation process and properties can be reversible. Section VI summarizes the results of the preceding sections. and 3. IN) were obtained from the supplier in dimensions of 1 cm  1 cm  1 cm. whose direct effect is described by the linear relation Di ¼ dij sj (1) where Di is the electric displacement. This direction corresponds to the axis of the electric field during poling. Initially Randomly Oriented PZT Ceramics PZT materials remain widely used despite reservations over their lead content. Ltd. This section demonstrates that the degree of domain texture established in conventional poling processes is constrained by microstructural aspects of these materials and can be quantitatively correlated with the measurable macroscopic properties. In our earlier work. Grain and non-1801 domain distribution in a ceramic with no initial preferred orientation in the unpoled state (a) and with preferred orientation in the unpoled state (b).42 (Panel B) was used to analyze the measured diffraction data in ˚ ˚ the range 1. After thermal annealing at 6001C for 2 h. The well-developed understanding of these materials and the ability to fine tune their performance using wellinvestigated doping strategies are confounded by limited understanding of the domain character of these materials.39 The starting crystallographic information (lattice parameters. the performance potential is superior to conventionally processed materials. PA) 24 h after poling. etc. or grain growth. Piezo Technologies.) was taken from prior refinements of this material. dielectric anisotropy.45 The time-of-flight (TOF) calibration constant difc was first refined for each detector. The samples were immersed in silicon oil and electrically poled using electric fields in the range 0.38. Even the static nature of the domain configurations is disputed. j 5 1. or expansion of favored orientations from domain wall motion. elastic behavior. Through this poling process and the development of an electric dipole.05 A od o2..22–27 Figure 2(b) illustrates the alignment of domains before and after poling in ceramics that possess an initial crys- (1) Experimental Procedure Soft PZT ceramics (K350. Preferred orientation after electrical poling was measured using the texture diffractometer High Pressure-Preferred Orientation (HIPPO) (Panel B).75 kV/mm for 10 min at room temperature.25 A using the Rietveld method.46 After refinement of the texture using a sample symmetry of À1. In the subsequent refinement. is an orientation-inducing process that changes the fraction of the 1801 domains and can change the fraction of non-1801 domains.32–34 Regardless of the static structure. be generated by either 1801 rotations or non-1801 rotations. Materials exhibiting an Aurivillius28 or Tungsten–bronze29–31 crystal structure are particularly valuable for generating ceramics with an initial crystallographic texture before poling because of the large surface energy anisotropy of their structures. within ranges allowed by internal stresses and fatigue effects. a silver electrode was painted on the major faces of the sample and the polarization and strain response were measured using a Sawyer–Tower circuit with a laser interferometer in response to a 2. the process of electrical poling establishes a bias in domain configurations that enables the functionality of these materials. II. Finally. 2. Unlike texture changes from plastic deformation. Additionally. Sections III and IV describe the synthesis of initially textured ceramics of these two respective crystal systems and the evolution of their domain structures and piezoelectric properties through electrical poling.

3 and Randle and Engler.4 The ODF can be described discretely.100 At the top. trends should be consistent with the expected textures developed across all methods. synchrotron sources have been used. Other differences are not apparent in Fig. The continuity and statistical accuracy of a given texture measurement can be affected by the relationship between grain size and counting statistics. For grain texture measurements. These range from spallation neutron sources to synchrotron sources to laboratory diffractometers. the Rietveld method38. a brief examination of some of the capabilities and limitations of these approaches is given. Today. four sample rotations are used for collection of 120 diffraction patterns.37.2300 Journal of the American Ceramic Society—Jones et al. which require fewer measurements.41. When surface-sensitive measurements or a large number of measurements are required. HIPPO also has a high count rate that results from its short (9 m) initial flight path. While different methods may obtain different results.98 In the middle. the X-ray pattern utilized a synchrotron source with a fixed wavelength in Bragg–Brentano geometry. we have . and 401 that are used for texture measurements. The diffraction patterns of the soft PZT ceramic used in Section II obtained from three of these instruments is shown in Fig. the neutron diffraction pattern was obtained from the instrument MRPD at the HiFAR reactor at the Australian Nuclear Science and Technology Organisation (ANSTO) using a fixed wavelength. diffraction techniques are most widely used for texture measurements35 and in this work. For example.. The resolution of these detectors depends on the scattering angle. has 30 detector panels at fixed diffraction angles of 1501. Therefore. the relative intensities in neutron and X-ray patterns are different as a result of the difference in atomic scattering and Lorentz-polarization factors. Once a diffraction pattern or a series of patterns are obtained. or continuously using spherical harmonic (SH) functions in Fourier space.2 Wenk. The two primary considerations in these approaches are: (1) instrument selection and (2) the method of interpretation of information contained in the diffraction pattern. No. other less complex texture measurements are often desirable. but the number of measurements required (largely a function of the material’s symmetry) can be large.42 MAUD was utilized for this purpose in this work. 901.37 Each TOF pattern is effectively a measured inverse pole figure for one sample direction. the intensities can be extracted individually or as part of a whole powder pattern-fitting routine. with improved resolution available at higher scattering angles. For example. Typically.39 is a common method of modeling the diffraction patterns and enabling intensity extraction. Neutron diffraction typically gives a better sampling of the bulk material and therefore has been used whenever possible. the laboratory diffractometer has an advantage. the neutron diffraction pattern was obtained on the TOF instrument HIPPO by summing all of the y 5 901 fixed-angle detectors. Panel B: Diffraction Methods for Measuring Texture Vol. all of which collect diffracted intensities as a function of TOF. the ODF can be calculated by pole figure inversion. the diffractometer HIPPO at the Los Alamos Neutron Science Center. Many different diffraction instruments are available by which to perform texture measurements. In this work.36. When higher resolution measurements are required. B1 and yet are critical to the capabilities of the instrument. At the bottom.43 The large number of neutron diffraction patterns obtained on the texture diffractometer HIPPO at the Los Alamos Neutron Science Center (120 diffraction patterns are common for texture analysis)36. Los Alamos Fig.99.45 National Laboratory. sometimes in three-crystal mode (a crystal analyzer on the diffracted beam). Commonly used software for using Rietveld methods for texture analysis are General Structure Analysis System (GSAS)40 and Materials Analysis Using Diffraction (MAUD). a method of interpretation of information contained within the pattern is necessary. B1. The Rietveld method can also be used on X-ray diffraction patterns. Details of pole figure inversion can be found in Kocks et al.44 often necessitates. and benefits from. B1. we have used a variety of approaches using X-ray and neutron diffraction. Here. Diffracted intensities of the soft commercial lead zirconate titanate using three different diffraction instruments. For the latter. 90.1 Bunge.39. 8 Diffraction methods for measuring texture must enable a quantitative and statistically significant interpretation of the orientation of domains and grains in the polycrystalline material. Pole figure inversion is the reconstruction of the 3D ODF from measurements of the intensities of crystal poles (the distribution of a single-crystal pole in sample space is a pole figure and the distribution of crystal poles in a single sample direction is an inverse pole figure). we have performed measurements using all of these various instrument types. the Rietveld method for texture analysis. The ‘‘best’’ method for texture measurements is often dependent on the material being examined and the availability of the given diffraction instruments. To obtain pole figures or inverse pole figures from diffraction data for use in pole figure inversion. illustrating some of the unique features of these instruments. For domain textures of initially randomly oriented materials. where the texture is expressed completely by intensity interchanges in symmetry-dependent reflections.

defined here as the minimum value in the strain hysteresis plot. There exist some materials in which the (h00) and (0k0) peaks are either low in intensity or highly overlapped with other peaks and the use of Eq. In these cases. However. Because non-1801 domain switching only occurs in this tetragonal structure through an interchange of 002 and 200 poles. was not constant during this entire time (triangular waveform). is of the same order of mag40 0.2 kV/ mm. For tetragonal symmetries. Polarization and strain hysteresis behavior of the soft lead zirconate titanate ceramic. the use of Eq. The measurable strain at subcoercive poling fields could be attributed to either mechanism. The d33 increases dramatically around a poling field of 1. Preferred orientation induced through non-1801 domain switching was measured after electrical poling using full-pattern Rietveld refinement and pole figure inversion methods. the 100 pole density (or.1 – 20 0. The macroscopic longitudinal strain generated from the electrical poling process is also shown in Fig.47 Electrical poling of bulk ceramics induces domain reorientation similar to that observed during polarization and strain hysteresis measurements. After poling with an electric field of 1. 5. 3. Therefore. 4. The polarization and strain hysteresis. Increasing the electric field beyond the coercive field reorients both 1801 and non-1801 domains.33%. In other words. 3.0 kV/mm. incomplete pole figures can be measured directly without the complexity of pole figure inversion or the Rietveld method. ranging from 0% to 0. conversely.3 Polarization [µC/cm2] 20 Strain [%] –2 –1 0 1 Electric Field [kV/mm] 2 0. the inverse pole figure parallel to the electric field consists of a single maximum at 002 and a single minimum at 200. The information presented in Fig. This macroscopic strain. although it will be shown later that a component of this strain is from non-1801 domain switching.0 – 40 –0. (B-1) and (B-2) on diffraction intensities obtained at various sample tilt angles (a). the 001 pole density is given by45 f001 ðmrdÞ ¼ 3 R I00h =I00h R þ 2I R I00h =I00h h00 =Ih00 ðB À 1Þ R where Ihlk is the integrated intensity of the hkl peak in a randomly oriented sample (cooled in the absence of applied fields and unpoled). (B-2) becomes difficult.21 (2) Results and Discussion The polarization and strain response of an initially unpoled soft PZT bulk ceramic to a cyclic bipolar electric field are shown in Fig. However. moreover.1 –2 –1 0 1 Electric Field [kV/mm] 2 Fig.. This small degree of domain switching results in a measurable value of d33 for poling fields below 1.August 2007 Texture and Anisotropy of Polycrystalline Piezoelectrics 2301 developed a simple calculation for determining the degree of domain preference based on the relative intensity of these peaks in a single scattering direction. Although the entire ODF is calculated through pole figure inversion methods. the 010 pole density) pole is given by20 R Ih00 =Ih00 R R Ih00 =Ih00 þ 2I0h0 =I0h0 f100 ðmrdÞ ¼ 2 ðB À 2Þ Using Eqs.e. The coercive field. any set of peaks with consistent c components and varying a and b components can be used for quantifying domain textures. d33. The 002 pole density distributions are reproduced in Fig. although the ‘‘pole 0 0. static electric fields are applied for longer time periods during electric poling. Poling with higher electric fields yields nominally higher piezoelectric coefficients. For orthorhombic symmetries with two possible orthogonal ferroelastic variants such as the bismuth titanate and lead metaniobate structures in this work.0 kV/mm. The fact that these strains are different for different loading times provides some evidence of a time dependence of domain reorientation during electrical poling. shown in Fig. The longitudinal piezoelectric coefficient. is typical of soft PZT ceramics measured in other commercially available soft PZT materials. the magnitude of strain is higher during electrical poling because the electric field is applied for 10 min. 3. The poling strain. identified from Fig. leading to polarization and strain accumulation that is retained upon removing the electric field. i.0 kV/mm.56 . or remanent strain obtained after poling. 4. Some domain switching is expected during electrical poling below the coercive field because the electric field is applied over relatively long times. a single pole figure is sufficient to illustrate the results. (B-2) cannot always be directly applied. Therefore. is a combination of both intergranular elastic strain and strain resulting from non-1801 domain switching (interchanging of the long (002) and short (200) lattice planes). is shown as a function of electric field amplitude during electrical poling in Fig. significant grain rotation or growth does not lead to preferred orientation in these or other poles during electrical poling. 4 and. Piezoelectricity is then allowed in the initially randomly oriented ceramic after a net electric dipole is developed in the bulk material through 1801 and non-1801 domain switching. a d33 of 380 pC/N is achieved. 5 is the same as that given in pole figures with fiber symmetry. is 1.2 nitude as the remanent strain obtained during measurement of the polarization and strain hysteresis (Fig. whereas the positive portion of the electric field was applied for only B3 min during measurement of the strain in Fig. 3). the remanent state. 3 as the coercive field of this material. these poles are the only texture components in this system.

subcoercive electric fields. In other words.25 mrd. figure’’ terminology is reserved for pole distributions plotted on an equal area projection. Measured Berlincourt d33 and poling strain evolution as a function of the applied electric field during poling.62 (sixth order) and 1. 5) using Eq. 1). 5 is the angle from the poling axis.5 f002 [mrd] 2.0 kV/mm. The solid line labeled saturation indicates the theoretical saturation distribution from Jones et al. However. we have strong confidence in the trends observed between 0 and 1.2302 Journal of the American Ceramic Society—Jones et al. Matthies et al. One context for discussing the errors in these values is through a comparison of the results produced from the different methods of pole figure inversion. 002 pole density (f002) distributions of tetragonal lead zirconate titanate as a function of poling electric field.53 Qualitatively.0 1.0 kV/mm). which is seen between the highest electric fields.50 (fourth order) mrd.45. The presentation of the measured pole density distribution with the maximum saturation distribution highlights opportunities for optimization in the degree of non-1801 domain switching achieved during electrical poling. we have reported reasonable repeatability of pole density measurements using different measurement techniques and pole figure inversion methods. Before interpreting the results from Fig. However. the development of a nonzero d33 coefficient is a function of 1801 and non-1801 domain switching. indicating a likely concurrent progression of both 1801 and non-1801 domain switching. the domain textures produced by electrical poling are weak by comparison and the width of the pole density peaks is broad. such large differences are not expected in these weaker textures. this method of pole figure inversion does not yield errors associated with each sample direction. 8 Fig. For example. the pole density distributions are represented as continuous functions.75 1. has recently shown promise for attaining greater domain switching during this process.25 1. For example. the domain distributions described here are related to the . a benefit of quantitative texture measurements is the capability to relate single-crystal properties and the polycrystalline ODF to bulk anisotropic properties (Fig. this is evidence of non-1801 domain switching in the bulk of the material under application of static. Different methods have been developed for the inversion procedure including discretization methods and the use of series expansion. 5.5 0. 1801 domain switching is typically considered to be the primary contributor to this polarization development. the non-1801 domain switching distributions measured in Fig.00 0. 5. In bulk ceramics.0 Saturation 2. albeit within different grains with different orientations as a means of balancing both mechanical strain and electrical charge at the domain wall interface. No. the maximum pole density value increases to the range 1.21 The maximum density in the saturation distribution of 3 mrd results from the three possible non-1801 domain orientations in tetragonal ceramics.46 The differences reported in these earlier examples are generated using fundamentally different representations of the ODF.0 0. 5 used the series expansion representation of spherical harmonics. Electric field amplitudes below 1. 5 that the preferred orientation of the 002 pole increases with an increasing electric field during poling. The domain-switching component is calculated from the domain orientation distributions (Fig. or electromechanical poling.75 0. In earlier work.51 and 1. 5 is 0. Because this series expansion method provides a continuous solution of pole density in every possible sample direction (regardless of the discrete measurement grid).0 kV/mm and reasonable confidence in the increasing trend above 1. Vol.21 in this work on a strongly textured aluminum sample and report a wide range of maximum pole density values produced by the various methods. The minimum change in the maximum f002 values in the measured data of Fig. (2).0 0 15 30 Random Field [kV/mm] 1. the use of different pole figure inversion methods yielded maximum f002 values of 1. 5) agrees with the trends observed in macroscopic strain and d33 (Fig. 4. no error bars are readily available for a given sample direction and thus confidence in observed trends has to be developed through other means. both of which can lead to the development of a net electric dipole.06 mrd. The units of f002 are mrd (Panel A).46 For example. it is worthwhile reviewing the character of these pole density representations. the evolution of preferred orientation during electrical poling (Fig.44 compare several different methods of pole figure inversion from data obtained using the same instrument as that used 3. 5 is the theoretical saturation distributions predicted from an analytical domain-switching model of tetragonal ferroelastic ceramics with an initial random orientation. we expect the errors in the values reported in Fig.1 mrd. 5 to be o0. 5 correlate with the evolution of d33 in Fig. Measurements of crystallographic texture are useful for qualitative correlations to measured properties and material behavior. 4. Because these experiments were conducted using neutron diffraction.48–51 Application of mechanical fields during the electrical poling process. 4). the maximum f002 values for compression domain textures measured using two different orders of spherical harmonics were 1. These differences are much larger than the approach expected within the same pole figure inversion method such as those used here.45. Thus. When the electric field amplitude during electrical poling exceeds the coercive field (1. Poling strain results from non-1801 domain switching and the evolution of intergranular elastic strain. Therefore.65 mrd for the same data. The strain associated with domain switching and the mechanically constrained boundary conditions of individual grains within the ceramic limit switching within individual grains and therefore limit the degree of preferred orientation that can be attained. 90.0 mrd.46 Additionally. The data presented in Fig.46 Also shown in Fig.0 kV/mm during electrical poling generate maximum 002 density values of o1. It is therefore apparent from Fig.5 1. The principle of pole figure inversion involves a calculation of the ODF in three dimensions (Euler angles) from 2D data (pole density values as a function of two sample directions in the form of pole figures or intensity deviations from a structure solution in a diffraction pattern). This seems to suggest that the use of different pole figure inversion techniques may produce a wide range of ODFs.50 45 60 α [degrees] 75 90 Fig.5 mrd of002 o2. Therefore.52. The angle a in Fig. Evolution of both types of domain switching may progress in parallel.50 1. Furthermore. However. consistent with observations in earlier work.

after Chang et al. The temperature at which poling is performed plays a similarly important role in the achievable degree of domain switching. The grain contains three non-1801 domain variants.59 have recently used thermal depoling experiments to demonstrate the changing magnitudes of tetragonality and domain wall stability as a function of temperature and dopant. the value of 0.01 1. 3 also imply that there is some relaxation as the field is removed.3 1.99 0 100 200 300 400 Temperature [°Celsius] Fig.4%– 0. 6.67 and the associated strain are lower. In other words. This discrepancy above 1. would produce a more accurate strain estimate. However. the preference for non-1801 domain orientations parallel to the poling axis initially increases with increasing temperature (Fig.02 1. Change in the tetragonality (c/a ratio) parallel to the poling axis for three different ceramic compositions measured in situ as a function of temperature. in essence. bÞ Â cos2 a ðsin aÞdadb (2) b¼0 Through Eq. An averaging of this domain-switching strain over all possible grain orientations is represented as an integral over the two pole figure angles a and b.4 f002 [mrd] 1. Above 1.04 1. The extraction of the domain-switching strain component from non-1801 domain distributions are one possible outcome of coupling texture measurements and macroscopic properties. These results are redrawn in Figs.0 0 50 100 150 200 250 300 350 Temperature [°Celsius] hard PZT PT 2303 macroscopic poling strain because the measurements quantitatively capture the degree of interchanging (‘‘switching’’) of the crystallographic a and c lattice parameters in every possible grain orientation. Such a grain yields a macroscopic strain of 0.0 kV/mm and below.59 hard PZT PT . These strains contribute to the difference between our measured strain and calculated domain-switching strain values.0 kV/mm.47 have reported the 111 lattice strain hysteresis and observed the remanent strains after similar loadings to be approximately 0. there is more elastic strain58 and therefore larger errors in the application of Eq. For switching in grain orientations that are not perfectly oriented with respect to the electric field. the domain wall mobility of a Sr-doped (hard) PZT ceramic decreases as a function of temperature.6 soft PZT 1. there is a small but steady increase in the preference for domain orientations parallel to the poling axis with increasing 1. the total measured macroscopic strain is a combination of both non-1801 domain switching (a small volume fraction of the material in which the a and c lattice parameters are interchanged) and intergranular elastic strains. subcoercive electric field cycling. For unsaturated switching. including tetragonality and stiffness. Thermal depoling is. yielding21 SZZ 1 0 ¼ Slattice 2p Z p=2 Z  a¼0 Fig.2 1. these efforts at coupling the macroscopic strain to texture remain a quantitative link between texture measurements and macroscopic properties of piezoelectric ceramics. 6 and 7. the calculated strains from non-1801 domain switching comprise just over half of the measured poling strain. 6). the tetragonality decreases continuously with temperature until the Curie temperature is reached (Fig. This texture–property relationship is best understood by considering a grain orientation in which the pseudocubic crystal axes are coincident with the sample axes.55 Hoffmann et al. after Chang et al. As a piezoelectric ceramic cools from an elevated poling temperature.46 Ideally. For the soft PZT ceramic reported thus far. A modified lead titanate (PT) ceramic exhibits a smaller degree of domain orientation in the as-poled state as compared with the other materials (T 5 251C in Fig. a second-rank tensor transformation yields an additional cos2a dependence. 5. Figure 5 suggests that the highest degree of domain switching is expected at the highest applied electric fields during poling. the reverse effect of the cooling that occurs after poling at elevated temperatures.56. although it exhibits similarly decreasing tetragonality. 4. although more intensive.5 1.6%. In mechanical compression.54. The reduced domain wall mobility in this material compared with the PZT compositions has also been expressed in its mechanical stress–strain behavior and reduced fracture toughness enhancement with crack extension.03 c/a ratio 1. (2). 7). the increase in tetragonality (c/a) and elastic stiffness can promote intergranular elastic stresses. In the absence of such an approach.0 kV/mm is contributed by the evolution of intergranular elastic strains.60 For this PT ceramic.00 0. Some prior studies have shown that the measured 111 lattice strains parallel to the loading axis can serve as an indicator of internal stress during electrical or mechanical loading.67(cÀa)/a if the two less-preferred domain orientations switch entirely to the orientation where [001] is parallel to the electric field. the calculated component of the macroscopic strain resulting from non-1801 domain switching is shown in Fig.59 2p  à Df001 ða. the change in the 001 pole density distribution (Df001) can be related to the macroscopic strain resulting from non-1801 domain switching. At 1. (2). the measured poling strains and the calculated strains from non-1801 domain switching are comparable. The ferroelectric hysteresis loops in Fig. 6).05 soft PZT 1. 7. coupling of a lattice strain distribution function with a lattice ODF. small changes in the composition and dopant can strongly influence the behavior of these materials. 002 pole density (f002) parallel to the poling axis for three different ceramic compositions measured in situ as a function of temperature. We have used this comparison in ferroelastic textures induced by mechanical compression46 and domain-switching strains produced during higher frequency. As stated earlier. where a is the angle between the axis undergoing lattice constant interchanging and the strain direction.1 1.57 The most significant error in such an approach is that the lattice parameters are assumed to be constant. Chang et al. In contrast to that of the soft PZT ceramic. These stresses compete with a decreasing do- main wall mobility to establish the final domain configuration found at room temperature after poling. For the textures represented in Fig.August 2007 Texture and Anisotropy of Polycrystalline Piezoelectrics 1.

The earliest process used to induce a crystallographic texture in bismuth titanate ceramics was hot forging. This strong mechanical influence persists through repeated thermal cycling and thermal depoling at temperatures approaching the Curie temperatures. this behavior is attributed to a reduced domain wall mobility resulting from doping that is internally strengthened with increasing temperature.3 soft PZT. In fact.5Ti4O15 phase extracted from the ODF provide the distribution of the 001 crystallographic pole throughout the entire sample orientation space. To describe the texture on as-sintered and polished surfaces.7 1. The materials have been ground to introduce surface residual stresses and initial domain textures.75 A schematic of the tape-casting process and the resulting texture in the sintered ceramic are shown in Fig.23 in which a uniaxial force is applied to the ceramic at or near the sintering temperature.76 The Na0.77 The ODF of the Na0. the software MAUD41.2 2. understand. 8. Because highly anisometric platelet-shaped particles are synthesized by a more complex route than conventional calcination.2304 2. Sputtered electrodes were applied to both major faces of the samples and were thin enough for diffraction from the substrate.05 mm. or the 2 Aurivillius-oxide crystal structure.6 50 100 150 soft PZT. The platelet-shaped particles are preferentially oriented parallel to the tape-casting plane by viscous forces during the shearing process (Panel C). the maximum piezoelectric response is observed perpendicular to the pressing direction. and 3) of in situ heating to temperatures just below the Curie temperature. 1 2. (1) Experimental Procedure Textured ceramics were fabricated using templates of composition Bi4Ti3O12 and a commercial. the same materials retain domain texture following brief excursions above the Curie temperature. Figure 8 shows the results of a similar in situ measurement of textures generated initially by mechanical grinding of the soft PZT and PT compositions. preferentially oriented by tape casting. 3 Journal of the American Ceramic Society—Jones et al. Vol.5Ti4O15 matrix powder (K15. with the platelet-shaped particles serving as templates for epitaxial grain growth through the fine matrix grains. A temperature of 2151C and an electric field of 7. reorienting the (001) planes normal to the applied force. grow at the expense of the matrix powder during sintering. This texturing mechanism has been called templated grain growth (TGG). These samples were then subjected to thermal cycling in increments of 501C to temperatures just below the Curie temperature. For both instruments. promoting a 001 fiber texture about the casting plane normal. although they are indistinguishable in both diffraction and property measurements because the sample symmetry is transversely isotropic. The data shown are for the heating cycles up to 2501C only as a resolution of the peaks is difficult at temperatures exceeding 2501C. Details of the processing can be found in Jones. 6). Piezo Technologies) in discrete fractions ranging from 0 wt% (untemplated) to 25 wt%. Within the tape-casting plane. 9(a).5Ti4O15 phase was determined using both neutron and X-ray diffraction in methods detailed earlier.65 tape casting was explored as a more commercially viable. 6) suggests a strong mechanical influence from surface grinding. III. 3 PT.22. calcined Na0. 2 PT. the two directions defined by the tape-casting geometry are the tape-casting direction (TCD) and the transverse direction (TD). Bi4Ti3O12.5Ti4O15 structure contains three pseudo-perovskite blocks separated by Bi2O21 layers. in the (001) plane. Unique samples were cut in which measurements were taken both parallel to the TCD and the ND.74 The larger platelets.63 The highly anisometric.5Bi4. The samples were polished using decreasing grit coarseness to a final alumina grit size of 0. 1 PT. No.42 was used to calculate the ODF as represented by a fourth-order SH function by full-pattern Rietveld refinement of the obtained diffraction patterns (Panel B).5Bi4. Electrical poling was performed in an oil bath heated to temperatures in the range 1501–2151C for 40 min. For property and diffraction measurements. the piezoelectric d33 coefficient is modest in bismuth titanate. and describe the role played by dopants that are designed to help pin or depin domain walls. more recent tape-casting work has limited the quantity of platelets by including only a small fraction within a fine matrix powder. These experiments were repeated two additional times and repeatability was demonstrated without substantial loss of the mechanically induced surface domain texture.8 1. the tape-casting process produces a ceramic with a fiber symmetry axis parallel to the tape-casting normal direction (ND). 2 soft PZT.28 Bismuth titanate ceramics are preferred for high-temperature sensors because the structure remains piezoelectric at higher temperatures than in other common ferroelectric ceramics.5Bi4. 90.26.1 f002 [mrd] 2. The recalculated 001 pole figures of the Na0.5 kV/mm were used for the sample on which diffraction measurements were made to deter- .0 1. Domain alignment expressed in the unit mrd for soft lead zirconate titanate (PZT) and a lead titanate (PT) material during repeated thermal cycles (1.61 Investigations of this type enable a new framework in which to investigate. high-capacity process. The strong degree of initial domain texture relative to those achieved by electrical poling (Fig. These results demonstrate that domain alignments can intensify as the elastic constants soften and the tetragonality decreases with increasing temperature.27. The first tape-casting process used powder composed completely of platelet-shaped particles66–68 and the obtained textures are analogous to those produced by hot forging.62 However. In bismuth titanate. Although hot forging is still being investigated. Because this ceramic exhibits a strong decrease in tetragonality with temperature (Fig. For each of the two materials. there is an increase in the surface domain textures with increasing temperature.9 1.78 Neutron diffraction was used to measure the global texture in the bulk ceramic using the texture diffractometer HIPPO. and Na substitutes for Bi evenly and complete2 ly only in the pseudo-perovskite blocks. Although the samples were heated to just below the Curie temperature of 3501C. an area detector diffractometer was utilized using CuKa incident radiation. In the resulting texture. samples were cut with different orientations relative to the sample axes. 8 200 250 Temperature [°Celsius] Fig. 2. an established approach to increase d33 in a preferred sample direction. contains two pseudo-perovskite blocks separated by Bi2O21 layers. 7). Textured Bismuth Titanate Oxides The prototypical bismuth titanate structure.5Bi4. because the spontaneous polarization direction is parallel to [100] and non-1801 domain switching occurs between [100] and [010]. temperature (Fig. namely molten salt methods. plate-like morphology of bismuth titanate expressed in anisometric single crystals64 is easily exploited in engineered processes to generate crystallographic texture. the data shown are limited to 2501C due to the inability to quantify accurately the degree of alignment in mechanically ground domain textures above this temperature. leading to a macroscopic fiber texture in the ceramic.

5 kV/mm.240 A and a Ge (111) crystal analyzer detector on the diffracted beam. H is the blade gap used. templated sample. used a parameter. An untemplated. and the d33 coefficient was measured on a Berlincourt d33 meter 24 h after poling.27. Therefore.69–72 A thorough examination of the flow behavior of a ceramic slurry during tape casting was conducted by Kim et al.26.22–24. The correlation between template fraction.August 2007 Texture and Anisotropy of Polycrystalline Piezoelectrics Panel C: Tape Casting and Texture Development 2305 Tape casting ceramic powders with the inclusion of shaped seed particles is an effective way to induce grain textures in ceramic materials. most investigations focus only on either the seed particle shape or the seed particle concentration in the slurry. to quantify the ratio between the pressure forces to the viscous forces. three independent methods for increasing texture in tape-casting systems can be devised: increasing the casting velocity. C1). was developed for Newtonian fluids. The initial preferred orientation of the templates then directs texture development of the matrix phase by epitaxial or topotaxial growth. Deformation during a process such as tape casting in any fluid can be due to both viscous. it is possible to calculate P for a given tape-casting experiment for the following geometry from the equation P¼ DPH 2 2mLU ðC À 1Þ DPH2 is the pressure driven forces and 2mLU the viscous driven forces Hslurry α Ho U x=L L x x=0 H y H1 Fig. beamline X18A. Texture in the bulk as a function of template fraction was measured using neutron diffraction.6 to 4. P. Between 0% and 25% template fraction.74 Nonetheless. this modest degree of orientation still proves to be valuable. While highly anisotropic ceramics can be created in this way.78 where it is compared with pole figures produced from other approaches.1 mrd. which describes that the interaction of plateletshaped particles leads to their ‘‘mutual parallelism.20 This instrumental setup was required to resolve the small difference between the (100) and (010) lattice planes. Kim et al. modest residual texture (Lotgering factor % 30%) was also previously acknowledged in Bi4Ti3O12 processed by TGG. Although the formulation used by Kim et al.74 To explore the untemplated texture evolution in greater detail.65–68. According to Fig. Because we have explored the relationship between the Lotgering degree of orientation indicator and the multiple in intensity of the 00l peaks. C1. and texture is shown in Fig. mine domain textures.’’67 Panel C describes this process more completely. the effects of viscosity and casting velocity are expected to have similar effects on texture in tape casting of even non-Newtonian fluids. while the relative density increases from 91% to 95%. the greatest piezoelectric response in textured BaTiO3 is found in microstructures with a maximum of 2. The ratio of the pressure forces to viscous forces determines the flow characteristics of the slurry. The maximum value of the 001 pole figure is reported in this paper as a texture indicator because the pole figure is a smooth and broad distribution that does not change unexpectedly with processing condition. 11(a).73 where DP is the pressure exerted by the slurry head (DP 5 rslurry  g  Hslurry). They assumed that the slurry would behave as a Newtonian fluid in order to simplify the analysis. and U is the casting velocity. (2) Results and Discussion Figure 10 shows a micrograph of a section of a pyrolyzed.6 mrd is obtained without the requirements of template synthesis and incorporation. From this analysis. quantitative .80 The residual texture observed in untemplated samples with a maximum of 2. This increase in viscous-driven forces is expected to increase preferred orientation. 11(a). Recent numerical methods demonstrate a high piezoelectric response in microstructures with modest degrees of texture.73 (Fig. The pole figure is given explicitly in Jones et al.9 mrd.and pressure-driven forces. both density and texture increase with increasing template fraction. using a wavelength of 1. an increase in either the slurry viscosity or casting velocity will effectively increase the amount of viscous-driven forces. Utilizing all process conditions and slurry viscosity. Viscous forces are the source of shear behavior necessary for particle rotation and alignment. Increasing the fraction of templates increases the sintered bulk texture because the templates possess an initial preferred orientation.’s analysis. Prior investigators have used the Lotgering degree of orientation indicator to describe the texture. consistent with the generally accepted theory of particle alignment in shearbased processes. increasing the slurry viscosity. These domain measurements using diffraction were conducted at the National Synchrotron Light ˚ Source (NSLS). an increase in the ratio of viscous forces will result in an increased degree of particle orientation. m is the viscosity of the slurry. Casting geometry described in Kim et al. the maximum value of the 001 pole figure increases from 2. Figure 10 shows that the templates are preferentially oriented during the tape-casting process. and increasing the template concentration.77 it is apparent that the textures produced in this work are modest compared with those in the earlier literature. The templates can be identified as platelet-shaped particles with a width in excess of 10 mm.79 The samples for which the piezoelectric d33 coefficient was measured were poled using an electric field of 6. density. L is the length of the doctor blade. From Kim et al.

Equations (B-1) and (B-2) are therefore reserved for initially randomly oriented ceramics. regardless of the mechanism. Consideration of both texture contributions is necessary for interpreting the resulting properties because both forms of preferred orientation contribute to the absolute volume fraction of any given domain orientation. or ceramics containing 0% template particles. respectively.5Bi4. (B-2) for initially randomly oriented ceramics is given by81 fh00 ½mrdŠ ¼ 2Zh00 þ 1 (4) The domain-switching fraction induced by electrical poling in initially textured ceramics and calculated by Eq. the possible mechanisms for the stronger surface texture are limited to: (1) preferential growth of particles initially oriented parallel to the surface. A determination of the acting mechanism cannot be distinguished from these measurements. only a small absolute number of domains can be aligned in any specimen direction where the initial grain orientations provide few possible domain orientation variants. the driving force for surface texture enhancement. Figures 12(a) and (b) illustrate the presence of both the initial crystallographic texture of the grain structure and poling-induced domain texture. Little densification occurs at 10001C. or (3) a combination of preferential growth and reorientation mechanisms. In initially textured ceramics.5Ti4O15 matrix powder. However. No. (B-2) would imply a complete description of preferred orientation. (3) is shown in Fig. the grain ðfhkl Þ and domain-switching (Z200) orientation distributions can combine multiplicatively to à describe the total preferred orientation of the 200 pole ðf200 Þ by81 grain à f200 ¼ f200 ð2Z200 þ 1Þ (5) Fig. Likewise. Eqs. the initial preferred orientation of the 200 pole . were electrically poled for further domain texture and property measurements. where the 2Z20011 component transforms the domain-switching fraction (Z200) into the unit mrd as described by Eq. texture analysis using surface-sensitive X-ray reflection geometry was used. For initially textured ceramics. The tape-casting plane is horizontal in the image and normal direction is vertical. such considerations exist regardless of the domain-switching fraction. Recall for orthorhombic bismuth titanate such as Na0. 10. however. However. In other words.77 High-resolution synchrotron X-ray diffraction was used to characterize the domain texture. The initial preferred orientation before electrical poling is shown in Fig. Section of a pyrolyzed tape containing 5% Bi4Ti3O12 templates and a Na0. The volume fraction of the 100 domain orientation20 was measured as a function of angle relative to the electric field by evaluating the (200) and (020) peaks. In orthorhombic bismuth titanate. Schematic of the tape-casting process and the resulting texture in the sintered ceramic for 001-oriented. is the promotion of relatively lowenergy (001) surfaces. (4). In bismuth titanate ceramics with an initial preferred oriengrain tation of the grains. The maximum value of the 001 pole figure on both the top and bottom as-sintered surfaces and a polished internal surface are plotted with the relative density as a function of sintering temperature in Fig. preferred orientation on the as-sintered surface develops more rapidly than on the internal polished surface. (2) reorientation of particles early during the sintering process. Because the surface is not initially more predisposed to sources of texture than the bulk. Untemplated ceramics. 12(a). only 1501C from the maximum sintering temperature. [001] [001] [001] [001] [hk0] Vol.5Ti4O15 that the directions of possible spontaneous polarization relative to the paraelectric tetragonal unit cell are [100] and [010]. 12(b). (B-1) and (B-2) do not account for the initial preferred orientation induced by grain-orientation processing because they are formulated on a relative change in intensities after application of an electric field. or the preference for the [100] (parallel to the spontaneous polarization) at the expense of the [010]. needle-shaped PbNb2O6 templates (b). the volume fraction of certain domain orientations can be restricted by the domain-switching fraction. the domain switching can instead be expressed by the volume fraction of the preferred domain orientation. Densification accelerates at 11001C and plateaus near 11251C. a representation of domain switching by the value f200 calculated from Eq. it is apparent that the surface texture is stronger than in the bulk. With increasing sintering temperature. this volume fraction is given as20 Zh00 ¼ R Ih00 =Ih00 1 À R þI R 2 Ih00 =Ih00 0h0 =I0h0 (3) where the relationship between the domain-switching fraction Zh00 and the absolute pole density value fh00 calculated from Eq. even in a textured ceramic with nearly perfect orientation. a measurement that is independent of the initial preferred orientation of the grains. it cannot be presumed that the texture in this system is more significantly predisposed at the surface by such effects as particle settling (at the bottom surface) or particle reorientation from slurry surface tension (at the top surface). 9. The implication of this consideration is that the ferroelectric and piezoelectric properties are derived from contributions by both the grain orientation distribution and the domain orientation distribution. In fully sintered ceramics.81 In other words.2306 [001] Journal of the American Ceramic Society—Jones et al. Because the degree of orientation at a sintering temperature of 10501C is nearly equivalent at the surface and in the bulk. The 56% relative density at this sintering temperature is only slightly larger than the relative density of the pyrolyzed ceramic.5Bi4. platelet-shaped Bi4Ti3O12 templates (a) and 001-oriented. 51%. This is consistent with viscous forces as the mechanism of particle rotation and alignment as described in Panel C. 8 [001] (a) (b) Fig. 90. 11(b).

Texture of the as-sintered and polished internal surfaces quantified by surface-sensitive X-ray diffraction measurements.5 3.21 Therefore.0 80 3.20). however.0 1200 maximum(f001) [mrd] 2307 1000 1050 1100 1150 Template Fraction [weight percent] Sintering Temperature [°Celsius] Fig. 13 for samples containing 0% templates (untemplated) and range from 5 to 10 pC/ N when poled parallel to the ND and from 19 to 30 pC/N when poled parallel to the TCD. The maximum 200 pole density value is approximately 2. the grain texture leads to easier domain switching in the tape-casting plane.20 demonstrate that the maximum value of domain orientation when poled parallel to the tape-casting plane is Z200 5 0. contribute less to the piezoelectric response of the bulk ceramic. However. (b) Degree of domain switching (Z200) induced from electrical poling (from Jones et al.0 maximum(f001) [mrd] 4.77). We have previously suggested that the easy realignment of the ferroelastic distortion directions within the tape-casting plane may contribute to the strong dependence of d33 on direction. (c) Resultant 200 pole figure after poling considering the contributions of both preferred grain and domain orientations in units of mrd (after Jones et al.0 25 (b) 100 Relative Density [%] 80 60 40 20 0 950 10. There is a reduced temperature dependence when poled perpendicular to the tape-casting plane because domain wall motion is not promoted in this direction.0 70 2. the values are much smaller and less dependent on temperature. All plots are equal area projections. 12.5 mrd (Fig. Thus. the preferred orientation or alignment of the individual component strains influences the degree of domain switching. 12(c). and a polished internal surface (). the temperature dependence of the d33 in the TCD may result from thermally activated ferroelectric domain wall motion in the tape-casting plane during electrical poling. Texture of the bulk ceramic quantified using neutron diffraction measurements. the independent measurement methods described here are required to assess independently the grain and domain orientation contributions to the final state of preferred orientation. pole figures of the initially unpoled ceramic were first generated.2 mrd. This can then influence both the attainable degree of switching during electrical poling as mentioned previously and also promote possible extrinsic contributions to the d33 coefficient measured in this direction. 12(c) could be obtained by measuring 200 pole figures directly on the poled ferroelectric material. therefore. 12(a)) to 2. Here. The smaller values are the result of fewer favorable grain orientations. no measurable degree of domain orientation was apparent when poled perpendicular to the tape-casting plane. the process of electrical poling increases the 200 pole density value parallel to the electric field from 1. The randomly oriented ceramic poled under equivalent poling conditions exhibits a piezoelectric d33 coefficient between the values measured in the two directions of a textured ceramic: B15 pC/N.18 (Fig. the in-plane direction of the casting process. the domain orientation distributions were measured by evaluating the relative intensity of the 200 and 020 diffraction peaks. grains with a [001] direction parallel to the electric field have less of a tendency for ferroelectric switching and. With these mechanisms in mind. because non-1801 domain switching involves mechanical straining or deformation of grains. Parallel to the ND. bottom (H).0 0. 12(b)). we have also been able to demonstrate the influence of initial grain orientation on the degree of non-1801 domain switching. By measuring these two forms of preferred orientation independently. The tape-casting plane is parallel to the horizontal plane of the pole figure. Thus. (b) Influence of sintering temperature in an untemplated sample on preferred orientation of the top (n). Fig.5 90 4.81).20 Thus.0 2.0 6.2 mrd (Fig.August 2007 (a) 100 Relative Density [%] Texture and Anisotropy of Polycrystalline Piezoelectrics 5.0 4. In contrast to tetragonal or rhombohedral perovskite symmetries. 11. and the relative density ( & ). Jones et al. However. A large temperature dependence of poling on the d33 coefficient is apparent parallel to the TCD. (a) Influence of template fraction on relative density ( & ) and degree of preferred orientation () sintered at 11251C. The final pole figure representing the degree of preference for the 200 pole in the poled ferroelectric material is shown in Fig. and the final state was calculated as a multiple of the two components. (a) 200 pole figure of a textured bismuth titanate ceramic in units of mrd (redrawn from Jones et al.5 60 0 5 10 15 20 2.0 8. the orthorhombic material here exhibits only two possible ferroelastic distortion directions. The final state of the microstructure as shown in Fig. The piezoelectric d33 coefficient as a function of orientation and poling temperature is shown in Fig. resulting from tape casting (grain texture) is enhanced by poling (domain texture) and the preferred orientation induced by both independent processes combines multiplicatively to completely describe preferred orientation in ceramics with both texture components. 12(c)). .

Polishing the unpoled material to this finish produces X-ray diffraction data that are indistinguishable from samples annealed above the Curie temperature. 13. These samples were poled parallel to the ND. The 10 wt% slurry was then cast at rates of 20 and 80 cm/min. Using the estimates for the shear rate. sample faces were polished to a fine grit (1 mm). (B-2). ½ 100Š. Because the strength of the induced texture is relatively weak.94 kV/ mm for 25 min at a temperature of 1401C. both the h00 and 0k0 pole densities are 1 mrd. (2) Results and Discussion In a randomly oriented ceramic. To describe the crystallographic texture of the grains. texture developed in lead metaniobate is linked to variations in the tape-casting process. modifications to the tape-casting process itself can affect the degree of texture developed during the process. samples were ramped to 12401C over 12 h. 9(a) and the normal direction (ND) is directed out of the tape-casting plane. commercial lead metaniobate ceramics (K81. Domain textures were also measured by whole pattern refinement via the Rietveld method using the neutron diffractometer HIPPO. a blade gap of 300 mm was used with a parallel doctor blade. The high-viscosity slurries were cast only using a 5 wt% seed particle concentration at a casting rate of 20 cm/min. The details of these approaches are described in Panel B and Key et al. 90. polarization directions exist. and 20% by weight of ceramic were used with low-viscosity slurries. d33 % 80 pC/N. where intensities from the unpoled R sample correspond to values of Ihkl . For property measurements. higher order spherical harmonics are not necessary in representing the ODF. 2. The ferroelectric phase exhibits an orthorhombic tungsten–bronze crystal structure29–31 where the a and b unit cell dimensions are ˚ substantially larger than the c dimension (a 5 17. while all other slurries were cast at only 20 cm/min.88 These seeds were cast with a commercial. Increasing the casting velocity and slurry viscosity increases the shear behavior of the slurry. Temperature was then decreased to room temperature over a 2-h span. For firing. b 5 17.85 Domain textures were represented in poled samples by using a secondorder SH texture model with fiber symmetry enforced about the poling axis. 10%. When poled. (1) Experimental Procedure For domain orientation measurements on initially untextured ceramics. Textured Lead Metaniobate Oxides Ceramics of lead metaniobate.94 kV/mm and a temperature of 1401 for 25 min.87 A) and the b axis is defined as the axis of ferroelastic elongation and is parallel to the spontaneous polarization. The ODF was represented as a second-order SH function and orthorhombic sample symmetry was enforced.83 Similar to orthorhombic bismuth titanate. single-crystal seed particles of the composition PbNb2O6 were grown from a melt following the method proposed by Li et al. Here.92 ˚ ˚ A. [010].5 Pa Á s for the high-viscosity slurry. high d33/d31 ratio ( % 6). calcined PbNb2O6 matrix powder (K81. Seed particle concentrations of 0%. Previous studies have shown that inducing crystallographic texture before poling can lead to improvements in piezoelectric properties. the volume fraction of domains with crystallographic [h00] and [0k0] directions oriented in any given sample direction would be equal. and TD. Both slurries exhibit shear thinning behavior and therefore the viscosities during casting can be estimated by fitting a best-fit line to the viscosity data.30. For all formulations. find use where their elevated Curie temperatures ( % 5601C). These laminates were pressed at 6. and 2. These results are compared with preferred domain orientation that is developed due to the application of an electric field and the resulting piezoelectric properties in initially textured and poled ceramics. which can be tracked by quantifying the P value for each individual slurry. or PbNb2O6. Piezo Technologies) were obtained in both an unpoled and poled condition.5Bi4. Piezo Technologies).87 Tape casting was performed using seeds to template preferred orientation. Changes from this value upon poling indicate an increase in domain texture relative to a crystallographic pole. Using a rationale supported by Panel C. Green tapes were cut and laminated into stacks of 10–20. Both of these methods are described in Panel B. Samples for X-ray diffraction were polished to a fine grit (1 mm) on the surface perpendicular to the poling direction in order to remove the sample electrode. The 150/510 peak doublet was evaluated here using a synchrotron X-ray source. No. IV. 8 Fig. TCD. Therefore.2308 Journal of the American Ceramic Society—Jones et al. and c 5 3. from Jones et al. and ½0 such that four possible coplanar 10Š. The commercial poling conditions used were 3. Before all diffraction experiments. The structure was first refined using data from an unpoled specimen and a starting structure equivalent to that reported by Labbe et al. samples of the high-viscosity 5 wt% slurry were electrically poled at a field of 3.20 The tape-casting direction (TCD) is in the tapecasting plane of the sample in Fig.63 A. MA). The shear rates developed during casting are estimated to be the ratio of the blade gap to the casting velocity. and low mechanical quality factor ( % 15) can be exploited. The samples were heated to 6001C over 3 h and held at this temperature for 2 h to burn out the binder. held at this temperature for 30 min. and furnace cooled to room temperature. the Rietveld method was used to calculate ODFs from measured neutron diffraction spectra using the instrument HIPPO and methods described earlier. the maximum allowable 0k0 pole density parallel to the poling direction is 2 mrd. polarization is confined to the aÀb plane of the crystal. 86 and Iverson et al. Measurements of the peak doublet were obtained at tilt angles (a) from 01 to 701 in 51 increments using Eq. randomly oriented ceramics.69.82 Switching by 901 and 1801 domains occurs between [100].0 Pa Á s for the low-viscosity slurry cast at 80 cm/min. polycrystalline ceramics of lead metaniobate exhibit a modest longitudinal piezoelectric coefficient. Additionally.84 The inclusion of seed particles with a high morphological aspect ratio in a tape-casting process can allow for the development of grain textures through processes such as TGG.8 Pa Á s for the low-viscosity slurries cast at 20 cm/min. several variations of the tape-casting slurry were devised.9 MPa using heated platens at a temperature of 381C.21 This value would occur only if all 901 . Middleboro. Piezoelectric d33 coefficient as a function of sample direction and poling temperature of textured Na0. For an initially randomly oriented ceramic.89 The general viscosity profiles for the two slurries containing a seed particle concentration of 5 wt% were measured using a Brookfield viscometer (Brookfield Engineering. Acicular.5Ti4O15 obtained without the use of templates and initially untextured. the viscosities at casting are estimated to be: 6. Vol. Two methods were used to measure domain textures from poled lead metaniobate using diffraction techniques: comparison of (hk0)-type peaks using synchrotron X-ray diffraction data and pole figure inversion methods using neutron diffraction data and the Rietveld method.

the maximum 150 pole density value is parallel to the poling direction (a 5 01) with decreasing values at higher angles to the poling direction. During casting. all of the laminates develop a maximum 010 texture parallel to the ND and a minimum 010 texture parallel to the TCD. Differences between absolute values can be attributed to differences between the penetration depth and sample volume examined during diffraction. Therefore. 16 correlate with these predictions: a 001-type preferred orientation parallel to the TCD and a 010-type preferred orientation parallel to the ND. 15. With greater particle orientation before firing. the degree of preferred orientation is dependent on other factors as described in Panel C. continuous and provides an interpolation between measured directions. Increasing the slurry viscosity (Fig. Because peaks of pure (h00) or (0k0) are either low in intensity or overlapped by other peaks in this structure.August 2007 Texture and Anisotropy of Polycrystalline Piezoelectrics Synchrotron X-ray diffraction Neutron diffraction Saturation 2309 3. However. resulting in increased preferred orientation in the TCD and ND. 9(b). [100] and [010]. The (150) and (510) were chosen because there is a relatively shallow angle (B111) between these crystal poles and the respective crystal axes. where hak. Increasing the casting velocity (Figs. any set of peaks with consistent c components and varying a and b components can be used for quantifying domain textures. slurry deformation was determined to be dominated by sheardriven forces. the templates are subject to shear forces that rotate the particles and align them within the tape-casting plane. This behavior inverts in the 001 pole figures with maxima in the TCD and minima in the ND. Such an interpolation is commonly used as a filter for experimental noise in measured intensities. One method involves domain orientation measurements at discrete sample orientations using X-ray diffraction in reflection geometry and a calculation of domain orientations based on relative peak intensity changes. The solid line labeled saturation indicates the theoretical saturation distribution from Jones et al.5 f150 [mrd] 2. 16(b) vs. Accounting for the casting geometry and slurry viscosity. The pole figures are recalculated from the ODF and are reproduced in Fig. which demonstrates a distinct elongated rectangular shape. 5).5 0. Figure 15 shows a micrograph of these particles. The increase in 0k0-type texture quantified in all methods is attributed to an increase in the volume fraction of domains oriented such that the angle between the polarization direction and the electric field is minimized. As illustrated in Fig. The long axis of the particles is parallel to the [001] crystallographic direction and the [100] and [010] directions are parallel to the short particle direction.5 1. Seed particles are used to fabricate textured ceramics. 14. The long axis of these particles is parallel to the crystallographic [001]. With the long axis of the particles parallel to the crystallographic [001]. These particles act as templates for anisotropic grain growth in the fired ceramic. 9(b)). Domain density distributions calculated using the synchrotron diffraction data are discrete because values are calculated from intensity measurements in discrete sample directions. In addition to the template concentration. whereas pole figures obtained from an ODF are continuous because the ODF is represented as a continuous SH function (similar to that of Fig. with the crystallographic [100] and [010] parallel to the shorter particle dimensions. general 001-type textures are expected to develop parallel to the TCD. the shear behavior of the slurry acts to align these particles within the tape-casting plane (Fig. the use of direct peak intensity comparisons is limited to those of (hk0) type. the amount of particle orientation should also be increased. The second method involves pole figure inversion methods using neutron diffraction data and a representation of the ODF using a series expansion of spherical harmonics. There is more scatter in the discrete data because each value is calculated individually. These particles were added to two slurries of different viscosity formulated after Galassi et al. Particle rotation and orientation is dependent on the amount of shear-driven forces. The pole density distributions generated by the two methods exhibit a difference in their absolute values and a difference in scatter.89 This means that the inclusion of even small amounts of seed particles should result in the development of preferred orientation. alignment of the ‘‘square-beam’’ template particles in the tape-casting plane results in the development of [001]-type preferred orientation in the TCD and [100] and [010] preferred orientations in the normal and transverse directions. 150 pole density (f150) distributions of orthorhombic lead metaniobate. (d)) results in an increase in both the 001 and 010 pole densities without the use of additional seed particles. The pole figures in Fig.21 domains were reoriented.0 Random 0. With the exception of the 0 wt%.87 This texture development is related to the morphology of the template particles and the degree of shear behavior developed during casting.and 010-type textures are expected to develop normal to the tape-casting plane. low-viscosity slurry.0 0 15 30 45 60 α [degrees] 75 90 Fig. shear forces will act to align seed particles relative to the tape-casting plane. respectively.21 The 150 pole density distributions of an initially randomly oriented lead metaniobate ceramic calculated using two different methods are shown in Fig. During casting. stronger textures can be achieved when the ceramic is fired. 16. The 010 and 001 pole figures are shown for each of the investigated tape-casting variations. 100.90 During casting. if the amount of shear-driven forces occurring during casting is increased. Collection of acicular seed particles of lead metaniobate grown from a melt.0 1. whereas pole figure inversion methods utilizing series expansion representations produce data that are Fig. 16(a)–(c)) during casting increases the number of templates that become aligned during casting.0 2. The two methods show agreement in that in both cases. 16(e)) results in a higher 010 pole . 14. Subsequently. orthotropic sample symmetry results with a specific TCD and preferred normal plane corresponding to the tape-casting plane. Increasing seed particle concentration (Figs. Slurry deformation during casting is composed of both shear-driven and pressure-driven forces. A metal-rolling type.

seed particle concentration. To better illustrate these correlations.52 0. 17. À~. V. suggesting that a tailored response can be induced through a combination of grain texturing. these domain distributions will contribute to the enhanced performance in new functional materials. and TCD. resulting in an increase in preferred orientation. In a similar manner.31 110 70 (a) (b) (c) Fig. The maximum 010 texture is found parallel to the ND. three different longitudinal piezoelectric coefficients are observed. those with monoclinic symmetry or monoclinic distortions of the unit cell).g. and symmetry on polycrystalline anisotropy. although they are intrinsic to the behavior of polycrystalline ceramics in the poled state. and casting velocity. In Section II. 17. a discussion on the influence of these lower-symmetry systems on the domain distributions and polycrystalline properties is relevant. Electrical poling parallel to the ND (normal to the tape-casting plane) results in the largest piezoelectric coefficient. For example. the d33 value is approximately 80 pC/N.33 yield unique domain distribution functions not yet considered.2310 Journal of the American Ceramic Society—Jones et al. For an originally random sample.91–93 Therefore. These directionally dependent piezoelectric coefficients correlate with the texture measurements in Fig. ~. the shear behavior of the slurry deformation is increased. For tetragonal ceramics. The spontaneous polarization direction in lead metaniobate is parallel to [010]. which is a value between the two coefficients when poled parallel to the TCD and ND. These distributions cannot be measured dip rectly using the methods described here. the piezoelectric response is dependent on the distribution of the 010 pole before electrical poling. followed by the TD. 8 Fig. d33 5 10 pC/N. Electrical poling parallel to the TCD results in a substantially lower piezoelectric coefficient. tape-cast lead metaniobate exhibits orthotropic sample symmetry and there are three distinct axes.32. and the longitudinal piezoelectric coefficient measured when electrical poling was performed parallel to each sample direction. 16(e). This indicates that increasing the preferred orientation of the 010 pole before electrical poling can increase the piezoelectric response in this direction after poling. Vol. anisotropy. is unique from the antip polar direction. the magnitude of electric field and temperature during poling. No. polycrystalline ceramics incorporating increasingly complex crystal systems (e. two of which are in the tape-casting plane (TCD and TD).18 d33 [pC/N] 10 ND TD 2. 10%. When the 5 wt% high-viscosity laminate is poled parallel to the ND. By increasing the casting velocity and slurry viscosity. 16. we described the degree of non-1801 domain switching using a pole density distribution function. Other Texture–Anisotropy Relationships There are a number of other piezoelectric systems not investigated in this work but are nonetheless interesting with regard to the influence of texture. these texture and piezoelectric coefficient measurements are shown in parallel in Fig. d33 5 110 pC/N. density in the ND than all of the other cases with the use of the lowest fraction of seed particles. 010 (top) and 001 (bottom) pole figures for the various tape-casting processes plotted on equal area projections. or 1801 p p domain switching) and additional polarization reorientations allowable by crystal symmetry. (a)–(c) are 0%. 90. the 010 pole density in each sample direction (b). and the minimum 010 mrd is parallel to the TCD. the degree of 1801 domain switching can be represented by a polarization distribution function. Unlike bismuth titanate. The polarization distribution function as a function of crystal symmetry and domain-switching can be calculated by modifying our earlier non-1801 domain-switching simulation21 to account for polarization inversion (~2 À ~ domain switching. and (e) is the 5% seed particles with a high-viscosity slurry. Therefore.87. The incorporated symmetries f010 [mrd] TCD TC 0. where the polar direction. and poling time. and 20% seed particles under the standard tape-casting conditions. Sample axes definitions (a). .. the 001 pole density distribution function described the distribution of the 001 pole relative to the poling axis and the 001 and 00 pole are 1 indistinguishable. Different strengths of texture can be induced by altering the slurry viscosity. Nonetheless. particularly with the increased availability of polycrystalline ceramics of stable monoclinic symmetries with continuing processing advances. Electrical poling parallel to the TD results in a piezoelectric coefficient of d33 5 70 pC/N. TD. (d) is the 10% seed particles with a blade speed of 80 cm/min.73 This equates to more particle rotation and orientation.

In ferroelectric ceramics. only a fraction of the total x-axis range (01oao1801) is shown. self-consistent. the polarization distribution function can be integrated to calculate the effective grain-averaged polarization using the equation hp3 i 1 ¼ 2 p0 Z p Because a single-crystal polarization of B95% is attainable in monoclinic symmetries without a polarization rotation mechanism. Because the polarization distribution function describes a statistical probability of the spontaneous polarization direction in every possible sample direction. the maximum value of fp is equal to the possible number of spontaneous polarization directions. Every aspect of these measurements demonstrates that the potential performance of these materials is critically tied to polarization processes that are impacted by the chemistry of added dopants.August 2007 1000 100 Texture and Anisotropy of Polycrystalline Piezoelectrics Monoclinic with polarization rotation Mononclinic (γ = 24°) Rhombohedral Tetragonal Orthorhombic 180° switching only Random distribution 2311 fp [mrd] 24 16 8 0 0 15 30 45 60 α [degrees] 75 90 Fig. whereas the second-rank strain tensor in Eq. Section II describes the evolution of these 3D orientational elements in initially randomly oriented polycrystalline PZT ceramics.975 . Table I. [010]. these results also suggest little motivation for the use of processes that induce initial grain texture to yield larger polarization fractions in low-symmetry materials. and the degeneracy of symmetry breaking that enables the piezoelectric effect. which are furp ther described in Table I. Number and Distribution of Possible Polarization Directions Relative to a Prototype Pseudo-Cubic Unit Cell for Various Crystal Systems and Resulting Attainable Fraction of Single-Crystal Polarization (/p3S/p0) in Initially Randomly Oriented Ceramics95 Crystal system Number of domain variants Polarization direction distribution in sample space /p3S/p0 O1 T R O2 MA (g 5 241) MA (g unconstrained) 4 6 8 12 24 N [100]. only non-1801 domain switching and polarization inversion may occur. Saturated polarization distribution functions for different crystal systems with different multiples and directions of possible spontaneous polarization. there may also exist polarization percolation networks70 or ferroelastic alignment mechanisms20 that can contribute either positively or negatively to the physically achievable polarization in textured ceramics. enabling the achievement of a higher degree of domain texture during poling. It is believed that crystal symmetries exhibiting more possible polarization directions and ferroelastic strain variants can be more self-compensating. /001S Toward corners of cube. Using Eq. defects within the crystals. In other words. include an MA-type monoclinic symmetry with a constrained polarization direction of 241 from the pseudo-cubic o0014(g). Upon application of an electric field in the unconstrained case. Whereas most investigations on these materials have previously relied upon interpreting the behavior of polycrystalline piezoelectrics as deviations from an ideal single-crystal response. 5 where the non-1801 domain switching induced by increasing electric field during poling only marginally increases the domain orientation distribution relative to the calculated saturated distribution. ½ 100Š. For clarity. uov 0. /011S pffiffi   1 1 2= tanð24o Þ [uuv]. polycrystalline ceramics of these symmetries may intrinsically enable better poling and a resulting higher fraction of realizable singlecrystal values in polycrystalline materials. although the first-rank polarization tensor (vector) is projected by a single cosine term. /111S Toward ffiedges of cube. polarization inversion. respectively. non-1801 domain switching.94 and an MA-type monoclinic symmetry with an unconstrained polarization direction in the monoclinic (010) plane.5% (for MA symmetry with an unconstrained polarization direction). VI. Eq. In the constrained case (g 5 241). there are physical limits to achieving such a high fraction of single-crystal polarization in real polycrystalline ceramics that are limited by intergranular stresses and strains. However. (6) is analogous to Eq.707 0. (2) is projected by cos2a.866 0. Thus. which further influences macroscopic anisotropies in piezoelectric and ferroelectric behavior. In all cases with a finite number of polarization direction possibilities.952 0. 18.95 Distribution represents saturation of initially randomly oriented polycrystalline ceramics.51 This was demonstrated earlier in Fig. the monoclinic and tetragonal symmetries have maximum values fp 5 24 and 6 mrd. a sample symmetry can be induced through poling. the intrinsic crystal symmetry of the individual orientations relates to the measurable macroscopic properties of the material. Figure 18 presents the distribution functions of the polarization direction ~ for various crystal systems. As discussed in Section III. An electromechanically coupled. this work aims to capture the available 3D orientational information so that the behavior of domain walls within individual grain orientations can be inferred and correlated with macroscopic properties.831 0. multiaxial constitutive model incorporating anisotropic crystal elasticity would be a suitable second approximation for investigating these interaction mechanisms in various crystal symmetries. and polarization rotation may occur.912 0. Summary and Outlook Different measurements and diffraction tools have been combined in this investigation to elicit information on the separate contributions from 1801 and non-1801 domains to the macroscopic response of ferroelectric ceramics. (6).7% (for orthorhombic) to 97. It is shown during electrical poling that domains oriented with the spontaneous polarization direction close to parallel to the applied electric field increase at the expense of other pðaÞ cos a sin a da a¼0 (6) where /p3S/p0 is the fraction of single-crystal polarization achievable in the polycrystalline material. (2). ½0 10Š Toward faces of cube. the fraction of single-crystal polarization achievable in polycrystalline materials is listed in Table I and varies from 70. Because every polycrystalline material has a distribution of crystallographic orientations and orientation relationships between grains.

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1987).S. Vol. Iowa from 2005 to 2006. Before this.S. he received his B.S and B. Jones is an Assistant Professor in the Department of Materials Science and Engineering at the University of Florida (UF). Keith Bowman joined the faculty as Assistant Professor at Purdue University in 1988 after receiving degrees from Case Western Reserve University (CWRU) (B. In 2007 he received the College of Engineering Mentoring Award and he was named to a Professorship of Engineering Education by courtesy. .D. Before this. 1981.S.S. He was promoted to Associate Professor in 1992.D. He served as a visiting professor at the University of New South Wales in Sydney. His research group has lead efforts to quantify and model preferred orientation and property anisotropy in metals. He was named the 2007 Outstanding Graduate Student for Materials Engineering. 90. No. He was named a Fellow of the American Ceramic Society in 2000. Australia from 2004 to 2005 and at Iowa State University in Ames.D. Dr. Germany in 1996 and again in 2002. He received his Ph. Professor Bowman has served as advisor or coadvisor to twenty master’s and eighteen doctoral students. His postdoctoral research focused on fracture and fatigue of ceramic materials.2314 Journal of the American Ceramic Society—Jones et al. and in situ characterization techniques. anisotropy. Jones’ current research interests at UF include structure–property relationships in electromechanical materials. 8 Jacob L. in Mechanical Engineering from Purdue University and worked in industry as a mechanical engineer. the Charles Murphy Undergraduate Teaching Award in 1995. in Materials Science and Engineering from Purdue University. and then promoted to Professor in 1996. Benjamin J. In 2003 Professor Bowman’s name was added to the Purdue Book of Great Teachers. 1983) and the University of Michigan (Ph. Keith Bowman also served as a visiting professor and received Alexander von Humboldt Research Awards at the Technical University of Darmstadt. Iverson received his Ph. he received an NSF International Research Fellowship to conduct postdoctoral research abroad at the University of New South Wales in Sydney. he received his M. Awards at Purdue University include receiving the Purdue Materials Engineering Best Teaching Award in 1992 and 1995 and Purdue’s highest teaching award. in Materials Science and Engineering from Purdue University in 2004 for his work on texture and anisotropy in bismuth titanate ceramics. Australia in 2003. in Materials Science and Engineering from Purdue University in 2007 for his work on texture and anisotropy in lead metaniobate. M. Before joining UF. ceramics and composites.

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