Universal Phase Diagram for High-Piezoelectric Perovskite Systems

Strong piezoelectricity in the perovskite-type PbZr(1-x)TixO3 (PZT) and Pb(Zn1/3Nb2/3)O3-PbTiO3 (PZN-PT) systems is generally associated with the existence of a morphotropic phase boundary (MPB) separating regions with rhombohedral and tetragonal symmetry. An x-ray study of PZN-9%PT has revealed the presence of a new orthorhombic phase at the MPB, and a near-vertical boundary between the rhombohedral and orthorhombic phases, similar to that found for PZT between the rhombohedral and monoclinic phases. We discuss the results in the light of a recent theoretical paper by Vanderbilt and Cohen, which attributes these low-symmetry phases to the high anharmonicity in these oxide systems.Comment: REVTeX file. 4 pages,=A0 4 figures embedde

Low-temperature phases in Pb(Zr0.52Ti0.48)O3: A neutron powder diffraction study

A neutron powder diffraction study has been carried out on Pb(Zr0.52Ti0.48)O3 in order to resolve an ongoing controversy about the nature of the low-temperature structure of this strongly-piezoelectric and technologically-important material. The results of a detailed and systematic Rietveld analysis at 20 K are consistent with the coexistence of two monoclinic phases having space groups Cm and Ic respectively, in the approximate ratio 4:1, and thus support the findings of a recent electron diffraction study by Noheda et al. [Phys. Rev. B 66, 060103 (2002)]. The results are compared to those of two recent conflicting neutron powder diffraction studies of materials of the same nominal composition by Hatch et al. [Phys. Rev. B 65, 212101 (2002)] and Frantti et al. [Phys. Rev. B 66, 064108 (2002)].Comment: RevTex4, 16 pages, 6 color figure

New Features of the Morphotropic Phase Boundary in the PbZr(1-x)TixO3 System

Recently a new monoclinic phase in the PbZr(1-x)TixO3 ceramic system has been reported by Noheda et al. for the composition x= 0.48. In the present work, samples with Ti contents of x= 0.47 and 0.50, which are both tetragonal below their Curie points, have been investigated. In the sample with x= 0.50, the tetragonal phase was found to transform to a monoclinic phase at about 200 K as the temperature was lowered. The sample with x= 0.47 showed a complicated region of phase coexistence between 440-320 K, becoming rhombohedral at around 300 K. No further symmetry change was found down to 20 K. Dielectric measurements for these two samples are also reported. On the basis of these results, a preliminary phase diagram is presented. Optimum compositional homogeneity is needed to properly characterize the new monoclinic region.Comment: 5 pages, 7 PS figures embedded. RevTeX and epsf macros. Presented at the 9th. European Meeting on Ferroelectricity, Prague, July 1999. To be published in "Ferroelectrics

The monoclinic phase in PZT: new light on morphotropic phase boundaries

A summary of the work recently carried out on the morphotropic phase boundary (MPB) of PZT is presented. By means of x-ray powder diffraction on ceramic samples of excellent quality, the MPB has been successfully characterized by changing temperature in a series of closely spaced compositions. As a result, an unexpected monoclinic phase has been found to exist in between the well-known tetragonal and rhombohedral PZT phases. A detailed structural analysis, together with the investigation of the field effect in this region of compositions, have led to an important advance in understanding the mechanisms responsible for the physical properties of PZT as well as other piezoelectric materials with similar morphotropic phase boundaries.Comment: 5 pages REVTeX file, 6 figures embedded. Presented at the Workshop on "Fundamental Physics of Ferroelectrics" held in Aspen, February 00. To appear in the proceeding

Static and Dynamic Magnetism in Underdoped Superconductor BaFe1.92_{1.92}Co0.08_{0.08}As2_2

We report neutron scattering measurements on single crystals of BaFe$_{1.92}$Co$_{0.08}$As$_2$. The magnetic Bragg peak intensity is reduced by 6 % upon cooling through T$_C$. The spin dynamics exhibit a gap of 8 meV with anisotropic three-dimensional (3d) interactions. Below T$_C$ additional intensity appears at an energy of $\sim$4.5(0.5) meV similar to previous observations of a spin resonance in other Fe-based superconductors. No further gapping of the spin excitations is observed below T$_C$ for energies down to 2 meV. These observations suggest the redistribution of spectral weight from the magnetic Bragg position to a spin resonance demonstrating the direct competition between static magnetic order and superconductivity.Comment: 4 pages, 4 figure

Spin Waves in the Ferromagnetic Ground State of the Kagome Staircase System Co3V2O8

Inelastic neutron scattering measurements were performed on single crystal Co3V2O8 wherein magnetic cobalt ions reside on distinct spine and cross-tie sites within kagome staircase planes. This system displays a rich magnetic phase diagram which culminates in a ferromagnetic ground state below Tc~6 K. We have studied the low-lying magnetic excitations in this phase within the kagome plane. Despite the complexity of the system at higher temperatures, linear spin-wave theory describes most of the quantitative detail of the inelastic neutron measurements. Our results show two spin-wave branches, the higher energy of which displays finite spin-wave lifetimes well below Tc, and negligible magnetic exchange coupling between Co moments on the spine sites.Comment: 4 pages and 4 figure

Phonon Properties of Knbo3 and Ktao3 from First-Principles Calculations

The frequencies of transverse-optical $\Gamma$ phonons in KNbO$_3$ and KTaO$_3$ are calculated in the frozen-phonon scheme making use of the full-potential linearized muffin-tin orbital method. The calculated frequencies in the cubic phase of KNbO$_3$ and in the tetragonal ferroelectric phase are in good agreement with experimental data. For KTaO$_3$, the effect of lattice volume was found to be substantial on the frequency of the soft mode, but rather small on the relative displacement patterns of atoms in all three modes of the $T_{1u}$ symmetry. The TO frequencies in KTaO$_3$ are found to be of the order of, but somehow higher than, the corresponding frequencies in cubic KNbO$_3$.Comment: 8 pages + 1 LaTeX figure, Revtex 3.0, SISSA-CM-94-00

Lattice dynamics reveals a local symmetry breaking in the emergent dipole phase of PbTe

Local symmetry breaking in complex materials is emerging as an important contributor to materials properties but is inherently difficult to study. Here we follow up an earlier structural observation of such a local symmetry broken phase in the technologically important compound PbTe with a study of the lattice dynamics using inelastic neutron scattering (INS). We show that the lattice dynamics are responsive to the local symmetry broken phase, giving key insights in the behavior of PbTe, but also revealing INS as a powerful tool for studying local structure. The new result is the observation of the unexpected appearance on warming of a new zone center phonon branch in PbTe. In a harmonic solid the number of phonon branches is strictly determined by the contents and symmetry of the unit cell. The appearance of the new mode indicates a crossover to a dynamic lower symmetry structure with increasing temperature. No structural transition is seen crystallographically but the appearance of the new mode in inelastic neutron scattering coincides with the observation of local Pb off-centering dipoles observed in the local structure. The observation resembles relaxor ferroelectricity but since there are no inhomogeneous dopants in pure PbTe this anomalous behavior is an intrinsic response of the system. We call such an appearance of dipoles out of a non-dipolar ground-state "emphanisis" meaning the appearance out of nothing. It cannot be explained within the framework of conventional phase transition theories such as soft-mode theory and challenges our basic understanding of the physics of materials