Condensation and Slow Dynamics of Polar Nanoregions in Lead Relaxors

It is now well established that the unique properties of relaxor ferroelectrics are due to the presence of polar nanoregions (PNR's). We present recent results from Neutron and Raman scattering of single crystals of PZN, PZN-xPT, and PMN. Both sets of measurements provide information on the condensation of the PNR's and on their slow dynamics, directly through the central peak and, indirectly, through their coupling to transverse phonons. A comparative analysis of these results allows identification of three stages in the evolution of the PNR's with decreasing temperature: a purely dynamic stage, a quasi-static stage with reorientational motion and a frozen stage. A model is proposed, based on a prior study of KTN, which explains the special behavior of the transverse phonons (TO and TA) in terms of their mutual coupling through the rotations of the PNR's.Comment: AIP 6x9 style files, 10 pages, 4 figures, Conference-Fundamental Physics of Ferroelectrics 200

Domain structure in the monoclinic Pm phase of Pb(Mg1/3Nb2/3)O3 - PbTiO3 single crystals

The domain structure of (1-x)Pb(Mg1/3Nb2/3)O3- xPbTiO3 single crystals with composition x ~ 0.33 in the range of the morphotropic phase boundary (MPB) was studied. Based on the analysis of spontaneous strain compatibility and charge of domain walls, we have established the permissible domain arrangements for the ferroelectric phases of different symmetry, which are expected to occur in the range of the MPB. Examination of (001)-oriented unpoled and electrically poled (along the [001] direction) crystal plates in polarizing microscope reveals a monophase state with the domain structure compatible with the structure theoretically predicted for the Mc monoclinic phase (space group Pm), which was recently discovered in the compositions close to the MPB by x-ray and neutron diffraction studies. In the unpoled crystal the 180 deg. walls between the domains whose spontaneous polarization vectors are parallel to the plane of the crystal plate (i.e. a-domains) are observed. The domain structure of the poled crystal is predominantly composed of crystallographically prominent Wf walls parallel to (001) (i.e. the plane of the crystal plate) and inclined S walls parallel to [110] or [1-10] direction. In poled and unpoled samples the optical rotatory polarization effect is found, which is related to the inhomogeneity of the sample resulting from the mixture of domains.Comment: PDF file, 30 pages, 15 figures (3 in color) collected on pp.18-3

Diffuse Neutron Scattering Study of Relaxor Ferroelectric (1-x)Pb(Zn1/3Nb2/3)O3-xPbTiO3(PZN-xPT)

Diffuse neutron scattering is a valuable tool to obtain information about the size and orientation of the polar nanoregions that are a characteristic feature of relaxor ferroelectrics. In this paper, we present new diffuse scattering results obtained on Pb(Zn1/3Nb2/3)O3 (PZN for short) and (1-x)Pb(Zn1/3Nb2/3)O3-xPbTiO3(PZN-xPT)single crystals (with x=4.5 and 9%), around various Bragg reflections and along three symmetry directions in the [100]-[011] zone. Diffuse scattering is observed around reflections with mixed indices, (100), (011) and (300), and along transverse and diagonal directions only. No diffuse scattering is found in longitudinal scans. The diffuse scattering peaks can be fitted well with a Lorentzian function, from which a correlation length is extracted. The correlation length increases with decreasing temperatures down to the transition at Tc, first following a Curie-Weiss law, then departing from it and becoming flat at very low temperatures. These results are interpreted in terms of three temperature regions: 1) dynamic polarization fluctuations (i.e. with a finite lifetime) at high temperatures, 2) static polarization reorientations (condensation of polar nanoregions) that can still reorient as a unit (relaxor behavior) at intermediate temperatures and 3) orientational freezing of the polar nanoregions with random strain fields in pure PZN or a structural phase transition in PZN-xPT at low temperatures. The addition of PT leads to a broadening of the diffuse scattering along the diagonal ([111]) relative to the transverse ([100]) direction, indicating a change in the orientation of the polar regions. Also, with the addition of PT, the polar nanoregions condense at a higher temperature above Tc.Comment: AIP 6x9 style files, 9 pages, 5 figures, Conference-Fundamental Physics of Ferroelectrics 200

Ground State of Relaxor Ferroelectric Pb(Zn1/3Nb2/3)O3Pb(Zn_{1/3}Nb_{2/3})O_3

High energy x-ray diffraction measurements on Pb(Zn$_{1/3}$Nb$_{2/3}$)O$_3$ (PZN) single crystals show that the system does not have a rhombohedral symmetry at room temperature as previously believed. The new phase (X) in the bulk of the crystal gives Bragg peaks similar to that of a nearly cubic lattice with a slight tetragonal distortion. The Bragg profile remains sharp with no evidence of size broadening due to the polar micro crystals (MC). However, in our preliminary studies of the skin, we have found the expected rhombohedral (R) phase as a surface state. On the other hand, studies on an electric-field poled PZN single crystal clearly indicate a rhombohedral phase at room temperature.Comment: 11 pages with 3 figure

Diffuse Neutron Scattering Study of a Disordered Complex Perovskite Pb(Zn1/3Nb2/3)O3 Crystal

Diffuse scattering around the (110) reciprocal lattice point has been investigated by elastic neutron scattering in the paraelectric and the relaxor phases of the disordered complex perovskite crystal-Pb(Zn1/3Nb2/3)O3(PZN). The appearance of a diffuse intensity peak indicates the formation of polar nanoregions at temperature T*, approximately 40K above Tc=413K. The analysis of this diffuse scattering indicates that these regions are in the shape of ellipsoids, more extended in the direction than in the direction. The quantitative analysis provides an estimate of the correlation length, \xi, or size of the regions and shows that \xi ~1.2\xi , consistent with the primary or dominant displacement of Pb leading to the low temperature rhombohedral phase. Both the appearance of the polar regions at T*and the structural transition at Tc are marked by kinks in the \xi curve but not in the \xi one, also indicating that the primary changes take place in a direction at both temperatures.Comment: REVTeX file. 4 pages, 3 figures embedded, New version after referee cond-mat/010605

Neutron scattering study of PbMg1/3_{1/3}Ta2/3_{2/3}O3_3 and BaMg1/3_{1/3}Ta2/3_{2/3}O3_3 complex perovskites

Neutron scattering investigations were carried out in PbMg$_{1/3}$Ta$_{2/3}$O$_3$ and BaMg$_{1/3}$Ta$_{2/3}$O$_3$ complex perovskites. The crystal structure of both compounds does not show any phase transition in the temperature range 1.5 -- 730 K. Whereas the temperature dependence of the lattice parameter of BaMg$_{1/3}$Ta$_{2/3}$O$_3$ follows the classical expectations, the lattice parameter of relaxor ferroelectric PbMg$_{1/3}$Ta$_{2/3}$O$_3$ exhibits anomalies. One of these anomalies is observed in the same temperature range as the peak in the dielectric susceptibility. We find that in PbMg$_{1/3}$Ta$_{2/3}$O$_3$, lead ions are displaced from the ideal positions in the perovskite structure at all temperatures. Consequently short-range order is present. This induces strong diffuse scattering with an anisotropic shape in wavevector space. The temperature dependences of the diffuse neutron scattering intensity and of the amplitude of the lead displacements are similar

A Neutron Elastic Diffuse Scattering Study of PMN

We have performed elastic diffuse neutron scattering studies on the relaxor Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_3$ (PMN). The measured intensity distribution near a (100) Bragg peak in the (hk0) scattering plane assumes the shape of a butterfly with extended intensity in the (110) and (1$\bar{1}$0) directions. The temperature dependence of the diffuse scattering shows that both the size of the polar nanoregions (PNR) and the integrated diffuse intensity increase with cooling even for temperatures below the Curie temperature $T_C \sim 213$ K.Comment: Submitted to PR

Disorder and relaxation mode in the lattice dynamics of PbMg1/3_{1/3}Nb2/3_{2/3}O3_3 relaxor ferroelectric

The low-energy part of vibration spectrum in PbMg$_{1/3}$Nb$_{2/3}$O$_3$ relaxor ferroelectric was studied by inelastic neutron scattering. We observed the coexistence of a resolution-limited central peak with strong quasielastic scattering. The line-width of the quasielastic component follows a $\Gamma_0+Dq^2$ dependence. We find that $\Gamma_0$ is temperature-dependent. The relaxation time follows the Arrhenius law well. The presence of a relaxation mode associated with quasi-elastic scattering in PMN indicates that order-disorder behaviour plays an important r\^ole in the dynamics of diffuse phase transitions

Competing orders in PZN-xPT and PMN-xPT relaxor ferroelectrics

Neutron and x-ray scattering studies on relaxor ferroelectric systems Pb(Zn$_{1/3}$Nb$_{2/3}$)O$_3$ (PZN), Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_3$ (PMN), and their solid solutions with PbTiO$_3$ (PT) have shown that inhomogeneities and disorder play important roles in the materials properties. Although a long-range polar order can be established at low temperature - sometimes with the help of an external electric field; short-range local structures called the ``polar nano-regions'' (PNR) still persist. Both the bulk structure and the PNR have been studied in details. The coexistence and competition of long- and short-range polar orders and how they affect the structural and dynamical properties of relaxor materials are discussed.Comment: Article submitted for JPSJ Special Topics (Novel States of Matter Induced by Frustration