arXiv subjects

G. Shirane

Publications and source records attributed to G. Shirane.

At least 37 records · Page 2Linked to original sources

arXiv2004

High q-resolution neutron scattering technique using triple-axis spectrometers

We present a new technique which brings a substantial increase of the wave-vector $q$-resolution of triple-axis-spectrometers by matching the measurement wave-vector $q$ to the reflection $τ_a$ of a perfect crystal analyzer. A relative Bragg width of $δ/Q \sim 10^{-4}$ can be achieved with reasonable collimation settings. This technique is very useful in measuring small structural changes and line broadenings that can not be accurately measured with conventional set-ups, while still keeping all the strengths of a triple-axis-spectrometer.

cond-mat.other↗

arXiv2004

Dual structures in PZN-xPT ferroelectric relaxors

We performed x-ray diffraction studies on a series of (1-$x$)Pb(Zn$_{1/3}$Nb$_{2/3}$)O$_3$-$x$PbTiO$_3$ (PZN-$x$PT) single crystals with different incident photon energies, and therefore different penetration depths. Our results show that outer-layers of $\sim 10$ to 50 $μ$m thick are present in all samples. The structure of those outer-layers is different from that of the inside of the crystals, by having much greater (rhombohedral) distortions. With increasing $x$, rhombohedral-type lattice distortions develop, both in the outer-layer and the inside.

cond-mat.mtrl-sci↗

arXiv2003

Characterization of low-energy magnetic excitations in chromium

The low-energy excitations of Cr, i.e. the Fincher-Burke (FB) modes, have been investigated in the transversely polarized spin-density-wave phase by inelastic neutron scattering using a single-(Q+-) crystal with a propagation vector (Q+-) parallel to [0,0,1]. The constant-momentum-transfer scans show that the energy spectra consist of two components, namely dispersive FB modes and an almost energy-independent cross section. Most remarkably, we find that the spectrum of the FB modes exhibits one peak at 140 K near Q = (0,0,0.98) and two peaks near Q = (0,0,1.02), respectively. This is surprising because Cr crystallizes in a centro-symmetric bcc structure. The asymmetry of those energy spectra decreases with increasing temperature. In addition, the observed magnetic peak intensity is independent of Q suggesting a transfer of spectral-weight between the upper and lower FB modes. The energy-independent cross section is localized only between the incommensurate peaks and develops rapidly with increasing temperature.

cond-mat.mtrl-sci↗

arXiv2003

Evidence of decoupled lattice distortion and ferroelectric polarization in the relaxor system PMN-xPT

We report high $q$-resolution neutron scattering data on PMN-$x$PT single crystals with $x=20%$ and 27%. No rhombohedral distortion occurs in the 20PT sample for temperatures as low as 50 K. On the other hand, the 27PT sample transforms into a rhombohedral phase below T$_C \sim 375$ K. Our data provide conclusive evidence that a new phase with an average cubic lattice is present in the bulk of this relaxor system at low PT concentration, in which the ferroelectric polarization and lattice distortion are decoupled. The rhombohedral distortion is limited to the outermost tens of microns of the crystal.

cond-mat.mtrl-sci↗

arXiv2003

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.

cond-mat.mtrl-sci↗

arXiv2003

Universal Static and Dynamic Properties of the Structural Transition in Pb(Zn1/3Nb2/3)O3

The relaxors Pb(Zn$_{1/3}$Nb$_{2/3}$)O$_{3}$ (PZN) and Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_{3}$ (PMN) have very similar properties based on the dielectric response around the critical temperature $T_{c}$ (defined by the structural transition under the application of an electric field). It has been widely believed that these materials are quite different below $T_{c}$ with the unit cell of PMN remaining cubic while in PZN the low temperature unit cell is rhombohedral in shape. However, this has been clarified by recent high-energy x-ray studies which have shown that PZN is rhombohedral only in the skin while the shape of the unit cell in the bulk is nearly cubic. In this study we have performed both neutron elastic and inelastic scattering to show that the temperature dependence of both the diffuse and phonon scattering in PZN and PMN is very similar. Both compounds show a nearly identical recovery of the soft optic mode and a broadening of the acoustic mode below $T_{c}$. The diffuse scattering in PZN is suggestive of an onset at the high temperature Burns temperature similar to that in PMN. In contrast to PMN, we observe a broadening of the Bragg peaks in both the longitudinal and transverse directions below $T_{c}$. We reconcile this additional broadening, not observed in PMN, in terms of structural inhomogeneity in PZN. Based on the strong similarities between PMN and PZN, we suggest that both materials belong to the same universality class and discuss the relaxor transition in terms of the three-dimensional Heisenberg model with cubic anisotropy in a random field.

cond-mat.mtrl-sci↗

arXiv2003

Electric Field Effects on the Diffuse Scattering in PZN-8%PT

We report measurements of the neutron diffuse scattering from a single crystal of the relaxor ferroelectric Pb(Zn_1/3Nb_2/3)O_3 doped with 8% PbTiO_3 (PZN-8%PT) for temperatures 100 K < T < 530 K and electric fields 0 kV/cm < E < 10 kV/cm. The diffuse scattering is strongly suppressed transverse to the (003) Bragg peak at 400 K for E = 2 kV/cm applied along the [001] direction. However, no change in the diffuse scattering is observed transverse to (300), even for field strengths up to 10 kV/cm. Thus the application of an external electric field in the tetragonal phase does not produce a macroscopically polarized state. This unusual behavior can be understood within the context of the Hirota et al. phase-shifted polar nanoregion (PNR) model of the relaxor diffuse scattering, since an electric field E oriented parallel to [001] would remove the shift of the nanoregions along [001] while preserving those along the orthogonal [100] direction.

cond-mat.mtrl-sci↗

arXiv2003

Dynamics and Structure of PMN and PZN

A review is given of recent neutron and x-ray scattering studies of the lead-oxide perovskite relaxor systems Pb(Zn1/3Nb2/3)O3-xPbTiO3 and Pb(Mg1/3Nb2/3)O3-xPbTiO3. X-ray measurements by Noheda et al. have established that these two systems exhibit nearly identical phase diagrams in which a rhombohedral-monoclinic-tetragonal structural sequence takes place with increasing PbTiO3 concentration. Recent high-energy x-ray and neutron measurements on single crystals of PZN and PMN-10PT, however, show that the rhombohedral distortions occur only in the outermost 20 - 40 microns, while the bulk of each crystal transforms into a new phase X, which has a nearly cubic unit cell. This situation is very similar to the structural behavior of pure PMN at Tc = 220 K. A simple model has been suggested that correlates phase X to the unique atomic displacements of the polar nanoregions, which are created at the Burns temperature.

cond-mat.str-el↗

arXiv2003

A Universal Phase Diagram for PMN-xPT and PZN-xPT

The phase diagram of the Pb(Mg1/3Nb2/3)O3 and PbTiO3 solid solution (PMN-xPT) indicates a rhombohedral ground state for x < 0.32. X-ray powder measurements by Dkhil et al. show a rhombohedrally split (222) Bragg peak for PMN-10%PT at 80 K. Remarkably, neutron data taken on a single crystal of the same compound with comparable q-resolution reveal a single resolution-limited (111) peak down to 50 K, and thus no rhombohedral distortion. Our results suggest that the structure of the outer layer of these relaxors differs from that of the bulk, which is nearly cubic, as observed in PZN by Xu et al.

cond-mat.mtrl-sci↗

arXiv2003

Spin waves and the origin of commensurate magnetism in Ba2CoGe2O7

The square-lattice antiferromagnet Ba2CoGe2O7 is studied by means of neutron diffraction and inelastic scattering. This material is isostructural to the well-known Dzyaloshinskii-Moriya helimagnet Ba2CuGe2O7, but exhibits commensurate long-range Neel order at low temperatures. Measurements of the spin wave dispersion relation reveal strong in-plane anisotropy that is the likely reason for the suppression of helimagnetism.

cond-mat.str-el↗

arXiv2003

Spin Wave Propagation in the Domain State of a Random Field Magnet

Inelastic neutron scattering with high wave-vector resolution has characterized the propagation of transverse spin wave modes near the antiferromagnetic zone center in the metastable domain state of a random field Ising magnet. A well-defined, long wavelength excitation is observed despite the absence of long-range magnetic order. Direct comparisons with the spin wave dispersion in the long-range ordered antiferromagnetic state reveal no measurable effects from the domain structure. This result recalls analogous behavior in thermally disordered anisotropic spin chains but contrasts sharply with that of the phonon modes in relaxor ferroelectrics.

cond-mat.dis-nn↗

arXiv2003

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

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.

cond-mat.str-el↗

arXiv2002

Structure and Dynamics of the Ferroelectric Relaxors Pb(Mg1/3Nb2/3)O3 and Pb(Zn1/3Nb2/3)O3

We review some of the current research on two of the ultra-high piezoelectric relaxors Pb(Mg1/3Nb2/3)O3 (PMN) and Pb(Zn1/3Nb2/3)O3 (PZN). The discovery of a monoclinic phase in Pb(Zr1-xTix)O3 (PZT) in 1999 by Noheda et al. forced a reassessment of the structural symmetries found near the morphotropic phase boundary in PZT, as well as in the PbTiO3 (PT) doped systems PZN-PT, and PMN-PT. All three systems are now known to have nearly identical phase diagrams that exhibit a rhombohedral-monoclinic-tetragonal structural sequence with increasing PbTiO3 concentration. The dynamical properties of these relaxors are controlled by the unique nature of the so-called polar nanoregions (PNR), which first appear at the Burns temperature Td as evidenced by the onset of diffuse scattering. That this diffuse scattering persists to temperatures below the Curie temperatures of PMN (220 K) and PZN (410 K) indicates that the phase transitions in these relaxors are very different from those observed in ordinary ferroelectrics. They also differ in this regard from what would be expected in the often-quoted model based on analogy with the random field effect.

cond-mat.mtrl-sci↗

arXiv2002

Magnetic field effects and magnetic anisotropy in lightly doped La_{2-x}Sr_xCuO_4

The effects of the application of a magnetic field on the diagonal stripe spin-glass phase is studied in lightly doped La_{2-x}Sr_xCuO_4 (x=0.014 and 0.024). With increasing magnetic field, the magnetic elastic intensity at the diagonal incommensurate (DIC) positions (1,\pmε,0) decreases as opposed to the increase seen in superconducting samples. This diminution in intensity with increasing magnetic field originates from a spin reorientation transition, which is driven by the antisymmetric exchange term in the spin Hamiltonian. On the other hand, the transition temperature, the incommensurability, and the peak width of the diagonal incommensurate correlations are not changed with magnetic field. This result suggests that the magnetic correlations are determined primarily by the charge disproportionation and that the geometry of the diagonal incommensurate magnetism is also determined by effects, that is, stripe formation which are not purely magnetic in origin. The Dzyaloshinskii-Moriya antisymmetric exchange is nevertheless important in determining the local spin structure in the DIC stripe phase.

cond-mat.str-el↗

arXiv2002

Development of Ferroelectric Order in Relaxor (1-x)Pb(Mg1/3Nb2/3)O3 - xPbTiO3

The microstructure and phase transition in relaxor ferroelectric Pb(Mg1/3Nb2/3)O3 (PMN) and its solid solution with PbTiO3 (PT), PMN-xPT, remain to be one of the most puzzling issues of solid state science. In the present work we have investigated the evolution of the phase symmetry in PMN-xPT ceramics as a function of temperature (20 K < T < 500 K) and composition (0 <= x <= 0.15) by means of high-resolution synchrotron x-ray diffraction. Structural analysis based on the experimental data reveals that the substitution of Ti^4+ for the complex B-site (Mg1/3Nb2/3)^4+ ions results in the development of a clean rhombohedral phase at a PT-concentration as low as 5%. The results provide some new insight into the development of the ferroelectric order in PMN-PT, which has been discussed in light of the kinetics of polar nanoregions and the physical models of the relaxor ferroelectrics to illustrate the structural evolution from a relaxor to a ferroelectric state.

cond-mat.mtrl-sci↗

arXiv2002

Mode-coupling and polar nanoregions in the relaxor ferroelectric Pb(Mg1/3Nb2/3)O3

We present a quantitative analysis of the phonon lineshapes obtained by neutron inelastic scattering methods in the relaxor ferroelectric Pb(Mg1/3Nb2/3)O3 (PMN). Differences in the shapes and apparent positions of the transverse acoustic (TA) and transverse optic (TO) phonon peaks measured in the (300) and (200) Brillouin zones at 690 K are well described by a simple model that couples the TA and soft TO modes in which the primary parameter is the wave vector and temperature-dependent TO linewidth Gamma(q,T). This mode-coupling picture provides a natural explanation for the uniform displacements of the polar nanoregions, discovered by Hirota et al., as the PNR result from the condensation of a soft TO mode that also contains a large acoustic component.

cond-mat.mtrl-sci↗

arXiv2002

New Magnetic Excitations in the Spin-Density-Wave of Chromium

Low-energy magnetic excitations of chromium have been reinvestigated with a single-Q crystal using neutron scattering technique. In the transverse spin-density-wave phase a new type of well-defined magnetic excitation is found around (0,0,1) with a weak dispersion perpendicular to the wavevector of the incommensurate structure. The magnetic excitation has an energy gap of E ~ 4 meV and at (0,0,1) exactly corresponds to the Fincher mode previously studied only along the incommensurate wavevector.

cond-mat.str-el↗

arXiv2002

Ferroelectric Dynamics in the Perovskite Relaxor PMN

We review results obtained from recent neutron scattering studies of the lead-oxide class of perovskite relaxors PMN and PZN. A ferroelectric soft mode has been identified in PMN at 1100 K that becomes overdamped near 620 K. This is the same temperature at which polar nanoregions (PNR) begin to form, denoted by Td, and suggests that a direct connection exists between the soft mode and the PNR. The appearance of diffuse scattering intensity at Td reported by Naberezhnov et al. lends further support to this picture. At lower temperature the soft mode in PMN reappears close to Tc = 213 K (defined only for E > Ec). These results are provocative because the dynamics below Tc are characteristic of an ordered ferroelectric state, yet they occur in a system that remains cubic on average at all temperatures. We discuss a coupled-mode model that successfully describes these data as well as those from earlier lattice dynamical studies of other perovskites such as BaTiO3.

cond-mat.mtrl-sci↗