arXiv subjects

G. Shirane

Publications and source records attributed to G. Shirane.

At least 55 records · Page 3Linked to original sources

arXiv2002

Phase diagram of the ferroelectric-relaxor (1-x)PbMg(1/3)Nb(2/3)O3-xPbTiO3

Synchrotron x-ray powder diffraction measurements have been performed on unpoled ceramic samples of (1-x)PbMg(1/3)Nb(2/3)O3-xPbTiO3 (PMN-xPT) with 30%<= x<= 39% as a function of temperature around the morphotropic phase boundary (MPB), which is the line separating the rhombohedral and tetragonal phases in the phase diagram. The experiments have revealed very interesting features previously unknown in this or related systems. The sharp and well-defined diffraction profiles observed at high and intermediate temperatures in the cubic and tetragonal phases, respectively, are in contrast to the broad features encountered at low temperatures. These peculiar characteristics, which are associated with the monoclinic phase of MC-type previously reported by Kiat et al and Singh et al., can only be interpreted as multiple coexisting structures with MC as the major component. An analysis of the diffraction profiles has allowed us to properly characterize the PMN-xPT phase diagram and to determine the stability region of the monoclinic phase, which extends from x= 31% to x= 37% at 20 K. The complex lansdcape of observed phases points to an energy balance between the different PMN-xPT phases which is intrinsically much more delicate than that of related systems such as PbZr(1-x)TixO3 or (1-x)PbZn(1/3)Nb(1/3)O3-xPbTiO3. These observations are in good accord with an optical study of x= 33% by Xu et al., who observed monoclinic domains with several different polar directions coexisting with rhombohedral domains, in the same single crystal.

cond-mat.mtrl-sci↗

arXiv2002

Ferroelectric Ordering in the Relaxor Pb(Mg1/3Nb2/3)O3 as Evidenced by Low-Temperature Phonon Anomalies

Neutron scattering measurements of the lowest-energy TO phonons in the relaxor Pb(Mg1/3Nb2/3)O3 (PMN) are reported for 10<=T<=750 K. The soft mode, which is overdamped by the polar nanoregions below the Burns temperature T_d = 620 K, surprisingly recovers below 220 K. The square of the soft mode energy hw0^2 increases linearly with decreasing temperature, and is consistent with the behavior of a ferroelectric soft mode. At 10 K, hw0 reaches 11 meV, the same value observed in ferroelectric Pb(Zn1/3Nb2/3)O3 at low-T. An unusual broadening of the TA phonon starts at T_d and disappears at 220 K, coincident with the recovery of the TO mode. These dynamics suggest that a well-developed ferroelectric state is established below 220 K.

cond-mat.mtrl-sci↗

arXiv2002

Electronic phase separation in lightly-doped La$_{2-x}$Sr$_x$CuO$_4$

The hole concentration dependence of the magnetic correlations is studied in very lightly-doped La$_{2-x}$Sr$_x$CuO$_4$ ($x<$0.02), which shows coexistence of a three-dimensional antiferromagnetic (AF) long-range ordered phase and a spin-glass phase at low temperatures. It is found that the spin-glass phase in the coexistence region also shows a diagonal spin modulation as in the pure spin-glass phase in La$_{2-x}$Sr$_x$CuO$_4$ (0.02$\le x\le$0.055). Below $x\sim$0.02 the diagonal stripe structure is the same as that in $x\sim$0.02 with a volume fraction almost proportional to hole concentration, suggesting that electronic phase separation of the doped holes occurs so that some regions with hole concentration $h_c\sim$0.02 and the rest with $h_c\sim$0 are formed. This result also indicates that the transition between the AF and spin-glass phase around $x$=0.02 is first order.

cond-mat.str-el↗

arXiv2002

Electric-field induced phase transitions in rhombohedral PZN-xPT

High-energy x-ray diffraction experiments peformed on rhombohedral (1-x)Pb(Zn1/3Nb2/3)O3-xPbTiO3(PZN-xPT) crystals with x= 4.5 and 8% show that an electric field applied along the [001] direction induces the tetragonal phase, as proposed by Park and Shrout. Our experiments reveal that in 4.5PT such phase change occurs via a third phase with monoclinic symmetry, MA, which is observed at intermediate field values. This is in agreement with first-principles calculations by Fu and Cohen predicting the rotation of the polarization between the rhombohedral and tetragonal phases in this material. A different polarization path between the rhombohedral and tetragonal phases, through a second monoclinic phase, MC, has been previously reported in 8PT. The microscopic characterization of these crystals allows us to explain the ultra-high macroscopic strain observed in PZN-x%PT under an electric field. Moreover, some unusual scattering profiles displayed by exceptionally good crystals, are experimental evidence of the high anharmonicities and near-degeneracy of the different phases in these extremely deformable materials.

cond-mat.mtrl-sci↗

arXiv2001

Monoclinic phase in the relaxor-based piezo-/ ferroelectric Pb(Mg$_{1/3}$Nb$_{2/3})O_3$-PbTiO$_3$ system

A ferroelectric monoclinic phase of space group $Cm$ ($M_A$ type) has been discovered in 0.65Pb(Mg$_{1/3}$Nb$_{2/3})O_3$-0.35PbTiO$_3$ by means of high resolution synchrotron X-ray diffraction. It appears at room temperature in a single crystal previously poled under an electric field of 43 kV/cm applied along the pseudocubic [001] direction, in the region of the phase diagram around the morphotropic phase boundary between the rhombohedral (R3m) and the tetragonal (P4mm) phases. The monoclinic phase has lattice parameters a = 5.692 A, b = 5.679 A, c = 4.050 A and $β$ = $90.15^{\circ}$, with the b$_m$-axis oriented along the pseudo-cubic [110] direction . It is similar to the monoclinic phase observed in PbZr$_{1-x}$Ti$_x$O$_3$, but different from that recently found in Pb(Zn$_{1/3}$Nb$_{2/3})O_3$-PbTiO$_3$, which is of space group $Pm$ ($M_C$ type).

cond-mat.mtrl-sci↗

arXiv2001

Static magnetic correlations near the insulating-superconducting phase boundary in La$_{2-x}$Sr$_{x}$CuO$_{4}$

An elastic neutron scattering study has been performed on several single crystals of La$_{2-x}$Sr$_{x}$CuO$_{4}$ for {\it x} near the lower critical concentration {\it x$_{c}$} for superconductivity. % In the insulating spin-glass phase ({\it x} = 0.04 and 0.053), the previously reported one-dimensional spin modulation along the orthorhombic {\it b}-axis is confirmed. % Just inside the superconducting phase ({\it x} = 0.06), however, two pairs of incommensurate magnetic peaks are additionally observed corresponding to the spin modulation parallel to the tetragonal axes. % These two types of spin modulations with similar incommensurabilities coexist near the boundary. % The peak-width $κ$ along spin-modulation direction exhibits an anomalous maximum in the superconducting phase near {\it x$_{c}$}, where the incommensurability $δ$ monotonically increases upon doping across the phase boundary. % These results are discussed in connection with the doping-induced superconducting phase transition.

cond-mat.supr-con↗

arXiv2001

Neutron Diffuse Scattering from Polar Nanoregions in the Relaxor Pb(Mg1/3Nb2/3)O3

We have studied the neutron diffuse scattering in the relaxor PMN. The diffuse scattering appears around the Burns temperature (~620K), indicating its origin from the polar nanoregions (PNR). While the relative diffuse intensities are consistent with previous reports, they are entirely different from those of the lowest-energy TO phonon. Because of that, it has been considered that this TO mode could not be the ferroelectric soft mode. Recently, a neutron scattering study has unambiguously shown that the TO mode does soften on cooling. If the diffuse scattering in PMN originates from the soft mode condensation, then the atomic displacements must satisfy the center of mass condition. But, the atomic displacements determined from diffuse scattering intensities do not fulfill this condition. To resolve this contradiction, we propose a simple model in which the total atomic displacement consists of two components: $δ_{CM}$ is created by the soft mode condensation, satisfying the center of mass condition, and, $δ_{shift}$ represents a uniform displacement of the PNR along their polar direction relative to the surrounding (unpolarized) cubic matrix. Within this framework, we can successfully describe the neutron diffuse scattering intensities observed in PMN.

cond-mat.mtrl-sci↗

arXiv2001

Soft Mode Dynamics Above and Below the Burns Temperature in the Relaxor Pb(Mg_1/3Nb_2/3)O_3

We report neutron inelastic scattering measurements of the lowest-energy transverse optic (TO) phonon branch in the relaxor Pb(Mg_1/3Nb_2/3)O_3 from 400 to 1100 K. Far above the Burns temperature T_d ~ 620 K we observe well-defined propagating TO modes at all wave vectors q, and a zone center TO mode that softens in a manner consistent with that of a ferroelectric soft mode. Below T_d the zone center TO mode is overdamped. This damping extends up to, but not above, the waterfall wave vector q_wf, which is a measure of the average size of the PNR.

cond-mat.mtrl-sci↗

arXiv2001

Phase diagram of the relaxor ferroelectric (1-x)PbZn(1/3)Nb(2/3)O3-xPbTiO3

Recently, a new orthorhombic phase has been discovered in the ferroelectric system Pb(Zn1/3Nb2/3)O3-xPbTiO3 (PZN-xPT) for x= 9%, and for x= 8% after the application of an electric field. In the present work, synchrotron x-ray measurements have been extended to higher concentrations, 10% <= x <=15%. The orthorhombic phase was observed for x= 10%, but, surprisingly, for x>= 11% only a tetragonal phase was found down to 20 K. The orthorhombic phase thus exists only in a narrow concentration range with near vertical phase boundaries on both sides. This orthorhombic symmetry (MC-type) is in contrast to the monoclinic MA-type symmetry recently identified at low temperatures in the PbZr(1-x)TixO3 (PZT) system over a triangle-shaped region of the phase diagram in the range x= 0.46-0.52. To further characterize this relaxor-type system neutron inelastic scattering measurements have also been performed on a crystal of PZN-xPT with x= 15%. The anomalous soft-phonon behaviour (''waterfall'' effect) previously observed for x= 0% and 8% is clearly observed for the 15% crystal, which indicates that the presence of polar nanoregions extends to large values of x.

cond-mat.mtrl-sci↗

arXiv2001

Anomalous transverse acoustic phonon broadening in the relaxor ferroelectric Pb(Mg_1/3Nb_2/3)O_3

The intrinsic linewidth $Γ_{TA}$ of the transverse acoustic (TA) phonon observed in the relaxor ferroelectric compound Pb(Mg$_{1/3}$Nb$_{2/3})_{0.8}$Ti$_{0.2}$O$_3$ (PMN-20%PT) begins to broaden with decreasing temperature around 650 K, nearly 300 K above the ferroelectric transition temperature $T_c$ ($\sim 360$ K). We speculate that this anomalous behavior is directly related to the condensation of polarized, nanometer-sized, regions at the Burns temperature $T_d$. We also observe the ``waterfall'' anomaly previously seen in pure PMN, in which the transverse optic (TO) branch appears to drop precipitously into the TA branch at a finite momentum transfer $q_{wf} \sim 0.15$ Å$^{-1}$. The waterfall feature is seen even at temperatures above $T_d$. This latter result suggests that the PNR exist as dynamic entities above $T_d$.

cond-mat.mtrl-sci↗

arXiv2001

Low symmetry phases in piezoelectric systems: PZN-xPT single crystal and powder

In this review we address some of the experimental challenges found in the x-ray diffraction characterization of the low-symmetry phases recently discovered in the PZT, PZN-PT and PMN-PT piezoelectric systems around their morphotropic phase boundaries. In particular, we discuss the need for special care in the preparation of powder samples made from single crystals in order to avoid degradation and peak-broadening effects.

cond-mat.mtrl-sci↗

arXiv2001

Hole concentration dependence of the magnetic moment in superconducting and insulating La2-xSrxCuO4

Recent neutron scattering measurements on the La2-xSrxCuO4 system have revealed a drastic change of the incommensurate static spin correlations from diagonal in the insulating region to parallel in the superconducting region. We report the doping dependence of the ordered magnetic moment for the hole concentration region 0.03 <= x <= 0.12, focusing on the relationship between the static magnetism and the superconductivity. The elastic magnetic crosssection decreases monotonically with increasing x for 0.03 <= x <= 0.07. We find that the ordered magnetic moment μvaries from ~0.18 (x=0.03) to \~0.06 μ_B/Cu (x=0.07). No significant anomaly is observed at the insulator-superconductor boundary (x ~ 0.055). The elastic magnetic crosssection is enhanced in the vicinity of x=0.12 whose resolution limited width peaks are observed in neutron scattering measurements and where the apparent magntic and superconducting transitions coincide.

cond-mat.supr-con↗

arXiv2001

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.

cond-mat.mtrl-sci↗

arXiv2000

Polarization rotation via a monoclinic phase in the piezoelectric 92%PbZn1/3Nb2/3O3-8%PbTiO3

The origin of ultrahigh piezoelectricity in the relaxor ferroelectric PbZn1/3Nb2/3O3-PbTiO3 was studied with an electric field applied along the [001] direction. The zero-field rhombohedral R phase starts to follow the direct polarization path to tetragonal symmetry via an intermediate monoclinic M phase, but then jumps irreversibly to an alternate path involving a different type of monoclinic distortion. Details of the structure and domain configuration of this novel phase are described. This result suggests that there is a nearby R-M phase boundary as found in the Pb(Ti,Zr)O3 system.

cond-mat.mtrl-sci↗

arXiv2000

Soft Phonon Anomalies in Relaxor Ferroelectrics

A review is given of the phonon anomalies, which have been termed ``waterfalls,'' that were recently discovered through a series of neutron inelastic scattering measurements on the lead-oxide relaxor systems PZN-xPT, PMN, and PZN. We discuss a simple coupled-mode model that has been used successfully to describe the basic features of the waterfall, and which relates this unusual feature to the presence of polar micro-regions.

cond-mat.mtrl-sci↗

arXiv2000

Dynamical effects of the nanometer-sized polarized domains in Pb(Zn1/3Nb2/3)O3

Recent neutron scattering measurements performed on the relaxor ferroelectric Pb[(Zn1/3Nb2/3)0.92Ti0.08]O3 (PZN-8%PT) in its cubic phase at 500 K, have revealed an anomalous ridge of inelastic scattering centered ~0.2 A-1 from the zone center (Gehring et al., Phys. Rev. Lett. 84, 5216 (2000)). This ridge of scattering resembles a waterfall when plotted as a phonon dispersion diagram, and extends vertically from the transverse acoustic (TA) branch near 4 meV to the transverse optic (TO) branch near 9 meV. No zone center optic mode was found. We report new results from an extensive neutron scattering study of pure PZN that exhibits the same waterfall feature. We are able to model the dynamics of the waterfall using a simple coupled-mode model that assumes a strongly q-dependent optic mode linewidth Gamma1(q) that increases sharply near 0.2 A-1 as one approaches the zone center. This model was motivated by the results of Burns and Dacol in 1983, who observed the formation of a randomly-oriented local polarization in PZN at temperatures far above its ferroelectric phase transition temperature. The dramatic increase in Gamma1 is believed to occur when the wavelength of the optic mode becomes comparable to the size of the small polarized micro-regions (PMR) associated with this randomly-oriented local polarization, with the consequence that longer wavelength optic modes cannot propagate and become overdamped. Below Tc=410 K, the intensity of the waterfall diminishes. At lowest temperatures ~30 K the waterfall is absent, and we observe the recovery of a zone center transverse optic mode near 10.5 meV.

cond-mat.mtrl-sci↗

arXiv2000

Macroscopic and Local Magnetic Moments in Si-doped CuGeO$_3$ with Neutron and $μ$SR Studies

The temperature-concentration phase diagram of the Si-doped spin-Peierls compound CuGeO$_{3}$ is investigated by means of neutron scattering and muon spin rotation spectroscopy in order to determine the microscopic distribution of the magnetic and lattice dimerised regions as a function of doping. The analysis of the zero-field muon spectra has confirmed the spatial inhomogeneity of the staggered magnetisation that characterises the antiferromagnetic superlattice peaks observed with neutrons. In addition, the variation of the macroscopic order parameter with doping can be understood by considering the evolution of the local magnetic moment as well as of the various regions contributing to the muon signal.

cond-mat.str-el↗

arXiv2000

Neutron Scattering study of Sr_2Cu_3O_4Cl_2

We report a neutron scattering study on the tetragonal compound Sr_2Cu_3O_4Cl_2, which has two-dimensional (2D) interpenetrating Cu_I and Cu_{II} subsystems, each forming a S=1/2 square lattice quantum Heisenberg antiferromagnet (SLQHA). The mean-field ground state is degenerate, since the inter-subsystem interactions are geometrically frustrated. Magnetic neutron scattering experiments show that quantum fluctuations lift the degeneracy and cause a 2D Ising ordering of the Cu_{II} subsystem. Due to quantum fluctuations a dramatic increase of the Cu_I out-of-plane spin-wave gap is also observed. The temperature dependence and the dispersion of the spin-wave energy are quantitatively explained by spin-wave calculations which include quantum fluctuations explicitly. The values for the nearest-neighbor superexchange interactions between the Cu_I and Cu_{II} ions and between the Cu_{II} ions are determined experimentally to be J_{I-II} = -10(2)meV and J_{II}= 10.5(5)meV, respectively. Due to its small exchange interaction, J_{II}, the 2D dispersion of the Cu_{II} SLQHA can be measured over the whole Brillouin zone with thermal neutrons, and a novel dispersion at the zone boundary, predicted by theory, is confirmed. The instantaneous magnetic correlation length of the Cu_{II} SLQHA is obtained up to a very high temperature, T/J_{II}\approx 0.75. This result is compared with several theoretical predictions as well as recent experiments on the S=1/2 SLQHA.

cond-mat.str-el↗