SrTiO3 displacive transition revisited via coherent X-ray diffraction

We present a coherent x-ray diffraction study of the antiferrodistortive displacive transition of SrTiO3, a prototypical example of a phase transition for which the critical fluctuations exhibit two length scales and two time scales. From the microbeam x-ray coherent diffraction patterns, we show that the broad (short-length scale) and the narrow (long-length scale) components can be spatially disentangled, due to 100-microm-scale spatial variations of the latter. Moreover, both components exhibit a speckle pattern, which is static on a approximately 10 mn time scale. This gives evidence that the narrow component corresponds to static ordered domains. We interpret the speckles in the broad component as due to a very slow dynamical process, corresponding to the well-known central peak seen in inelastic neutron scattering.     

Observation of nanoscale 180 degrees stripe domains in ferroelectric PbTiO3 thin films

We report the observation of periodic 180 degrees stripe domains below the ferroelectric transition in thin films. Epitaxial PbTiO3 films of thickness d=1.6 to 42 nm on SrTiO3 substrates were studied using x-ray scattering. Upon cooling below T(C), satellites appeared around Bragg peaks indicating the presence of 180 degrees stripe domains of period Lambda=3.7 to 24 nm. The dependence of Lambda on d agrees well with theory including epitaxial strain effects, while the suppression of T(C) for thinner films is significantly larger than that expected solely from stripe domains.     

Multiple time scales in diffraction measurements of diffusive surface relaxation

We grew SrTiO3 on SrTiO3(001) by pulsed laser deposition, using x-ray scattering to monitor the growth in real time. The time-resolved small-angle scattering exhibits a well-defined length scale associated with the spacing between unit-cell high surface features. This length scale imposes a discrete spectrum of Fourier components and rate constants upon the diffusion equation solution, evident in multiple exponential relaxation of the "anti-Bragg" diffracted intensity. An Arrhenius analysis of measured rate constants confirms that they originate from a single activation energy.     

Determination of inelastic critical scattering at a first order phase transition in the CDW structure of 1TTaS2 using Mössbauer diffraction

We report Mössbauer diffraction measurements of the temperature dependence of the elastic and inelastic intensities at the (100) Bragg reflection in 1TTaS₂. These measurements use a newly developed microfoil conversion electron (MICE) spectrometry. They cover the temperature range from 19°C to 100°C, bracketing the first order 1T₁ to 1T₂ phase transition in the charge density wave structure at 79°C. The elastic Bragg peak shows a discontinuity at the phase transition as reported by Moret and Colella. The inelastic scattering shows a significant peak near the phase transition. This peak is interpreted as inelastic critical scattering at this first order phase transition.     

Elastic and anelastic relaxations in the relaxor ferroelectric Pb(Mg1/3Nb2/3)O3: I. Strain analysis and a static order parameter

The structural evolution of Pb(Mg(1/3)Nb(2/3))O(3) (PMN) has been reviewed in terms of characteristic temperatures, length scales and timescales, with a view to considering the overall relaxor behaviour from the perspectives of strain and elasticity. A conventional analysis of lattice parameter data in terms of spontaneous strain and strain/order parameter coupling shows that even though a normal phase transition does not occur the relaxor ordering process is accompanied by a significant volume strain which follows the pattern of a static order parameter evolving according to that expected for a tricritical phase transition with T(c) ≈ 350 K. This matches the evolution of the intensity of the elastic central peak in neutron scattering spectra, and reflects the development of static (or quasistatic) polar nanoregions (PNRs) as if by a mean-field phase transition. Use of a Landau free energy expansion, which includes Γ4(-) order parameter components to describe ferroelectric contributions and an R1(+) order parameter to describe cation ordering together with their formal coupling with strain, then allows the pattern of elastic softening expected for a cubic → rhombohedral phase transition to be anticipated. The extent to which observed softening differs from this static mean-field pattern serves to highlight the additional roles of local heterogeneity and relaxation dynamics in determining the relaxor properties of PMN.     

Unconventional magnetic correlations in DyB2C and HoB2C

Layered borocarbides RB2C (R=Dy, Ho, and Er) have been studied by powder neutron diffraction at 2-30 K. ErB2C has two-sublattice antiferromagnetic order below T(N)=16.3 K, but DyB2C and HoB2C show a coexistence of a conventional canted k=(000) ferromagnetic structure and unconventional magnetic correlations. The k=(000) phase orders at T(c)=8.5 K (DyB2C) and 7.1 K (HoB2C), but low-Q diffraction peaks from the unconventional correlations appear above T(c) with different critical temperatures for different peaks: at 8, 10.5, and 15.7 K for HoB2C. This scattering is fitted as diffraction from a Warren-type random magnetic layer lattice and may result from quadrupolar interactions between R3+ spins.     

Electric-field-induced soft-mode hardening in SrTiO3 films

We have studied electric-field-induced Raman scattering in SrTiO3 thin films using an indium-tin-oxide/SrTiO3/SrRuO3 structure grown by pulsed laser deposition. The soft mode polarized along the field becomes Raman active. Experimental data for electric-field-induced hardening of the soft modes and the tuning of the static dielectric constant are in agreement described by the Lyddane-Sachs-Teller formalism. The markedly different behavior of the soft modes in thin films from that in the bulk is explained by the existence of local polar regions.     

Ordering process of Cu3Pt from short-range order state studied by in-situ TEM observation

The state of short-range order (SRO) and the ordering process in Cu3Pt have been studied by the in-situ transmission electron microscope observation method. In order to detect weak diffraction-patterns and weak image-contrasts, an imaging plate system and/or digital-process of video-recorded signals were applied. It is confirmed that above the critical temperature for ordering, Tc, the alloy shows diffuse scattering in its electron diffraction pattern. The appearance of the diffuse scattering indicates that the "disordered" Cu3Pt (designated as A1) has an SRO-state in thermoequilibrium. Dark field images taken by using the diffuse scattering shows a fine dot-contrast, which indicates the presence of "microdomains". The dot-contrast is flickering at higher temperatures, but the rate of flickering decreases with falling temperature and finally stops before reaching Tc. On further decreasing temperature, some of the microdomains grow up to large domains of the long period superstructure (L12-s) phase. This indicates that the transformation to L12-s via SRO proceeds without a process of nucleation even though the transformation is of a first-order.     

Unusual behavior of the ferroelectric polarization in PbTiO3/SrTiO3 superlattices

Artificial PbTiO3/SrTiO3 superlattices were constructed using off-axis rf magnetron sputtering. X-ray diffraction and piezoelectric atomic force microscopy were used to study the evolution of the ferroelectric polarization as the ratio of PbTiO3 to SrTiO3 was changed. For PbTiO3 layer thicknesses larger than the 3-unit cell SrTiO3 thickness used in the structure, the polarization is found to be reduced as the thickness is decreased. This observation confirms the primary role of the depolarization field in the polarization reduction in thin films. For the samples with ratios of PbTiO3 to SrTiO3 of less than one, a surprising recovery of ferroelectricity that cannot be explained by electrostatic considerations was observed.     

Photoemission from buried interfaces in SrTiO3/LaTiO3 superlattices

We have measured photoemission spectra of SrTiO3/LaTiO3 superlattices with a topmost SrTiO3 layer of variable thickness. A finite coherent spectral weight with a clear Fermi cutoff was observed at chemically abrupt SrTiO3/LaTiO3 interfaces, indicating that an "electronic reconstruction" occurs at the interface between the Mott insulator LaTiO3 and the band insulator SrTiO3. For SrTiO3/LaTiO3 interfaces annealed at high temperatures (approximately 1000 degrees C), which leads to Sr/La atomic interdiffusion and hence to the formation of La(1-x)Sr(x)TiO3-like material, the intensity of the incoherent part was found to be dramatically reduced whereas the coherent part with a sharp Fermi cutoff was enhanced due to the spread of charge. These important experimental features are well reproduced by layer dynamical-mean-field-theory calculation.     

明胶水溶液分形性质的光散射研究

本文通过动态光散射技术并结合静态光散射及粘滞系数实验研究了明胶水溶液在不同温度、不同浓度下的分形性质。当Ｔ＞Ｔｇｅｌ时（Ｔｇｅｌ为胶凝临界温度），水为明胶的良好溶剂。明胶分子在水溶液中符合自避无规行走模型，分维ｄｆ＝５／３。当Ｔ＜Ｔｇｅｌ时，明胶水溶液需经历从溶液到凝胶的胶凝过程。在胶凝过程中，动态光散射弛豫谱分段具有指数衰减和随后的伸展指数两种模式，且伸展指数衰减的宽度参数β逐渐从０．８减少到胶凝点的０．６７，与此相对应，分维由５／３逐渐增加到２．０。在胶凝点，通过静态光散射及粘滞系数实验测得分维为２．０。     

Improved multiferroic properties of La-doped 0.6BiFeO₃-0.4SrTiO₃ solid solution ceramics

The 0.6(Bi1-xLax)FeO 3-0.4SrTiO 3(x = 0,0.1) multiferroic ceramics are prepared by a modified Pechini method to study the effect of substitution of SrTiO3 and La in BiFeO3.The X-ray diffraction patterns confirm the single phase characteristics of all the compositions each with a rhombohedral structure.The magnetic properties of the ceramics are significantly improved by a solid solution with SrTiO3 and substitution of La.The values of the dielectric constant ε r and loss tangent tan δ of all the samples decrease with increasing frequency and become constant at room temperature.The La-doped 0.6BiFeO3-0.4SrTiO3 ceramics exhibit improved dielectric and ferroelectric properties,with higher dielectric constant enhanced remnant polarization(Pr) and lower leakage current at room temperature.Compared with a anti-ferromagnetic BiFeO3 compound,the 0.6(Bi0.9La0.1)FeO3-0.4SrTiO3 sample shows the optimal ferromagnetism with remnant magnetization M r ～ 0.135 emμ/g and ferroelectricity with Pr ～ 5.94 μC/cm 2 at room temperature.     

Structure of SrTiO3 films on Si

The epitaxial deposition of oxides on silicon opens the possibility of incorporating their diverse properties into silicon-device technology. Deposition of SrTiO(3) on silicon was first reported over a decade ago, but growing the coherent, lattice-matched films that are critical for many applications has been difficult for thicknesses beyond 5 unit cells. Using a combination of density functional calculations and x-ray diffraction measurements, we determine the atomic structure of coherent SrTiO(3) films on silicon, finding that the Sr concentration at the interface varies with the film thickness. The structures with the lowest computed energies best match the x-ray diffraction. During growth, Sr diffuses from the interface to the surface of the film; the increasing difficulty of Sr diffusion with film thickness may cause the disorder seen in thicker films. The identification of this unique thickness-dependent interfacial structure opens the possibility of modifying the interface to improve the thickness and quality of metal oxide films on silicon.     

Central peak in the strontium titanate crystal near the tetragonal-to-cubic phase transition

Raman spectra of the SrTiO3 crystal have been measured in wide temperature (22?C316 K) and frequency (2?C1020 cm^?1) ranges. It has been shown that a central peak appears in low-frequency Raman spectra at temperatures above 70 K. In the spectral geometry with polarization rotation near the temperature T _c = 106 K of the cubic-to-tetragonal phase transition, the central peak exhibits properties of the order-disorder phase transition. Such a behavior of the central peak has been explained by the interaction of the low-frequency soft mode E _g with the relaxation mode near T _c .     

Two dimensional XY type magnetism in intercalated graphite: an elastic and inelastic neutron scattering study

Stage-2 CoCl₂-GIC approximates a two-dimensional easy-plane (XY) ferromagnet on a triangular lattice. It has been found in prior work to order in two steps, with the intermediate phase showing long-ranged ferromagnetic correlations within the intercalate plane, but no correlations between neighboring planes. We have probed the wave vector and temperature dependence of the static and dynamic spin correlations in detail, including measurements of the critical scattering, the quasielastic scattering from vortex diffusion and the spin wave excitations with and without an external magnetic field. Some of the predictions for a Kosterlitz-Thouless type transition are met in this compound, at least qualitatively, including an apparent jump in the spin stiffness at the critical point and the existence of a diffusive central peak in the scattering function possibly originating from vortex autocorrelations. However, there are some inconsistencies between our observations and recent analytical studies as well as Monte Carlo-molecular dynamics simulations of the vortex dynamics that prevent unambigous assignment of the upper critical temperature as a vortex-binding transition.     

Resonant soft x-ray scattering from stepped surfaces of SrTiO3

We studied the resonant diffraction signal from stepped surfaces of SrTiO(3) at the Ti 2p → 3d (L(2,3)) resonance in comparison with x-ray absorption (XAS) and specular reflectivity data. The steps on the surface form an artificial superstructure suitable as a model system for resonant soft x-ray diffraction. A small step density on the surface is sufficient to produce a well defined diffraction peak. We determined the optical parameters of the sample across the resonance and found that the differences between the energy dependence of the x-ray absorption signal, the specular reflectivity and the step-related peak reflect the different quantities probed in these signals. When recorded at low incidence or detection angles, XAS and specular reflectivity spectra are strongly distorted by the changes of the angle of total reflection with energy. The resonant diffraction spectrum is less affected and can be used as a spectroscopic probe even in less favorable geometries.     

Ideal soft mode-type quantum phase transition and phase coexistence at quantum critical point in 18O-exchanged SrTiO3

The quantum ferroelectric phase transition of 18O-exchanged SrTiO3 (x% exchanged SrTiO3 is abbreviated as STO18-x) was investigated by Raman scattering as a function of x. The result indicates the ideal soft mode-type quantum ferroelectric phase transition of STO18-x, where the 18O exchange enhances the softening of the soft mode by the suppression of quantum fluctuation. In the vicinity of the quantum critical point (x approximately xc=33%), the system results in the ferroelectric-paraelectric phase coexistence state, in clear contrast to the homogeneous ferroelectric phase in STO18-x, whose x is sufficiently larger than xc. Simultaneously, the softening of the soft mode becomes strongly rounded with the underdamped oscillation. The present result indicates that the sensitivity of the soft phonon vibration to the mass disorder is dramatically enhanced in the vicinity of the quantum critical point.     

Transport through graphene on SrTiO3

We report transport measurements through graphene on SrTiO(3) substrates as a function of magnetic field B, carrier density n, and temperature T. The large dielectric constant of SrTiO(3) very effectively screens long-range electron-electron interactions and potential fluctuations, making Dirac electrons in graphene virtually noninteracting. The absence of interactions results in an unexpected behavior of the longitudinal resistance in the N=0 Landau level and in a large suppression of the transport gap in nanoribbons. The "bulk" transport properties of graphene at B=0 T, on the contrary, are completely unaffected by the substrate dielectric constant.     

Crystal imperfections and structural phase transitions in perovskites

High‐resolution X-ray scattering measurements of the antiferrodistortive phase transitions in the perovskites SrTiO₃, RbCaF₃ and KMnF₃ have recently revealed the existence of two length scales in the critical scattering above T_e . Here we review these observations and discuss how they might be related to the well known existence of two time scales (the "central peak" problem) in the critical dynamic response function above T_e . We reach the tentative conclusion that within a few degrees of T_e both the time and length scales of the fluctuations are strongly influenced by defects and that the intrinsic critical behaviour is swamped by these effects in most crystals.     

Pressure-induced phase transition(s) in KMnF3 and the importance of the excess volume for phase transitions in perovskite structures

We report a pressure-dependent investigation of KMnF(3) by x-ray diffraction up to 30 GPa. The results are discussed in the framework of Landau theory and in relation to the isostructural phase transition in SrTiO(3). The phase transition temperature near 186 K in KMnF(3) shifts to room temperature at a critical pressure of P(c) = 3.4 GPa; the pressure dependence of the transition point follows ΔP(c)/ΔT(c) = 0.0315 GPa K(-1). The transition becomes second order under high pressure, close to the tricritical point. The phase transition is determined by the rotation of MnF(6) octahedra with their simultaneous expansion along the rotation axis. The rotation angle was found to increase to 10.5° at 24 GPa. An additional anomaly was observed at higher pressure around 25 GPa, suggesting a further phase transition.