A Resonant X-ray Scattering Study of Octahedral Tilt Ordering in LaMnO3_3 and Pr1−x_{1-x}Cax_xMnO3_3

We report an x-ray scattering study of octahedral tilt ordering in the manganite series Pr$_{1-x}$Ca$_x$MnO$_3$ with x=0.4 and 0.25 and in LaMnO$_3$. The sensitivity to tilt ordering is achieved by tuning the incident x-ray energy to the L$_I$, L$_{II}$ and L$_{III}$ absorption edges of Pr and La, respectively. The resulting energy-dependent profiles are characterized by a dipole-resonant peak and higher energy fine structure. The polarization dependence is predominantly $\sigma$-to-$\pi$ and the azimuthal dependence follows a sin-squared behavior. These results are similar to those obtained in recent x-ray scattering studies of orbital ordering carried out in these same materials at the Mn K edge. They lead to a description of the cross-section in terms of Templeton scattering in which the tilt ordering breaks the symmetry at the rare earth site. The most interesting result of the present work is our observation that octahedral tilt ordering persists above the orbital ordering transition temperatures in all three samples. Indeed, we identify separate structural transitions which may be associated with the onset of orbital and tilt ordering, respectively, and characterize the loss of tilt ordering versus temperature in LaMnO$_3$.Comment: 24 pages, 8 figure

Coherent X-ray Scattering from Manganite Charge and Orbital Domains

We report coherent x-ray scattering studies of charge and orbital domains in manganite systems. The experiments were carried out on LaMnO_3 and Pr_{0.6}Ca_{0.4}MnO_3, with the incident photon energy tuned near the Mn K edge. At room temperature, the orbital speckle pattern of LaMnO_3 was observed to be constant over a timescale of at least minutes, which is indicative of static orbital domains on this timescale. For Pr_{0.6}Ca_{0.4}MnO_3, both charge and orbital speckle patterns were observed. The observation of the latter rules out the presence of fast orbital fluctuations, while long time series data-- on the order of several minutes-- were suggestive of slow dynamic behavior. In contrast, the charge order speckle patterns were static.Comment: 6 pages, 4 figure

Electronic Structure and Phase Transition in V2O3: Importance of 3d Spin-Orbit Interaction and Lattice Distortion

The 3d electronic structure and phase transition in pure and Cr doped V2O3 are theoretically investigated in relation to the 3d spin-orbit interaction and lattice distortion. A model consisting of the nearest-neighbor V ion pair with full degeneracy of the 3d orbitals is studied within the many-body point of view. It is shown that each V ion with S=1 spin state has a large orbital magnetic moment $\sim 0.7 \mu_{\rm B}$ and no orbital ordering occurs in the antiferromagnetic insulating (AFI) phase. The anomalous resonant Bragg reflection found in the AFI phase is attributed to the magnetic ordering. In the AFI and paramagnetic insulating (PI) phases, Jahn-Teller like lattice instability leads to tilting of the V ion pairs from the corundum c-axis and this causes large difference in the orbital occupation between the paramagnetic metal and the insulating phases, which is consistent with linear dichroic V 2p XAS measurements. To understand the AFI to PI transition, a model spin Hamiltonian is also proposed. The transition is found to be simultaneous order-disorder transition of the magnetic moments and tilting directions of the V ion pairs. Softening of elastic constant C44 and abrupt change in short range spin correlations observed at the transition are also explained.Comment: 18 pages, 16 figure

X-ray Resonant Scattering Studies of Orbital and Charge Ordering in Pr1−x_{1-x}Cax_xMnO3_3

We present the results of a systematic x-ray scattering study of the charge and orbital ordering in the manganite series Pr$_{1-x}$Ca$_x$MnO$_3$ with $x$=0.25, 0.4 and 0.5. The temperature dependence of the scattering at the charge and orbital wavevectors, and of the lattice constants, was characterized throughout the ordered phase of each sample. It was found that the charge and orbital order wavevectors are commensurate with the lattice, in striking contrast to the results of earlier electron diffraction studies of samples with $x$=0.5. High momentum-transfer resolution studies of the x=0.4 and 0.5 samples further revealed that while long-range charge order is present, long-range orbital order is never established. Above the charge/orbital ordering temperature T$_o$, the charge order fluctuations are more highly correlated than the orbital fluctuations. This suggests that charge order drives orbital order in these samples. In addition, a longitudinal modulation of the lattice with the same periodicity as the charge and orbital ordering was discovered in the x=0.4 and 0.5 samples. For x=0.25, only long-range orbital order was observed with no indication of charge ordering, nor of an additional lattice modulation. We also report the results of a preliminary investigation of the loss of charge and orbital ordering in the x=0.4 sample by application of a magnetic field. Finally, the polarization and azimuthal dependence of the charge and orbital ordering in these compounds is characterized both in the resonant and nonresonant limits, and compared with the predictions of current theories. The results are qualitatively consistent with both cluster and LDA+U calculations of the electronic structure.Comment: 37 pages, 22 figure

Correlated Polarons in Dissimilar Perovskite Manganites

We report x-ray scattering studies of broad peaks located at a (0.5 0 0)/(0 0.5 0)-type wavevector in the paramagnetic insulating phases of La_{0.7}Ca_{0.3}MnO_{3} and Pr_{0.7}Ca_{0.3}MnO_{3}. We interpret the scattering in terms of correlated polarons and measure isotropic correlation lengths of 1-2 lattice constants in both samples. Based on the wavevector and correlation lengths, the correlated polarons are found to be consistent with CE-type bipolarons. Differences in behavior between the samples arise as they are cooled through their respective transition temperatures and become ferromagnetic metallic (La_{0.7}Ca_{0.3}MnO_{3}) or charge and orbitally ordered insulating (Pr_{0.7}Ca_{0.3}MnO_{3}). Since the primary difference between the two samples is the trivalent cation size, these results illustrate the robust nature of the correlated polarons to variations in the relative strength of the electron-phonon coupling, and the sensitivity of the low-temperature ground state to such variations.Comment: 13 pages, 6 figure

Resonant x-ray diffraction study of the magnetoresistant perovskite Pr0.6Ca0.4MnO3

We report a x-ray resonant diffraction study of the perovskite Pr0.6Ca0.4MnO3. At the Mn K-edge, this technique is sensitive to details of the electronic structure of the Mn atoms. We discuss the resonant x-ray spectra measured above and below the charge and orbital ordering phase transition temperature (TCOO = 232 K), and present a detailed analysis of the energy and polarization dependence of the resonant scattering. The analysis confirms that the structural transition is a transition to an orbitally ordered phase in which inequivalent Mn atoms are ordered in a CE-type pattern. The Mn atoms differ mostly by their 3d orbital occupation. We find that the charge disproportionation is incomplete, 3d^{3.5-\delta} and 3d^{3.5+\delta} with \delta\ll0.5 . A revised CE-type model is considered in which there are two Mn sublattices, each with partial e_{g} occupancy. One sublattice consists of Mn atoms with the 3x^{2}-r^{2} or 3y^{2}-r^{2} orbitals partially occupied, the other sublattice with the x^{2}-y^{2} orbital partially occupied.Comment: 15 pages, 15 figure

Substrate-induced strain effects on Pr_{0.6}Ca_{0.4}MnO_{3} films

We report the characterization of the crystal structure, low-temperature charge and orbital ordering, transport, and magnetization of Pr_{0.6}Ca_{0.4}MnO_{3} films grown on LaAlO_{3}, NdGaO_{3}, and SrTiO_{3} substrates, which provide compressive (LaAlO_{3}) and tensile (NdGaO_{3} and SrTiO_{3}) strain. The films are observed to exhibit different crystallographic symmetries than the bulk material, and the low-temperature ordering is found to be more robust under compressive-- as opposed to tensile-- strain. In fact, bulk-like charge and orbital ordering is not observed in the film grown on NdGaO_{3}, which is the substrate that provides the least amount of nominal and measured, but tensile, strain. This result suggests the importance of the role played by the Mn--O--Mn bond angles in the formation of charge and orbital ordering at low temperatures. Finally, in the film grown on LaAlO_{3}, a connection between the lattice distortion associated with orbital ordering and the onset of antiferromagnetism is reported.Comment: 12 pages, 7 figure

Local optical excitations in metals

U of I OnlyThesi

Recent Highlights of X-Ray Magnetic Scattering Studies from Surfaces.

Abstract not availableJRC.E-Institute for Transuranium Elements (Karlsruhe

Recent Highlights of X-Ray Magnetic Scattering Studies from Surfaces

In this work, recent studies of surface magnetism, as observed by x-ray scattering techniques, are described. The experiments were concerned with uranium dioxide crystals for which x-ray resonance effects enhance the small magnetic signal from the surface. The main result is that, in contrast to the bulk which exhibits a discontinuous magnetic ordering transition, both the (001) and (111) surface layers order continuously. This is reminiscent of the general phenomenon of surface wetting, but had not been previously observed for magnetic materials. Magnetic reflectivity studies show further that the near-surface magnetic layers are more disordered than layers deep in the bulk, even at low temperatures