We report the first direct resonant soft x-ray scattering observations of orbital ordering. We have studied the low temperature phase of La$_{0.5}$Sr$_{1.5}$MnO$_4$, a compound that displays charge and orbital ordering. Previous claims of orbital ordering in such materials have relied on observations at the Manganese $K$ edge. These claims have been questioned in several theoretical studies. Instead we have employed resonant soft x-ray scattering at the manganese $L_{III}$ and $L_{II}$ edges which probes the orbital ordering directly. Energy scans at constant wavevector are compared to theoretical predictions and suggest that at all temperatures there are two separate contributions to the scattering, direct orbital ordering and strong cooperative Jahn - Teller distortions of the Mn$^{3+}$ ions.
We investigate the high temperature phase of layered manganites, and demonstrate that the charge-orbital phase transition without magnetic order in La$_{0.5}$Sr$_{1.5}$MnO$_4$ can be understood in terms of the density wave instability. The orbital ordering is found to be induced by the nesting between segments of Fermi surface with different orbital characters. The simultaneous charge and orbital orderings are elaborated with a mean field theory. The ordered orbitals are shown to be $d_{x^2-y^2} pm d_{3z^2-r^2}$.
The magnon dispersion in the charge, orbital and spin ordered phase in La(0.5)Sr(1.5)MnO(4) has been studied by means of inelastic neutron scattering. We find an excellent agreement with a magnetic interaction model basing on the CE-type superstructure. The magnetic excitations are dominated by ferromagnetic exchange parameters revealing a nearly-one dimensional character at high energies. The nearest neighbor ferromagnetic interaction in La(0.5)Sr(1.5)MnO(4) is significantly larger than the one in the metallic ferromagnetically ordered manganites. The large ferromagnetic interaction in the charge/orbital ordered phase appears to be essential for the capability of manganites to switch between metallic and insulating phases.
The magnetic correlations in the charge- and orbital-ordered manganite La(0.5)Sr(1.5)MnO(4) have been studied by elastic and inelastic neutron scattering techniques. Out of the well-defined CE-type magnetic structure with the corresponding magnons a competition between CE-type and ferromagnetic fluctuations develops. Whereas ferromagnetic correlations are fully suppressed by the static CE-type order at low temperature, elastic and inelastic CE-type correlations disappear with the melting of the charge-orbital order at high temperature. In its charge-orbital disordered phase, La(0.5)Sr(1.5)MnO(4) exhibits a dispersion of ferromagnetic correlations which remarkably resembles the magnon dispersion in ferromagnetically ordered metallic perovskite manganites.
We studied the charge-orbital ordering in the superlattice of charge-ordered insulating Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ and ferromagnetic metallic La$_{0.5}$Sr$_{0.5}$MnO$_3$ by resonant soft x-ray diffraction. A temperature-dependent incommensurability is found in the orbital order. In addition, a large hysteresis is observed that is caused by phase competition between insulating charge ordered and metallic ferromagnetic states. No magnetic phase transitions are observed in contrast to bulk, confirming the unique character of the superlattice. The deviation from the commensurate orbital order can be directly related to the decrease of ordered-layer thickness that leads to a decoupling of the orbital-ordered planes along the c axis.
We describe a strategy for using resonant soft x-ray scattering (RSXS) to study the electronic structure of transition metal oxide quantum wires. Using electron beam lithography and ion milling, we have produced periodic, patterned arrays of colossal magnetoresistance (CMR) phase La(1-x)Sr(x)MnO(3) consisting of ~ 5000 wires, each of which is 80 nm in width. The scattered intensity exhibits a series of peaks that can be interpreted as Bragg reflections from the periodic structure or, equivalently, diffraction orders from the grating-like structure. RSXS measurements at the Mn L(2,3) edge, which has a large magnetic cross section, show clear evidence for a magnetic superstructure with a commensurate period of five wires, which we interpret as commensurately modulated antiferromagnetism. This superstructure, which is accompanied by non-trivial reorganization of the magnetization within each wire, likely results from classical dipole interactions among the wires. We introduce a simple, exactly soluble, analytic model of the scattering that captures, semi-quantitatively, the primary features in the RSXS data; this model will act as a foundation for forthcoming, detailed studies of the magnetic structure in these systems.
S.B. Wilkins
,P.D. Spencer
,P.D. Hatton
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(2003)
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"Direct observation of orbital ordering in La$_{0.5}$Sr$_{1.5}$MnO$_4$ using soft x-ray diffraction"
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Stuart Wilkins
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