Orbital excitations in CMR progenitor of LaMnO3 studied by resonant inelastic x-ray scattering

We present a formula for the calculation of K-edge resonant inelastic x-ray scattering on transition metal compounds, based on a local interaction between the valence shell electrons and the $1s$ core hole. Extending a previous result, we include explicit momentum dependence and a basis with multiple core-hole sites. We apply this formula to a single-layered charge, orbital and spin ordered manganite, La$_{0.5}$Sr$_{1.5}$MnO$_4$, and obtain good agreement with experimental da...

We investigated the origin of the energy splitting observed in the resonant x-ray scattering (RXS) in manganites. Using thin film samples with controlled lattice parameters and orbital states at a fixed orbital filling, we estimated that the contribution of the interatomic Coulomb interaction relative to the Jahn-Teller mechanism is insignificant and at most 0.27. This indicates that RXS probes mainly Jahn-Teller distortion in manganites.

We review our recent x-ray scattering studies of charge and orbital order in doped manganites, with specific emphasis on the role of orbital correlations in Pr_1-xCa_xMnO_3. For x=0.25, we find an orbital structure indistinguishable from the undoped structure with long range orbital order at low temperatures. For dopings 0.3<x<0.5, we find scattering consistent with a charge and orbitally ordered CE-type structure. While in each case the charge order peaks are resolution limi...

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 patte...

We report the observation of temperature dependent electronic excitations in various manganites utilizing resonant inelastic x-ray scattering (RIXS) at the Mn K-edge. Excitations were observed between 1.5 and 16 eV with temperature dependence found as high as 10 eV. The change in spectral weight between 1.5 and 5 eV was found to be related to the magnetic order and independent of the conductivity. On the basis of LDA+U and Wannier function calculations, this dependence is ass...

A theory of resonant x-ray scattering in perovskite manganites is developed by applying the group theory to the correlation functions of the pseudospin operators for the orbital degree of freedom. It is shown that static and dynamical informations of the orbital state are directly obtained from the elastic, diffuse and inelastic scatterings due to the tensor character of the scattering factor. We propose that the interaction and its anisotropy between orbitals are directly id...

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 $\si...

We present an analysis of the dependence of the resonant orbital order and magnetic scattering spectra on the spin configuration. We consider an arbitrary spin direction with respect to the local crystal field axis, thus lowering significantly the local symmetry. To evaluate the atomic scattering in this case, we generalized the Hannon-Trammel formula and implemented it inside the framework of atomic multiplet calculations in a crystal field. For an illustration, we calculate...

We have studied the orbital ordering (OO) in La0.5Sr1.5MnO4 and its soft x-ray resonant diffraction spectroscopic signature at the Mn L2, L3 edges. We have modelled the system in second quantization as a small planar cluster consisting of a central Mn atom, with the first neighbouring shells of oxygen and Mn atoms. For the effective Hamiltonian we consider Slater-Koster parameters, charge transfer and electron correlation energies obtained from previous measurements on mang...

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...