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We report on the observation of orbital excitations in YVO3 by means of resonant inelastic x-ray scattering (RIXS) at energies across the vanadium L3 and oxygen K absorption edges. Due to the excellent experimental resolution we are able to resolve t he intra-t2g excitations at 0.1-0.2 eV, 1.07 eV, and 1.28 eV, the lowest excitations from the t2g into the eg levels at 1.86 eV, and further excitations above 2.2 eV. For the intra-t2g excitations at 0.1-0.2 eV, the RIXS peaks show small shifts of the order of 10-40 meV as a function of temperature and of about 13-20 meV as a function of the transferred momentum q||a. We argue that the latter reflects a finite dispersion of the orbital excitations. For incident energies tuned to the oxygen K edge, RIXS is more sensitive to intersite excitations. We observe excitations across the Mott-Hubbard gap and find an additional feature at 0.4 eV which we attribute to two-orbiton scattering, i.e., an exchange of orbitals between adjacent sites. Altogether, these results indicate that both superexchange interactions and the coupling to the lattice are important for a quantitative understanding of the orbital excitations in YVO3.
83 - J. Reul , L. Fels , N. Qureshi 2013
Compounds with intermediate-size transition metals such as Fe or Mn are close to the transition between charge-transfer systems and Mott-Hubbard systems. We study the optical conductivity sigma(omega) of insulating layered LaSrFeO_4 in the energy ran ge 0.5 - 5.5 eV from 15 K to 250 K by the use of spectroscopic ellipsometry in combination with transmittance measurements. A multipeak structure is observed in both sigma^a(omega) and sigma^c(omega). The layered structure gives rise to a pronounced anisotropy, thereby offering a means to disentangle Mott-Hubbard and charge-transfer absorption bands. We find strong evidence that the lowest dipole-allowed excitation in LaSrFeO_4 is of Mott-Hubbard type. This rather unexpected result can be attributed to Fe 3d - O 2p hybridization and in particular to the layered structure with the associated splitting of the e_g level. In general, Mott-Hubbard absorption bands may show a strong dependence on temperature. This is not the case in LaSrFeO_4, in agreement with the fact that spin-spin and orbital-orbital correlations between nearest neighbors do not vary strongly below room temperature in this compound with a high-spin 3d^5 configuration and a Neel temperature of T_N = 366 K.
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