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.
We study optical excitations across the Mott gap in the multi-orbital Mott-Hubbard insulators RVO3. The multi-peak structure observed in the optical conductivity can be described consistently in terms of the different 3d^3 multiplets or upper Hubbard
bands. The spectral weight is very sensitive to nearest-neighbor spin-spin and orbital-orbital correlations and thus shows a pronounced dependence on both temperature and polarization. Comparison with theoretical predictions based on either rigid orbital order or strong orbital fluctuations clearly rules out the latter. Both, the line shape and the temperature dependence give clear evidence for the importance of excitonic effects.
