Dispersion of the dielectric function of a charge-transfer insulator

We study the problem of dielectric response in the strong coupling regime of a charge transfer insulator. The frequency and wave number dependence of the dielectric function $\epsilon ({\bf q},\omega)$ and its inverse $\epsilon ^{-1}({\bf q},\omega)$ is the main object of consideration. We show that the problem, in general, cannot be reduced to a calculation within the Hubbard model, which takes into account only a restricted number of electronic states near the Fermi energy. The contribution of the rest of the system to the longitudinal response (i.e. to $\epsilon ^{-1}({\bf q},\omega)$) is essential for the whole frequency range. With the use of the spectral representation of the two-particle Green's function we show that the problem may be divided into two parts: into the contributions of the weakly correlated and the Hubbard subsystems. For the latter we propose an approach that starts from the correlated paramagnetic ground state with strong antiferromagnetic fluctuations. We obtain a set of coupled equations of motion for the two-particle Green's function that may be solved by means of the projection technique. The solution is expressed by a two particle basis that includes the excitonic states with electron and hole separated at various distances. We apply our method to the multiband Hubbard (Emery) model that describes layered cuprates. We show that strongly dispersive branches exist in the excitonic spectrum of the 'minimal' Emery model ($1/U_d=U_p=t_{pp}=0$) and consider the dependence of the spectrum on finite oxygen hopping $t_{pp}$ and on-site repulsion $U_p$. The relationship of our calculations to electron energy loss spectroscopy is discussed.Comment: 22 pages, 5 figure

The dynamics of a hole in a CuO_4 plaquette: electron energy-loss spectroscopy of Li_2CuO_2

We have measured the energy and momentum dependent loss function of Li_2CuO_2 single crystals by means of electron energy-loss spectroscopy in transmission. Using the same values for the model parameters, the low-energy features of the spectrum as well as published Cu 2p_(3/2) x-ray photoemission data of Li_2CuO_2 are well described by a cluster model that consists of a single CuO_4 plaquette only. This demonstrates that charge excitations in Li_2CuO_2 are strongly localized.Comment: 5 pages, 5 figure

One-dimensional dynamics of the d-electrons in α′\alpha'-NaV2_{2}O5_{5}

We have studied the electronic properties of the ladder compound $\alpha'$-NaV$_{2}$O$_{5}$, adopting a joint experimental and theoretical approach. The momentum-dependent loss function was measured using electron energy-loss spectroscopy in transmission. The optical conductivity derived from the loss function by a Kramers-Kronig analysis agrees well with our results from LSDA+U band-structure calculations upon application of an antiferromagnetic alignment of the V~3$d_{xy}$ spins along the legs and an on-site Coulomb interaction U of between 2 and 3 eV. The decomposition of the calculated optical conductivity into contributions from transitions between selected energy regions of the DOS reveals the origin of the observed anisotropy of the optical conductivity. In addition, we have investigated the plasmon excitations related to transitions between the vanadium states within an effective 16 site vanadium cluster model. Good agreement between the theoretical and experimental loss function was obtained using the hopping parameters derived from the tight binding fit to the band-structure and moderate Coulomb interactions between the electrons within the ab plane.Comment: 23 pages, 8 figures; submitted to PR

Valence band excitations in V_2O_5

We present a joint theoretical and experimental investigation of the electronic and optical properties of vanadium pentoxide. Electron energy-loss spectroscopy in transmission was employed to measure the momentum-dependent loss function. This in turn was used to derive the optical conductivity, which is compared to the results of band structure calculations. A good qualitative and quantitative agreement between the theoretical and the experimental optical conductivity was observed. The experimentally observed anisotropy of the optical properties of V_2O_5 could be understood in the light of an analysis of the theoretical data involving the decomposition of the calculated optical conductivity into contributions from transitions into selected energy regions of the conduction band. In addition, based upon a tight binding fit to the band structure, values are given for the effective V3d_xy-O2p hopping terms and are compared to the corresponding values for alpha'-NaV_2O_5.Comment: 6 pages (revtex),6 figures (jpg

Temperature dependence of optical spectral weights in quarter-filled ladder systems

The temperature dependence of the integrated optical conductivity I(T) reflects the changes of the kinetic energy as spin and charge correlations develop. It provides a unique way to explore experimentally the kinetic properties of strongly correlated systems. We calculated I(T) in the frame of a t-J-V model at quarter-filling for ladder systems, like NaV_2O_5, and show that the measured strong T dependence of I(T) for NaV_2O_5 can be explained by the destruction of short range antiferromagnetic correlations. Thus I(T) provides detailed information about super-exchange and magnetic energy scales.Comment: 4 pages, 5 figure

Electron Correlation Effects in Resonant Inelastic X-ray Scattering of NaV2O5

Element- and site-specific resonant inelastic x-ray scattering spectroscopy (RIXS) is employed to investigate electron correlation effects in {$\rm NaV_2O_5$}. In contrast to single photon techniques, RIXS at the vanadium $L_3$ edge is able to probe $d-d^*$ transitions between V d-bands. A sharp energy loss feature is observed at -1.56 eV, which is well reproduced by a model calculation including correlation effects. The calculation identifies the loss feature as excitation between the lower and upper Hubbard bands and permits an accurate determination of the Hubbard interaction term $U= 3.0 \pm 0.2$ eV.Comment: 15 pages, four figures, accepted to Phys. Rev. Let

Polarized x-ray absorption spectra of CuGeO3 at the Cu and Ge K edges

Polarized x-ray absorption near edge structure (XANES) spectra at both the Cu and the Ge K-edges of CuGeO3 are measured and calculated relying on the real-space multiple-scattering formalism within a one-electron approach. The polarization components are resolved not only in the unit cell coordinate system but also in a local frame attached to the nearest neighborhood of the photoabsorbing Cu atom. In that way, features which resist a particular theoretical description can be identified. We have found that it is the out-of-CuO4-plane p_{z'} component which defies the one-electron calculation based on the muffin-tin potential. For the Ge K-edge XANES, the agreement between the theory and the experiment appears to be better for those polarization components which probe more compact local surroundings than for those which probe regions with lower atomic density. Paper published in Phys. Rev. B 66, 155119 (2002) and available on-line at http://link.aps.org/abstract/PRB/v66/e155119.Comment: 15 pages, 6 figures. Published in Physical Review B, abstract available on-line at http://link.aps.org/abstract/PRB/e15511

Elektronen-Energieverlustspektroskopie von quasi-eindimensionalen Kupraten und Vanadaten

In a combination of experimental and theoretical methods in this thesis the electronic structures of quasi-one-dimensional cuprates and vanadates were studied. For this the momentum-dependent loss function was measured by means of the electron energy-loss spectroscopy in transmission on monocrystals of Li_2CuO_2, CuGeO_3, V_2O_5 and #alpha#'-NaVO_5. The comparison of the experimental data with results from band-structure and cluster calculations allowed conclusions on the mobility and correlations of the electrons in these systems.Available from TIB Hannover / FIZ - Fachinformationszzentrum Karlsruhe / TIB - Technische InformationsbibliothekSIGLEDEGerman