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E. Benckiser

Publications and source records attributed to E. Benckiser.

25 records · Page 2Linked to original sources

Orbital superexchange and crystal field simultaneously at play in YVO3: resonant inelastic x-ray scattering at the V L edge and the O K edge

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 the 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.

cond-mat.str-el↗

Orbital control of noncollinear magnetic order in nickelate heterostructures

We have used resonant x-ray diffraction to develop a detailed description of antiferromagnetic ordering in epitaxial superlattices based on two-unit-cell thick layers of the strongly correlated metal LaNiO3. We also report reference experiments on thin films of PrNiO3 and NdNiO3. The resulting data indicate a spiral state whose polarization plane can be controlled by adjusting the Ni d-orbital occupation via two independent mechanisms: epitaxial strain and quantum confinement of the valence electrons. The data are discussed in the light of recent theoretical predictions.

cond-mat.str-el↗

Magnetic proximity effect in $\mathbf{YBa_2Cu_3O_7/La_{2/3}Ca_{1/3}MnO_3}$ and $\mathbf{YBa_2Cu_3O_7/LaMnO_{3+δ}}$ superlattices

Using neutron reflectometry and resonant x-ray techniques we studied the magnetic proximity effect (MPE) in superlattices composed of superconducting YBa$_2$Cu$_3$O$_7$ (YBCO) and ferromagnetic-metallic (FM-M) La$_{0.67}$Ca$_{0.33}$MnO$_{3}$ (LCMO) or ferromagnetic-insulating (FM-I) LaMnO$_{3+δ}$ (LMO). We find that the MPE strongly depends on the electronic state of the manganite layers, being pronounced for the FM-M LCMO and almost absent for FM-I LMO. We also detail the change of the magnetic depth profile due to the MPE and provide evidence for its intrinsic nature.

cond-mat.str-el↗

Dimensionality Control of Electronic Phase Transitions in Nickel-Oxide Superlattices

The competition between collective quantum phases in materials with strongly correlated electrons depends sensitively on the dimensionality of the electron system, which is difficult to control by standard solid-state chemistry. We have fabricated superlattices of the paramagnetic metal LaNiO3 and the wide-gap insulator LaAlO3 with atomically precise layer sequences. Using optical ellipsometry and low-energy muon spin rotation, superlattices with LaNiO3 as thin as two unit cells are shown to undergo a sequence of collective metalinsulator and antiferromagnetic transitions as a function of decreasing temperature, whereas samples with thicker LaNiO3 layers remain metallic and paramagnetic at all temperatures. Metal-oxide superlattices thus allow control of the dimensionality and collective phase behavior of correlated-electron systems.

cond-mat.str-el↗

Orbital reflectometry

The occupation of d-orbitals controls the magnitude and anisotropy of the inter-atomic electron transfer in transition metal oxides and hence exerts a key influence on their chemical bonding and physical properties. Atomic-scale modulations of the orbital occupation at surfaces and interfaces are believed to be responsible for massive variations of the magnetic and transport properties, but could thus far not be probed in a quantitative manner. Here we show that it is possible to derive quantitative, spatially resolved orbital polarization profiles from soft x-ray reflectivity data, without resorting to model calculations. We demonstrate that the method is sensitive enough to resolve differences of 3 % in the occupation of Ni e_g orbitals in adjacent atomic layers of a LaNiO3-LaAlO3 superlattice, in good agreement with ab-initio electronic-structure calculations. The possibility to quantitatively correlate theory and experiment on the atomic scale opens up many new perspectives for orbital physics in d-electron materials.

cond-mat.str-el↗

Collective orbital excitations in orbitally ordered YVO3 and HoVO3

We study orbital excitations in the optical absorption spectra of YVO3 and HoVO3. We focus on an orbital absorption band observed at 0.4 eV for polarization E parallel c. This feature is only observed in the intermediate, monoclinic phase. By comparison with the local crystal-field excitations in VOCl and with recent theoretical predictions for the crystal-field levels we show that this absorption band cannot be interpreted in terms of a local crystal-field excitation. We discuss a microscopic model which attributes this absorption band to the exchange of two orbitals on adjacent sites, i.e., to the direct excitation of two orbitons. This model is strongly supported by the observed dependence on polarization and temperature. Moreover, the calculated spectral weight is in good agreement with the experimental result.

cond-mat.str-el↗

Optical study of orbital excitations in transition-metal oxides

The orbital excitations of a series of transition-metal compounds are studied by means of optical spectroscopy. Our aim was to identify signatures of collective orbital excitations by comparison with experimental and theoretical results for predominantly local crystal-field excitations. To this end, we have studied TiOCl, RTiO3 (R=La, Sm, Y), LaMnO3, Y2BaNiO5, CaCu2O3, and K4Cu4OCl10, ranging from early to late transition-metal ions, from t_2g to e_g systems, and including systems in which the exchange coupling is predominantly three-dimensional, one-dimensional or zero-dimensional. With the exception of LaMnO3, we find orbital excitations in all compounds. We discuss the competition between orbital fluctuations (for dominant exchange coupling) and crystal-field splitting (for dominant coupling to the lattice). Comparison of our experimental results with configuration-interaction cluster calculations in general yield good agreement, demonstrating that the coupling to the lattice is important for a quantitative description of the orbital excitations in these compounds. However, detailed theoretical predictions for the contribution of collective orbital modes to the optical conductivity (e.g., the line shape or the polarization dependence) are required to decide on a possible contribution of orbital fluctuations at low energies, in particular in case of the orbital excitations at about 0.25 eV in RTiO3. Further calculations are called for which take into account the exchange interactions between the orbitals and the coupling to the lattice on an equal footing.

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