Contiguous 3d and 4f magnetism: towards strongly correlated 3d electrons in YbFe2Al10

We present magnetization, specific heat, and 27Al NMR investigations on YbFe2Al10 over a wide range in temperature and magnetic field. The magnetic susceptibility at low temperatures is strongly enhanced at weak magnetic fields, accompanied by a ln(T0/T) divergence of the low-T specific heat coefficient in zero field, which indicates a ground state of correlated electrons. From our hard X-ray photo emission spectroscopy (HAXPES) study, the Yb valence at 50 K is evaluated to be 2.38. The system displays valence fluctuating behavior in the low to intermediate temperature range, whereas above 400 K, Yb3+ carries a full and stable moment, and Fe carries a moment of about 3.1 mB. The enhanced value of the Sommerfeld Wilson ratio and the dynamic scaling of spin-lattice relaxation rate divided by T [27(1/T1T)] with static susceptibility suggests admixed ferromagnetic correlations. 27(1/T1T) simultaneously tracks the valence fluctuations from the 4f -Yb ions in the high temperature range and field dependent antiferromagnetic correlations among partially Kondo screened Fe 3d moments at low temperature, the latter evolve out of an Yb 4f admixed conduction band.Comment: To appear in Phys. Rev. Let

Quantitative study of valence and configuration interaction parameters of the Kondo semiconductors CeM2Al10 (M = Ru, Os and Fe) by means of bulk-sensitive hard x-ray photoelectron spectroscopy

The occupancy of the 4f^n contributions in the Kondo semiconductors CeM2Al10(M = Ru, Os and Fe) has been quantitatively determined by means of bulk-sensitive hard x-ray photoelectron spectroscopy (HAXPES) on the Ce 3d core levels. Combining a configuration interaction scheme with full multiplet calculations allowed to accurately describe the HAXPES data despite the presence of strong plasmon excitations in the spectra. The configuration interaction parameters obtained from this analysis -- in particular the hybridization strength V_eff and the effective f binding energy Delta_f -- indicate a slightly stronger exchange interaction in CeOs2Al10 compared to CeRu2Al10, and a significant increase in CeFe2Al10. This verifies the coexistence of a substantial amount of Kondo screening with magnetic order and places the entire CeM2Al10 family in the region of strong exchange interactions.Comment: 9 pages, 4 figures, submitted to Physical Review

Bulk and surface electronic properties of SmB6: a hard x-ray photoelectron spectroscopy study

We have carried out bulk-sensitive hard x-ray photoelectron spectroscopy (HAXPES) measurements on in-situ cleaved and ex-situ polished SmB6 single crystals. Using the multiplet-structure in the Sm 3d core level spectra, we determined reliably that the valence of Sm in bulk SmB6 is close to 2.55 at ~5 K. Temperature dependent measurements revealed that the Sm valence gradually increases to 2.64 at 300 K. From a detailed line shape analysis we can clearly observe that not only the J=0 but also the J=1 state of the Sm 4f 6 configuration becomes occupied at elevated temperatures. Making use of the polarization dependence, we were able to identify and extract the Sm 4f spectral weight of the bulk material. Finally, we revealed that the oxidized or chemically damaged surface region of the ex-situ polished SmB6 single crystal is surprisingly thin, about 1 nm only.Comment: 11 pages, 8 figure

Intricacies of the Co3+^{3+} spin state in Sr2_2Co0.5_{0.5}Ir0.5_{0.5}O4_4: an x-ray absorption and magnetic circular dichroism study

We report on a combined soft x-ray absorption and magnetic circular dichroism (XMCD) study at the Co-$L_{3,2}$ on the hybrid 3$d$/5$d$ solid state oxide Sr$_2$Co$_{0.5}$Ir$_{0.5}$O$_4$ with the K$_2$NiF$_4$ structure. Our data indicate unambiguously a pure high spin state $(S=2)$ for the Co$^{3+}$ (3$d^6$) ions with a significant unquenched orbital moment $L_z/2S_z=0.25$ despite the sizeable elongation of the CoO$_6$ octahedra. Using quantitative model calculations based on parameters consistent with our spectra, we have investigated the stability of this high spin state with respect to the competing low spin and intermediate spin states.Comment: 7 pages, 4 figure

Low-temperature coherence in the periodic Anderson model: Predictions for photoemission of heavy Fermions

We present numerically exact predictions of the periodic and single-impurity Anderson models to address photoemission experiments on heavy Fermion systems. Unlike the single impurity model the lattice model is able to account for the enhanced intensity, dispersion, and apparent weak temperature dependence of the Kondo resonant peak seen in recent controversial photoemission experiments. We present a consistent interpretation of these results as a crossover from the impurity regime to an effective Hubbard model regime described by Nozieres.Comment: 4 pages, 3 figure

Long-range interactions in the effective low energy Hamiltonian of Sr2IrO4: a core level resonant inelastic x-ray scattering study

We have investigated the electronic structure of Sr2IrO4 using core level resonant inelastic x-ray scattering. The experimental spectra can be well reproduced using ab initio density functional theory based multiplet ligand field theory calculations, thereby validating these calculations. We found that the low-energy, effective Ir t2g orbitals are practically degenerate in energy. We uncovered that covalency in Sr2IrO4, and generally in iridates, is very large with substantial oxygen ligand hole character in the Ir t2g Wannier orbitals. This has far reaching consequences, as not only the onsite crystal-field energies are determined by the long range crystal-structure, but, more significantly, magnetic exchange interactions will have long range distance dependent anisotropies in the spin direction. These findings set constraints and show pathways for the design of d^5 materials that can host compass-like magnetic interactions

Electronically highly cubic conditions for Ru in alpha-RuCl3

We studied the local Ru 4d electronic structure of alpha-RuCl3 by means of polarization dependent x-ray absorption spectroscopy at the Ru-L2,3 edges. We observed a vanishingly small linear dichroism indicating that electronically the Ru 4d local symmetry is highly cubic. Using full multiplet cluster calculations we were able to reproduce the spectra excellently and to extract that the trigonal splitting of the t2g orbitals is -12 $\pm10$ meV, i.e. negligible as compared to the Ru 4d spin-orbit coupling constant. Consistent with our magnetic circular dichroism measurements, we found that the ratio of the orbital and spin moments is 2.0, the value expected for a Jeff = 1/2 ground state. We have thus shown that as far as the Ru 4d local properties are concerned, alpha-RuCl3 is an ideal candidate for the realization of Kitaev physics

Electronic signature of the vacancy ordering in NbO (Nb3O3)

We investigated the electronic structure of the vacancy-ordered 4d-transition metal monoxide NbO (Nb3O3) using angle-integrated soft- and hard-x-ray photoelectron spectroscopy as well as ultra-violet angle-resolved photoelectron spectroscopy. We found that density-functional-based band structure calculations can describe the spectral features accurately provided that self-interaction effects are taken into account. In the angle-resolved spectra we were able to identify the so-called vacancy band that characterizes the ordering of the vacancies. This together with the band structure results indicates the important role of the very large inter-Nb-4d hybridization for the formation of the ordered vacancies and the high thermal stability of the ordered structure of niobium monoxide

Orbitally driven spin-singlet dimerization in SS=1 La4_{4}Ru2_{2}O10_{10}

Using x-ray absorption spectroscopy at the Ru-$L_{2,3}$ edge we reveal that the Ru$^{4+}$ ions remain in the $S$=1 spin state across the rare 4d-orbital ordering transition and spin-gap formation. We find using local spin density approximation + Hubbard U (LSDA+U) band structure calculations that the crystal fields in the low temperature phase are not strong enough to stabilize the $S$=0 state. Instead, we identify a distinct orbital ordering with a significant anisotropy of the antiferromagnetic exchange couplings. We conclude that La$_{4}$Ru$_{2}$O$_{10}$ appears to be a novel material in which the orbital physics drives the formation of spin-singlet dimers in a quasi 2-dimensional $S$=1 system.Comment: 5 pages, 4 figures, and 1 tabl