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Register a new userLocal symmetry and magnetic anisotropy in multiferroic MnWO4 and antiferromagnetic CoWO4 studied by soft x-ray absorption spectroscopy
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Soft x-ray absorption experiments on the transition metal L2,3 edge of multiferroic MnWO4 and antiferromagnetic CoWO4 are presented. The observed linear polarization dependence, analyzed by full-multiplet calculations, is used to determine the ground state wave function of the magnetic Mn2+ and Co2+ ions. The impact of the local structure and the spin-orbit coupling on the orbital moment is discussed in terms of the single-ion anisotropy. It is shown that the orbital moment in CoWO4 is responsible for the collinear antiferromagnetism, while the small size of spin-orbit coupling effects make spiral magnetic order in MnWO4 possible, enabling the material to be multiferroic.
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We have studied the local electronic structure of LaMn0.5Co0.5O3 using soft-x-ray absorption spectroscopy at the Co-L_3,2 and Mn-L_3,2 edges. We found a high-spin Co^{2+}--Mn^{4+} valence state for samples with the optimal Curie temperature. We discovered that samples with lower Curie temperatures contain low-spin nonmagnetic Co^{3+} ions. Using soft-x-ray magnetic circular dichroism we established that the Co^{2+} and Mn^{4+} ions are ferromagnetically aligned. We revealed also that the Co^{2+} ions have a large orbital moment: m_orb/m_spin ~ 0.47. Together with model calculations, this suggests the presence of a large magnetocrystalline anisotropy in the material and predicts a non-trivial temperature dependence for the magnetic susceptibility.
The Fe(1+x)Sb compound has been synthesized close to stoichiometry with x = 0.023(8). The compound was investigated by 57Fe Mossbauer spectroscopy in the temperature range 4.2 - 300 K. The antiferromagnetic ordering temperature was found as 232 K i.e. much higher than for the less stoichiometric material. Regular iron was found to occupy two different positions in proportion 2:1. They differ by the electric quadrupole coupling constants and both of them exhibit extremely anisotropic electric field gradient tensor (EFG) with the asymmetry parameter equal one. The negative component of both EFGs is aligned with the c-axis of the hexagonal unit cell, while the positive component is aligned with the <120> direction. Hence, a model describing deviation from the NiAs P63/mmc symmetry group within Fe-planes has been proposed. Spectra in the magnetically ordered state could be explained by introduction of the incommensurate spin spirals propagating through the iron atoms in the direction of the c-axis with a complex pattern of the hyperfine magnetic fields distributed within a-b plane. Hyperfine magnetic field pattern of spirals due to major regular iron is smoothed by the spin polarized itinerant electrons, while the minor regular iron exhibits hyperfine field pattern characteristic of the highly covalent bonds to the adjacent antimony atoms. The excess interstitial iron orders magnetically at the same temperature as the regular iron, and magnetic moments of these atoms are likely to form two-dimensional spin glass with moments lying in the a-b plane. The upturn of the hyperfine field for minor regular iron and interstitial iron is observed below 80 K. Magneto-elastic effects are smaller than for FeAs, however the recoilless fraction increases significantly upon transition to the magnetically ordered state.
We have measured the intricate temperature dependence of the Co L2,3 x-ray absorption spectra (2p-3d excitations) of CoO. To allow for accurate total electron yield measurements, the material has been grown in thin film form on a metallic substrate in order to avoid charging problems usually encountered during electron spectroscopic studies on bulk CoO samples. The changes in spectra due to temperature are in good agreement with detailed ligand-field calculations indicating that these changes are mostly due to thermal population of closely lying excited states, originating from degenerate t2g levels lifted by the spin-orbit coupling. Magnetic coupling in the ordered phase, modeled as a mean-field exchange field, mixes in excited states inducing a tetragonal charge density. The spin-orbit coupling induced splitting of the low energy states results in a non-trivial temperature dependence for the magnetic susceptibility.
To clarify how the electronic state of Sr1-xLaxRuO3 evolves with La doping, we conducted photoemission (PES) experiments using soft x-rays. The spectral shape of the Ru 4d derived peak near the Fermi level changes significantly with increasing x. This variation indicates that a spectral weight transfer from the coherent to incoherent component occurs due to an enhancement of the electron correlation effect. Resonant PES experiments at the La 3d_{5/2} edge have confirmed that there is no significant contribution of the La 5d state in the energy range where the spectral weight transfer is observed. Using the dependence of the photoelectron mean free path on the photon energy, we subtracted the surface components from the PES spectra and confirmed that the enhancement of the electron correlation effect with La doping is an intrinsic bulk phenomenon. On the other hand, a large portion of the coherent component remains at the Fermi level up to x = 0.5, reflecting that the Ru 4d state still has itinerant characteristics. Moreover, we found that the PES spectra hardly depend on the temperature and do not exhibit a discernible change with magnetic ordering, suggesting that the temperature variation of the exchange splitting does not follow the prediction of the Stoner theory. The presently obtained experimental results indicate that the electron correlation effect plays an important role in Sr1-xLaxRuO3 and that the Ru 4d electrons possess both local and itinerant characteristics.
Soft and hard X-ray photoelectron spectroscopy (PES) has been performed for one of the heavy fermion system CeRu$_2$Si$_2$ and a $4f$-localized ferromagnet CeRu$_2$Ge$_2$ in the paramagnetic phase. The three-dimensional band structures and Fermi surface (FS) shapes of CeRu$_2$Si$_2$ have been determined by soft X-ray $h u$-dependent angle resolved photoelectron spectroscopy (ARPES). The differences in the Fermi surface topology and the non-$4f$ electronic structures between CeRu$_2$Si$_2$ and CeRu$_2$Ge$_2$ are qualitatively explained by the band-structure calculation for both $4f$ itinerant and localized models, respectively. The Ce valences in CeRu$_2X_2$ ($X$ = Si, Ge) at 20 K are quantitatively estimated by the single impurity Anderson model calculation, where the Ce 3d hard X-ray core-level PES and Ce 3d X-ray absorption spectra have shown stronger hybridization and signature for the partial $4f$ contribution to the conduction electrons in CeRu$_2$Si$_2$.
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