Search

We have studied in-gap states in epitaxial CoFe2O4(111), which potentially acts as a perfect spin filter, grown on a Al2O3(111)/Si(111) structure by using ellipsometry, Fe L2,3-edge x-ray absorption spectroscopy (XAS), and Fe L2,3-edge resonant inelastic x-ray scattering (RIXS), and revealed the relation between the in-gap states and chemical defects due to the Fe2+ cations at the octahedral sites (Fe2+ (Oh) cations). The ellipsometry measurements showed the indirect band gap of 1.24 eV for the CoFe2O4 layer and the Fe L2,3-edge XAS confirmed the characteristic photon energy for the preferential excitation of the Fe2+ (Oh) cations. In the Fe L3-edge RIXS spectra, a band-gap excitation and an excitation whose energy is smaller than the band-gap energy (Eg = 1.24 eV) of CoF2O4, which we refer to as "below-band-gap excitation (BBGE)" hereafter, were observed. The intensity of the BBGE was strengthened at the preferential excitation energy of the Fe2+ (Oh) cations. In addition, the intensity of the BBGE was significantly increased when the thickness of the CoFe2O4 layer was decreased from 11 to 1.4 nm, which coincides with the increase in the site occupancy of the Fe2+ (Oh) cations with decreasing the thickness. These results indicate that the BBGE comes from the in-gap states of the Fe2+ (Oh) cations whose density increases near the heterointerface on the bottom Al2O3 layer. We have demonstrated that RIXS measurements and analyses in combination with ellipsometry and XAS are effective to provide an insight into in-gap states in thin-film oxide heterostructures.

We have probed the crystalline electric-field ground states of pure $|J = 7/2, J_z = \pm 5/2\rangle$ as well as the anisotropic $c$-$f$ hybridization in both valence fluctuating systems $\alpha$- and $\beta$-YbAlB$_4$ by linear polarization dependence of angle-resolved core level photoemission spectroscopy. Interestingly, the small but distinct difference between \abyb was found in the polar angle dependence of linear dichroism, indicating the difference in the anisotropy of $c$-$f$ hybridization which may be essential to a heavy Fermi liquid state in $\alpha$-YbAlB$_4$ and a quantum critical state in $\beta$-YbAlB$_4$.

We report experimentally observed linear dichroism in angle-resolved core-level photoemission spectra of PrIr2Zn20 and PrB6 in cubic symmetry. The different anisotropic 4f charge distributions between the compounds due to the crystalline-electric-field splitting are responsible for the difference in the linear dichroism, which has been verified by spectral simulations with the full multiplet theory for a single-site Pr3+ ion in cubic symmetry. The observed linear dichroism and polarization-dependent spectra in two different photoelectron directions for PrIr2Zn20 are reproduced by theoretical analysis for the Gamma_3 ground state, whereas those of the Pr 3d and 4d core levels indicate the Gamma_5 ground state for PrB6., Comment: 6 pages, 4 figures

We report a combined study for the electronic structures of ferromagnetic CeAgSb$_2$ using soft X-ray absorption (XAS), magnetic circular dichroism (XMCD), and angle-resolved photoemission (ARPES) spectroscopies. The Ce $M_{4, 5}$ XAS spectra show very small satellite structures, reflecting a strongly localized character of the Ce $4f$ electrons. The linear dichroism effects in the Ce $M_{4, 5}$ XAS spectra demonstrate the ground state Ce $4f$ symmetry of $\Gamma{_6}$, the spatial distribution of which is directed along the $c$-axis. The XMCD results give support to the picture of local-moment magnetism in CeAgSb$_2$. Moreover it is also found that the theoretical band dispersions for LaAgSb$_2$ provides better description of the ARPES band structures than those for CeAgSb$_2$. Nevertheless, ARPES spectra at the Ce $3d$-$4f$ resonance show the momentum dependence for the intensity ratio between Ce $4f^{1}_{5/2}$ and $4f^{1}_{7/2}$ peaks in a part of the Brillouin zone, suggesting the non-negligible momentum dependent hybridization effect between the Ce $4f$ and the conduction electrons. This is associated with the moderate mass enhancement in CeAgSb$_2$., Comment: to be published in Journal of the Physical Society of Japan

We have examined the local 3d electronic structures of Co-Au multinuclear complexes with the medicinal molecules D-penicillaminate (D-pen) [Co{Au(PPh3)(D-pen)}2]ClO4 and [Co3{Au3(tdme)(D-pen)3}2] by Co L_2,3-edge soft X-ray absorption (XAS) spectroscopy, where PPh3 denotes triphenylphosphine and tdme stands for 1,1,1-tris[(diphenylphosphino)methyl]ethane. The Co L_2,3-edge XAS spectra indicate the localized ionic 3d electronic states in both materials. The experimental spectra are well explained by spectral simulation for a localized Co ion under ligand fields with the full multiplet theory, which verifies that the ions are in the low-spin Co3+ state in the former compound and in the high-spin Co2+ state in the latter., Comment: 7 pages, 5 figures. To be published in J. Phys. Soc. Jpn

We have successfully observed linear dichroism in angle-resolved Yb3+ 3d5/2 core-level photoemission spectra for YbB12 in cubic symmetry. Its anisotropic 4f charge distribution due to the crystal-field splitting is responsible for the linear dichroism, which has been verified by spectral simulations using ionic calculations with the full multiplet theory for a single-site Yb3+ ion in cubic symmetry. The observed linear dichroism as well as the polarization-dependent spectra in two different photoelectron directions for YbB12 are quantitatively reproduced by theoretical analysis for the Gamma_8 ground state, indicating the Gamma_8 ground-state symmetry for the Yb3+ ions mixed with the Yb2+ state., Comment: 5 pages, 3 figures, to be published in J. Phys. Soc. Jpn. (Letters)

We show that the strongly correlated 4f-orbital symmetry of the ground state is revealed by linear dichroism in core-level photoemission spectra as we have discovered for YbRh2Si2 and YbCu2Si2. Theoretical analysis tells us that the linear dichroism reflects the anisotropic charge distributions resulting from crystalline electric field. We have successfully determined the ground-state 4f symmetry for both compounds from the polarization-dependent angle-resolved core-level spectra at a low temperature well below the first excitation energy. The excited-state symmetry is also probed by temperature dependence of the linear dichroism where the high measuring temperatures are of the order of the crystal-field-splitting energies., Comment: 6 pages, 4 figures, to be published in J. Phys. Soc. Jpn. (Letters)

Undoped and slightly Eu-doped SmB6 show the opening of a gap with decreasing temperature below ~150 K. The spectral shapes near the Fermi level (EF) at 15 K have shown strong increase in intensity of a peak at a binding energy (EB) of around 12 meV with decreasing the photon energy (hn) from 17 eV down to 7 eV. Angle resolved spectra of SmB6 measured at hn = 35 eV just after the in-situ cleavage showed clear dispersions of several bands in the EB region from EF to 4 eV. Spin-polarized photoelectron spectra were then measured at 12 K and light incidence angle of ~50 deg. In contrast to the lack of spin polarization for the linearly polarized light excitation, clear spin polarization was observed in the case of circularly polarized light excitation. The two prominent peaks at EB~12 and ~150 meV have shown opposite signs of spin polarization which are reversed when the helicity of the light is reversed. The sign and the magnitude of spin- polarization are consistent with a theoretical prediction for the 6H5/2 and 6H7/2 states., Comment: all correspondence should be addressed to ssmsuga@gmail.com

Hard X-ray and extremely low energy bulk-sensitive photoelectron spectroscopy has been performed in the temperature range of 100-330 K for Fe3O4. In the high temperature phase just above the Verwey transition, the intensity at the Fermi level (EF) is still negligible, but it increases gradually with further increasing the temperature (250 K, 330 K) in consistence with the temperature dependence of the conductivity. The spectral behaviors near EF with temperature are well explained by the model, which takes the polaron effect into account., Comment: 5 pages, 3 figures