Akira Sekiyama

Probing bulk states of correlated electron systems by high-resolution resonance photoemission

Electron correlations are known to play an important role in determining the unusual physical properties of a variety of compounds. Such properties include high-temperature superconductivity, heavy fermion behaviour and metal-to-insulator transitions. High-resolution photoelectron spectroscopy (PES) provides a means of directly probing the electronic states (particularly those near the Fermi level) in these materials, but the short photoelectron mean free paths (⩽5 Å) associated with the low excitation energies conventionally used (⩽120 eV) make this a surface-sensitive technique. Now that high-resolution PES is possible at much higher energies, with mean free paths as long as 15 Å (ref. 6), it should become feasible to probe the bulk electronic states in these materials. Here we demonstrate the power of this technique by applying it to the cerium compounds CeRu2Si2 and CeRu2. Previous PES studies of these compounds revealed very similar spectra for the Ce 4f electronic states, yet it is expected that such states should be different owing to their differing degrees of hybridization with other valence bands. Our determination of the bulk Ce 4f electronic states of these compounds resolves these differences.

Performance of a very high resolution soft x-ray beamline BL25SU with a twin-helical undulator at SPring-8

We report on the excellent performance of a newly constructed soft x-ray helical undulator beamline BL25SU of SPring-8 for photon energies 500–1800 eV. The full beamline was designed to perform very high resolution soft x-ray spectroscopy of solids with using high brilliance, highly circularly polarized undulator radiation. The grazing incidence monochromator employs varied-line-spacing plane gratings which operate in convergent light from a spherical mirror and focuses monochromatic light onto the exit slit. A resolving power in excess of 15 000 was measured at 540 and 870 eV for a grating with a central groove density of 600 lines/mm from the photoemission spectra of Au. A resolving power of more than 20 000 is estimated near 870 eV for a grating with a central groove density of 1000 lines/mm. A photon flux of more than 1×1011 photons/s/100 mA/0.02% b.w. is supplied onto the sample between 500 and 1800 eV with very low amount of higher-order light. The low heat load from the twin-helical undulator gives...

Prominent quasiparticle peak in the photoemission spectrum of the metallic phase of V2O3.

We present the first observation of a prominent quasiparticle peak in the photoemission spectrum of the metallic phase of V2O3 and report new spectral calculations that combine the local-density approximation with the dynamical mean-field theory (using quantum Monte Carlo simulations) to show the development of such a distinct peak with decreasing temperature. The experimental peak width and weight are significantly larger than in the theory.

Direct k-space mapping of the electronic structure in an oxide-oxide interface.

The interface between LaAlO(3) and SrTiO(3) hosts a two-dimensional electron system of itinerant carriers, although both oxides are band insulators. Interface ferromagnetism coexisting with superconductivity has been found and attributed to local moments. Experimentally, it has been established that Ti 3d electrons are confined to the interface. Using soft x-ray angle-resolved resonant photoelectron spectroscopy we have directly mapped the interface states in k space. Our data demonstrate a charge dichotomy. A mobile fraction contributes to Fermi surface sheets, whereas a localized portion at higher binding energies is tentatively attributed to electrons trapped by O vacancies in the SrTiO(3). While photovoltage effects in the polar LaAlO(3) layers cannot be excluded, the apparent absence of surface-related Fermi surface sheets could also be fully reconciled in a recently proposed electronic reconstruction picture where the built-in potential in the LaAlO(3) is compensated by surface O vacancies serving also as a charge reservoir.

Bulk 4f Electronic States of Ce-Based Heavy Fermion System Probed by High-Resolution Resonance Photoemission

“Bulk-sensitive” Ce 3 d -4 f resonance photoemission (RPES) with an unprecedentedly high resolution has revealed a clear difference of bulk Ce 4 f spectral weights of heavy fermion system CeRu 2 Si 2 and CeRu 2 Ge 2 in the region of the tail of the Kondo peak and its spin-orbit partner. The significant spectral difference in both materials is in strong contrast to the mutually similar “surface-sensitive” 4 d -4 f RPES. The obtained bulk-sensitive spectra are well reproduced by a single impurity model. Consideration of the crystalline electric field splitting is important for estimating a realistic Kondo temperature from the bulk 4 f spectra.

Twin helical undulator beamline for soft X-ray spectroscopy at SPring-8

A very high resolution soft X-ray beamline, BL25SU, has been designed and is under construction at SPring-8. Completely right or left circularly polarized light is supplied on a common axis of a newly designed twin helical undulator. A helicity modulation up to 10 Hz can be performed using five kicker magnets. The fundamental radiation covers the region 0.5-3 keV. Higher-order radiation is rather weak on the axis. A monochromator with varied-line-spacing plane gratings is installed to cover the region below 1.5 keV. A very high resolution beyond 10(4) is expected for the whole energy region.

The prominent 5d-orbital contribution to the conduction electrons in gold

We have examined the valence-band electronic structures of gold and silver in the same column in the periodic table with nominally filled d orbitals by means of a recently developed polarization-dependent hard x-ray photoemission. Contrary to a common expectation, it is found that the 5d-orbital electrons contribute prominently to the conduction electrons in gold while the conduction electrons in silver are to some extent free-electron-like with negligible 4d contribution, which could be related to a well-known fact that gold is more stable than silver in air. The 4d electron correlation effects are found to be essential for the conduction electron character in silver.

High-energy photoemission on Fe3O4: Small polaron physics and the Verwey transition

We have studied the electronic structure and charge ordering (Verwey) transition of magnetite (Fe3O4) by soft X-ray photoemission. Due to the enhanced probing depth and the use of different surface preparations we are able to distinguish surface and volume effects in the spectra. The pseudogap behavior of the intrinsic spectra and its temperature dependence give evidence for the existence of strongly bound small polarons consistent with both dc and optical conductivity. Together with other recent structural and theoretical results our findings support a picture in which the Verwey transition contains elements of a cooperative Jahn-Teller effect, stabilized by local Coulomb interaction.

Kondo Lattice Effects of YbAl3 Suggested by Temperature Dependence of High-Accuracy High-Energy Photoelectron Spectroscopy

By use of high-resolution soft X-rays, intrinsic temperature dependences of bulk Yb 4f photoelectron spectra were obtained for fractured surfaces of high-purity YbAl 3 single crystals. The spectra ...

Technique for bulk Fermiology by photoemission applied to layered ruthenates

We report the Fermi surfaces of the superconductor