Detecting halfmetallic electronic structures of spintronic materials in a magnetic field.

Band-gap engineering is one of the fundamental techniques in semiconductor technology and also applicable in next generation spintronics using the spin degree of freedom. To fully utilize the spintronic materials, it is essential to optimize the spin-dependent electronic structures in the operando conditions by applying magnetic and/or electric fields. Here we present an advanced spectroscopic technique to probe the spin-polarized electronic structures by using magnetic circular dichroism (MCD) in resonant inelastic soft X-ray scattering (RIXS) under an external magnetic field. Thanks to the spin-selective dipole-allowed transitions in RIXS-MCD, we have successfully demonstrated the direct evidence of the perfectly spin-polarized electronic structures for the prototypical halfmetallic Heusller alloy [Formula: see text]. RIXS-MCD is a promising tool to probe the spin-dependent carriers and band-gap induced in the buried magnetic layers in an element specific way under the operando conditions.

Ce electronic states in Nd(0.45-x)Ce(x)Sr0.55MnO3 probed by x-ray absorption spectroscopy and photoemission.

We have investigated the Ce 4f electronic states in the Ce-doped manganites Nd(0.45-x)Ce(x)Sr0.55MnO3 (NCSMO) by means of x-ray absorption spectroscopy (XAS) and hard x-ray photoelectron spectroscopy (HAXPES). The Ce 3d XAS shows that the Ce ions exist in the form of the Ce(3+) and Ce(4+) mixed-valent states, and we have found that the XAS spectral features change with temperature. The Ce 3d XAS and HAXPES spectra for NCSMO agree reasonably well with calculated results based on the single-impurity Anderson model, which takes into account the atomic multiplets and two valence bands. The estimated Ce bulk valence of Nd0.15Ce0.3Sr0.55MnO3 decreases from 3.44 to 3.30 with cooling.

Photoemission spectroscopy and the unusually robust one-dimensional physics of lithium purple bronze.

Temperature-dependent photoemission spectroscopy in Li(0.9)Mo(6)O(17) contributes to evidence for one-dimensional (1D) physics that is unusually robust. Three generic characteristics of the Luttinger liquid are observed: power law behavior of the k-integrated spectral function down to temperatures just above the superconducting transition, k-resolved lineshapes that show holon and spinon features, and quantum critical (QC) scaling in the lineshapes. Departures of the lineshapes and the scaling from expectations in the Tomonaga-Luttinger model can be partially described by a phenomenological momentum broadening that is presented and discussed. The possibility that some form of 1D physics obtains even down to the superconducting transition temperature is assessed.

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.

High resolution, low hν photoelectron spectroscopy with the use of a microwave excited rare gas lamp and ionic crystal filters.

The need for not only bulk sensitive but also extremely high resolution photoelectron spectroscopy for studying detailed electronic structures of strongly correlated electron systems is growing rapidly. Moreover, easy access to such a capability in one's own laboratory is desirable. Demonstrated here is the performance of a microwave excited rare gas (Xe, Kr, and Ar) lamp combined with ionic crystal filters (sapphire, CaF(2), and LiF), which can supply three strong lines near the photon energy of hnyu hν=8.4, 10.0, and 11.6 eV, with the hν resolution of better than 600 µeV for photoelectron spectroscopy. Its performance is demonstrated on some materials by means of both angle-integrated and angle-resolved measurements.

Coexistence of strongly mixed-valence and heavy-fermion character in SmOs4Sb12 studied by soft- and hard-X-ray spectroscopy.

Sm-based heavy-fermion compound SmOs4Sb12 has been investigated by soft x-ray (hnu=1070-1600 eV) and hard x-ray (HX; hnu=7932 eV) spectroscopy. The HX photoemission spectroscopy clearly demonstrates that the strongly mixed-valence state and the heavy-fermion state coexist in the bulk. It is found that the Sm valence decreases below 100 K, indicating that the Kondo coherence develops with approaching the proposed Kondo temperature. Our theoretical analyses suggest that the origin of the coexistence in SmOs4Sb12 is the coincidence of two conditions, namely, (i) the energy difference between Sm divalent and trivalent states is very small and (ii) the hybridization between Sm 4f and conduction electrons is weak.

Three-dimensional bulk fermiology of CeRu2Ge2 in the paramagnetic phase by soft x-ray hnu-dependent (700-860 eV) ARPES.

By virtue of the soft x-ray angle-resolved photoelectron spectroscopy, the three-dimensional bulk fermiology has been successfully performed for a strongly correlated Ce compound, ferromagnet CeRu2Ge2 in the paramagnetic phase. A clear difference of the Fermi surface topology from either band calculation or de Haas-van Alphen results in the ferromagnetic phase is observed and interpreted by considering the difference of the 4f contribution to the Fermi surfaces in the paramagnetic phase.

Spatial chemical inhomogeneity and local electronic structure of Mn-doped Ge ferromagnetic semiconductors.

We have investigated the chemical distributions and the local electronic structure of potential diluted magnetic semiconductor Ge0.94Mn0.06 single crystals using scanning photoelectron microscopy (SPEM), x-ray absorption spectroscopy (XAS), and photoemission spectroscopy (PES). The SPEM image shows the stripe-shaped microstructures, which arise from the chemical phase separation between the Mn-rich and Mn-depleted phases. The Mn 2p XAS shows that the Mn ions in the Mn-rich region are in the divalent high-spin Mn2+ states but that they do not form metallic Mn clusters. The Mn 3d PES spectrum exhibits a peak centered at approximately 4 eV below E(F) and the negligible spectral weight near E(F). This study suggests that the observed ferromagnetism in Ge1-xMnx arises from the phase-separated Mn-rich phase.

Mutual experimental and theoretical validation of bulk photoemission spectra of Sr1-xCaxVO3.

We report high-resolution high-energy photoemission spectra together with parameter-free LDA + DMFT (local density approximation + dynamical mean-field theory) results for Sr1-xCaxVO3, a prototype 3d(1) system. In contrast to earlier investigations the bulk spectra are found to be insensitive to x. The good agreement between experiment and theory confirms the bulk sensitivity of the high-energy photoemission spectra.

Filling of the mott-hubbard gap in the high temperature photoemission spectrum of (V0.972Cr0.028)2O3.

Photoemission spectra of the paramagnetic insulating phase of (V0.972Cr0.028)2O3, taken in ultrahigh vacuum up to the unusually high temperature (T) of 800 K, reveal a property unique to the Mott-Hubbard (MH) insulator that has not been observed previously. With increasing T the MH gap is filled by spectral weight transfer, in qualitative agreement with high-T theoretical calculations combining dynamical mean field theory and band theory in the local density approximation.

Localized character of 4f electrons in CeRhx (x=2,3) and CeNix (x=2,5).

We have measured Ce 4f spectral weights of extremely alpha-like Ce transition metal intermetallic compounds CeRhx (x=2,3) and CeNix (x=2,5) by using the bulk-sensitive resonant photoemission technique at the Ce M5(3d(5/2)-->4f) edge. High energy resolution and longer escape depth of photoemitted electron at this photon energy enabled us to distinguish the sharp Kondo resonance tails at the Fermi level, which can be well described by the Gunnarsson-Schönhammer calculation based on the Anderson impurity Hamiltonian. On the other hand, the itinerant 4f band description shows big discrepancies, which implies that Ce 4f electrons retain localized characters even in extremely alpha-like compounds.

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.

Electronic structure of YbXCu(4) (X = In, Cd, Mg) investigated by high-resolution photoemission spectroscopy.

The valence-band electronic structure of YbXCu(4) (X = In, Cd, Mg) has been investigated by means of temperature-dependent high-energy-resolution photoemission spectroscopy using a He I resonance line (hnu = 21.22 eV) and synchrotron radiation (hnu = 800 eV). Intensities of the structure due to the Yb(2+) 4f(7/2) states in the He I spectra of YbInCu(4) and YbCdCu(4) gradually increase with decreasing temperature from 300 to 10 K, and Yb(2+) 4f(7/2) structures are clearly observed as peaks near the Fermi level (E(F)) at 10 K. The enhancement of the Yb(2+) 4f(7/2) peak from 50 to 10 K is much greater for YbInCu(4) than for YbCdCu(4). On the other hand, the Yb(2+) 4f(7/2) states of YbMgCu(4) are observed as a broad structure near E(F). In the synchrotron radiation photoemission spectra of YbInCu(4) and YbCdCu(4), the structures due to the Yb(2+) and Yb(3+) 4f states are recognized at all temperatures. The intensity ratio Yb(2+)/Yb(3+) gradually increases with decreasing temperature. The energy separations between the Yb(2+) and Yb(3+) 4f structures of YbInCu(4) increase from 50 to 20 K. For YbMgCu(4), on the other hand, almost only the Yb(2+) structures are observed and little temperature dependence has been detected.

High-resolution soft X-ray absorption spectroscopy of solids.

The present research deals with the high-resolution soft x-ray absorption spectra (XAS) of Si, Ce- and Sm- compounds measured at BL25SU of SPring-8. The spectra are compared with theoretical results. The Si 1s spectrum shows good agreement with the calculated empty density of states so far reported. The Ce 3d spectra are very sensitive to the local electronic structure. The Sm 3d XAS of SmS shows clear temperature dependence, which is partly explained by a calculation for Sm2+ ion.

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 (< or = 5 A) associated with the low excitation energies conventionally used (< or = 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 A (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.

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.