arXiv subjects

A. Sekiyama

Publications and source records attributed to A. Sekiyama.

At least 19 recordsLinked to original sources

arXiv2025

Fingerprints of Mott and Slater gaps in the core-level photoemission spectra of antiferromagnetic iridates

We present Ir $4f$ core-level hard-x-ray photoemission spectroscopy (HAXPES) experiments conducted across antiferromagnetic (AFM) ordering transition in Ruddlesden-Popper iridates Sr$_2$IrO$_4$ and Sr$_3$Ir$_2$O$_7$. The Ir $4f$ spectra exhibit distinct changes between the AFM and paramagnetic (PM) phases, with the spectral difference $I_\text{PM}-I_\text{AFM}$ showing a contrasting behavior in the two compounds. By employing computational simulations using the local-density approximation combined with the dynamical mean-field theory method, we elucidate that $I_\text{PM}-I_\text{AFM}$ primary reflects the Slater or Mott-Hubbard character of the AFM insulating state rather than material specific details. This sensitivity to fine low-energy electronic structure arises from the dependence of charge-transfer responses to the sudden creation of a localized core hole on both metal-insulator transitions and long-range AFM ordering. Our result broadens the applications of core-level HAXPES as a tool for characterization of electronic structure.

cond-mat.str-el↗

arXiv2025

Simultaneous probes of pseudogap and disorder by hard x-ray photoemission applied for a candidate thermoelectric Al-Pd-Ru quasicrystal

The bulk electronic structure of Al-Pd-Ru quasicrystal (QC) have been investigated by hard X-ray photoemission spectroscopy (HAXPES). We have found an intrinsic pseudogap structure in which the spectral weight in the vicinity of the Fermi level (E_F) is remarkably suppressed at any photon energy. The valence-band HAXPES spectra and the asymmetry of the core-level peaks indicate a contribution of the Al sites to the electronic structure in the vicinity of E_F with less contributions from the Pd and Ru sites. The disorder effects are found in the core-level lineshapes of the Al-Pd-Ru QC, of which the widths are much broader than those of the other reference crystalline solids with less disorder.

cond-mat.mtrl-sci↗

arXiv2025

Hybridized and Localized 4f Electronic States of Nd-based Intermetallic Compounds in Cubic Symmetry Probed by High-Energy Photoemission

We have performed soft and hard X-ray photoemission spectroscopies on NdTi2Al20 and NdBe13 which show antiferromagnetic ordering at low temperatures. The Nd 3d core-level photoemission and Nd 3d-4f valence-band resonant photoemission spectra show finite 4f4 initial-state components in addition to the 4f3 configurations attributed to the c-f hybridization effects in NdTi2Al20, while the 4f3 initial-state components with localized character are dominant in NdBe13. These results imply the emergence of overscreening channel due to the two-channel Kondo effect in NdTi2Al20 through the the strong c-f hybridization effect.

cond-mat.str-el↗

arXiv2024

Bulk superconductivity in Pb-substituted BiS$_{\bf 2}$-based compounds studied by hard-x-ray spectroscopy

In this study, we investigate the bulk electronic structure of Pb-substituted LaO$_{0.5}$F$_{0.5}$BiS$_2$ single crystals, using two types of hard-x-ray spectroscopy. High-energy-resolution fluorescence-detected x-ray absorption spectroscopy revealed a spectral change at low temperatures. Using density functional theory (DFT) simulations, we find that the temperature-induced change originates from a structural phase transition, similar to the pressure-induced transition in LaO$_{0.5}$F$_{0.5}$BiS$_2$. This finding suggests that the mechanism of bulk superconductivity induced by Pb substitution is the same as that under high pressure. Furthermore, a novel low-valence state with a mixture of divalent and trivalent Bi ions is discovered using hard x-ray photoemission spectroscopy with the aid of DFT calculations.

cond-mat.supr-con↗

arXiv2023

Impact of the ground-state $4f$ symmetry for anisotropic $cf$-hybridization in the heavy fermion superconductor CeNi$_{2}$Ge$_{2}$

We report the ground-state symmetry of the Ce $4f$ states in the heavy fermion superconductor CeNi$_{2}$Ge$_{2}$, yielding anisotropic $cf$-hybridization between the Ce $4f$ states and conducting electrons. By analyzing linear dichroism in soft x-ray absorption and core-level hard x-ray photoemission spectra, the $4f$ symmetry is determined as $Σ$-type $Γ_{7}$, promoting predominant hybridization with the conducting electrons originating from the Ge site. The band structures probed by the soft x-ray angle-resolved photoemission indicates that the Ge $4p$ components contribute to the band renormalization through the anisotropic hybridization effects, suggesting that the control of the electronic structures of Ge orbital gives an impact to achieve the exotic phenomena in CeNi$_{2}$Ge$_{2}$.

cond-mat.str-el↗

arXiv2020

The Prominent Charge-Transfer Effects of Trinuclear Complexes with Nominally High Nickel Valences

Recently synthesized Rh-Ni trinuclear complexes hexacoordinated with sulfur ions, 3-aminopropanethiolate (apt) metalloligand [Ni{Rh(apt)$_{3}$}$_{2}$](NO$_{3}$)$_{n}$ ($n$ = 2, 3, 4), are found to be chemically interconvertible between the nominal Ni$^{2+}$ and Ni$^{4+}$ states. In order to clarify the origins of their interconvertible nature and the stability of such a high oxidation state as the tetravalency from the physical point of view, we have systematically investigated the local 3$d$ electronic structures of [Ni{Rh(apt)$_{3}$}$_{2}$](NO$_{3}$)$_{n}$ by means of soft X-ray core-level absorption spectroscopy (XAS). The experimental data have been reproduced by the single-site configuration-interaction cluster-model simulations, which indicate that the charge-transferred configurations are more stable than the nominal $d$-electron-number configuration for $n=3,4$ leading to the prominent charge-transfer effects. These are also supported by S $K$-edge XAS of [Ni{Rh(apt)$_{3}$}$_{2}$](NO$_{3}$)$_{n}$. Our results imply that the found charge-transfer effects have a key role to realize the interconvertible nature as well as the stability of the high oxidization state of the Ni ions.

cond-mat.str-el↗

arXiv2018

Half-metallicity of Mn2VAl ferrimagnet revealed by resonant inelastic soft x-ray scattering under magnetic field

Detailed information on the electronic states of both V and Mn 3d electrons in the ferrimagnet Mn2VAl is obtained by the bulk sensitive resonant inelastic soft x-ray scattering (SX-RIXS) excited with the circularly polarized light under an external magnetic field for the first time. The results under the V L-edge excitation have revealed the negligible partial density of states (PDOS) of the V 3d states around the Fermi energy as well as their rather localized character. Under the Mn L-edge excitation, on the other hand, the spectra are dominated by fluorescence with clear magnetic circular dichroism with noticeable excitation photon energy dependence. Compared with the theoretical prediction of the RIXS spectra based on the density-functional-theory band structure calculation, an itinerant, spin-dependent character of the Mn 3d states and decays of the Mn 2p core states are confirmed in consistence with the half-metallicity of the Mn 3d states.

cond-mat.mtrl-sci↗

arXiv2017

Electronic Structure and Magnetic Properties of Half-metallic Ferrimagnet Mn$_{2}$VAl Probed by Soft X-ray Spectroscopies

We have studied the electronic structure of ferrimagnetic Mn2VAl single crystal by means of soft X-ray absorption spectroscopy (XAS), X-ray absorption magnetic circular dichroism (XMCD) and resonant soft X-ray inelastic scattering (RIXS). We have successfully observed the XMCD signals for all constitute elements, supporting the spin polarized states at the Fermi level. The Mn $L_{2,3}$ XAS and XMCD spectra are reproduced by the spectral simulation based on density-functional theory (DFT), indicating itinerant character of the Mn 3d states. On the other hand, V $3d$ electrons are rather localized since the ionic model can qualitatively explain the V $L_{2,3}$ XAS and XMCD spectra as well as the local dd excitation revealed by V $L_3$ RIXS.

cond-mat.str-el↗

arXiv2017

Raman and fluorescence contributions to resonant inelastic soft x-ray scattering on LaAlO$_3$/SrTiO$_3$ heterostructures

We present a detailed study of the Ti 3$d$ carriers at the interface of LaAlO$_3$/SrTiO$_3$ heterostructures by high-resolution resonant inelastic soft x-ray scattering (RIXS), with special focus on the roles of overlayer thickness and oxygen vacancies. Our measurements show the existence of interfacial Ti 3$d$ electrons already below the critical thickness for conductivity and an increase of the total interface charge up to a LaAlO$_3$ overlayer thickness of 6 unit cells before it levels out. By comparing stoichiometric and oxygen deficient samples we observe strong Ti 3$d$ charge carrier doping by oxygen vacancies. The RIXS data combined with photoelectron spectroscopy and transport measurements indicate the simultaneous presence of localized and itinerant charge carriers. However, it is demonstrated that the relative amount of localized and itinerant Ti $3d$ electrons in the ground state cannot be deduced from the relative intensities of the Raman and fluorescence peaks in excitation energy dependent RIXS measurements, in contrast to previous interpretations. Rather, we attribute the observation of either the Raman or the fluorescence signal to the spatial extension of the intermediate state reached in the RIXS excitation process.

cond-mat.mtrl-sci↗

arXiv2016

Three-dimensional electronic structures and the metal-insulator transition in Ruddlesden-Popper iridates

In this study, we systematically investigate 3D momentum($\hbar k$)-resolved electronic structures of Ruddlesden-Popper-type iridium oxides Sr$_{n+1}$Ir$_n$O$_{3n+1}$ using soft-x-ray (SX) angle-resolved photoemission spectroscopy (ARPES). Our results provide direct evidence of an insulator-to-metal transition that occurs upon increasing the dimensionality of the IrO$_2$-plane structure. This transition occurs when the spin-orbit-coupled $j_{\rm eff}$=1/2 band changes its behavior in the dispersion relation and moves across the Fermi energy. In addition, an emerging band along the $Γ$(0,0,0)-R($π$,$π$,$π$) direction is found to play a crucial role in the metallic characteristics of SrIrO$_3$. By scanning the photon energy over 350 eV, we reveal the 3D Fermi surface in SrIrO$_3$ and $k_z$-dependent oscillations of photoelectron intensity in Sr$_3$Ir$_2$O$_7$. In contrast to previously reported results obtained using low-energy photons, folded bands derived from lattice distortions and/or magnetic ordering make significantly weak (but finite) contributions to the $k$-resolved photoemission spectrum. At the first glance, this leads to the ambiguous result that the observed $k$-space topology is consistent with the unfolded Brillouin zone (BZ) picture derived from a non-realistic simple square or cubic Ir lattice. Through careful analysis, we determine that a superposition of the folded and unfolded band structures has been observed in the ARPES spectra obtained using photons in both ultraviolet and SX regions. To corroborate the physics deduced using low-energy ARPES studies, we propose to utilize SX-ARPES as a powerful complementary technique, as this method surveys more than one whole BZ and provides a panoramic view of electronic structures.

cond-mat.str-el↗

arXiv2015

Photoemission System with Polarized Hard X-rays for Probing Ground State Symmetry of Strongly Correlated Materials

We have developed a polarized hard X-ray photoemission (HAXPES) system to study the ground-state symmetry of strongly correlated materials. The linear polarization of the incoming X-ray beam is switched by the transmission-type phase retarder composed of two diamond (100) crystals. The best degree of the linear polarization $P_L$ is $-0.96$, containing the vertical polarization component of 98%. A newly developed low temperature two-axis manipulator enables easy polar and azimuthal rotations to select the detection direction of photoelectrons. The lowest temperature achieved is 9 K, offering us a chance to access the ground state even for the strongly correlated electron systems in cubic symmetry. The co-axial sample monitoring system with the long-working-distance microscope enables us to keep measuring the same region on the sample surface before and after rotation procedures. Combining this sample monitoring system with a micro-focused X-ray beam by means of an ellipsoidal Kirkpatrick-Baez mirror (25 $μ$m $\times$ 25 $μ$m (FWHM)), we have demonstrated the polarized valence-band HAXPES on NiO for voltage application as resistive random access memories to reveal the origin of the metallic spectral weight near the Fermi level.

cond-mat.str-el↗

arXiv2015

Soft X-ray Angle Resolved Photoemission with Micro Positioning Techniques for Metallic V$_2$O$_3$

We have performed soft-X-ray angle resolved photoemission for metallic V$_2$O$_3$. Combining a micro focus beam (40 x 65 $μ$m$^2$) and micro positioning techniques with a long working distance microscope, we have succeeded in observing band dispersions from tiny cleavage surfaces with typical size of the several tens of $μ$m. The photoemission spectra show a clear position dependence reflecting the morphology of the cleaved sample surface. By selecting high quality flat regions on the sample surface, we have succeeded in band mapping using both photon-energy and polar-angle dependences, opening the door to three-dimensional ARPES for typical three dimensional correlated materials where large cleavage planes are rarely obtained.

cond-mat.str-el↗

arXiv2014

Dimensionality-tuned electronic structure of nickelate superlattices explored by soft-x-ray angle resolved photoelectron spectroscopy

The electronic and magnetic properties of epitaxial LaNiO3/LaAlO3 superlattices can be tuned by layer thickness and substrate-induced strain. Here, we report on direct measurements of the k-space-resolved electronic structure of buried nickelate layers in superlattices under compressive strain by soft x-ray photoemission. After disentangling strong extrinsic contributions to the angle-dependent signal caused by photoelectron diffraction, we are able to extract Fermi surface information from our data. We find that with decreasing LaNiO3 thickness down to two unit cells (2 uc) quasiparticle coherence becomes strongly reduced, in accord with the dimension-induced metal-to-insulator transition seen in transport measurements. Nonetheless, on top of a strongly incoherent background a residual Fermi surface can be identified in the 2 uc superlattice whose nesting properties are consistent with the spin-density wave (SDW) instability recently reported. The overall behavior of the Ni 3d spectra and the absence of a complete gap opening indicate that the SDW phase is dominated by strong order parameter fluctuations.

cond-mat.str-el↗

arXiv2014

Bulk Nature of Layered Perovskite Iridates beyond the Mott Scenario : An Approach from Bulk Sensitive Photoemission Study

We present genuine bulk Ir 5d jeff states of layered perovskite iridates obtained by hard-x-ray photoemission spectroscopy (HAXPES) with s- and p-polarized lights. HAXPES spectra of Sr2IrO4 and Ba2IrO4 are well reproduced by the quasi-particle densities of states calculated by the local density approximation with dynamical mean-field theory (LDA+DMFT). It is demonstrated that the insulating nature of the iridates is triggered by antiferromagnetic correlation (Slater type) combined with electron correlation (Mott type). The extremely-low-energy bulk-sensitive photoemission spectroscopy reveals "bad metallic" states in the paramagnetic phase of the iridates, suggesting strongly renormalized metallic states above the Neel temperature as predicted by the LDA+DMFT.

cond-mat.str-el↗

arXiv2013

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

The interface between LaAlO3 and SrTiO3 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 SrTiO3. While photovoltage effects in the polar LaAlO3 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 LaAlO3 is compensated by surface O-vacancies serving also as charge reservoir.

cond-mat.str-el↗

arXiv2013

Intrinsic Correlated Electronic Structure of CrO2 Revealed by Hard X-ray Photoemission Spectroscopy

Bulk-sensitive hard x-ray photoemission spectroscopy (HAXPES) reveals for as-grown epitaxial films of half-metallic ferromagnetic CrO2(100) a pronounced screening feature in the Cr 2p3/2 core level and an asymmetry in the O 1s core level. This gives evidence of a finite, metal-type Fermi edge, which is surprisingly not observed in HAXPES. A spectral weight shift in HAXPES away from the Fermi energy is attributed to single-ion recoil effects due to high energy photoelectrons. In conjunction with inverse PES the intrinsic correlated Mott-Hubbard-type electronic structure is unravelled, yielding an averaged Coulomb correlation energy Uav ~ 3.2 eV.

cond-mat.str-el↗

arXiv2013

Photoemission Spectroscopy and the Unusually Robust One Dimensional Physics of Lithium Purple Bronze

Temperature dependent photoemission spectroscopy in Li0.9Mo6O17 contributes to evidence for one dimensional 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.

cond-mat.str-el↗

arXiv2010

Electron correlation in FeSe superconductor studied by bulk-sensitive photoemission spectroscopy

We have investigated the electronic structures of recently discovered superconductor FeSe by soft-x-ray and hard-x-ray photoemission spectroscopy with high bulk sensitivity. The large Fe 3d spectral weight is located in the vicinity of the Fermi level (EF), which is demonstrated to be a coherent quasi-particle peak. Compared with the results of the band structure calculation with local-density approximation, Fe 3d band narrowing and the energy shift of the band toward EF are found, suggesting an importance of the electron correlation effect in FeSe. The self energy correction provides the larger mass enhancement value (Z^-1=3.6) than in Fe-As superconductors and enables us to separate a incoherent part from the spectrum. These features are quite consistent with the results of recent dynamical mean-field calculations, in which the incoherent part is attributed to the lower Hubbard band.

cond-mat.supr-con↗