arXiv subjects

A. Higashiya

Publications and source records attributed to A. Higashiya.

15 recordsLinked to original sources

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

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↗

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↗

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↗

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

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↗

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↗

arXiv2010

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.

cond-mat.str-el↗

arXiv2010

Different Evolution of Intrinsic Gap in Kondo Semiconductors SmB6 and YbB12

Dependence of the spectral functions on temperature and rare-earth substitution was examined in detail for Kondo semiconductor alloys Sm1-xEuxB6 and Yb1-xLuxB12 by bulk-sensitive photoemission. It is found that the 4f lattice coherence and intrinsic (small) energy gap are robust for SmB6 against the Eu substitution up to x = 0.15 while both collapse by Lu substitution already at x = 0.125 for YbB12. Our results suggest that the mechanism of the intrinsic gap formation is different between SmB6 and YbB12 although they were so far categorized in the same kind of Kondo semiconductors.

cond-mat.str-el↗

arXiv2010

Evidence for the constancy of U in the Mott transition of V2O3

We have performed high-resolution hard X-ray photoemission spectroscopy for the metal-insulator transition (MIT) system (V(1-x)Cr(x))2O3 in the paramagnetic metal, paramagnetic insulator and antiferromagentic insulator phases. The quality of the spectra enables us to conclude that the on-site Coulomb energy U does not change through the MIT, which eliminate all but one theoretical MIT scenario in this paradigm material.

cond-mat.str-el↗

arXiv2007

Electronic structures of CeRu$_2X_2$ ($X$ = Si, Ge) in the paramagnetic phase studied by soft X-ray ARPES and hard X-ray photoelectron spectroscopy

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 $hν$-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$_2$.

cond-mat.str-el↗

arXiv2005

Charge dynamics in strongly correlated one-dimensional Cu-O chain systems revealed by inelastic X-ray scattering

We report on the Cu 1s resonant inelastic X-ray scattering (RIXS) of Cu-O one-dimensional (1D) strongly correlated insulator systems with contrasting atomic arrangements, namely edge-sharing CuGeO3 and corner-sharing Sr2CuO3. Owing to good statistics of the high-resolution RIXS data, so far unresolved fine structures are revealed. Detailed photon-energy and momentum dependence of the RIXS spectra in comparison with theoretical calculations has clarified the natures of the low-energy charge excitations and hybridization of the electronic states.

cond-mat.str-el↗

arXiv2004

Driving mechanisms behind the various phases in manganese perovskites revealed by Mn 2p resonance photoemission

Unusual temperature and doping dependence of the Mn 3d spectral functions of manganese perovskites Nd1-xSrxMnO3 has been revealed by the high-resolution Mn 2p-3d resonance photoemission. The temperature-dependent spectra cannot be explained by any theoretical model currently under debate, while showing evidence for a microscopic and dynamic phase segregation. The experimental results strongly suggest that the competition of both the dynamical and static Jahn-Teller effects with ferromagnetic ordering at high and low temperatures, respectively, is responsible for the actual electronic states.

cond-mat.str-el↗

arXiv2002

High-resolution Photoemission Study of Cd2Re2O7

High-resolution bulk-sensitive photoemission has been measured for pyrochlore oxide Cd2Re2O7. Temperature variations of the spectral shapes between 20 and 250 K are obviously observed for the Re 4f inner core and the valence band spectra. The Re 5d states are dominant for the DOS near the Fermi level.

cond-mat.str-el↗