Combining photoemission and optical spectroscopies for reliable valence determination in YbS and Yb metal
M. Matsunami, A. Chainani, M. Taguchi, R. Eguchi, Y. Ishida, Y. Takata, H. Okamura, T. Nanba, M. Yabashi, K. Tamasaku, Y. Nishino, T. Ishikawa, Y. Senba, H. Oha… 展开作者
M. Matsunami, A. Chainani, M. Taguchi, R. Eguchi, Y. Ishida, Y. Takata, H. Okamura, T. Nanba, M. Yabashi, K. Tamasaku, Y. Nishino, T. Ishikawa, Y. Senba, H. Ohashi, A. Ochiai, S. Shin
Hard x-ray photoemission and optical spectroscopies have been performed on YbS and Yb metal to determine the precise $f$-electron occupation. A comparison of the photoemission spectra with the energy loss functions in bulk and surface, obtained from optical reflectivity, enables us to distinguish between the energy loss satellite of Yb$^{2+}$ peak and Yb$^{3+}$ multiplet. The results clearly indicate a purely divalent Yb state except for the surface of YbS. We demonstrate that the present method is highly reliable in identifying the electronic structure and the mean valence in $f$-electron systems.
Recently, $α$-$\textrm{RuCl}_3$ has attracted much attention as a possible material realization of the honeycomb Kitaev model, which may stabilize a quantum-spin-liquid state. Compared to extensive studies on its magnetic properties, there is still a lack of understanding on its electronic structure, which is strongly related with its Kitaev physics. Here, the electronic structure of $α$-$\textrm{RuCl}_3$ is investigated by photoemission (PE) and inverse photoemission (IPE) spectroscopies. The band gap, directly measured from PE/IPE spectra, is found to be 1.9 eV, much larger than previous est…
The basic theory of photoemission, inverse photoemission, Auger-electron and appearance-potential spectroscopy is developed within a unified framework starting from Fermi's golden rule. The spin-resolved and temperature-dependent appearance-potential spectroscopy of band-ferromagnetic transition metals is studied in detail. It is shown that the consideration of electron correlations and orbitally resolved transition-matrix elements is essential for a quantitative agreement with experiments for Ni.
Xclaim (x-ray core level atomic multiplets) is a graphical interface for the calculation of core-hole spectroscopy and ground state properties within a charge-transfer multiplet model taking into account a many-body hamiltonian with Coulomb, spin-orbit, crystal-field, and hybridization interactions. Using Hartree-Fock estimates for the Coulomb and spin-orbit interactions and ligand field parameters (crystal-field, hybridization and charge-transfer energy) the program can calculate x-ray absorption spectroscopy (XAS), x-ray photoemission spectroscopy (XPS), photoemission spectrospcy (PES) and i…
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 $Γ{_6}$, the spatial distribution of which is directed along the $c$-axis. The XMCD results give support to the picture of local-moment magn…
We have performed a photoemission spectroscopy (PES) study of CeM2Al10 (M = Fe, Ru, and Os) to directly observe the electronic structure involved in the unusual magnetic ordering. Soft X-ray resonant (SXR) PES provides spectroscopic evidence of the hybridization between conduction and Ce 4f electrons (c-f hybridization) and the order of the hybridization strength (Ru < Os < Fe). High-resolution (HR) PES of CeRu2Al10 and CeOs2Al10, as compared with that of CeFe2Al10, identifies two structures that can be ascribed to structures induced by the c-f hybridization and the antiferromagnetic ordering,…
In a system with strong local repulsive interactions it should be more difficult to add an electron than to extract one. We make this idea precise by deriving various exact sum rules for the one-particle spectral function independent of the details of the Hamiltonian describing the system and of the nature of the ground state. We extend these results using a variational ansatz for the superconducting ground state and low lying excitations. Our results shed light on the striking asymmetry in the tunneling spectra of high Tc superconductors and should also be useful in estimating the local dopin…
The joint density of states (JDOS) of Bi2Sr2CaCu2O8+x is calculated by evaluating the autocorrelation of the single particle spectral function A(k,omega) measured from angle resolved photoemission spectroscopy (ARPES). These results are compared with Fourier transformed (FT) conductance modulations measured by scanning tunneling microscopy (STM). Good agreement between the two experimental probes is found for two different doping values examined. In addition, by comparing the FT-STM results to the autocorrelated ARPES spectra with different photon polarization, new insight on the form of the S…
Recent realization of well-controlled quantum simulators of the triangular-lattice Fermi-Hubbard model, including the triangular optical lattices loaded with ultracold Fermions and the heterostructures of the transition-metal dichalcogenides, as well as the more advanced techniques to probe them, pave the way for studying frustrated Fermi-Hubbard physics. Here, we theoretically predict asymmetric photoemission and tunneling spectroscopies for a lightly hole-doped and electron-doped triangular Mott antiferromagnet, and reveal two distinct types of magnetic polarons: a \emph{lightly} renormalize…
Relaxation energies for photoemission, when an occupied electronic state is excited, and for inverse photoemission, when an empty state is filled, are calculated within the density functional theory with application to Nd$_{2-x}$Ce$_x$CuO$_4$. The associated relaxation energies are obtained by computing differences in total energies between the ground state and an excited state in which one hole or electron is added into the system. The relaxation energies of f-electrons are found to be of the order of several eV's, indicating that f-bands will appear substantially away from the Fermi energy (…
The electronic properties of the Mn:GaSe interface, produced by evaporating Mn at room temperature on an epsilon-GaSe(0001) single crystal surface, have been studied by soft X-ray spectroscopies. Substitutional effects of Mn replacing Ga cations and Mn-Se hybridization effects are found both in core level and valence band photoemission spectra. The Mn cation valence state is probed by XAS measurements at the Mn L-edge, which indicate that Mn diffuses into the lattice as a Mn2+ cation with negligible crystal field effects. The Mn spectral weight in the valence band is probed by resonant photoem…
We compare efforts to extract self energies and fluctuation spectra of the cuprates using optical and photoemission techniques. The fluctuations have contributions from both the coherent and incoherent parts of the band, which are spread over the full bare bandwidth of >2eV. Many experimental studies concentrate on the coherent part of the band and hence miss higher energy fluctuations. Our study establishes the universal presence of high energy bosonic fluctuations across various spectroscopies as a key ingredient in the high temperature superconducting cuprates.
High-resolution hard X-ray photoemission measurements have been performed to clarify the electronic structure originating from the strong correlation between electrons in bulk Ce 3$d$ core-level spectra of CeNi$_{1-x}$Co$_x$Ge$_2$ (0 $\leq$ $x$ $\leq$ 1). In the Ce 3$d_{5/2}$ core-level spectra, the variation of satellite structures ($f^2$ peaks) shows that the hybridization strength between Ce 4$f$- and conduction electrons gradually increases with Co concentration in good agreement with the results of Ce 3$d-4f$ and 4$d-4f$ resonant photoemission spectroscopies. Particularly, in Ce 3$d_{3/2}…
We have analyzed experimental evidence for an anomalous transfer of spectral weight from high to low energy scales in both electron and hole doped cuprates as a function of doping. X-ray scattering, optical and photoemission spectra are all found to show that the high energy spectral weight decreases with increasing doping at a rate much faster than predictions of the large $U-$limit calculations. The observed doping evolution is however well-described by an intermediate coupling scenario where the effective Hubbard $U$ is comparable to the bandwidth. The experimental spectra across various sp…
The localized-to-itinerant transition of f electrons lies at the heart of heavy-fermion physics, but has only been directly observed in single-layer Ce-based materials. Here, we report a comprehensive study on the electronic structure and nature of the Ce 4f electrons in the heavy-fermion superconductor Ce2PdIn8, a typical n=2 CenMmIn3n+2m compound, using high-resolution and 4d-4f resonance photoemission spectroscopies. The electronic structure of this material has been studied over a wide temperature range, and hybridization between f and conduction electrons can be clearly observed to form a…
Unified description of cuprate superconductors by fractionalized electrons emerging from integrated analyses of photoemission spectra and quasiparticle interference
Sophia University（上智大学）；RIKEN Center for Emergent Matter Science（理化学研究所物质结构科学中心）；National Institute for Materials Science（国立材料研究所）；RIKEN Center for Computational Science（理化学研究所计算科学中心）；Schrödinger Inc.（薛定谔公司）；University of Tokyo（东京大学）；Ames National Laboratory（艾姆斯国家实验室）；Iowa State University（爱荷华州立大学）；ISSP, University of Tokyo（东京大学国际超导材料研究中心）；Kyoto University（京都大学）
The experimental finding of an ubiquitous kink in the nodal direction of angle-resolved photoemission spectroscopies of superconducting cuprates has been reproduced theoretically. Our model is built upon the Migdal-Eliashberg theory for the electron self-energy within the phonon-coupling scenario. Following this perturbative approach, a numerical evaluation of the bare band dispersion energy in terms of the electron-phonon coupling parameter $λ$ allows a unified description of the nodal-kink effect. Our study reveals that distinction between $λ$ and the technically defined mass-enhancement par…
In order to realize superconductivity in cuprates with the T'-type structure, not only chemical substitution (Ce doping) but also post-growth reduction annealing is necessary. In the case of thin films, however, well-designed reduction annealing alone without Ce doping can induce superconductivity in the T'-type cuprates. In order to unveil the origin of superconductivity in the Ce-undoped T'-type cuprates, we have performed bulk-sensitive hard x-ray photoemission and soft x-ray absorption spectroscopies on superconducting and non-superconducting Nd$_{2-x}$Ce$_x$CuO$_4$ ($x=$ 0, 0.15, and 0.19…
Kondo scaling of $4f$-electron states and the Kondo singlet breakdown in heavy fermions
Helmholtz-Zentrum Berlin für Materialien und Energie（柏林亥姆霍兹材料与能源中心）；Heidelberg University（海德堡大学）；Synchrotron SOLEIL（SOLEIL同步辐射中心）；Université de Rennes, CNRS, Institut des Sciences Chimiques de Rennes-UMR6226（雷恩大学，法国国家科学研究中心，雷恩化学科学研究所）；Université de Lorraine, CNRS, Institut Jean Lamour（洛林大学，法国国家科学研究中心，让·拉穆尔研究所）；National Synchrotron Radiation Research Center（国家同步辐射研究中心）
We report studies of the electronic structure and elementary excitations of doped and undoped cuprate chains, ladders and planes. Using high energy spectroscopies such as x-ray absorption, core level photoemission and angle resolved photoemission spectroscopy, important information regarding the charge distribution and hole dynamics can be obtained. The comparison of the experimental data with suitable theoretical models sets constraints on the parameters entering into the model calculations, and offers insight into the important physical quantities governing the electronic structure of these …
We investigated the electronic structure of the Si(111)--7$\times$7 surface below 20 K by scanning tunneling and photoemission spectroscopies and by density functional theory calculations. Previous experimental studies have questioned the ground state of this surface, which is expected to be metallic in a band picture because of the odd number of electrons per unit cell. Our differential conductance spectra instead show the opening of an energy gap at the Fermi level and a significant temperature dependence of the electronic properties, especially for the adatoms at the center of the unfaulted…
Photoemission insights into lanthanide-based crystals
St. Petersburg State University（圣彼得堡国立大学）；Moscow Institute of Physics and Technology (State University)（莫斯科物理技术学院（国立大学））；Kristall- und Materiallabor, Physikalisches Institut, Goethe University Frankfurt（法兰克福歌德大学物理学院晶体与材料实验室）；Donostia International Physics Center (DIPC)（多诺西亚国际物理中心）；University of the Basque Country UPV/EHU（巴斯克大学）；IKERBASQUE, Basque Foundation for Science（伊克尔巴斯基克科学基金会）
Ultrafast spectroscopies have become an important tool for elucidating the microscopic description and dynamical properties of quantum materials. In particular, by tracking the dynamics of non-thermal electrons, a material's dominant scattering processes -- and thus the many-body interactions between electrons and collective excitations -- can be revealed. Here we present a new method for extracting the electron-phonon coupling strength in the time domain, by means of time and angle-resolved photoemission spectroscopy (TR-ARPES). This method is demonstrated in graphite, where we investigate th…
Intriguing properties of the misfit layered chalcogenide (LaS)$_{1.196}$VS$_2$ crystals were investigated by transport, optical measurements, angle-resolved photoemission (ARPES) and x-ray diffraction. Although no clear anomaly is found in transport properties as a function of temperature, a large spectral weight transfer, up to at least 1 eV, is observed by both optical and photoemission spectroscopies. ARPES reveals that a nearly filled band with negative curvature, close enough from the Fermi level at 300K to produce metallic-like behaviour as observed in optical conductivity spectra. At lo…
Re-examination of electronic structure of dilute Kondo transition-metal ions substituted into a Heavy Fermion compound
Waseda University（早稻田大学）；University of Tokyo（东京大学）；National Institutes for Quantum Science and Technology（量子科学技术研究开发机构）；Japan Synchrotron Radiation Research Institute（日本同步辐射研究所）；Kumamoto University（熊本大学）
