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Electron quasiparticles play a crucial role in simplifying the description of many-body physics in solids with surprising success. Conventional Landau's Fermi-liquid and quasiparticle theories for high-temperature superconducting cuprates have, however, received skepticism from various angles. A path-breaking framework of electron fractionalization has been established to replace the Fermi-liquid theory for systems that show the fractional quantum Hall effect and the Mott insulating phenomena; whether it captures the essential physics of the pseudogap and superconducting phases of cuprates is still an open issue. Here, we show that excitonic excitation of optimally doped Bi$_2$Sr$_2$CaCu$_2$O$_{8+\delta}$ with energy far above the superconducting-gap energy scale, about 1 eV or even higher, is unusually enhanced by the onset of superconductivity. Our finding proves the involvement of such high-energy excitons in superconductivity. Therefore, the observed enhancement in the spectral weight of excitons imposes a crucial constraint on theories for the pseudogap and superconducting mechanisms. A simple two-component fermion model which embodies electron fractionalization in the pseudogap state well explains the change, pointing toward a novel route for understanding the electronic structure of superconducting cuprates.

The magnetic properties and the electronic excitations of the new diluted magnetic semiconductor Ba$_{1-x}$K$_{x}$(Zn$_{1-y}$Mn$_{y}$)$_{2}$As$_{2}$ have been studied by x-ray magnetic circular dichroism (XMCD) and resonant inelastic x-ray scattering (RIXS) at the Mn $L_{2,3}$ edge. The sum rule analysis of the XMCD spectra yields the net spin moment of $0.45\mu_{\text{B}}$/Mn and the small orbital moment of $0.05\mu_{\text{B}}$/Mn. This indicates that the Mn atoms are in the high-spin configurations of $d^{5}$, whereas the presence of competing ferromagnetic and antiferromagnetic interactions between the Mn ions reduces the net spin moment. RIXS spectra show broad peaks from 1 to 6 eV energy loss, which originate from the $d$-$d$ crystal field excitations of the Mn ions. Based on a comparison of the RIXS line shapes with those of Ga$_{1-x}$Mn$_{x}$As, we conclude that the ground state of Mn in Ba$_{1-x}$K$_{x}$(Zn$_{1-y}$Mn$_{y}$)$_{2}$As$_{2}$ consists not only of the charge-transferred $3d^{5}\underline{L}$ electron configuration ($\underline{L}$: ligand hole) with weakly bound holes as in Ga$_{1-x}$Mn$_{x}$As, but also of the pure $3d^{5}$ configuration with free holes.

Quantum phase transitions play an important role in shaping the phase diagram of high-temperature cuprate superconductors. These cuprates possess intertwined orders which interact strongly with superconductivity. However, the evidence for the quantum critical point associated with the charge order in the superconducting phase remains elusive. Here we show the short-range charge orders and the spectral signature of the quantum fluctuations in La$_{2-x}$Sr$_x$CuO$_4$ (LSCO) near the optimal doping using high-resolution resonant inelastic X-ray scattering. On performing calculations through a diagrammatic framework, we discovered that the charge correlations significantly soften several branches of phonons. These results elucidate the role of charge order in the LSCO compound, providing evidence for quantum critical scaling and discommensurations associated with charge order., Comment: 9 pages, 4 figures

The superconductivity of cuprates, which has been a mystery ever since its discovery decades ago, is created through doping electrons or holes into a Mott insulator. There, however, exists an inherent electron-hole asymmetry in cuprates. The layered crystal structures of cuprates enable collective charge excitations fundamentally different from those of three-dimensional metals, i.e., acoustic plasmons. Acoustic plasmons have been recently observed in electron-doped cuprates by resonant inelastic X-ray scattering (RIXS); in contrast, there is no evidence for acoustic plasmons in hole-doped cuprates, despite extensive measurements. This contrast led us to investigate whether the doped holes in cuprates La$_{2-x}$Sr$_x$CuO$_4$ are conducting carriers or are too incoherent to induce collective charge excitation. Here we present momentum-resolved RIXS measurements and calculations of collective charge response via the loss function to reconcile the aforementioned issues. Our results provide unprecedented spectroscopic evidence for the acoustic plasmons and long sought conducting p holes in hole-doped cuprates.

We report on the development of a high-resolution and highly efficient beamline for soft-X-ray resonant inelastic X-ray scattering (RIXS) located at Taiwan Photon Source. This beamline adopts an optical design that uses an active grating monochromator (AGM) and an active grating spectrometer (AGS) to implement the energy compensation principle of grating dispersion. Active gratings are utilized to diminish defocus, coma and higher-order aberrations as well as to decrease the slope errors caused by thermal deformation and optical polishing. The AGS is mounted on a rotatable granite platform to enable momentum-resolved RIXS measurements with scattering angle over a wide range. Several high-precision instruments developed in house for this beamline are briefly described. The best energy resolution obtained from this AGM-AGS beamline was 12.4 meV at 530 eV, achieving a resolving power 42,000, while the bandwidth of the incident soft X-rays was kept at 0.5 eV. To demonstrate the scientific impacts of high-resolution RIXS, we present an example of momentum-resolved RIXS measurements on a high-temperature superconducting cuprate, La$_{2-x}$Sr$_x$CuO$_4$. The measurements reveal the A$_{1g}$ apical oxygen phonons in superconducting cuprates, opening a new opportunity to investigate the coupling between these phonons and charge density waves., Comment: 9 pages, p figures, submitted to J. of Synchrotron Radiation. Revise expression

"Why are the tin isotopes soft?" has remained, for the past decade, an open problem in nuclear structure physics: models which reproduce the isoscalar giant monopole resonance (ISGMR) in the "doubly-closed shell" nuclei, $^{90}$Zr and $^{208}$Pb, overestimate the ISGMR energies of the open-shell tin and cadmium nuclei, by as much as 1 MeV. In an effort to shed some light onto this problem, we present results of detailed studies of the ISGMR in the molybdenum nuclei, with the goal of elucidating where--and how--the softness manifests itself between $^{90}$Zr and the cadmium and tin isotopes. The experiment was conducted using the $^{94,96,98,100}$Mo($\alpha,\alpha^\prime$) reaction at $E_\alpha = 386$ MeV. A comparison of the results with relativistic, self-consistent Random-Phase Approximation calculations indicates that the ISGMR response begins to show softness in the molybdenum isotopes beginning with $A=92$., Comment: Accepted for publication to Physics Letters B

We present X-ray spectroscopic evidence for the evolution of valence-specific spin states and tetragonal distortions in single-layer cobaltates. Measurements of Co $L_3$-edge resonant inelastic X-ray scattering reveal the $t_{2g}$ electronic structure of Co for hole-doped La$_{2-x}$Sr$_x$CoO$_4$ ($x$ = 0.5, 0.7 and 0.8). As the Sr-doping $x$ increases, the tetragonal splitting of the $t_{2g}$ states of high-spin Co$^{2+}$ decreases, whereas that of low-spin Co$^{3+}$ increases and the fraction of high-spin Co$^{3+}$ increases. The results enable us to clarify the origin of the change of magnetic anisotropy and in-plane resistivity in a mixed-valence cobaltate caused by the interplay of spin-orbit coupling and tetragonal distortion., Comment: 8 pages, 6 figures. published in Phys. Rev. B online 12 August 2021

We have constructed and tested a novel plastic-scintillator-based solid-state active proton target for use in nuclear spectroscopic studies with nuclear reactions induced by an ion beam in inverse kinematics. The active target system, named Stack Structure Solid organic Scintillator Active Target (S4AT), consists of five layers of plastic scintillators, each with a 1-mm thickness. To determine the reaction point in the thickness direction, we exploit the difference in the energy losses due to the beam particle and the charged reaction product(s) in the scintillator material. S4AT offers the prospect of a relatively thick target while maintaining a good energy resolution. By considering the relative energy loss between different layers, the energy loss due to unreacted beam particles can be eliminated. Such procedure, made possible by the multi-layer structure, is essential to eliminate the effect of unreacted accompanying beam particles, thus enabling its operation at a moderate beam intensity of up to a few Mcps. We evaluated the performance of S4AT by measuring the elastic proton-proton scattering using a 70-MeV proton beam at Cyclotron and Radioisotope Center (CYRIC), Tohoku University., Comment: 32 pages, 14 figures

We carried out temperature-dependent (20 - 550 K) measurements of resonant inelastic X-ray scattering on LaCoO$_3$ to investigate the evolution of its electronic structure across the spin-state crossover. In combination with charge-transfer multiplet calculations, we accurately quantized the renormalized crystal-field excitation energies and spin-state populations. We show that the screening of the on-site Coulomb interaction of 3d electrons is orbital selective and coupled to the spin-state crossover in LaCoO$_3$. The results establish that the gradual spin-state crossover is associated with a relative change of Coulomb energy versus bandwidth, leading to a Mott-type insulator-to-metal transition., Comment: 6 pages, 4 figures. Submitted to Phys. Rev. Lett

We report the first empirical demonstration that resonant inelastic x-ray scattering (RIXS) is sensitive to \emph{collective} magnetic excitations in $S=1$ systems by probing the Ni $L_3$-edge of La$_{2-x}$Sr$_x$NiO$_4$ ($x = 0, 0.33, 0.45$). The magnetic excitation peak is asymmetric, indicating the presence of single and multi spin-flip excitations. As the hole doping level is increased, the zone boundary magnon energy is suppressed at a much larger rate than that in hole doped cuprates. Based on the analysis of the orbital and charge excitations observed by RIXS, we argue that this difference is related to the orbital character of the doped holes in these two families. This work establishes RIXS as a probe of fundamental magnetic interactions in nickelates opening the way towards studies of heterostructures and ultra-fast pump-probe experiments., Comment: 8 pages, 4 figures, see ancillary files for the supplemental material

The magnetic correlations within the cuprates have undergone intense scrutiny as part of efforts to understand high temperature superconductivity. We explore the evolution of the magnetic correlations along the nodal direction of the Brillouin zone in La2-xSrxCuO4, spanning the doping phase diagram from the anti-ferromagnetic Mott insulator at x = 0 to the metallic phase at x = 0.26. Magnetic excitations along this direction are found to be systematically softened and broadened with doping, at a higher rate than the excitations along the anti-nodal direction. This phenomenology is discussed in terms of the nature of the magnetism in the doped cuprates. Survival of the high energy magnetic excitations, even in the overdoped regime, indicates that these excitations are marginal to pairing, while the influence of the low energy excitations remains ambiguous., Comment: 8 pages, 6 figures

Resonant inelastic x-ray scattering is used to investigate the electronic origin of orbital polarization in nickelate heterostructures taking $\mathrm{LaTiO_3-LaNiO_3-3x(LaAlO_3)}$, a system with exceptionally large polarization, as a model system. We find that heterostructuring generates only minor changes in the Ni $3d$ orbital energy levels, contradicting the often-invoked picture in which changes in orbital energy levels generate orbital polarization. Instead, O $K$-edge x-ray absorption spectroscopy demonstrates that orbital polarization is caused by an anisotropic reconstruction of the oxygen ligand hole states. This provides an explanation for the limited success of theoretical predictions based on tuning orbital energy levels and implies that future theories should focus on anisotropic hybridization as the most effective means to drive large changes in electronic structure and realize novel emergent phenomena., Comment: Accepted for publication in Physical Review Letters. 6 pages, 4 figures

The first known magnetic mineral, magnetite (Fe$_3$O$_4$), has unusual properties which have fascinated mankind for centuries; it undergoes the Verwey transition at $T_{\rm V}$ $\sim$120 K with an abrupt change in structure and electrical conductivity. The mechanism of the Verwey transition however remains contentious. Here we use resonant inelastic X-ray scattering (RIXS) over a wide temperature range across the Verwey transition to identify and separate out the magnetic excitations derived from nominal Fe$^{2+}$ and Fe$^{3+}$ states. Comparison of the RIXS results with crystal-field multiplet calculations shows that the spin-orbital $dd$ excitons of the Fe$^{2+}$ sites arise from a tetragonal Jahn-Teller active polaronic distortion of the Fe$^{2+}$O$_6$ octahedra. These low-energy excitations, which get weakened for temperatures above 350 K but persist at least up to 550 K, are distinct from optical excitations and best explained as magnetic polarons.

Measurements of spin excitations are essential for an understanding of spin-mediated pairing for superconductivity; and resonant inelastic X-ray scattering (RIXS) provides a considerable opportunity to probe high-energy spin excitations. However, whether RIXS correctly measures the collective spin excitations of doped superconducting cuprates remains under debate. Here we demonstrate distinct Raman- and fluorescence-like RIXS excitations of Bi$_{1.5}$Pb$_{0.6}$Sr$_{1.54}$CaCu$_{2}$O$_{8+{\delta}}$ in the mid-infrared energy region. Combining photon-energy and momentum dependent RIXS measurements with theoretical calculations using exact diagonalization provides conclusive evidence that the Raman-like RIXS excitations correspond to collective spin excitations, which are magnons in the undoped Mott insulators and evolve into paramagnons in doped superconducting compounds. In contrast, the fluorescence-like shifts are due primarily to the continuum of particle-hole excitations in the charge channel. Our results show that under the proper experimental conditions RIXS indeed can be used to probe paramagnons in doped high-$T_c$ cuprate superconductors.

The layered transition metal dichalcogenides host a rich collection of charge density wave (CDW) phases in which both the conduction electrons and the atomic structure display translational symmetry breaking. Manipulating these complex states by purely electronic methods has been a long-sought scientific and technological goal. Here, we show how this can be achieved in 1T-TaS2 in the two-dimensional (2D) limit. We first demonstrate that the intrinsic properties of atomically-thin flakes are preserved by encapsulation with hexagonal boron nitride in inert atmosphere. We use this facile assembly method together with TEM and transport measurements to probe the nature of the 2D state and show that its conductance is dominated by discommensurations. The discommensuration structure can be precisely tuned in few-layer samples by an in-plane electric current, allowing continuous electrical control over the discommensuration-melting transition in 2D.

We investigated the electronic and magnetic properties of fully oxidized BaFeO3 thin films, which show ferromagnetic-insulating properties with cubic crystal structure, by hard x-ray photoemission spectroscopy (HAXPES), x-ray absorption spectroscopy (XAS) and soft x-ray magnetic circular dichroism (XMCD). We analyzed the results with configuration-interaction (CI) cluster-model calculations for Fe4+, which showed good agreement with the experimental results. We also studied SrFeO3 thin films, which have an Fe4+ ion helical magnetism in cubic crystal structure, but are metallic at all temperatures. We found that BaFeO3 thin films are insulating with large magnetization (2.1muB/formula unit) under ~ 1 T, using valence-band HAXPES and Fe 2p XMCD, which is consistent with the previously reported resistivity and magnetization measurements. Although Fe 2p core-level HAXPES and Fe 2p XAS spectra of BaFeO3 and SrFeO3 thin films are quite similar, we compared the insulating BaFeO3 to metallic SrFeO3 thin films with valence-band HAXPES. The CI cluster-model analysis indicates that the ground state of BaFeO3 is dominated by d5L (L: ligand hole) configuration due to the negative charge transfer energy, and that the band gap has significant O 2p character. We revealed that the differences of the electronic and magnetic properties between BaFeO3 and SrFeO3 arise from the differences in their lattice constants, through affecting the strength of hybridization and bandwidth., Comment: 8 pages, 5 figures

We studied the charge-orbital ordering in the superlattice of charge-ordered insulating Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ and ferromagnetic metallic La$_{0.5}$Sr$_{0.5}$MnO$_3$ by resonant soft x-ray diffraction. A temperature-dependent incommensurability is found in the orbital order. In addition, a large hysteresis is observed that is caused by phase competition between insulating charge ordered and metallic ferromagnetic states. No magnetic phase transitions are observed in contrast to bulk, confirming the unique character of the superlattice. The deviation from the commensurate orbital order can be directly related to the decrease of ordered-layer thickness that leads to a decoupling of the orbital-ordered planes along the c axis., Comment: 4 pages, 5 figures

Charge dynamics and its critical behavior are investigated near the metal-insulator transition of layered-nickelate R2-xSrxNiO4 (R=Nd, Eu). The polarized x-ray absorption spectroscopy experiment clearly shows the multi-orbital nature which enables the x2-y2-orbital-based checkerboard-type charge ordering or correlation to persist up to the critical doping region (x sim 1). In the barely metallic region proximate to the charge-ordered insulating phase, the nominal carrier density estimated from the Hall coefficient markedly decreases in accord with development of the pseudogap structure in the optical conductivity spectrum, while the effective mass is least enhanced. The present findings combined with the results of recent angle-resolved photoemission spectroscopy show that the pseudogap in the metal-insulator critical state evolves due to the checkerboard-type charge correlation to extinguish the coherent-motion carriers in a characteristic momentum (k)-dependent manner with lowering temperature., Comment: 7 pages, 6 figures. Accepted in Physical Review B

We investigated the magnetic structure of an orthorhombic YMnO3 thin film by resonant soft x-ray and hard x-ray diffraction. We observed a temperature-dependent incommensurate magnetic reflection below 45 K and a commensurate lattice-distortion reflection below 35 K. These results demonstrate that the ground state is composed of coexisting E-type and cycloidal states. Their different ordering temperatures clarify the origin of the large polarization to be caused by the E-type antiferromagnetic states in the orthorhombic YMnO3 thin film., Comment: 4 pages, 6 figures

Static charge-density wave (CDW) and spin-density wave (SDW) order has been convincingly observed in La-based cuprates for some time. However, more recently it has been suggested by quantum oscillation, transport and thermodynamic measurements that density wave order is generic to underdoped cuprates and plays a significant role in YBa_2Cu_3O_{6+delta} (YBCO). We use resonant soft x-ray scattering at the Cu L and O K edges to search for evidence of density wave order in Ortho-II and Ortho-VIII oxygen-ordered YBCO. We report a null result -- no evidence for static CDW order -- in both Ortho-II and Ortho-VIII ordered YBCO. While this does not rule out static CDW order in the CuO_2 planes of YBCO, these measurements place limits on the parameter space (temperature, magnetic field, scattering vector) in which static CDW order may exist. In addition, we present a detailed analysis of the energy and polarization dependence of the Ortho-II superstructure Bragg reflection [0.5 0 0] at the Cu L edge. The intensity of this peak, which is due to the valence modulations of Cu in the chain layer, is compared with calculations using atomic scattering form factors deduced from x-ray absorption measurements. The calculated energy and polarization dependence of the scattering intensity is shown to agree very well with the measurement, validating the approach and providing a framework for analyzing future resonant soft x-ray scattering measurements., Comment: 11 pages, 9 figures

The magnetic properties of as-grown Ga$_{1-x}$Mn$_{x}$As have been investigated by the systematic measurements of temperature and magnetic field dependent soft x-ray magnetic circular dichroism (XMCD). The {\it intrinsic} XMCD intensity at high temperatures obeys the Curie-Weiss law, but residual spin magnetic moment appears already around 100 K, significantly above Curie temperature ($T_C$), suggesting that short-range ferromagnetic correlations are developed above $T_C$. The present results also suggest that antiferromagnetic interaction between the substitutional and interstitial Mn (Mn$_{int}$) ions exists and that the amount of the Mn$_{int}$ affects $T_C$., Comment: 4 pages, 4 figures

Ca_1-xSr_xRuO_3, which is ferromagnetic for Sr concentration x > 0.3, has been studied by x-ray magnetic circular dichroism (XMCD) in Ru 3p and O 1s core-level x-ray absorption. XMCD signals appear at x ~ 0.3 and monotonically increases with x in the ferromagnetic phase. While the monotonic increase of the XMCD signals with x is of a typical Stoner-type, the absence of appreciable change in the spectral line shapes of both the Ru 3p and O 1s XMCD spectra indicate that the itinerant-electron ferromagnetism in Ca_1-xSr_xRuO_3 is influenced by strong electron correlation., Comment: 5 pages, 4 figures, accepted in Phys. Rev. B 1 page, correct the 4th affiliation 5 page, modifiy 9th reference

Based on measurements of soft x-ray magnetic scattering and symmetry considerations, we demonstrate that the magnetoelectric effect in TbMn$_2$O$_5$ arises from an internal field determined by $\vec{S}_{\vec{q}} \times {\vec{S}_{-\vec{q}}}$ with $\vec{S}_{\vec{q}}$ being the magnetization at modulation vector $\vec{q}$, whereas the magneto-elastic effect in the exchange energy governs the response to external electric fields. Our results set fundamental symmetry constraints on the microscopic mechanism of multiferroicity in frustrated magnets.

We performed a soft x-ray magnetic circular dichroism (XMCD) study of a Zn$_{1-x}$V$_x$O thin film which showed small ferromagnetic moment. Field and temperature dependences of V 2$p$ XMCD signals indicated the coexistence of Curie-Weiss paramagnetic, antiferromagnetic, and possibly ferromagnetic V ions, quantitatively consistent with the magnetization measurements. We attribute the paramagnetic signal to V ions substituting Zn sites which are somewhat elongated along the c-axis.

We have performed photoemission and soft x-ray absorption studies of pyrochlore-type Ru oxides, namely, the filling-control system Sm$_{2-x}$Ca$_x$Ru$_2$O$_7$ and the bandwidth-control system Sm$_{2-x}$Bi$_x$Ru$_2$O$_7$, which show insulator-to-metal transition with increasing Ca and Bi concentration, respectively. Core levels and the O 2$p$ valence band in Sm$_{2-x}$Ca$_x$Ru$_2$O$_7$ show almost the same amount of monotonous upward energy shifts with Ca concentration, which indicates that the chemical potential is shifted downward due to hole doping. The Ru 4$d$ band in Sm$_{2-x}$Ca$_x$Ru$_2$O$_7$ is also shifted toward the Fermi level ($E_F$) with hole doping and the density of states (DOS) at $E_F$ increases. The core levels in Sm$_{2-x}$Bi$_x$Ru$_2$O$_7$, on the other hand, do not show clear energy shifts except for the Ru 3$d$ core level, whose line shape change also reflects the increase of metallic screening with Bi concentration. We observe pronounced spectral weight transfer from the incoherent to the coherent parts of the Ru 4d $t_{2g}$ band with Bi concentration, which is expected for a bandwidth-control Mott-Hubbard system. The increase of the DOS at $E_F$ is more abrupt in the bandwidth-control Sm$_{2-x}$Bi$_x$Ru$_2$O$_7$ than in the filling-control Sm$_{2-x}$Ca$_x$Ru$_2$O$_7$, in accordance with a recent theoretical prediction. Effects of charge transfer between the Bi 6$sp$ band and the Ru 4$d$ band are also discussed., Comment: 11 pages, 6 figures

We report on the results of x-ray absorption (XAS), x-ray magnetic circular dichroism (XMCD), and photoemission experiments on {\it n}-type Zn$_{1-x}$Co$_x$O ($x=0.05$) thin film, which shows ferromagnetism at room temperature. The XMCD spectra show a multiplet structure, characteristic of the Co$^{2+}$ ion tetrahedrally coordinated by oxygen, suggesting that the ferromagnetism comes from Co ions substituting the Zn site in ZnO. The magnetic field and temperature dependences of the XMCD spectra imply that the non-ferromagnetic Co ions are strongly coupled antiferromagnetically with each other., Comment: 5pages, 4figures

We have studied the electronic structure of the diluted magnetic semiconductor Ga$_{1-x}$Mn$_{x}$N ($x$ = 0.0, 0.02 and 0.042) grown on Sn-doped $n$-type GaN using photoemission and soft x-ray absorption spectroscopy. Mn $L$-edge x-ray absorption have indicated that the Mn ions are in the tetrahedral crystal field and that their valence is divalent. Upon Mn doping into GaN, new state were found to form within the band gap of GaN, and the Fermi level was shifted downward. Satellite structures in the Mn 2$p$ core level and the Mn 3$d$ partial density of states were analyzed using configuration-interaction calculation on a MnN$_{4}$ cluster model. The deduced electronic structure parameters reveal that the $p$-$d$ exchange coupling in Ga$_{1-x}$Mn$_{x}$N is stronger than that in Ga$_{1-x}$Mn$_{x}$As., Comment: 6pages, 10figures. To be published to Phys. Rev. B

Measurements of polarization-dependent soft x-ray absorption reveal that the electronic states determining the low-energy excitations of Na$_{x}$CoO$_2$ have predominantly $a_{1g}$ symmetry with significant O $2p$ character. A large transfer of spectral weight observed in O $1s$ x-ray absorption provides spectral evidence for strong electron correlations in the layered cobaltates. Comparing Co $2p$ x-ray absorption with calculations based on a cluster model, we conclude that Na$_{x}$CoO$_2$ exhibits a charge-transfer electronic character rather than a Mott-Hubbard character.