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J. Okamoto

Publications and source records attributed to J. Okamoto.

At least 19 recordsLinked to original sources

Orbital-specific Itinerancy and Localization in a Kagome Magnet

The kagome lattice naturally hosts flat bands, Dirac fermions, and van Hove singularities, yet whether its geometry can stabilize orbital-selective phases - a hallmark of Hund's physics in multi-orbital correlated systems - has remained an open question. Here, we combine resonant inelastic X-ray scattering with density functional theory and dynamical mean-field theory to demonstrate that YMn$_6$Sn$_6$ exhibits a spontaneous orbital differentiation into coexisting itinerant and localized electrons within the same Mn $3d$ manifold. Orbitals directed along Mn-Mn bonds provide coherent quasiparticles and metallic bands, while those pointing toward ligands become strongly correlated and display non-Fermi-liquid behavior. Hund's intra-atomic exchange suppresses orbital fluctuations, stabilizing this dichotomy and providing a natural double-exchange-like mechanism for the observed ferromagnetic bilayer coupling. Our work establishes YMn$_6$Sn$_6$ as a kagome platform where orbital selectivity, flat-band topology, and Hund's metallicity converge - revealing that geometric frustration and correlation-driven orbital differentiation can cooperatively design exotic quantum phases beyond the canonical paradigms of Mott physics or band topology alone.

cond-mat.str-el

Quantum critical behavior of cuprate superconductors observed by inelastic X-ray scattering

Progress toward a complete understanding of cuprate superconductors has been hindered by their intricate phase diagram, potentially linked to a quantum critical point (QCP). However, conclusive evidence for the QCP is lacking, as the presumed QCP is buried under the superconducting dome, disguising its presence. Here, we use high-resolution resonant inelastic X-ray scattering to examine the dynamical charge-charge correlation in La$_{2-x}$Sr$_x$CuO$_4$ and uncover the quantum critical scaling, a key feature required for a QCP. Specifically, \djh{we observed that the inverse correlation lengths for various dopings and temperatures collapsed onto a universal scaling curve, yielding a critical exponent $\nu$ of $0.74 \pm 0.08$. The non-negativity of this exponent confirms the presence of a QCP. Remarkably, the value of $\nu$ suggests that while the QCP is manifested through the charge-density wave, other orders also participate, such that the QCP appears to belong to the universality class characterized by the O(4) symmetry, reminiscent of the microscopic SO(4) symmetry in the Hubbard model at half-filling. Further analysis indicates that the QCP is highly dissipative with a short quasi-particle lifetime, reflecting the intertwined quantum fluctuations due to its being buried inside the superconducting state.

cond-mat.str-el

First Extraction of the Matter Radius of $^{132}$Sn via Proton Elastic Scattering at 200 MeV/Nucleon

The angular distribution of the differential cross sections for proton elastic scattering from $^{132}$Sn at 196-210 MeV/nucleon was successfully measured over a momentum transfer range of 0.80 to 2.1 fm$^{-1}$. Using a relativistic impulse approximation, the root-mean-square matter radius of $^{132}$Sn was extracted to be $4.758^{+0.023}_{-0.024}$ fm, which was compared with the state-of-the-art ab initio calculations. Combined with the charge radius measured at ISOLDE, there are no theoretical calculations consistent with both matter and charge radii within the experimental errors.

nucl-ex

Non-reciprocal circular dichroism of axial phonons coupled to ferro-rotational order

Circular dichroism (CD) in X-ray absorption, defined as the difference in absorption between opposite circular polarizations, is fundamentally enabled by the breaking of time-reversal symmetry or inversion symmetry. It is therefore sensitive to magnetism, chirality, and their interplay. In contrast, the sample symmetry alone is insufficient to determine whether CD in resonant inelastic X-ray scattering (RIXS) is allowed. Rather, RIXS-CD is governed by both the sample symmetry and the scattering geometry. Here, using RIXS, we identify circularly polarized phonons coupled to ferro-rotational order in MnTiO$_3$, which we refer to as ferro-axial phonons. Their excitations provide a direct demonstration of non-reciprocal RIXS-CD, in which the dichroic response changes upon reversing the propagation direction of the incident X-rays, although the system globally preserves both inversion and time-reversal symmetries. We propose that a condensate of these phonons, manifested as standing waves, underlies the ferro-rotational order in MnTiO$_3$. The observed non-reciprocal CD reflects the interplay among photon helicity, phonon polarization, and ferro-rotational order.

cond-mat.str-el

Altermagnetic boosting of chiral phonons

Chirality characterizes the asymmetry between a structure and its mirror image and underlies a wide range of chiral functionalities. In crystallographically chiral materials, phonons with non-zero linear momentum $\textbf{k}$ can acquire a $k$-induced longitudinal magnetization, giving rise to chiral phonons. Helical spin order, with its proper screw-type configuration, breaks all mirror symmetries and therefore carries magnetic chirality. Such helical spins also generate non-relativistic spin splitting for any quasiparticle excitations propagating along the screw axis. To explore the possible connection between chiral phonons and magnetic chirality, we investigated the crystallographically polar and chiral compound (Mn,Ni)$_3$TeO$_6$, which hosts three distinct states: a paramagnetic state, a helical spin state with magnetic chirality, and a collinear spin state without magnetic chirality. We find an approximately tenfold enhancement of chiral-phonon coupling in the helical spin state along the screw axis, compared with both the paramagnetic and collinear spin states. These results identify a new route to amplify chiral phonons through an altermagnetic effect arising from the broken parity-time symmetry in helical spins. %from non-relativistic spin splitting.

cond-mat.str-el

Bimagnon dispersion of La2CuO4 probed by resonant inelastic X-ray scattering

We report on the study of the magnetic excitations of Mott insulator La2CuO4 by using resonant inelastic x-ray scattering (RIXS) and cluster calculations within the framework of exact diagonalization. Our results demonstrate experimentally that the bimagnon excitation in Cu L-edge RIXS is enhanced if the incident x-ray energy is slightly above the absorption edge. Through incident-energy-dependent momentum-resolved RIXS, we investigated the excitation of the bimagnon with predominantly A1 symmetry. The bimagnons of La2CuO4 exhibit a nearly flat dispersion with momentum along the Cu-O bond direction. This observation agrees with the bimagnon dispersion from the calculations on a single-band Hubbard model rather than a Heisenberg model with only the nearest neighbor exchange interaction. This means that the effect of the higher-order spin couplings such as the cyclic or ring exchange interactions caused by the coherent motion of electrons beyond nearest-neighbor sites is important for understanding the bimagnon dynamics of cuprates.

cond-mat.str-el

Out-of-phase Plasmon Excitations in the Trilayer Cuprate Bi$_2$Sr$_2$Ca$_2$Cu$_3$O$_{10+\delta}$

Within a homologous series of cuprate superconductors, variations in the stacking of CuO$_2$ layers influence the collective charge dynamics through the long-range Coulomb interactions. We use O $K$-edge resonant inelastic x-ray scattering to reveal plasmon excitations in the optimally-doped trilayer Bi$_2$Sr$_2$Ca$_2$Cu$_3$O$_{10+\delta}$. The observed plasmon exhibits nearly $q_z$-independent dispersion and a large excitation gap of approximately 300 meV. This mode is primarily ascribed to the $\omega_{-}$ mode, where the charge density on the outer CuO$_2$ sheets oscillates out of phase while the density in the inner sheet remains unaltered at $q_z=0$. The intensity of the acoustic $\omega_3$ mode is relatively weak and becomes vanishingly small near $(q_x, q_y)=(0, 0)$. This result highlights a qualitative change in the eigenmode of the dominant low-energy plasmon with the number of CuO$_2$ layers.

cond-mat.str-el

Spin-orbit-entangled electronic structure of Ba$_2$CaOsO$_6$ studied by O $K$-edge resonant inelastic X-ray scattering

Transition-metal ions with $5d^2$ electronic configuration in a cubic crystal field are prone to have a vanishing dipolar magnetic moment but finite higher-order multipolar moments, and they are expected to exhibit exotic physical properties. Through an investigation using resonant inelastic X-ray spectroscopy (RIXS), Raman spectroscopy, and theoretical ligand-field (LF) multiplet and $ab initio$ calculations, we fully characterized the local electronic structure of Ba$_2$CaOsO$_6$, particularly, the crystal-field symmetry of the 5$d^2$ electrons in this anomalous material. The low-energy multiplet excitations from RIXS at the oxygen $K$ edge and Raman-active phonons both show no splitting. These findings are consistent with the ground state of Os ions dominated by magnetic octupoles. Obtained parameters pave the way for further realistic microscopic studies of this highly unusual class of materials, advancing our understanding of spin-orbit physics in systems with higher-order multipoles.

cond-mat.str-el

Exciton dynamics uncovering electron fractionalization in superconducting cuprates

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$_{8+δ}$ 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.

cond-mat.str-el

Magnetic Properties and Electronic Configurations of Mn Ions in the Diluted Magnetic Semiconductor Ba$_{1-x}$K$_{x}$(Zn$_{1-y}$Mn$_{y}$)$_{2}$As$_{2}$ Studied by X-ray Magnetic Circular Dichroism and Resonant Inelastic X-ray Scattering

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 $0.45μ_{\text{B}}$/Mn and the small orbital moment of $0.05μ_{\text{B}}$/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.

cond-mat.str-el

Quantum fluctuations of charge order induce phonon softening in a superconducting cuprate

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.

cond-mat.supr-con

Acoustic plasmons and conducting carriers in hole-doped cuprate superconductors

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.

cond-mat.str-el

Evolution of valence-specific spin states and local distortions in La$_{2-x}$Sr$_x$CoO$_4$

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.

cond-mat.str-el

Compressional-mode resonances in the molybdenum isotopes: Emergence of softness in open-shell nuclei near A=90

"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($α,α^\prime$) reaction at $E_α= 386$ 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 $A=92$.

nucl-ex

Development of the Soft X-ray AGM-AGS RIXS Beamline at Taiwan Photon Source

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.

physics.ins-det

Novel multi-layer plastic-scintillator-based solid active proton target for inverse-kinematics experiments

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.

physics.ins-det

Coulomb correlations intertwined with spin and orbital excitations in LaCoO$_3$

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.

cond-mat.str-el

Doping Dependence of Collective Spin and Orbital Excitations in Spin 1 Quantum Antiferromagnet La$_{2-x}$Sr$_x$NiO$_4$ Observed by X-rays

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.

cond-mat.str-el