arXiv subjects

Jun Okamoto

Publications and source records attributed to Jun Okamoto.

At least 19 recordsLinked to original sources

arXiv2026

Selective coupling of high-order phonons in La2-xSrxCuO4

In crystals and molecules with strong coupling between the charge carriers and atomic vibrations, high order harmonics of the vibrational excitations can be observed with intensity following the Franck-Condon envelope. Here, we uncover a new regime of electron-phonon coupling in La2-xSrxCuO4 using resonant inelastic X-ray scattering. In the undoped compound, we find sharp peaks at approximately 85$\pm$5 meV, 180$\pm$7 meV, and 330$\pm$5 meV with no observable dispersion, and an absence of appreciable intensity from other modes observed in Raman spectroscopy in this energy range. The 180 meV and 330 meV excitations have energies approximately consistent with two-phonon and four-phonon in-plane Cu-O bond stretching mode, suggesting that the resonantly excited valence electrons strongly couple to this mode. These excitations exhibit significant doping dependence, eventually becoming unresolvable at 10% hole doping, where the low energy charge excitations are dominated by dispersive plasmons. The observation of selective coupling to even-ordered phonons and stark contrast with the Raman spectra indicate anomalous electron-phonon coupling beyond the Franck-Condon picture. One intriguing possibility is the existence of locally paired quasiparticles in insulating cuprates.

cond-mat.str-el↗

arXiv2026

Spectroscopic evidence for a molecular orbital Kondo insulator

A Kondo insulator (KI) is a prototypical example of a highly entangled phase of matter, where many-body interactions between local moments and delocalized electrons engender the non-magnetic insulating ground state. Conventionally, the local moments arise from atomic multiplet states with a narrow bandwidth, limiting Kondo coherence to low temperatures. Here, we realize a new paradigm for constructing the KI state with hybridized molecular orbitals in FeSb2. Resonant inelastic X-ray scattering (RIXS) at the Fe L-edge reveals distinct signatures of band-like continuum states and localized states. Comparisons with first-principles calculations establish a mixed-configuration ground state with hybridized Fe d-Sb p molecular orbitals as basis states. By systematically investigating the RIXS momentum, temperature, and doping dependences, we find propagating collective modes commensurate with many-body charge and spin excitations. Our results pave the way for understanding the emerging class of unconventional d electron insulators and engineering high temperature Kondo many-body states.

cond-mat.str-el↗

arXiv2026

Collective spin excitations in trilayer nickelate La$_4$Ni$_3$O$_{10}$

Ruddlesden-Popper (RP) nickelates have recently emerged as a new family of high-temperature superconductors. In bilayer RP nickelates, magnetic excitations with large exchange couplings have been observed, supporting a spin-mediated pairing mechanism. Whether comparable spin correlations persist in trilayer nickelates, however, remains unknown. Here, we present a Ni $L$-edge resonant inelastic X-ray scattering (RIXS) study of La$_4$Ni$_3$O$_{10}$ single crystals. While the orbital excitations remain similar to those of La$_3$Ni$_2$O$_{7}$, the collective spin excitations in La$_4$Ni$_3$O$_{10}$ exhibit a comparable bandwidth of about $60$ meV but substantially suppressed spectral weight, implying a weaker electronic correlation in the trilayer compounds. Our results underscore the three-dimensional and multi-orbital electronic character in La$_4$Ni$_3$O$_{10}$, highlighting important differences from the bilayer nickelates. These findings provide crucial insights into the evolution of magnetism across the RP nickelate family and its connection to superconductivity.

cond-mat.supr-con↗

arXiv2025

Possibility of ferro-octupolar order in Ba$_2$CaOsO$_6$ assessed by X-ray magnetic dichroism measurements

Localized $5d^2$ electrons in a cubic crystal field possess multipoles such as electric quadrupoles and magnetic octupoles. We studied the cubic double perovskite Ba$_2$CaOsO$_6$ containing the Os$^{6+}$ ($5d^2$) ions, which exhibits a phase transition to a `hidden order' below $T^* \sim$ 50 K, by X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) at the Os $L_{2,3}$ edge. The cubic ligand-field splitting between the $t_{2g}$ and $e_g$ levels of Os $5d$ was deduced by XAS to be $\sim$4 eV. Ligand-field (LF) multiplet calculation under fictitious strong magnetic fields indicated that the exchange interaction between nearest-neighbor octupoles should be as strong as $\sim$1.5 meV if a ferro-octupolar order is stabilized in the `hidden-ordered' state, consistent with the exchange interaction of $\sim$1 meV previously predicted theoretically using model and density functional theory calculations. The temperature dependence of the XMCD spectra was consistent with a $\sim$18 meV residual cubic splitting of the lowest $J_{\rm eff} =$ 2 multiplet state into the non-Kramers $E_g$ doublet ground state and the $T_{2g}$ triplet excited state.

cond-mat.str-el↗

arXiv2025

Persistent paramagnons in high-temperature infinite-layer nickelate superconductors

The recent discovery of high-temperature superconductivity in hole-doped SmNiO$_2$, exhibiting the record-high transition temperature $T_c$ among infinite-layer (IL) nickelates, has opened a new avenue for exploring design principles of superconductivity. Experimentally determining the electronic structure and magnetic interactions in this new system is crucial to elucidating the mechanism behind the enhanced superconductivity. Here, we report a Ni $L$-edge resonant inelastic x-ray scattering (RIXS) study of superconducting Sm-based IL nickelate thin films Sm$_{1-x-y-z}$Eu$_x$Ca$_y$Sr$_z$NiO$_2$ (SECS). Dispersive paramagnonic excitations are observed in both optimally and overdoped SECS samples, supporting a spin-fluctuation-mediated pairing scenario. However, despite the two-fold enhancement of $T_c$ in the Sm-based nickelates compared to their Pr-based counterparts, the effective exchange coupling strength is reduced by approximately $20\%$. This behavior contrasts with hole-doped cuprates, where magnetic interactions correlate positively with $T_c$, highlighting essential differences in their superconducting mechanisms.

cond-mat.supr-con↗

arXiv2025

Enhanced Superconductivity and Mixed-dimensional Behaviour in Infinite-layer Samarium Nickelate Thin Films

Rare-earth infinite-layer nickelates represent an emerging class of unconventional superconductors, with materials synthesis largely limited to early lanthanide compounds. Here, we report the synthesis and characterization of phase-pure superconducting samarium-based infinite-layer nickelate thin films, including the first demonstration of Sm$_{1-x}$Sr$_x$NiO$_2$, along with co-doped variants incorporating europium and calcium. These films, grown on LSAT (001) substrates, exhibit coherent lattice structures up to $\sim$ 9 nm thickness with minimal stacking faults. The co-doped compounds achieve a record-small $c$-axis parameter of 3.26 {\AA} and display remarkable superconducting transition temperatures up to 32.5 K. These results establish a clear correlation between decreasing $c$-axis parameter and increasing critical temperature across different rare-earth systems. In addition, angle-dependent magnetoresistance investigations reveal the existence of a hybrid mixture of 2D and 3D superconductivity in this novel system with enhanced coupling between the rare-earth 5d and Ni 3d orbitals, confirmed by resonant inelastic X-ray scattering experiments. As the concentration of Eu increases, the system exhibits a clear tendency towards 3D superconductivity. Furthermore, we observe distinctive negative magnetoresistance in the europium-containing samples. These findings advocate clear materials design principles for higher transition temperatures and exotic physics in infinite-layer nickelate superconductors through structural engineering of the rare-earth site.

cond-mat.supr-con↗

arXiv2024

Visualizing Shape Functionals via Sinkhorn Multidimensional Scaling

In this paper, we present Sinkhorn multidimensional scaling (Sinkhorn MDS) as a method for visualizing shape functionals in shape spaces. This approach uses the Sinkhorn divergence to map these infinite-dimensional spaces into lower-dimensional Euclidean spaces. We establish error estimates for the embedding generated by Sinkhorn MDS compared to the unregularized case. Moreover, we validate the method through numerical experiments, including visualizations of the classical Dido's problem and two newly introduced shape functionals: the double-well and Sinkhorn cone-type shape functionals. Our results demonstrate that Sinkhorn MDS effectively captures and visualizes shapes of shape functionals.

math.OC↗

arXiv2024

On segmentation by total variation type energies of Kobayashi-Warren-Carter type with fidelity

We consider a total variation type energy which measures the jump discontinuities different from usual total variation energy. Such a type of energy is obtained as a singular limit of the Kobayashi-Warren-Carter energy with minimization with respect to the order parameter. We consider the Rudin-Osher-Fatemi type energy by replacing relaxation term by this type of total variation energy. We show that all minimizers are piecewise constant if the data function in the fidelity term is continuous in one-dimensional setting. Moreover, the number of jumps is bounded by an explicit constant involving a constant related to the fidelity. This is quite different from conventional Rudin-Osher-Fatemi energy where a minimizer has no jumps if the data has no jumps. Our results give an upper bound of the number of segments in a segmentation problem. The existence of a minimizer is guaranteed in multi-dimensional setting when the data is bounded.

math.AP↗

arXiv2024

Spin Excitations and Flat Electronic Bands in a Cr-based Kagome Superconductor

In the quest for topology- and correlation-driven quantum states, kagome lattice materials have garnered significant interest for their band structures, featuring flat bands (FBs) from the quantum destructive interference of the electronic wavefunction. Tuning an FB to the chemical potential could induce electronic instabilities and emergent orders. Despite extensive studies, direct evidence of FBs tuned to the chemical potential and their role in emergent orders in bulk materials remains lacking. Using angle-resolved photoemission spectroscopy, resonant inelastic X-ray scattering, and density functional theory, we show that the low-energy structure of the Cr-based kagome metal superconductor {\Cr} is dominated by FBs at the Fermi level. We also observe low-energy magnetic excitations evolving across the low-temperature transition, largely consistent with the FB shift. Our results suggest that the low-temperature order contains a magnetic origin and that the kagome FBs may play a role in the emergence of this order.

cond-mat.str-el↗

arXiv2023

Giant X-ray circular dichroism in a time-reversal invariant altermagnet

X-ray circular dichroism, arising from the contrast in X-ray absorption between opposite photon helicities, serves as a spectroscopic tool to measure the magnetization of ferromagnetic materials and identify the handedness of chiral crystals. Antiferromagnets with crystallographic chirality typically lack X-ray magnetic circular dichroism because of time-reversal symmetry, yet exhibit weak X-ray natural circular dichroism. Here, we report the observation of giant natural circular dichroism in the Ni $L_3$-edge X-ray absorption of Ni$_3$TeO$_6$, a polar and chiral antiferromagnet with effective time-reversal symmetry. To unravel this intriguing phenomenon, we propose a phenomenological model that classifies the movement of photons in a chiral crystal within the same symmetry class as that of a magnetic field. The coupling of X-ray polarization with the induced magnetization yields giant X-ray natural circular dichroism, revealing the altermagnetism of Ni$_3$TeO$_6$. Our findings provide evidence for the interplay between magnetism and crystal chirality in natural optical activity. Additionally, we establish the first example of a new class of magnetic materials exhibiting circular dichroism with time-reversal symmetry.

cond-mat.str-el↗

arXiv2023

Fractional time differential equations as a singular limit of the Kobayashi-Warren-Carter system

This paper is concerned with a singular limit of the Kobayashi-Warren-Carter system, a phase field system modelling the evolutions of structures of grains. Under a suitable scaling, the limit system is formally derived when the interface thickness parameter tends to zero. Different from many other problems, it turns out that the limit system is a system involving fractional time derivatives, although the original system is a simple gradient flow. A rigorous derivation is given when the problem is reduced to a gradient flow of a single-well Modica-Mortola functional in a one-dimensional setting.

math.AP↗

arXiv2023

Performance of prototype Dual Gain Multilayer Thick GEM with high-intensity heavy-ion beam injections in low-pressure hydrogen gas

A prototype Dual Gain Multilayer Thick Gas Electron Multilyer (DG-M-THGEM) with an active area of 10 cm $\times$ 10 cm was manufactured aiming at the production of a large-volume active-target time projection chamber which can work under the condition of high-intensity heavy-ion beam injections. The DG-M-THGEM has a alternating structure of electrodes and insulators. Effective gas gains of two regions, which are called beam and recoil regions, are separately controlled. Performance of the prototype DG-M-THGEM in hydrogen gas at a pressure of 40 kPa was evaluated. Irradiating a $^{132}$Xe beam, an effective gas gain lower than 100 with a charge resolution of 3% was achieved in the beam region while the effective gas gain of 2000 was maintained in the recoil region. Position distributions of measured charges along the beam axis were investigated in order to evaluate gain uniformity in the high intensity beam injection. The gain shift was estimated by simulations considering space charges in the drift region. The gain shift was suppressed within 3% even at the beam intensity of 2.5 $\times$ 10$^{6}$ particles per second.

physics.ins-det↗

arXiv2022

Graph gradient flows : from discrete to continuum

This paper gives a framework to study a continuum limit of a gradient flow on a graph where the number of vertices increases in an appropriate way. As examples we prove the convergence of a discrete total variation flow and a discrete Allen--Cahn flow on discretised tori to their respective continuum limits.

math.AP↗

arXiv2022

On a singular limit of the Kobayashi--Warren--Carter energy

By introducing a new topology, a representation formula of the Gamma limit of the Kobayashi-Warren-Carter energy is given in a multi-dimensional domain. A key step is to study the Gamma limit of a single-well Modica-Mortola functional. The convergence introduced here is called the sliced graph convergence, which is finer than conventional $L^1$ convergence, and the problem is reduced to a one-dimensional setting by a slicing argument.

math.AP↗

arXiv2020

Post-growth annealing effects on charge and spin excitations in Nd$_{2-x}$Ce$_x$CuO$_4$

We report a Cu K- and L$_3$-edge resonant inelastic x-ray scattering study of charge and spin excitations of bulk Nd$_{2-x}$Ce$_x$CuO$_4$, with focus on post-growth annealing effects. For the parent compound Nd$_2$CuO$_4$ ($x = 0$), a clear charge-transfer gap is observed in the as-grown state, whereas the charge excitation spectra indicate that electrons are doped in the annealed state. This is consistent with the observation that annealed thin-film and polycrystalline samples of RE$_2$CuO$_4$ (RE = rare earth) can become metallic and superconducting at sufficiently high electron concentrations without Ce doping. For $x = 0.16$, a Ce concentration for which it is known that oxygen reduction destroys long-range antiferromagnetic order and induces superconductivity, we find that the high-energy spin excitations of non-superconducting as-grown and superconducting annealed crystals are nearly identical. This finding is in stark contrast to the significant changes in the low-energy spin excitations previously observed via neutron scattering.

cond-mat.supr-con↗

arXiv2020

Revealing the site selective local electronic structure of Co$_{3}$O$_{4}$ using $2p3d$ resonant inelastic X-ray scattering

We investigate mixed-valence oxide Co$_3$O$_4$ using Co $2p3d$ resonant inelastic X-ray scattering (RIXS). By setting resonant edges at Co$^{2+}$ and Co$^{3+}$ ions, the $dd$ excitations on the two Co sites are probed selectively, providing detailed information on the local electronic structure of Co$_3$O$_4$. The $2p3d$ RIXS result reveals the $^4$T$_{2}$ excited state of tetrahedral Co$^{2+}$ site at 0.5 eV beyond the discriminative power of optical absorption spectroscopies. Additionally, the $^3$T$_{2g}$ excited stated at 1.3 eV is uniquely identified for the octahedral Co$^{3+}$ site. Guided by cluster multiplet simulations, the ground-state character of the Co$^{2+}$ and Co$^{3+}$ site is determined to be high-spin $^4$A$_{2}$(T$_d$) and low-spin $^1$A$_{1g}$(O$_h$), respectively. This indicates that only the Co$^{2+}$ site is magnetically active site at low-temperatures in Co$_3$O$_4$. The ligand-to-metal charge transfer analysis suggests a formation of a strong covalent bonding between Co and O ions at the Co$^{3+}$ site, while Co$^{2+}$ is rather ionic.

cond-mat.mtrl-sci↗

arXiv2020

A finer singular limit of a single-well Modica--Mortola functional and its applications to the Kobayashi--Warren--Carter energy

An explicit representation of the Gamma limit of a single-well Modica--Mortola functional is given for one-dimensional space under the graph convergence which is finer than conventional $L^1$-convergence or convergence in measure. As an application, an explicit representation of a singular limit of the Kobayashi-Warren-Carter energy, which is popular in materials science, is given. Some compactness under the graph convergence is also established. Such formulas, as well as compactness, is useful to characterize the limit of minimizers the Kobayashi-Warren-Carter energy. To characterize the Gamma limit under the graph convergence, a new idea which is especially useful for one-dimensional problem is introduced. It is a change of parameter of the variable by arc-length parameter of its graph, which is called unfolding by the arc-length parameter in this paper.

math.AP↗

arXiv2019

Random discretization of O'Hara knot energy

We considered random discrete approximation of O'Hara energy. O'Hara energy is the energy defined for a knot, and O'Hara energy was introduced for defining the standard shape for each knot class (equivalence class by ambient isotopy) by variational method. In the case of a specific exponent, due to energy invariance under Moebius transformation, this energy is called Moebius energy. Although discretization for various Moebius energies has been defined to analyse the shape of the minimizer so far, only Gamma-convergence to the original energy has been shown for a conventional discretization. In this study, we are successful to show locally uniform convergence and compactness of discrete energy in a space based on optimal transport theory, by introducing random discrete approximation of O'Hara energy using random variable.

math.CA↗