arXiv subjects

M. Isobe

Publications and source records attributed to M. Isobe.

At least 19 recordsLinked to original sources

arXiv2026

High temperature transitions in Ruddlesden-Popper nickelates La$_{n+1}$Ni$_{n}$O$_{3n+1}$

The discovery of superconductivity at $15\,\mathrm{K}$ in the infinite-layer nickelate $(\mathrm{Nd},\mathrm{Sr})\mathrm{NiO}_2$, followed by superconductivity at $80\,\mathrm{K}$ in the Ruddlesden--Popper phase $\mathrm{La}_3\mathrm{Ni}_2\mathrm{O}_7$, has ushered in a new era of nickelate research. Despite this progress, large discrepancies between reports exist. Here, we investigate the complete series of bulk-stable $\mathrm{La}_{n+1}\mathrm{Ni}_n\mathrm{O}_{3n+1}$ compounds using a comprehensive set of experimental techniques, including PXRD, single-crystal XRD, electron microscopy, heat capacity, differential scanning calorimetry, magnetic susceptibility, and transport measurements, over a broad temperature range from $2$ to $1000\,\mathrm{K}$. By studying high-quality single crystals, we identify a previously underappreciated high-temperature phase transition in Ruddlesden--Popper nickelates $\mathrm{La}_{n+1}\mathrm{Ni}_n\mathrm{O}_{3n+1}$ distinct from the one going to a tetragonal phase.

cond-mat.supr-con↗

arXiv2025

Multiorbital character of the density wave in trilayer nickelate superconductors

Ruddlesden-Popper nickelates exhibit high-temperature superconductivity closely intertwined with charge and spin density waves. However, fundamental questions persist regarding the interplay between the associated density wave (DW) fluctuations and superconductivity, as well as the orbital character and symmetry underlying the DW instabilities. Here we utilize polarized Raman scattering to investigate the phononic and electronic Raman responses of the trilayer nickelate La$_4$Ni$_3$O$_{10}$ across its concomitant charge and spin density wave transitions. In addition to distinct phonon anomalies occurring below the transition temperature, we observe a depletion of continuum spectral weight up to 114 meV and a pronounced peak centered at this energy. By combining momentum-selective information from polarized electronic Raman scattering with Raman-response model calculations based on a multiorbital Raman vertex in a reconstructed two-orbital DW state involving both Ni-3$d_{x^2 - y^2}$ and Ni-3$d_{z^2}$ orbitals, we identify 114 meV as the energy scale $2\Delta_\mathrm{DW}$ of the DW gap, characterized by incoherent opening and non-mean-field behavior. Furthermore, the model calculations reveal that the corresponding $2\Delta_\mathrm{DW}$ peak has a multiorbital origin, requiring both orbital contributions and their mixing beyond single-orbital projections, thus shedding light on the nature of the DW instabilities in La$_4$Ni$_3$O$_{10}$.

cond-mat.str-el↗

arXiv2025

Floating zone growth at high oxygen pressures in Ruddlesden-Popper bilayer nickelate Y$_{y}$Sr$_{3-y}$Ni$_{2-x}$Al$_{x}$O$_{7-\delta}$

With the discovery of superconductivity under pressure in the Ruddlesden-Popper (RP) bilayer La$_3$Ni$^{2.5+}_2$O$_7$ and trilayer La$_4$Ni$^{2.66+}_3$O$_{10}$, a new field of nickelate superconductors opened up. In this respect, Sr-Ni-O RP-type phases represent alternative systems that exist with partial cation substitution. We demonstrate that by Y-doping in Sr$_{3}$Ni$_{2-x}$Al$_{x}$O$_7$ (SNAO), as Y$_{y}$Sr$_{3-y}$Ni$_{2-x}$Al$_{x}$O$_7$ (YSNAO), the drawback of an insulating ground state is overcome, and a significant decrease in resistivity is achieved with crystals exhibiting semiconducting behavior. We employ optical floating zone (OFZ) growth at 10 bar oxygen partial pressure to explore the phase formation in a narrow region of Y-Sr-Ni-Al-O and investigate via DFT the general stability of the pure Sr-Ni-O scenario. Using extensive diffraction and spectroscopy, as well as transport and magnetization measurements, the structural, chemical, electrical, and magnetic properties of the as-grown and reduced compounds were investigated. The optimal growth of YSNAO allows for large high quality crystals suitable for neutron studies. In the Al-free growth, a known $n=1$ RP system with Sr$_{1.66}$Y$_{0.33}$NiO$_{4-\delta}$, from which the first single crystals were obtained, was further confirmed, opening the door for future exploration of \textit{A}-site substituted RP-type phases without Ni-site disorder.

cond-mat.supr-con↗

arXiv2024

Magnetic ground state of the dimer-based hexagonal perovskite Ba$_{3}$ZnRu$_{2}$O$_{9}$

We investigate the magnetic ground state of single crystals of the ruthenium-dimer-based hexagonal perovskite Ba$_{3}$ZnRu$_{2}$O$_{9}$ using magnetic susceptibility and resonant inelastic x-ray scattering (RIXS) measurements. While a previous study on powder samples exhibited intriguing magnetic behavior, questions about whether the spin state within a Ru$_{2}$O$_{9}$ dimer is a conventional $S = 3/2$ dimer or an orbital-selective $S = 1$ dimer were raised. The RIXS spectra reveal magnetic excitations from Hund's intraionic multiplet and intradimer spin-triplet transitions. The observed transition energies of the Hund's intraionic multiplets align with the $S=3/2$ ground state, contrasting with the theoretically proposed orbital-selective $S=1$ dimer state. High-temperature magnetic susceptibility analysis confirms the realization of the spin $S=3/2$ dimer state, and the extracted intradimer coupling is consistent with the spin-triplet transition energy observed in the RIXS spectra. These results highlights the ability of "spectroscopic fingerprinting" by RIXS to determine the magnetic ground states of complex materials.

cond-mat.str-el↗

arXiv2024

Charge-exchange measurements of high-energy fast ions in LHD using negative-ion neutral beam injection

A new sightline geometry for the fast-ion D-alpha (FIDA) diagnostic on the Large Helical Device (LHD) has been confirmed to measure signals for high-energy fast ions produced by negative-ion neutral beam injection. The newly installed sightline uses a 180 keV tangential negative-ion neutral beamline as the active source. Due to the small angle between the beamline and FIDA sightline, the relative velocity between fast ions and injected neutrals is small. This allows for high-energy fast ions just below the beam injection energy to produce measurable Doppler-shifted FIDA emission. Experiments were conducted at LHD in order to compare the new sightline, which views a high-energy negative-ion tangential beamline, and the old sightline, which views a low-energy perpendicular positive-ion neutral beamline. The measured FIDA signal is validated against predictions from the synthetic fast-ion diagnostic code FIDASIM with a distribution function modelled by the 5D transport code GNET. The results of the experiment confirm that reducing the viewing angle with a tangential active beam allows FIDA diagnostic to view high-energy fast ions with a sufficient signal-to-noise ratio.

physics.plasm-ph↗

arXiv2024

Metastable ordered states induced by low temperature annealing of {\delta}-Ag2/3V2O5

In {\delta}-Ag2/3V2O5 with charge degrees of freedom in V, it is known that the charge ordering state and physical properties of V that appear at low temperatures depend strongly on the ordering state of Ag. In this study, we focused on the Ag ions in the interlayer and studied the structure using synchrotron radiation powder diffraction in dependence on temperature. We found that when the sample is slowly cooled from room temperature and ordering occurs at the Ag sites, V4+/V5+ charge ordering of V and subsequent V4+-V4+ structural dimers are produced. Although quenching the sample from room temperature suppresses the ordering of Ag, annealing at around 160 K promotes partial ordering of Ag and allows a metastable phase to be realized. This metastable phase is maintained even when the temperature is lowered again, producing a remarkable change in low-temperature properties. These results indicate that the ordered state of Ag, which is the key to control the charge-ordered state and physical properties, can be controlled by low-temperature annealing. The results of this study may provide a methodology for the realization of metastable states in a wide range of material groups of vanadium compounds, where competition among various charge ordered states underlies the physical properties.

cond-mat.str-el↗

arXiv2024

Investigation of spin excitations and charge order in bulk crystals of the infinite-layer nickelate LaNiO$_2$

Recent x-ray spectroscopic studies have revealed spin excitations and charge density waves in thin films of infinite-layer (IL) nickelates. However, clarifying whether the origin of these phenomena is intrinsic to the material class or attributable to impurity phases in the films has presented a major challenge. Here we utilize topotactic methods to synthesize bulk crystals of the IL nickelate LaNiO$_2$ with crystallographically oriented surfaces. We examine these crystals using resonant inelastic x-ray scattering (RIXS) at the Ni $L_3$-edge to elucidate the spin and charge correlations in the bulk of the material. While we detect the presence of prominent spin excitations in the crystals, fingerprints of charge order are absent at the ordering vectors identified in previous in thin-film studies. These results contribute to the understanding of the bulk properties of LaNiO$_2$ and establish topotactically synthesized crystals as viable complementary specimens for spectroscopic investigations.

cond-mat.str-el↗

arXiv2023

Single crystal synthesis, structure, and magnetism of Pb$_{10-x}$Cu$_x$(PO$_4$)$_6$O

The recent claim of superconductivity above room temperature in Pb$_{10-x}$Cu$_x$(PO$_4$)$_6$O with 0.9 < $x$ < 1 (referred to as LK-99) has sparked considerable interest. To minimize the influence of structural defects and impurity phases on the physical properties, we have synthesized phase-pure single crystals with $x \sim 1$. We find that the crystals are highly insulating and optically transparent. X-ray analysis reveals an uneven distribution of the substituted Cu throughout the sample. Temperature ($T$) dependent magnetization measurements for $ 2 \leq T \leq 800$ K reveal the diamagnetic response characteristic of a non-magnetic insulator, as well as a small ferromagnetic component, possibly originating from frustrated exchange interactions in Cu-rich clusters in the Pb$_{10-x}$Cu$_x$(PO$_4$)$_6$O structure. No anomalies indicative of phase transitions are observed. We therefore rule out the presence of superconductivity in Pb$_{9}$Cu(PO$_4$)$_6$O crystals, and provide some considerations on the origin of anomalies previously reported in experiments on polycrystalline specimen.

cond-mat.supr-con↗

arXiv2023

Phase formation in hole- and electron-doped rare-earth nickelate single crystals

The recent discovery of superconductivity in hole-doped infinite-layer nickelates has triggered a great interest in the synthesis of novel nickelate phases, which have primarily been examined in thin film samples. Here, we report the high-pressure optical floating zone (OFZ) growth of various perovskite and perovskite-derived rare-earth nickelate single-crystals, and investigate the effects of hole-, electron-, and self-doping. For hole-doping with Ca and Sr, we observe phase separations during the growth process when a substitution level of 8% is exceeded. A similar trend emerges for electron-doping with Ce and Zr. Employing lower doping levels allows us to grow sizeable crystals in the perovskite phase, which exhibit significantly different electronic and magnetic properties than the undoped parent compounds, such as a decreased resistivity and a suppressed magnetic response. Our insights into the doping-dependent phase formation and the resulting properties of the synthesized crystals reveal limitations and opportunities for the exploration and manipulation of electronic states in rare-earth nickelates.

cond-mat.str-el↗

arXiv2021

Magnetic correlations in infinite-layer nickelates: an experimental and theoretical multi-method study

We report a comprehensive study of magnetic correlations in LaNiO$_{2}$, a parent compound of the recently discovered family of infinite-layer (IL) nickelate superconductors, using multiple experimental and theoretical methods. Our specific heat, muon-spin rotation ($\mu$SR), and magnetic susceptibility measurements on polycrystalline LaNiO$_{2}$ show that long-range magnetic order remains absent down to 2 K. Nevertheless, we detect residual entropy in the low-temperature specific heat, which is compatible with a model fit that includes paramagnon excitations. The $\mu$SR and low-field static and dynamic magnetic susceptibility measurements indicate the presence of short-range magnetic correlations and glassy spin dynamics, which we attribute to local oxygen non-stoichiometry in the average infinite-layer crystal structure. This glassy behavior can be suppressed in strong external fields, allowing us to extract the intrinsic paramagnetic susceptibility. Remarkably, we find that the intrinsic susceptibility shows non-Curie-Weiss behavior at high temperatures, in analogy to doped cuprates that possess robust non-local spin fluctuations. The distinct temperature dependence of the intrinsic susceptibility of LaNiO$_{2}$ can be theoretically understood by a multi-method study of the single-band Hubbard model in which we apply complementary cutting-edge quantum many-body techniques (dynamical mean-field theory, cellular dynamical mean-field theory and the dynamical vertex approximation) to investigate the influence of both short- and long-ranged correlations. Our results suggest a profound analogy between the magnetic correlations in parent (undoped) IL nickelates and doped cuprates.

cond-mat.str-el↗

arXiv2021

Formation of orbital molecules on a pyrochlore lattice induced by A-O bond covalency

The pyrochlore ruthenate In$_2$Ru$_2$O$_7$ displays a subtle competition between spin-orbital entanglement and molecular orbital formation. At room temperature, a spin-orbit-entangled singlet state was identified. With decreasing temperature, In$_2$Ru$_2$O$_7$ undergoes multiple structural transitions and eventually forms a nonmagnetic ground state with semi-isolated Ru$_2$O units on the pyrochlore lattice. The dominant hopping through the Ru-O-Ru linkage leads to molecular orbital formation within the Ru$_2$O units. This molecular orbital formation is unique in that it involves the O$^{2-}$ anions, unlike the transition-metal dimers observed in systems with edge-sharing octahedra. We argue that the covalent character of In-O bonds plays a pivotal role in the structural transitions and molecular orbital formation and such bonding character of "$A$-site" ions is an important ingredient for electronic phase competition in complex transition metal oxides.

cond-mat.str-el↗

arXiv2020

Tunneling-tip-induced collapse of the charge gap in the excitonic insulator Ta$_2$NiSe$_5$

Tuning many-body electronic phases by an external handle is of both fundamental and practical importance in condensed matter science. The tunability mirrors the underlying interactions, and gigantic electric, optical and magnetic responses to minute external stimuli can be anticipated in the critical region of phase change. The excitonic insulator is one of the exotic phases of interacting electrons, produced by the Coulomb attraction between a small and equal number of electrons and holes, leading to the spontaneous formation of exciton pairs in narrow-gap semiconductors/semimetals. The layered chalcogenide Ta$_2$NiSe$_5$ has been recently discussed as such an excitonic insulator with an excitation gap of ~250 meV below $T_c$ = 328 K. Here, we demonstrate a drastic collapse of the excitation gap in Ta$_2$NiSe$_5$ and the realization of a zero-gap state by moving the tip of a cryogenic scanning tunneling microscope towards the sample surface by a few angstroms. The collapse strongly suggests the many-body nature of the gap in the insulating state of Ta$_2$NiSe$_5$, consistent with the formation of an excitonic state. We argue that the collapse of the gap is driven predominantly by the electrostatic charge accumulation at the surface induced by the proximity of the tip and the resultant carrier doping of the excitonic insulator. Our results establish a novel phase-change function based on excitonic insulators.

cond-mat.str-el↗

arXiv2019

Validating the ASCOT modelling of NBI fast ions in Wendelstein 7-X stellarator

The first fast ion experiments in Wendelstein 7-X were performed in 2018. They are one of the first steps in demonstrating the optimised fast ion confinement of the stellarator. The fast ions were produced with a neutral beam injection (NBI) system and detected with infrared cameras (IR), a fast ion loss detector (FILD), fast ion charge exchange spectroscopy (FIDA), and post-mortem analysis of plasma facing components. The fast ion distribution function in the plasma and at the wall is being modelled with the ASCOT suite of codes. They calculate the ionisation of the injected neutrals and the consecutive slowing down process of the fast ions. The primary output of the code is the multidimensional fast ion distribution function within the plasma and the distribution of particle hit locations and velocities on the wall. Synthetic measurements based on ASCOT output are compared to experimental results to assess the validity of the modelling. This contribution presents an overview of the various fast ion measurements in 2018 and the current modelling status. The validation and data-analysis is on-going, but the wall load IR modelling already yield results that match with the experiments.

physics.plasm-ph↗

arXiv2018

Almost pure $J_{\mathrm{eff}} = 1/2$ Mott state of In$_2$Ir$_2$O$_7$ in the limit of reduced inter-site hopping

The pyrochlore iridate In$_2$Ir$_2$O$_7$ is a strong $J_{\mathrm{eff}} = 1/2$ Mott insulator with frustrated magnetism. Despite the large trigonal crystal field, a small admixture of $J_{\mathrm{eff}} = 3/2$ component in the $J_{\mathrm{eff}} = 1/2$ bands and a small splitting of $J_{\mathrm{eff}} = 3/2$ bands are observed as compared with other pyrochlore iridates A$_2$Ir$_2$O$_7$ (A: trivalent cation). We argue that the reduced inter-site hopping between the $J_{\mathrm{eff}} = 1/2$ and the $J_{\mathrm{eff}} = 3/2$ manifold plays a predominant role in the distinct behavior of In$_2$Ir$_2$O$_7$ compared with other A$_2$Ir$_2$O$_7$. The effect of the intersite hopping should not be dismissed in the local physics of spin-orbital-entangled $J_{\mathrm{eff}} = 1/2$ Mott insulators.

cond-mat.str-el↗

arXiv2018

Infrared phonon spectra of quasi-one-dimensional Ta$_2$NiSe$_5$ and Ta$_2$NiS$_5$

Using a combination of infrared ellipsometry, time-domain terahertz spectroscopy, and far-infrared reflectometry we have obtained the $ac$-plane complex dielectric function of monoclinic ($C2/c$) Ta$_2$NiSe$_5$ and orthorhombic ($Cmcm$) Ta$_2$NiS$_5$ single crystals. The identified dipole-active phonon modes polarized along $a$ and $c$ axes are in good agreement with density functional theory calculations. With increasing temperature the $a$-axis phonon modes of Ta$_2$NiSe$_5$ become poorly discernible, as they are superimposed on the electronic background which gradually fills the energy gap near the monoclinic-to-orthorhombic phase transition temperature $T_c$ = 326 K. In Ta$_2$NiS$_5$, which does not exhibit such a structural transition and remains orthorhombic down to low temperatures, the $a$-axis phonon modes are superimposed on a persistent broad electronic mode centered near 16 meV. We attribute this difference to strongly overlapping exciton-phonon complexes in Ta$_2$NiSe$_5$, as opposed to isolated instances of the same in Ta$_2$NiS$_5$, and find this to be in good agreement with an excitonic insulator state below $T_c$ in the former, as compared to the absence of one in the latter.

cond-mat.str-el↗

arXiv2018

Microscopic investigation of the weakly correlated noncentrosymmetric superconductor SrAuSi$_3$

SrAuSi$_3$ is a noncentrosymmetric superconductor (NCS) with $T_c$ = 1.54 K, which to date has been studied only via macroscopic techniques. By combining nuclear magnetic resonance (NMR) and muon-spin rotation ($\mu$SR) measurements we investigate both the normal and the superconducting phase of SrAuSi$_3$ at a local level. In the normal phase, our data indicate a standard metallic behavior with weak electron correlations and a Korringa constant $S_\mathrm{exp} = 1.31 \times 10^{-5}$ sK. The latter, twice the theoretical value, can be justified by the Moriya theory of exchange enhancement. In the superconducting phase, the material exhibits conventional BCS-type superconductivity with a weak-coupling s-wave pairing, a gap value $\Delta(0)$ = 0.213(2) meV, and a magnetic penetration depth $\lambda(0)$ = 398(2) nm. The experimental proof of weak correlations in SrAuSi$_{3}$ implies that correlation effects can be decoupled from those of antisymmetric spin-orbit coupling (ASOC), thus enabling accurate band-structure calculations in the weakly-correlated NCSs.

cond-mat.supr-con↗

arXiv2016

Intrinsic Proton NMR Studies of Mg(OH)$_2$ and Ca(OH)$_2$

We studied the short proton free induction decay signals and the broad ^1H NMR spectra of Mg(OH)2 and Ca(OH)2 powders at 77-355 K and 42 MHz using pulsed NMR techniques. Using a Gaussian-type back extrapolation procedure for the obscured data of the proton free induction decay signals, we obtained more precise values of the second moments of the Fourier-transformed broad NMR spectra than those in a previous report [Y. Itoh and M. Isobe, J. Phys. Soc. Jpn. Vol. 84, 113601 (2015)] and compared with the theoretical second moments. The decrease in the second moment could not account for the large decrease in the magnitude of the intrinsic proton spin-lattice relaxation rate 1/T_1 from Mg(OH)2 to Ca(OH)2. The analysis of 1/T_1 $propto$ exp(-E_g/k_BT) with E_g~0.01 eV points to a local hopping mechanism, and that of 1/T_1 $propto$ T^n with n~0.5 points to an anharmonic rattling mechanism.

cond-mat.mtrl-sci↗

arXiv2016

Extrinsic Proton NMR Studies of Mg(OH)$_2$ and Ca(OH)$_2$

We studied narrow $^1$H NMR spectra of Mg(OH)$_2$ and Ca(OH)$_2$ powders at 100$-$355 K and 42$-$59 MHz using pulsed NMR techniques. The Fourier transformed NMR spectra of the proton free-induction signals show the superposition of broad and narrow components, which can be assigned to immobile protons and extrinsic mobile protons, respectively. We found that a narrow spectrum develops on heating above about $T_c$ = 260 K and widens above a Larmor frequency of about $f_c$ = 50 MHz for Mg(OH)$_2$. The temperature-induced NMR spectrum and the characteristic frequency $f_c$ of 50 MHz are the noteworthy features of the nuclear spin fluctuation spectra of the extrinsic protons.

cond-mat.mtrl-sci↗