arXiv subjects

Shintaro Ishiwata

Publications and source records attributed to Shintaro Ishiwata.

At least 19 recordsLinked to original sources

arXiv2026

Systematic global structure search of bismuth-based binary systems under pressure using machine learning potentials

Machine learning potentials (MLPs) have significantly advanced global crystal structure prediction by enabling efficient and accurate property evaluations. In this study, global structure searches are performed for 11 bismuth-based binary systems, including Na-Bi, Ca-Bi, and Eu-Bi, under pressures ranging from 0 to 20 GPa, employing polynomial MLPs developed specifically for these systems. The searches reveal numerous compounds not previously reported in the literature and identify all experimentally known compounds that are representable within the explored configurational space. These results highlight the robustness and reliability of the current MLP-based structure search. The study provides valuable insights into the discovery and design of novel bismuth-based materials under both ambient and high-pressure conditions.

cond-mat.mtrl-sci↗

arXiv2026

Magnetoelastic mapping of the high-field phase diagram in the topological cubic helimagnet SrFeO$_{3}$

The cubic perovskite SrFeO$_{3}$ is a prototypical centrosymmetric itinerant magnet that hosts a quadruple-${\mathbf Q}$ hedgehog-antihedgehog lattice and exhibits a complex magnetic-field-temperature phase diagram. Yet, the microscopic mechanism underlying the emergence of its versatile multiple-${\mathbf Q}$ phases remains unresolved. Here, we reveal the field-orientation dependence of the magnetic phase diagram and establish an effective spin Hamiltonian for SrFeO$_{3}$ that incorporates a cubic single-ion anisotropy together with bilinear and biquadratic interactions in momentum space, which originate from the spin-charge coupling. In addition, we observe magnetoelastic signatures of a redistribution of the ligand-hole density upon entering the forced ferromagnetic phase. These findings emphasize the pivotal importance of electronic itinerancy arising from the formation of a ligand-hole band in stabilizing multiple-${\mathbf Q}$ phases.

cond-mat.str-el↗

arXiv2025

Enhanced thermopower in a magnetic semiconductor EuTe4 with multiple charge-density-wave instabilities/

We investigate the layered magnetic semiconductor EuTe4, focusing on its intricate charge-density wave (CDW) states near and above room temperature through single-crystal X-ray diffraction (XRD), magnetic, and thermoelectric measurements.The XRD measurement revealed that the CDW state inducing the polar lattice distortion persists even at 650 K, demonstrating its remarkable thermal stability. Notably, the Seebeck coefficient near room temperature reaches values exceeding 500 uVK-1. This large Seebeck coefficient, not fully captured by a simple band calculation, is comparable to those observed in heavy-electron semiconducting oxides, suggesting the importance of electron correlation and spin/lattice instabilities. Furthermore, potentially reflecting the competition of two types of CDW states, the thermal conductivity near room temperature is as low as 0.02 Wcm-1K-1. As a result, the thermoelectric figure of merit zT reaches 0.22 at 460 K. These findings establish EuTe4 as a compelling platform to explore novel types of thermoelectric materials with multiple electronic instability.

cond-mat.mtrl-sci↗

arXiv2025

A rutile-based homologous series Na(PtO$_2$)$_{2\it{n}+1}$ discovered by computationally assisted high-pressure synthesis

Layered transition metal oxides typified by the Ruddlesden-Popper phase have been extensively studied for its applications in high-temperature superconductivity, catalysis, and battery technologies. Despite the remarkable structural diversity and catalytic functionality of platinum oxides, the exploration of layered polymorphs has remained significantly constrained mainly due to the high inertness of platinum. Here, we discover a new homologous series of layered ternary oxides, Na(PtO$_2$)$_{2\it{n}+1}$, by a combination of highly oxidizing high-pressure methods and density functional theory (DFT) calculations. This series features unprecedented layered structural motifs, rutile-based PtO$_6$ octahedra and one-dimensional PtO$_4$ square-planar columns, which enables systematic control of dimensionality. Furthermore, we demonstrate a computationally-assisted identification of isomeric and putative members of this homologous series as confirmed by controlled synthesis and quantitative analysis of diffuse scattering data. This approach provides an effective platform for the exhaustive exploration of metastable transition metal oxides with rich structural variations.

cond-mat.mtrl-sci↗

arXiv2025

Exploration of metastable A-site-ordered perovskites (Ca,Ba)FeO3-δ by computationally-guided multi-step synthesis

Perovskite-type iron oxides with Fe4+ ions have attracted much attention for their versatile helimagnetic phases. While the introduction of a layered A-site ordered structure to AFeO3 with Fe4+ ions potentially lead to novel helimagnetic phases, the synthetic pathway spanning high pressure range is apparently difficult to elucidate. Here, we explored new A-site ordered perovskite-type iron oxides (Ca,Ba)FeO3-δ with Fe4+ ions with the support of first-principles calculations evaluating thermodynamic stability at selected pressures and chemical compositions. Among the six types of putative A-site ordered perovskites with and without oxygen vacancy, only two types of oxygen-deficient perovskites CaBaFe2O6-δ and Ca(Ba0.9Ca0.1)2Fe3O9-δ (δ~1) were successfully obtained by high-pressure synthesis, being consistent with the DFT-based convex-hull calculations. Considering the evaluated stability of the putative perovskites at selected pressures, we adopted low-temperature topotactic oxidation using ozone at ambient pressure and obtained the oxidized perovskites CaBaFe2O6-δ (δ~0.4) and Ca(Ba0.9Ca0.1)2Fe3O9-δ (δ~0.6), potentially showing novel helimagnetic phases. This study demonstrates that computational visualization of multi-step synthetic pathways involving high pressure can accelerate the search for new metastable perovskites with rich magnetic phases.

cond-mat.mtrl-sci↗

arXiv2024

Observation of converse flexoelectric effect in topological semimetals

A strong coupling between electric polarization and elastic deformation in solids is an important factor in creating useful electromechanical nanodevices. Such coupling is typically allowed in insulating materials with inversion symmetry breaking as exemplified by the piezoelectric effect in ferroelectric materials. Therefore, materials with metallicity and centrosymmetry have tended to be out of scope in this perspective. Here, we report the observation of giant elastic deformation by the application of an alternating electric current in topological semimetals (V,Mo)Te2, regardless of the centrosymmetry. Considering the crystal and band structures and the asymmetric measurement configurations in addition to the absence of the electromechanical effect in a trivial semimetal TiTe2, the observed effect is discussed in terms of a Berry-phase-derived converse flexoelectric effect in metals. The observation of the flexoelectric effect in topological semimetals paves a way for a new type of nanoscale electromechanical sensors and energy harvesting.

cond-mat.mtrl-sci↗

arXiv2024

Multiband Metallic Ground State in Multilayered Nickelates La$_3$Ni$_2$O$_7$ and La$_4$Ni$_3$O$_{10}$ Probed by $^{139}$La-NMR at Ambient Pressure

We report a $^{139}$La-NMR study of polycrystalline samples of multi($n$)-layered nickelates, La$_3$Ni$_2$O$_{7-δ}$ ($n=2$) and La$_4$Ni$_3$O$_{10-δ}$ ($n=3$), at ambient pressure. Measurements of the nuclear magnetic resonance (NMR) spectra and nuclear spin relaxation rate ($1/T_1$) indicate the emergence of a density wave order with a gap below $T^*\sim150$ K for La$_3$Ni$_2$O$_{7-δ}$ and $\sim130$ K for La$_4$Ni$_3$O$_{10-δ}$. The finite value of $1/T_1$ below $T^*$ indicates metallic ground states with the remaining density of states at the Fermi level ($E_{\rm F}$) under the density wave order. These features are attributed to multiple $d$ electron bands with different characteristics. Above $T^*$, the gradual decrease in $1/T_1T$ upon cooling implies the presence of a band with flat dispersion near $E_{\rm F}$. From our microscopic probes, we point out that these nickelates ($n=2$ and $3$) possess similar electronic states despite the difference in the formal valence of the Ni-$d$ electron states, which provides a basis for understanding the novel high-$T_{\rm c}$ superconductivity under high pressures.

cond-mat.str-el↗

arXiv2024

Band-asymmetry-driven nonreciprocal electronic transport in a helimagnetic semimetal α-EuP$_3$

Chiral magnetic textures give rise to unconventional magnetotransport phenomena such as the topological Hall effect and nonreciprocal electronic transport. While the correspondence between real-space magnetic topology/symmetry and such transport phenomena has been well established, a microscopic understanding based on the spin-dependent band structure in momentum space remains elusive. Here we demonstrate how a chiral magnetic structure in real space introduces an asymmetry in the electronic band structure and triggers a nonreciprocal electronic transport in a centrosymmetric helimagnet α-EuP$_3$. The magnetic structure of α-EuP$_3$ is highly tunable by a magnetic field and closely coupled to its semi-metallic electronic band structure, enabling a systematic study across chiral and achiral magnetic phases on the correspondence between nonreciprocal transport and electronic band asymmetry. Our findings reveal how a microscopic change in the magnetic configuration of charge carriers can lead to nonreciprocal electronic transport, paving the way for designing chiral magnets with desirable properties.

cond-mat.mtrl-sci↗

arXiv2024

Unveiling the orbital-selective electronic band reconstruction through the structural phase transition in TaTe$_2$

Tantalum ditelluride TaTe$_2$ belongs to the family of layered transition metal dichalcogenides but exhibits a unique structural phase transition at around 170 K that accompanies the rearrangement of the Ta atomic network from a "ribbon chain" to a "butterfly-like" pattern. While multiple mechanisms including Fermi surface nesting and chemical bonding instabilities have been intensively discussed, the origin of this transition remains elusive. Here we investigate the electronic structure of single-crystalline TaTe$_2$ with a particular focus on its modifications through the phase transition, by employing core-level and angle-resolved photoemission spectroscopy combined with first-principles calculations. Temperature-dependent core-level spectroscopy demonstrates a splitting of the Ta $4f$ core-level spectra through the phase transition indicative of the Ta-dominated electronic state reconstruction. Low-energy electronic state measurements further reveal an unusual kink-like band reconstruction occurring at the Brillouin zone boundary, which cannot be explained by Fermi surface nesting or band folding effects. On the basis of the orbital-projected band calculations, this band reconstruction is mainly attributed to the modifications of specific Ta $5d$ states, namely the $d_{XY}$ orbitals (the ones elongating along the ribbon chains) at the center Ta sites of the ribbon chains. The present results highlight the strong orbital-dependent electronic state reconstruction through the phase transition in this system and provide fundamental insights towards understanding complex electron-lattice-bond coupled phenomena.

cond-mat.str-el↗

arXiv2023

Superconductivity in a ferroelectric-like topological semimetal SrAuBi

Given the rarity of metallic systems that exhibit ferroelectric-like transitions, it is apparently challenging to find a system that simultaneously possesses superconductivity and ferroelectric-like structural instability. Here, we report the observation of superconductivity at 2.4 K in a layered semimetal SrAuBi characterized by strong spin-orbit coupling (SOC) and ferroelectric-like lattice distortion. Single crystals of SrAuBi have been successfully synthesized and found to show a polar-nonpolar structure transition at 214 K, which is associated with the buckling of Au-Bi honeycomb lattice. On the basis of the band calculations considering SOC, we found significant Rashba-type spin splitting and symmetry-protected multiple Dirac points near the Fermi level. We believe that this discovery opens up new possibilities of pursuing exotic superconducting states associated with the semimetallic band structure without space inversion symmetry and the topological surface state with the strong SOC.

cond-mat.supr-con↗

arXiv2023

Real-Space Observation of Ligand Hole State in Cubic Perovskite SrFeO$_3$

An anomalously high valence state sometimes shows up in transition-metal oxide compounds. In such systems, holes tend to occupy mainly the ligand $p$ orbitals, giving rise to interesting physical properties such as superconductivity in cuprates and rich magnetic phases in ferrates. However, no one has ever observed the distribution of ligand holes in real space. Here, we report a successful observation of the spatial distribution of valence electrons in cubic perovskite SrFeO$_3$ by high-energy X-ray diffraction experiments and precise electron density analysis using a core differential Fourier synthesis method. A real-space picture of ligand holes formed by the orbital hybridization of Fe 3$d$ and O 2$p$ is revealed. The anomalous valence state in Fe is attributed to the considerable contribution of the ligand hole, which is related to the metallic nature and the absence of Jahn-Teller distortions in this system.

cond-mat.str-el↗

arXiv2023

Ultrafast Control of Crystal Structure in a Topological Charge-Density-Wave Material

Optical control of crystal structures is a promising route to change physical properties including topological nature of a targeting material. Time-resolved X-ray diffraction measurements using the X-ray free-electron laser are performed to study the ultrafast lattice dynamics of VTe$_2$, which shows a unique charge-density-wave (CDW) ordering coupled to the topological surface states as a first-order phase transition. A significant oscillation of the CDW amplitude mode is observed at a superlattice reflection as well as Bragg reflections. The frequency of the oscillation is independent of the fluence of the pumping laser, which is prominent to the CDW ordering of the first-order phase transition. Furthermore, the timescale of the photoinduced 1$T^{\prime\prime}$ to 1$T$ phase transition is independent of the period of the CDW amplitude mode.

cond-mat.str-el↗

arXiv2022

Superconductivity in a Magnetic Rashba Semimetal EuAuBi

We report the observation of superconductivity with multiple magnetic ordering and Rashba-type spin-orbit coupling in a layered polar semimetal EuAuBi. Magnetic transition is observed at 4 K, followed by a superconducting transition at 2.2 K, which is sensitive to the crystal surface conditions. The upper critical field Hc2 of 9.8 T for the out-of-plane field is three times higher than that for the in-plane field, which can be associated with the two-dimensional structure or the surface state. On the basis of first-principles calculations, it is found that the characteristic Hc2 possibly reflects the anisotropic modification of the Fermi surface by the effective combination of Rashba-type spin splitting and Zeeman spin splitting enhanced by Eu moments.

cond-mat.supr-con↗

arXiv2022

Possible helimagnetic order in Co4+-containing perovskites Sr1-xCaxCoO3

We systematically synthesized perovskite-type oxides Sr1-xCaxCoO3 containing unusually high valence Co4+ ions by a high pressure technique, and investigated the effect of systematic lattice change on the magnetic and electronic properties. As the Ca content x exceeds about 0.6, the structure changes from cubic to orthorhombic, which is supported by the first-principles calculations of enthalpy. Upon the orthorhombic distortion, the ground state remains to be apparently ferromagnetic with a slight drop of the Curie temperature. Importantly, the compounds with x larger than 0.8 show antiferromagnetic behavior with positive Weiss temperatures and nonlinear magnetization curves at lowest temperature, implying that the ground state is noncollinear antiferromagnetic or helimagnetic. Considering the incoherent metallic behavior and the suppression of the electronic specific heat at high x region, the possible emergence of a helimagnetic state in Sr1-xCaxCoO3 is discussed in terms of the band-width narrowing and the double-exchange mechanism with the negative charge transfer energy as well as the spin frustration owing to the next-nearest neighbor interaction.

cond-mat.mtrl-sci↗

arXiv2022

Spin-charge coupling and decoupling in perovskite-type iron oxides (Sr$_{1-x}$Ba$_x$)$_{2/3}$La$_{1/3}$FeO$_3$

The perovskite-type iron oxide Sr$_{2/3}$La$_{1/3}$FeO$_3$ is known to show characteristic spin-charge ordering (SCO), where sixfold collinear spin ordering and threefold charge ordering are coupled with each other. Here, we report the discovery of a spin-charge decoupling and an antiferromagnetic (AFM) state competing with the SCO phase in perovskites (Sr$_{1-x}$Ba$_x$)$_{2/3}$La$_{1/3}$FeO$_3$. By comprehensive measurements including neutron diffraction, M$ö$ssbauer spectroscopy, and x-ray absorption spectroscopy, we found that the isovalent Ba$^{2+}$ substitution systematically reduces the critical temperature of the SCO phase and additionally yields the spin-charge decoupling in $x$ > 0.75. Whereas the ground state remains in the SCO phase in the whole $x$ region, an unexpected G-type AFM phase with incoherent charge ordering or charge fluctuation appears as the high-temperature phase in the range of $x$ > 0.75. Reflecting the competing nature between them, the G-type AFM phase partially exists as a metastable state in the SCO phase at low temperatures. We discuss the origin of the spin-charge decoupling and the emergence of the G-type AFM phase with charge fluctuation in terms of the bandwidth reduction by the Ba substitution.

cond-mat.str-el↗

arXiv2022

Spin-orbit-derived giant magnetoresistance in a layered magnetic semiconductor AgCrSe2

Two-dimensional magnetic materials have recently attracted great interest due to their unique functions as the electric field control of a magnetic phase and the anomalous spin Hall effect. For such remarkable functions, a spin-orbit coupling (SOC) serves as an essential ingredient. Here we report a giant positive magnetoresistance in a layered magnetic semiconductor AgCrSe2, which is a manifestation of the subtle combination of the SOC and Zeeman-type spin splitting. When the carrier concentration approaches the critical value of 2.5\times10^18 cm^-3, a sizable positive magnetoresistance of ~400 % emerges upon the application of magnetic fields normal to the conducting layers. Based on the magneto-Seebeck effect and the first-principles calculations, the unconventional magnetoresistance is ascribable to the enhancement of effective carrier mass in the SOC induced J = 3/2 state, which is tuned to the Fermi level through the Zeeman splitting enhanced by the p-d coupling. This study demonstrates a new aspect of the SOC-derived magnetotransport in two-dimensional magnetic semiconductors, paving the way to novel spintronic functions.

cond-mat.str-el↗

arXiv2022

Magnetic generation and switching of topological quantum phases in a trivial semimetal $α{\mathrm{-EuP}}_3$

Topological materials have drawn increasing attention owing to their rich quantum properties, as highlighted by a large intrinsic anomalous Hall effect (AHE) in Weyl and nodal-line semimetals. However, the practical applications for topological electronics have been hampered by the difficulty in the external control of the band topology. Here we demonstrate a magnetic-field-induced switching of band topology in $α{\mathrm{-EuP}}_3$, a magnetic semimetal with a layered crystal structure derived from black phosphorus. When the magnetic field is applied perpendicular to the single mirror plane of the monoclinic structure, a giant AHE signal abruptly emerges at a certain threshold magnetization value, giving rise to a prominently large anomalous Hall angle of $\left|Θ_{\mathrm{AHE}}\right| \sim 20^{\circ}$. When the magnetic field is applied along the inter-layer direction, which breaks the mirror symmetry, the system shows a pronounced negative longitudinal magnetoresistance. On the basis of electronic structure calculations and symmetry considerations, these anomalous magneto-transport properties can be considered as manifestations of two distinct topological phases: topological nodal-line and Weyl semimetals, respectively. Notably, the nodal-line structure is composed of bands with the same spin character and spans a wide energy range around the Fermi level. These topological phases are stabilized via the exchange coupling between localized Eu-4$f$ moments and mobile carriers conducting through the phosphorus layers. Our findings provide a realistic solution for external manipulation of band topology, enriching the functional aspects of topological materials.

cond-mat.str-el↗

arXiv2021

High-Pressure Synthesis of a Massive and Non-Symmorphic Dirac Semimetal Candidate MoP$_4$

Single crystal and polycrystalline samples of MoP$_4$ with a black-phosphorus-derived structure have been successfully synthesized by a high-pressure technique. The polycrystalline samples show a large positive magnetoresistance and a small negative Seebeck coefficient at low temperatures, reflecting a semi-metallic nature with high-mobility electrons. Consistent with the transport properties, the band structure calculation reveals a semi-metallic state with the presence of two types of Dirac nodes slightly below the Fermi level. The Dirac node along the $Γ$-X direction normal to the phosphorus layers is gapped out in the presence of spin-orbit coupling (SOC), whereas the band crossing at the Z-point is immune to SOC because of the non-symmorphic symmetry. This work demonstrates a great potential of phosphorus-based layered Zintl compounds for topological semimetal candidates allowing chemical band engineering.

cond-mat.mtrl-sci↗