arXiv subjects

Taka-hisa Arima

Publications and source records attributed to Taka-hisa Arima.

At least 19 recordsLinked to original sources

arXiv2026

Polarized neutron diffraction with ex-situ $^3$He neutron spin filter and two-dimensional detector for noncollinear incommensurate magnetic order

Polarized neutron scattering has been widely used for studying magnetic orders in condensed matter. A typical setup for this technique is a triple-axis spectrometer with a ferromagnetic single-crystal monochromator and analyzer, which is suited for point-by-point measurements within the horizontal scattering plane. However, this setup cannot fully meet the demands of recent studies on complex magnetic orders with emergent cross-correlated phenomena. For instance, multiferroics, magnetic skyrmions, and other topologically nontrivial magnetic orders tend to have incommensurate magnetic modulation vectors running along various directions in reciprocal space, which cannot be captured by measurements restricted to the horizontal scattering plane. To overcome these limitations, we have developed an experimental setup combining a $^3$He neutron spin filter ($^3$He-NSF) and a two-dimensional (2D) detector, which enables us to analyze the polarization of neutrons scattered away from the horizontal plane. We also establish a data reduction procedure to convert the 2D intensity maps into three-dimensional intensity distributions in reciprocal space, correcting for the effect of imperfect $^3$He polarization. This method is applied to single-crystal diffraction measurements on the multiferroic material Mn$_3$WO$_6$, which exhibits complex incommensurate magnetic orders. We have successfully observed polarization-dependent intensities of out-of-plane incommensurate magnetic reflections, demonstrating the effectiveness of the present method for analyzing complex magnetic structures.

cond-mat.str-el↗

arXiv2026

Molecular-Orbital Degeneracy Lifting and Suppression of a Flat-Band Metal in a Tetrahedral Cluster System NbSeI

The lifting of degenerate electronic states has been extensively studied in transition metal compounds, where diverse quantum phenomena arise from the degrees of freedom of d electrons on individual atoms. In contrast, transition metal compounds containing high-symmetry clusters composed of multiple transition-metal atoms are expected to host a broader range of emergent phenomena due to the entanglement of the electronic degrees of freedom across multiple atoms. Here, we report the discovery of two distinct structural responses associated with molecular-orbital-degeneracy lifting in NbSeI, which comprises Nb4 tetrahedral clusters with molecular orbital degrees of freedom and whose cubic average crystal structure is predicted to host a flat-band metallic state. Below 106 K, NbSeI is a molecular-orbital-ordered nonmagnetic insulator with orthorhombic symmetry. Above this temperature, the average structure becomes face-centered cubic without superlattice formation, while local symmetry breaking associated with pronounced local distortions of the Nb4 tetrahedra lifts the molecular-orbital degeneracy. This local symmetry breaking occurs without cooperative long-range order and stabilizes a nonmagnetic insulating state instead of the flat-band metallic state predicted for the cubic average structure.

cond-mat.str-el↗

arXiv2026

Real-space determination of orbital states driving successive phase transitions in FeV2O4

Direct experimental access to orbital states in strongly correlated materials remains a major challenge, despite their central role in driving coupled structural and magnetic phase transitions. In systems where electronic correlations, electron-lattice coupling, and relativistic spin-orbit interactions compete on comparable energy scales, even first-principles calculations often yield multiple metastable solutions, hindering the unambiguous identification of the ground state. Here, we demonstrate that the orbital states of the spinel oxide FeV2O4, which possesses active orbital degrees of freedom on both Fe and V ions, are uniquely resolved by combining valence electron density (VED) analysis based on state-of-the-art synchrotron x-ray diffraction with spin-polarized density-functional-theory calculations. Our results reveal that temperature-dependent rearrangements of orbital occupations drive successive structural transitions that accompany collinear and noncoplanar ferrimagnetic orders, establishing a direct correspondence between orbital anisotropy and spin structure. More broadly, this work shows that experimentally determined VED provides a decisive real-space constraint on competing theoretical solutions, offering a powerful and broadly applicable framework for elucidating the microscopic mechanisms of complex phase transitions in strongly correlated electron systems.

cond-mat.str-el↗

arXiv2026

Observation of complex orbital order in MnV2O4

Orbital ordering in vanadium spinel oxides with a geometrically frustrated pyrochlore structure has been a subject of controversy, owing to competing theoretical models and the absence of direct experimental evidence. Here we combine high-precision single-crystal synchrotron x-ray diffraction with core differential fourier synthesis to visualize the valence electron density (VED) of the orbital-ordered ground state in real space. By carefully investigating multiple-scattering artifacts, we identify the low-temperature structure as belonging to the I41/amd space group. The reconstructed VED around the V sites reveals an orbital-ordered state distinct from both previously proposed real- and complex-orbital models. Our results resolve the long-standing controversy in MnV2O4 and establish a route to identifying orbital states in frustrated spin-orbital systems.

cond-mat.str-el↗

arXiv2026

Observation of g-wave altermagnetic multipole

Over the past few years, altermagnets have emerged as a new class of collinear magnets with broken time-reversal symmetry, offering novel opportunities for spintronics beyond conventional magnets. Rather than from net magnetization, as in ferromagnets, the unconventional time-reversal symmetry breaking of altermagnets originates from antiferroic magnetic dipoles locked to higher-order multipoles. Here we report the direct visualization of a $g$-wave altermagnetic multipole in the canonical altermagnet CrSb. Combining high-energy synchrotron X-ray diffraction with valence electron density (VED) analysis, we uncover a pronounced directional anisotropy of the VED distribution alternating between Cr sublattices. This evidences the antiferroic order of electric hexadecapoles predicted in $g$-wave altermagnets. Its coexistence with antiferroic magnetic dipoles induces ferroic magnetic multipoles, as probed by polarized neutron diffraction. We further identify a microscopic model of altermagnetism that directly relates the $g$-wave multipole and the $g$-wave spin splitting. Through direct observation and quantification of multipoles, this study provides a real-space fingerprint of altermagnetism and establishes a general probe of hidden multipole order in quantum materials.

cond-mat.str-el↗

arXiv2026

Automatic Termination Strategy of Inelastic Neutron-scattering Measurement Using Bayesian Optimization for Bin-width Selection

Currently, an excessive amount of event data is being obtained in four-dimensional inelastic neutron-scattering experiments. A method for automatic bin-width optimization of multidimensional histograms has been developed and recently validated on real inelastic neutron-scattering data. However, measuring beyond the equipment resolution leads to inefficient use of valuable beam time. To improve experimental efficiency, an automatic termination strategy is essential. We propose a Bayesian-optimization-based method to compute a stopping criterion that can support online decisions on whether to continue or terminate an experiment. In the proposed method, the bin-width optimization is performed using Bayesian optimization to efficiently compute the optimal bin widths. The experiment is terminated when the optimal bin widths become smaller than the target resolutions. In numerical experiments using real inelastic neutron-scattering data, the optimal bin widths decrease as the number of events increases. Even the optimal bin widths for data downsampled to 1/5 are comparable with the resolutions limited by the sample size, choppers, and so on. This implies excessive measurement of the inelastic neutron experiments for the moment. Moreover, we found that Bayesian optimization can reduce the search cost to approximately 10% of an exhaustive search in our numerical experiments.

physics.data-an↗

arXiv2026

Single-crystal structural phase diagram of stoichiometric bilayer nickelate La3Ni2O7 under hydrostatic pressure

The bilayer nickelate La3Ni2O7 has attracted intense interest following the discovery of high-temperature superconductivity under pressure, representing the first nickelate superconductor realized in bulk form. However, the crystal structure of the superconducting phase remains under active discussion, complicating efforts to establish its microscopic origin. Here we resolve these structural controversies by establishing a definitive pressure-temperature phase diagram, including the superconducting region of stoichiometric La3Ni2O7 single crystals under hydrostatic conditions using helium as the pressure-transmitting medium. At ambient pressure, La3Ni2O7 adopts a polar orthorhombic Am2m structure characterized by charge order between inequivalent Ni sites and NiO6 octahedral tilting. Upon compression, the system undergoes a direct transition from the charge-ordered Am2m phase to the tetragonal I4/mmm phase near 10 GPa, coinciding with the onset of bulk superconductivity. These results establish the intrinsic structural evolution of La3Ni2O7 and provide a structural framework for microscopic theories of nickelate superconductivity.

cond-mat.supr-con↗

arXiv2026

Density-wave phases, anisotropic transport, and Planckian dissipation in single crystals of the superconductor La3Ni2O7

Pressure-induced superconductivity in bilayer nickelates provides a platform for investigating intertwined roles of charge/spin orders and electric transport in unconventional superconductivity. However, important quantitative information on the transport, such as the absolute value of the resistivity, the anisotropy, and the scattering rate of carriers, remains insufficient due to the lack of accurate measurements using large single crystals. Here we establish a high-precision pressure-temperature phase diagram of high-quality La3Ni2O7 single crystals, by measuring the in-plane and out-of-plane resistivities. We resolve two distinct anomalies associated with density-wave formation with contrasting pressure dependences. The pressure-induced structural transition enhances not only the resistivity values for both directions, but also its anisotropy at low temperatures, demonstrating a pronounced effect of density-wave order on the charge dynamics. Superconductivity with zero-resistance emerges near the boundary where the density-wave phases are fully suppressed, and above Tc, the resistivity exhibits a temperature-linear dependence over a wide temperature range while the scattering rate falls within a regime of the Planckian limit. Our results show that pressure dramatically changes the anisotropic charge transport via modifying density-wave orders, and eventually produces a pronounced strange-metal state with strong scatterings, from which superconductivity develops. This establishes robust density-wave correlations and Planckian dissipation as remarkable features of La3Ni2O7.

cond-mat.supr-con↗

arXiv2026

Visualization of Co 3d high- and low-spin states via valence electron density

Properties of trivalent cobalt oxides are governed by the spin and orbital states of Co3+ ions, which are strongly coupled to their local coordination environments and chemical bonding. However, direct real-space access to the electronic states has remained challenging. Here, we determine the Co 3d states in the quasi-one-dimensional cobalt oxide Ca3Co2O6 by combining synchrotron X-ray diffraction with valence electron density (VED) analysis based on core differential Fourier synthesis. The reconstructed VED reveals distinct anisotropic distributions at two crystallographically inequivalent Co sites with octahedral and trigonal-prismatic coordination geometries. The octahedral site exhibits a characteristic VED consistent with a low-spin configuration, whereas the trigonal-prismatic site shows pronounced anisotropy that cannot be described solely by crystal electric field (CEF) effects. Quantitative analysis demonstrates that this anisotropy originates from the interplay of CEF effects, spin-orbit coupling, and ligand-assisted 3d-4p hybridization, reflecting partially unquenched orbital angular momentum and its role in the Ising magnetism. These results establish a general framework for understanding site-dependent electronic structure and chemical bonding in transition-metal oxides through real-space VED analysis.

cond-mat.str-el↗

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↗

arXiv2026

Collinear ferromagnetism with reduced moment length in kagome magnet Nd3Ru4Al12

We determine the magnetic ground state of the kagome lattice magnet Nd3Ru4Al12 by single-crystal neutron diffraction, supported by experiments with polarized neutrons. We identify this material as a collinear ferromagnet ("hex-FM") with uniform moment length mc = 2.1 μB/Nd and ordering vector Q = 0, in contrast to a previous, seminal report that proposed unequal moment lengths on two Nd sites, here called the "ortho-FM" state. Our analysis of the flipping ratio in polarized neutron scattering is consistent with the hex-FM state. The results provide a microscopic basis for understanding the large fluctuation-induced Hall and Nernst responses near TC = 41 K, as previously reported for Nd3Ru4Al12.

cond-mat.str-el↗

arXiv2026

Frustration of harmonic and solitonic helimagnetism on the body-centered tetragonal lattice of GdAlSi

The triangular lattice antiferromagnet (TLAF) with nearest-neighbor exchange interaction is a model platform in the field of frustrated magnetism. Here, anharmonic (`up-up-down') and harmonic (`120 degree') magnetic states compete, because the fundamental helimagnetic wave and its higher harmonic are degenerate in energy. We show that a body-centered tetragonal lattice (BCTL) can realize a similar frustration of harmonic and anharmonic helimagnetic states, and that the tetragonal magnetic Weyl semimetal GdAlSi realizes this scenario. In an applied magnetic field, resonant elastic X-ray scattering reveals a competition of harmonic cycloidal and solitonic double-Q states, well consistent with mean-field calculations. Our work provides a new paradigm for frustration physics in BCTL materials.

cond-mat.str-el↗

arXiv2026

Low energy excitations in A-site ordered SmBaMn2O6

The electron in a solid can be considered a bound state of the three independent, fundamental degrees of freedom creating quasi-particles: spinons, carrying the electron spin; plasmons carrying the collective charge mode and orbitons carrying its orbital degree of freedom. These fundamental degrees of freedom could form ordering states in which dynamics or collective motions could occurr and manifest as low-energy excitations. The exotic properties that appear in the materials exhibiting these electronic orderings are associated with these low-energy excitations. Although the orbital order (OO) and its coupling to the spin system creates very interesting phenomena, the microscopic origin of OO has been much less explored than other electronic properties as it is very difficult to directly access experimental information from OO. Due to the recent improvement in energy resolution and flux, soft x-ray resonant inelastic scattering (RIXS) allows for a re-examination of orbital excitations in manganites. Here, we present a study of low energy excitations in half doped A-site ordered SmBaMn_{2}O_{6} through a combination of RIXS and soft x-ray resonant elastic scattering (REXS) measurements. The obtained experimental data confirm the OO at \mathbf{q} = (0.25, 0.25, 0) and find various low energy excitations below 200 meV. while several excitations can be assigned to be of magnetic and phononic origin, a group of excitations between 80 and 200 meV show a temperature dependence distinctively following that of the OO making them possible candidates for orbital excitations.

cond-mat.str-el↗

arXiv2026

Experimental quantification of electronic symmetry breaking through orbital hybridization phase

Symmetry classification of crystal structures has been central to predicting physical properties of materials. While such structural classification identifies which physical responses are symmetry-allowed, the magnitudes of these responses are governed by the degree of symmetry breaking in the electronic state. However, a well-defined quantitative descriptor for the electronic symmetry breaking has been established only in limited cases such as electric polarization and magnetization. No analogous descriptor exists for most other types, including chirality. Here, we propose an experimental framework for quantifying electronic symmetry breaking from the anisotropy of valence electron density distribution. We show that the orbital hybridization phases governing this anisotropy can be uniquely determined under site symmetry constraints. Applying this framework to structurally chiral transition-metal silicides, we determine hybridization phases from their valence electron densities observed by synchrotron X-ray diffraction. From the obtained complex hybridization, we quantify an electronic chirality $χ$ and theoretically demonstrate that it is directly proportional to circular dichroism, establishing $χ$ as a predictive descriptor of chiral responses. This approach is systematically applicable to various point groups, offering a general route to quantifying electronic symmetry breaking and predicting associated physical properties.

cond-mat.str-el↗

arXiv2026

Bond-density-wave orders induced by geometric frustration in the kagome metal CeRu3Si2

Geometric frustration gives rise to vast manifolds of degenerate ground states and competing orders in spin and charge systems. Typically, classical ground states are governed by a local ``zero-sum constraint" that relieves frustrated antiferromagnetic interactions or Coulomb repulsion. To date, the paradigm of geometric frustration has yielded a rich landscape of emergent phases, from spin ices and quantum spin liquids to charge glasses. However, an analogous phase rooted in chemical bonding has yet to be firmly demonstrated. Here we report the discovery of bond-density-wave orders induced by geometric frustration in the kagome metal CeRu$_3$Si$_2$ above room temperature. Through synchrotron X-ray diffraction, real-space transmission electron microscopy, and model calculations, we observe two distinct long-period superlattices with harmonic and anharmonic structural modulations. Crucially, interlayer bonds between kagome planes modulate in a sublattice-selective manner to fulfill the zero-sum constraint on the kagome lattice. We demonstrate the potential of kagome metals to host complex bond-ordered states constrained by geometric frustration and establish chemical bonding as a distinct pathway to frustration physics in quantum materials even above room temperature.

cond-mat.str-el↗

arXiv2026

Magnetoelectric Control of Toroidal Moment in Ferroaxial Crystal PbMn$_{2}$Ni$_{6}$Te$_{3}$O$_{18}$

Ferroic multipole orders break some symmetry and often activate unique physical properties, such as nonreciprocal directional dichroism and linear magnetoelectric effects. Here, we demonstrate the control of magnetic toroidal orientation in PbMn$_{2}$Ni$_{6}$Te$_{3}$O$_{18}$ through the application of electric and magnetic fields in two distinct configurations. Through directional dichroism, we successfully visualize magnetic ferrotoroidic domains, establishing the intrinsic coupling among magnetic toroidal moment, crystallographic ferroaxial moment, and magnetoelectric monopoles. Our findings not only present an effective pathway for controlling magnetic toroidal moment but also provide a novel approach for investigating ferroaxial ordering.

cond-mat.str-el↗

arXiv2026

Polar, checkerboard charge order in bilayer nickelate La3Ni2O7

Competing charge and spin orders are central to uncovering the nature of unconventional superconductivity. Here we utilize synchrotron X-ray diffraction on a high-quality single crystal to reveal the charge order of La$_3$Ni$_2$O$_7$ at ambient pressure, which competes with the high-temperature superconducting phase under pressure. Enabled by the high synchrotron photon flux and a large dynamic range, we resolve faint reflections -- nearly four orders of magnitude weaker than the main Bragg reflections -- that were overlooked in prior diffraction studies. This observation evidences a broken glide-mirror symmetry, leading to a polar crystal structure, rather than the widely used centrosymmetric structure model. The polarity is induced by checkerboard charge order on nickel sites in combination with octahedral tilting, reminiscent of bilayer manganese oxides. Our results provide a foundation for understanding phase competition and the mechanism of pressure-induced superconductivity in bilayer nickelates.

cond-mat.supr-con↗

arXiv2026

Stripe antiferromagnetism in van der Waals metal HoTe3 decoupled from charge density wave order

The $R\mathrm{Te}_3$ ($R = \text{rare earth}$) family of layered van der Waals (vdW) compounds hosts coexisting magnetic and charge density wave (CDW) orders, yet the interplay between these degrees of freedom remains little explored. Combining polarized and unpolarized neutron diffraction on single-crystal $\mathrm{HoTe}_3$, we identify two distinct antiferromagnetic (AFM) phases, both exhibiting a collinear $\uparrow\uparrow\downarrow\downarrow$ motif within individual vdW layers. The two phases are distinguished by the vdW stacking of magnetic layers: ferromagnetic (FM) stacking in the higher-temperature AFM-II phase, here termed ``vertical-stripe'', and AFM stacking in the AFM-I ground state, here termed ``tilted-stripe''; the two phases have propagation vectors $\boldsymbol{q}_{\mathrm{m2}} = (0.48, 0, 0)$ and $\boldsymbol{q}_{\mathrm{m1}} = (0.5, 0.5, 0)$, respectively. In contrast to the CDW-driven exotic magnetism in $\mathrm{DyTe}_3$, $\mathrm{TbTe}_3$, and $\mathrm{GdTe}_3$, we find no evidence for coupling between magnetism and CDW in $\mathrm{HoTe}_3$. The relative alignment between AFM and CDW propagation vectors, as well as single-ion anisotropy, are likely essential for generating coupled spin/charge orders in layered vdW systems.

cond-mat.str-el↗