arXiv subjects

Yuichi Yamasaki

Publications and source records attributed to Yuichi Yamasaki.

At least 19 recordsLinked to original sources

arXiv2026

Intrinsic single crystals of MnTe altermagnet

We report the synthesis methodology, structure, and intrinsic properties of ultra-high quality single crystals of MnTe, an archetypal altermagnet. The crystals, obtained from self-flux method, are nearly free from crystal imperfections and disproportionate chemical compositions as seen by various investigation methods. In measurements under quasi free-standing configuration minimizing stress induced effects, the crystals exhibit complex and anisotropic domain kinetics in both superheating and supercooling regimes around the altermagnetic transition at $T_{\mathrm{N}} = 310\,\mathrm{K}$. An Anderson insulating state is observed below $T_{\mathrm{MI}}\approx 150\,\mathrm{K}$ with a carrier density of about $1.6\times 10^{17}\,\mathrm{cm}^{-3}$, being sharply contrast to metallic states usually seen in Te-deficit samples. Nevertheless, hallmarks of altermagnetism, anomalous Hall effect and X-ray magnetic circular dichroism signal, are robust in this intrinsic limit, however with significantly reduced magnitudes.

cond-mat.str-el↗

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↗

arXiv2025

X-ray magnetic circular dichroism originating from the $T_{z}$ term in collinear altermagnets under trigonal crystal field

We investigate the microscopic origin and spectral features of X-ray magnetic circular dichroism (XMCD) in collinear antiferromagnets with trigonal crystal fields, using $α$-MnTe as a prototypical example. Although such systems exhibit zero net magnetization, we demonstrate that XMCD can emerge from the anisotropic magnetic dipole operator $T_{z}$, arising from quadrupolar spin distributions. By constructing a complete multipole basis and analyzing the symmetry conditions under trigonal distortion, we identify specific spin and orbital configurations that enable a finite XMCD response. Further, we employ both one-electron and multi-electron models, including spin-orbit coupling and Coulomb interactions, to calculate the XMCD spectra for various $d^n$ configurations. Our findings provide theoretical benchmarks for XMCD in altermagnets and highlight the key role of orbital symmetry and magnetic anisotropy in realizing observable dichroic effects.

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

Lattice-commensurate skyrmion texture in a centrosymmetric breathing kagome magnet

Skyrmion lattices (SkL) in centrosymmetric materials typically have a magnetic period on the nanometer-scale, so that the coupling between magnetic superstructures and the underlying crystal lattice cannot be neglected. Here, we reveal the commensurate locking of a SkL to the atomic lattice in Gd$_3$Ru$_4$Al$_{12}$ via high-resolution resonant elastic x-ray scattering (REXS). Weak easy-plane magnetic anisotropy, demonstrated here by a combination of ferromagnetic resonance and REXS, penalizes placing a skyrmion core on a site of the atomic lattice. Under these conditions, a commensurate SkL, locked to the crystal lattice, is stable at finite temperatures -- but gives way to a competing incommensurate ground state upon cooling. We discuss the role of Umklapp-terms in the Hamiltonian for the formation of this lattice-locked state, its magnetic space group, the role of slight discommensurations, or (line) defects in the magnetic texture, and contrast our findings with the case of SkLs in noncentrosymmetric material platforms.

cond-mat.str-el↗

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↗

arXiv2021

Photoinduced Transient States of Antiferromagnetic Orderings in La${}_{1/3}$Sr${}_{2/3}$FeO${}_{3}$ and SrFeO${}_{3}$ Thin Films Observed through Time-resolved Resonant Soft X-ray Scattering

The relationship between the magnetic interaction and photoinduced dynamics in antiferromagnetic perovskites is investigated in this study. In La${}_{1/3}$Sr${}_{2/3}$FeO${}_{3}$ thin films, commensurate spin ordering is accompanied by charge disproportionation, whereas SrFeO${}_{3}$ thin films show incommensurate helical antiferromagnetic spin ordering due to increased ferromagnetic coupling compared to La${}_{1/3}$Sr${}_{2/3}$FeO${}_{3}$. To understand the photoinduced spin dynamics in these materials, we investigate the spin ordering through time-resolved resonant soft X-ray scattering. In La${}_{1/3}$Sr${}_{2/3}$FeO${}_{3}$, ultrafast quenching of the magnetic ordering within 130 fs through a nonthermal process is observed, triggered by charge transfer between the Fe atoms. We compare this to the photoinduced dynamics of the helical magnetic ordering of SrFeO${}_{3}$. We find that the change in the magnetic coupling through optically induced charge transfer can offer an even more efficient channel for spin-order manipulation.

cond-mat.str-el↗

arXiv2020

Complete phase diagram of Sr$_{1-x}$La$_x$FeO$_3$ with versatile magnetic and charge ordering

A detailed electronic phase diagram of perovskite-type oxides Sr$_{1-x}$La$_x$FeO$_3$ $(0\leq x \leq 0.5)$ was established by synchrotron X-ray diffraction, magnetization, and transport measurements for polycrystalline samples synthesized by a high-pressure technique. Among three kinds of helimagnetic phases in SrFeO$_3$ at zero field, two of them showing multiple-${\it q}$ helimagnetic spin textures tend to rapidly disappear in cubic symmetry upon the La substitution with $x$ less than 0.1, which accompanies the loss of metallic nature. On the other hand, the third helimagnetic phase apparently remains robustly in Sr$_{1-x}$La$_x$FeO$_3$ with $x$ higher than 0.1, followed by merging to the spin/charge ordered phase with $x\sim 1/3$. We propose an important role of itinerant ligand holes on the emergence of multiple-${\it q}$ states and a possible link between the third (putative single-${\it q}$) helimagnetic phase in SrFeO$_3$ and the spin/charge ordered phase in Sr$_{2/3}$La$_{1/3}$FeO$_3$.

cond-mat.str-el↗

arXiv2020

Topological Nernst effect of the two-dimensional skyrmion lattice

The topological Hall effect (THE) and its thermoelectric counterpart, the topological Nernst effect (TNE), are hallmarks of the skyrmion lattice phase (SkL). We observed the giant TNE of the SkL in centrosymmetric Gd$_2$PdSi$_3$, comparable in magnitude to the largest anomalous Nernst signals in ferromagnets. Significant enhancement (suppression) of the THE occurs when doping electrons (holes) to Gd$_2$PdSi$_3$. On the electron-doped side, the topological Hall conductivity approaches the characteristic threshold $\sim 1000\,\left(\mathrm{Ωcm}\right)^{-1}$ for the intrinsic regime. We use the filling-controlled samples to confirm Mott's relation between TNE and THE and discuss the importance of Gd-5d orbitals for transport in this compound.

cond-mat.str-el↗

arXiv2020

Soft X-ray Vortex Beam detected by In-line Holography

We demonstrate the in-line holography for soft x-ray vortex beam having an orbital angular momentum. A hologram is recorded as an interference between a Bragg diffraction wave from a fork grating and a divergence wave generated by a Fresnel zone plate. The obtained images exhibit fork-shaped interference fringes, which confirms the formation of the vortex beam. By analyzing the interference image, we successfully obtained the spiral phase distribution. The results demonstrate that the in-line holography technique is promising for the characterization of topological magnets, such as magnetic skyrmions.

physics.optics↗

arXiv2020

Metastable solitonic states in the strained itinerant helimagnet FeGe

The tensile strain is a promising tool for creation and manipulation of magnetic solitonic textures in the chiral helimagnets via tunable control of magnetic anisotropy and Dzyaloshinskii-Moriya interaction. Here, by using the in-situ resonant small-angle x-ray scattering we demonstrate that the skyrmion and chiral soliton lattices can be achieved as metastable states in FeGe lamella as distinct states or even simultaneously by combining the tensile strain and magnetic fields in various orientations with respect to the deformation. The small-angle scattering data are discussed in the frame of the analytical model which is sufficient to describe the experimental results for soliton lattice. By using the experimental results and analytical theory, unwinding of the metastable skyrmions in the perpendicular magnetic field as seen by small-angle scattering experiment was analyzed by the micromagnetic simulation.

cond-mat.mes-hall↗

arXiv2020

High-field depinned phase and planar Hall effect in skyrmion-host Gd$_2$PdSi$_3$

For the skyrmion-hosting intermetallic Gd$_2$PdSi$_3$ with centrosymmetric hexagonal lattice and triangular net of rare earth sites, we report a thorough investigation of the magnetic phase diagram. Our work reveals a new magnetic phase with isotropic value of the critical field for all orientations, where the magnetic ordering vector $\mathbf{q}$ is depinned from its preferred directions in the basal plane. This is in contrast to the highly anisotropic behavior of the low field phases, such as the skyrmion lattice (SkL), which are easily destroyed by in-plane magnetic field. The bulk nature of the SkL and of other magnetic phases was evidenced by specific-heat measurements. Resistivity anisotropy, likely originating from partial gapping of the density of states along $\mathbf{q}$ in this RKKY magnet, is picked up via the planar Hall effect (PHE). The PHE confirms the single-$\mathbf{q}$ nature of the magnetic order when the field is in the hexagonal plane, and allows to detect the preferred directions of $\mathbf{q}$. For field aligned perpendicular to the basal plane, several scenarios for the depinned phase (DP), such as tilted conical order, are discussed on the basis of the data.

cond-mat.str-el↗

arXiv2020

Skyrmion phase and competing magnetic orders on a breathing kagome lattice

Magnetic skyrmion textures are realized mainly in non-centrosymmetric, e.g. chiral or polar, magnets. Extending the field to centrosymmetric bulk materials is a rewarding challenge, where the released helicity / vorticity degree of freedom and higher skyrmion density result in intriguing new properties and enhanced functionality. We report here on the experimental observation of a skyrmion lattice (SkL) phase with large topological Hall effect and an incommensurate helical pitch as small as 2.8 nm in metallic Gd3Ru4Al12, which materializes a breathing kagomé lattice of Gadolinium moments. The magnetic structure of several ordered phases, including the SkL, is determined by resonant x-ray diffraction as well as small angle neutron scattering. The SkL and helical phases are also observed directly using Lorentz transmission electron microscopy. Among several competing phases, the SkL is promoted over a low-temperature transverse conical state by thermal fluctuations in an intermediate range of magnetic fields.

cond-mat.str-el↗

arXiv2019

Metamagnetic transitions and magnetoelectric responses in a chiral polar helimagnet Ni$_2$InSbO$_6$

Magnetic-field effect on the magnetic and electric properties in a chiral polar ordered corundum Ni$_2$InSbO$_6$ has been investigated. Single-crystal soft x-ray and neutron diffraction measurements confirm long-wavelength magnetic modulation. The modulation direction tends to align along the magnetic field applied perpendicular to the polar axis, suggesting that the nearly proper-screw type helicoid should be formed below 77\,K. The application of a high magnetic field causes a metamagnetic transition. In a magnetic field applied perpendicular to the polar axis, a helix-to-canted antiferromagnetic transition takes place through the intermediate soliton lattice type state. On the other hand, a magnetic field applied along the polar axis induces a first-order metamagnetic transition. These metamagnetic transitions accompany a change in the electric polarization along the polar axis.

cond-mat.mtrl-sci↗

arXiv2019

Augmented Magnetic Octupole in Kagome Antiferromagnets Detectable via X-ray Magnetic Circular Dichroism

The magneto-optical Kerr effect (MOKE) has recently been discovered in antiferromagnetic Kagome lattice Mn3Sn. Since the compound exhibits a coplanar $120^\circ$ antiferromagnetic (AFM) order, the magnetic moments cancel each other, and the net magnetization is almost zero. However, the MOKE is allowed due to the lack of the time-reversal symmetry (TRS) of the AFM order. X-ray magnetic circular dichroism (XMCD) can detect a difference in up and down the spin density of states (DOS), and thus XMCD originating from the spin operator, the so-called Sz term, should be negligibly small as well as the net magnetization. Nonetheless, we show that XMCD originating from the magnetic dipole operator, the so-called Tz term, should remain uncancelled in the AFM with the broken TRS. Moreover, we clarify that there is a strong link between the Tz term and the augmented magnetic octupole (AMO), which suggests that XMCD can be an effective approach for analyzing multipole moments in antiferromagnets.

cond-mat.str-el↗

arXiv2018

Skyrmion lattice with a giant topological Hall effect in a frustrated triangular-lattice magnet

Geometrically frustrated magnets provide abundant opportunities for discovering complex spin textures, which sometimes yield unconventional electromagnetic responses in correlated electron systems. It is theoretically predicted that magnetic frustration may also promote a topologically nontrivial spin state, i.e., magnetic skyrmions, which are nanometric spin vortices. Empirically, however, skyrmions are essentially concomitant with noncentrosymmetric lattice structures or interfacial-symmetry-breaking heterostructures. Here, we report the emergence of a Bloch-type skyrmion state in the frustrated centrosymmetric triangular-lattice magnet Gd2PdSi3. We identified the field-induced skyrmion phase via a giant topological Hall response, which is further corroborated by the observation of in-plane spin modulation probed by resonant x-ray scattering. Our results exemplify a new gold mine of magnetic frustration for producing topological spin textures endowed with emergent electrodynamics in centrosymmetric magnets.

cond-mat.str-el↗