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H. Sagayama

Publications and source records attributed to H. Sagayama.

16 recordsLinked to original sources

Chiral Antiferromagnetism from Momentum-Space Resonance in a 2D Semiconductor

Understanding the principles governing the emergence of chiral quantum phases is a fundamental challenge, not only for uncovering new mechanisms of quantum-state formation but also for realizing giant electronic responses and transport phenomena arising from chirality and topology. While Fermi-surface instabilities in metals can stabilize complex ordered states through multiple competing scattering channels, their microscopic origin is often obscured by the complexity of the underlying electronic structure, limiting the development of general microscopic design principles. Here, we introduce a complementary strategy based on the simplicity of semiconductor band extrema. Using the layered van der Waals semiconductor GdGaI, whose low-energy electronic structure consists of simple electron and hole valleys, we discover the spontaneous emergence of an intertwined chiral triple-$q$ antiferromagnetic state accompanied by a cooperative reconstruction of the electron-hole band edges, beyond the conventional expectation of a single-$q$ ground state. This collective reconstruction generates substantial momentum-space Berry curvature, giving rise to a pronounced spontaneous anomalous Hall effect despite the semiconducting character and negligible net magnetization. Remarkably, this chiral state is realized within an atomically well-defined ($\approx2a$), topologically nontrivial magnetic texture, showing that such collective quantum states can emerge at an exceptionally small length scale from a simple two-dimensional magnetic semiconductor. More broadly, our results introduce a remarkably simple design concept for chiral quantum matter: using simple semiconductor band extrema as building blocks for resonance-like interplay in momentum space, providing a route to Berry curvature, topological transport, and emergent quantum phases.

cond-mat.str-el

Mass enhancement and metal-nonmetal transition driven by d-f hybridization in perovskites La1-xPrxCuO3

We report the large electron-mass enhancement and the metal to nonmetal transition upon the Pr doping in perovskite-type La1-xPrxCuO3. With increasing the Pr content x around 0.6, the LaCuO3-type three-dimensional structure with trivalent Cu ions changes to the quasi-one-dimensional structure with nearly divalent Cu ions, which accompanies significant changes in the electronic properties. Based on the resistivity, optical conductivity, specific heat measurements and the first-principles calculations, we discuss the formation of a nearly localized nonmetallic state stabilized by the hybridization between Cu 3d, O 2p, and Pr 4f orbitals in the quasi-one-dimensional lattice. The present perovskite-type cuprates offer a unique opportunity to explore novel quantum phases of correlated electrons in low-dimensional lattice, where the spin/charge/orbital degrees of freedom of A- and B-site ions are entangled.

cond-mat.str-el

Multi-step topological transitions among meron and skyrmion crystals in a centrosymmetric magnet

Topological swirling spin textures, such as skyrmions and merons, have recently attracted much attention as a unique building block for high-density magnetic information devices. The controlled transformation among different types of such quasi-particles is an important challenge, while it was previously achieved only in a few non-centrosymmetric systems characterized by Dzyaloshinskii-Moriya interaction. Here, we report an experimental discovery of multi-step topological transitions among a variety of meron and skyrmion crystal states in a centrosymmetric magnet GdRu$_2$Ge$_2$. By performing the detailed magnetic structure analysis based on resonant X-ray and neutron scattering experiments as well as electron transport measurements, we have found that this compound hosts periodic lattice of elliptic skyrmions, meron/anti-meron pairs, and circular skyrmions as a function of external magnetic field. The diameter of these objects is as small as 2.7 nm, which is almost two orders of magnitude smaller than typical non-centrosymmetric magnets. Such an intricate manner of topological magnetic transitions are well reproduced by a theoretical model considering the competition between RKKY interactions at inequivalent wave vectors. The present findings demonstrate that even a simple centrosymmetric magnet with competing interactions can be a promising material platform to realize a richer variety of nanometric magnetic quasi-particles with distinctive symmetry and topology, whose stability may be tunable by various external stimuli.

cond-mat.mtrl-sci

Breathing pyrochlore magnet CuGaCr$_{4}$S$_{8}$: Magnetic, thermodynamic, and dielectric properties

We investigate the crystallographic and magnetic properties of a chromium-based thiospinel CuGaCr$_{4}$S$_{8}$. From a synchrotron x-ray diffraction experiment and structural refinement, Cu and Ga atoms are found to occupy the tetrahedral $A$-sites in an alternate way, yielding breathing pyrochlore Cr network. CuGaCr$_{4}$S$_{8}$ undergoes a magnetic transition associated with a structural distortion at 31 K in zero magnetic field, indicating that the spin-lattice coupling is responsible for relieving the geometrical frustration. When applying a pulsed high magnetic field, a sharp metamagnetic transition takes place at 40 T, followed by a 1/2-magnetization plateau up to 103 T. These phase transitions accompany dielectric anomalies, suggesting the presence of helical spin correlations in low-field phases. The density-functional-theory calculation reveals that CuGaCr$_{4}$S$_{8}$ is dominated by antiferromagnetic and ferromagnetic exchange couplings within small and large tetrahedra, respectively, in analogy with CuInCr$_{4}$S$_{8}$. We argue that $A$-site-ordered Cr thiospinels serve as an excellent platform to explore diverse magnetic phases along with pronounced magnetoelastic and magnetodielectric responses.

cond-mat.mtrl-sci

Complex magnetic phase diagram with a small phase pocket in a three-dimensional frustrated magnet CuInCr$_{4}$S$_{8}$

Frustrated magnets with a strong spin-lattice coupling can show rich magnetic phases and the associated fascinating phenomena. A promising platform is the breathing pyrochlore magnet CuInCr$_{4}$S$_{8}$ with localized $S=3/2$ Cr$^{3+}$ ions, which is proposed to be effectively viewed as an $S=6$ Heisenberg antiferromagnet on the face-centered-cubic lattice. Here, we unveil that CuInCr$_{4}$S$_{8}$ exhibits a complex magnetic phase diagram with a small phase pocket ($A$ phase) by means of magnetization, magnetostriction, magnetocapacitance, and magnetocaloric-effect measurements in pulsed high magnetic fields of up to 60 T. Remarkably, the appearance of $A$ phase is accompanied by anomalous magnetostrictive and magnetocapacitive responses, suggesting the emergence of helimagnetism in contrast to the neighboring commensurate magnetic phases. Besides, the high-entropy nature is confirmed in the high-temperature side of $A$ phase. These features are potentially related to a thermal fluctuation-driven multiple-$q$ state caused by the magnetic frustration, which has been theoretically predicted but yet experimentally undiscovered.

cond-mat.str-el

Zoology of multiple-Q spin textures in a centrosymmetric tetragonal magnet with itinerant electrons

Magnetic skyrmion is a topologically stable particle-like swirling spin texture potentially suitable for high-density information bit, which was first observed in noncentrosymmetric magnets with Dzyaloshinskii-Moriya interaction. Recently, nanometric skyrmion has also been discovered in centrosymmetric rare-earth compounds, and the identification of their skyrmion formation mechanism and further search of nontrivial spin textures are highly demanded. Here, we have exhaustively studied magnetic structures in a prototypical skyrmion-hosting centrosymmetric tetragonal magnet GdRu2Si2, by performing the resonant X-ray scattering experiments. We identified a rich variety of double-Q magnetic structures, including the antiferroic order of meron(half-skyrmion)/anti-meronlike textures with fractional local topological charges. The observed intricate magnetic phase diagram has been successfully reproduced by the theoretical framework considering the four-spin interaction mediated by itinerant electrons and magnetic anisotropy. The present results will contribute to the better understanding of the novel skyrmion formation mechanism in this centrosymmetric rare-earth compound, and suggest that itinerant electrons can ubiquitously host a variety of unique multiple-Q spin orders in a simple crystal lattice system.

cond-mat.mtrl-sci

High-pressure synthesis of Ba$_2$RhO$_4$, a rhodate analogue of the layered perovskite Sr-ruthenate

A new layered perovskite-type oxide Ba$_2$RhO$_4$ was synthesized by a high-pressure technique with the support of convex-hull calculations. The crystal and electronic structure were studied by both experimental and computational tools. Structural refinements for powder x-ray diffraction data showed that Ba$_2$RhO$_4$ crystallizes in a K$_2$NiF$_4$-type structure, isostructural to Sr$_2$RuO$_4$ and Ba$_2$IrO$_4$. Magnetic, resistivity, and specific heat measurements for polycrystalline samples of Ba$_2$RhO$_4$ indicate that the system can be characterized as a correlated metal. Despite the close similarity to its Sr$_2$RuO$_4$ counterpart in the electronic specific heat coefficient and the Wilson ratio, Ba$_2$RhO$_4$ shows no signature of superconductivity down to 0.16 K. Whereas the Fermi surface topology has reminiscent pieces of Sr$_2$RuO$_4$, an electron-like e$_g$-($d_{x^2-y^2}$) band descends below the Fermi level, making of this compound unique also as a metallic counterpart of the spin-orbit-coupled Mott insulator Ba$_2$IrO$_4$.

cond-mat.str-el

Electronic charge transfer driven by spin cycloidal structure

Muon spin rotation and resonant soft X-ray scattering experiments on prototype multiferroics RMn2O5 (R = Y, Sm) are used to demonstrate that the local electric displacements are driven by the spin-current (SC) mechanism. Small local electric displacements were evaluated by observing spin polarization at ligand O ions, for which implanted muons served as an extremely sensitive probe. Our results for YMn2O5 provide evidence that the spin polarization of O ions forming a spin cycloid chain with Mn spins increases in proportion to the vector spin chirality (Si x Sj ) of the Mn ions. This relationship strongly indicates that the charge transfer between O and Mn ions is driven by the SC mechanism, which leads to the ferroelectricity accompanying O spin polarization.

cond-mat.str-el

Nanometric square skyrmion lattice in a centrosymmetric tetragonal magnet

Magnetic skyrmions are topologically stable spin swirls with particle-like character and potentially suitable for the design of high-density information bits. While most known skyrmion systems arise in noncentrosymmetric systems with Dzyaloshinskii-Moriya interaction, also centrosymmetric magnets with a triangular lattice can give rise to skyrmion formation, with geometrically-frustrated lattice being considered essential in this case. Until today, it remains an open question if skyrmions can also exist in the absence of both geometrically-frustrated lattice and inversion symmetry breaking. Here, we discover a square skyrmion lattice state with 1.9 nm diameter skyrmions in the centrosymmetric tetragonal magnet GdRu2Si2 without geometrically-frustrated lattice by means of resonant X-ray scattering and Lorentz transmission electron microscopy experiments. A plausible origin of the observed skyrmion formation is four-spin interactions mediated by itinerant electrons in the presence of easy-axis anisotropy. Our results suggest that rare-earth intermetallics with highly-symmetric crystal lattices may ubiquitously host nanometric skyrmions of exotic origins.

cond-mat.mtrl-sci

Room-temperature Low-field Colossal Magneto-resistance in Double-perovskite Manganite

The gigantic decrease of resistance by an applied magnetic field, which is often referred to as colossal magnetoresistance (CMR), has been an attracting phenomenon in strongly correlated electron systems. The discovery of CMR in manganese oxide compounds has developed the science of strong coupling among charge, orbital, and spin degrees of freedom. CMR is also attracting scientists from the viewpoint of possible applications to sensors, memories, and so on. However, no application using CMR effect has been achieved so far, partly because the CMR materials which satisfy all of the required conditions for the application, namely, high operating temperature, low operating magnetic field, and sharp resistive change, have not been discovered. Here we report a resistance change of more than two-orders of magnitude at a magnetic field lower than 2 T near 300 K in an A-site ordered NdBaMn_2_O_6_ crystal. When temperature and a magnetic field sweep from insulating (metallic) phase to metallic (insulating) phase, the insulating (metallic) conduction changes to the metallic (insulating) conduction within 1 K and 0.5 T, respectively. The CMR is ascribed to the melting of the charge ordering. The entropy change which is estimated from the B-T phase diagram is smaller than what is expected for the charge and orbital ordering. The suppression of the entropy change is attributable to the loss of the short range ferromagnetic fluctuation of Mn spin moments, which an important key of the high temperature and low magnetic field CMR effect.

cond-mat.str-el

Cluster-based Haldane state in edge-shared tetrahedral spin-cluster chain: Fedotovite K$_2$Cu$_3$O(SO$_4$)$_3$

Fedotovite K$_2$Cu$_3$O(SO$_4$)$_3$ is a candidate of new quantum spin systems, in which the edge-shared tetrahedral (EST) spin-clusters consisting of Cu$^{2+}$ are connected by weak inter-cluster couplings to from one-dimensional array. Comprehensive experimental studies by magnetic susceptibility, magnetization, heat capacity, and inelastic neutron scattering measurements reveal the presence of an effective $S$ = 1 Haldane state below $T \cong 4$ K. Rigorous theoretical studies provide an insight into the magnetic state of K$_2$Cu$_3$O(SO$_4$)$_3$: an EST cluster makes a triplet in the ground state and one-dimensional chain of the EST induces a cluster-based Haldane state. We predict that the cluster-based Haldene state emerges whenever the number of tetrahedra in the EST is $even$.

cond-mat.str-el

High-pressure synthesis of an unusual antiferromagnetic metal CaCoO$_{3}$ with GdFeO$_{3}$-type perovskite structure

The GdFeO$_{3}$-type perovskite CaCoO$_{3}$ has been successfully synthesized by high-pressure oxygen annealing for the oxygen deficient perovskite. A detailed structural analysis based on synchrotron X-ray diffraction data and a thermogravimetric analysis show that the valence of Co is +4 and the sample is free from oxygen deficiency. This compound shows an antiferromagnetic ordering at 95 K, which has presumably helical spin arrangement, with keeping the incoherent metallic state down to the lowest temperature. This work demonstrates that the Co$^{4+}$-perovskite oxides exhibit a variety of magnetic phases by the band-width control through the lattice distortion.

cond-mat.str-el

Tomonaga-Luttinger spin liquid in the spin-1/2 inequilateral diamond-chain compound K$_3$Cu$_3$AlO$_2$(SO$_4$)$_4$

K$_3$Cu$_3$AlO$_2$(SO$_4$)$_4$ is a highly one-dimensional spin-1/2 inequilateral diamond-chain antiferromagnet. Spinon continuum and spin-singlet dimer excitations are observed in the inelastic neutron scattering spectra, which is in excellent agreement with a theoretical prediction: a dimer-monomer composite structure, where the dimer is caused by strong antiferromagnetic (AFM) coupling and the monomer forms an almost isolated quantum AFM chain controlling low-energy excitations. Moreover, muon spin rotation/relaxation spectroscopy shows no long-range ordering down to 90~mK, which is roughly three orders of magnitude lower than the exchange interaction of the quantum AFM chain. K$_3$Cu$_3$AlO$_2$(SO$_4$)$_4$ is, thus, regarded as a compound that exhibits a Tomonaga-Luttinger spin liquid behavior at low temperatures close to the ground state.

cond-mat.str-el

Three superconducting phases with different categories of pairing in hole- and electron-doped LaFeAs$_{1-x}$P$_x$O

The phase diagram of LaFeAs$_{1-x}$P$_x$O system has been extensively studied through hole- and electron-doping as well as As/P-substitution. It has been revealed that there are three different superconducting phases with different Fermi surface (FS) topologies and thus with possibly different pairing glues. One of them is well understood as spin fluctuation-mediated superconductivity within a FS nesting scenario. Another one with the FSs in a bad nesting condition must be explained in a different context such as orbital or spin fluctuation in strongly correlated electronic system. In both phases, $T$-linear resistivity was commonly observed when the superconducting transition temperature $T_{\rm c}$ becomes the highest value, indicating that the strength of bosonic fluctuation determines $T_{\rm c}$. In the last superconducting phase, the nesting condition of FSs and the related bosonic fluctuation are moderate. Variety of phase diagram characterizes the multiple orbital nature of the iron-based superconductors which are just near the boundary between weak and strong correlation regimes.

cond-mat.supr-con

Size of Orbital Ordering Domain Controlled by the Itinerancy of the 3d Electrons in a Manganite Thin Film

An electronic effect on a macroscopic domain structure is found in a strongly correlated half-doped manganite film Nd$_{0.5}$Sr$_{0.5}$MnO3 grown on a (011) surface of SrTiO3. The sample has a high-temperature (HT) phase free from distortion above 180K and two low-temperature (LT) phases with a large shear-mode strain and a concomitant twin structure. One LT phase has a large itinerancy (A-type), and the other has a small itinerancy (CE-type), while the lattice distortions they cause are almost equal. Our x ray diffraction measurement shows that the domain size of the LT phase made by the HT-CE transition is much smaller than that by the HT-A transition, indicating that the difference in domain size is caused by the electronic states of the LT phases.

cond-mat.str-el

Electric Control of Spin Helicity in a Magnetic Ferroelectric

Magnetic ferroelectrics or multiferroics, which are currently extensively explored, may provide a good arena to realize a novel magnetoelectric function. Here we demonstrate the genuine electric control of the spiral magnetic structure in one of such magnetic ferroelectrics, TbMnO3. A spin-polarized neutron scattering experiment clearly shows that the spin helicity, clockwise or counter-clockwise, is controlled by the direction of spontaneous polarization and hence by the polarity of the small cooling electric field.

cond-mat.str-el