arXiv subjects

K. Tomiyasu

Publications and source records attributed to K. Tomiyasu.

16 recordsLinked to original sources

arXiv2022

Observation of topological $Z_2$ vortex fluctuations in the frustrated Heisenberg magnet NaCrO$_2$

Spin fluctuations in the triangular-lattice Heisenberg antiferromagnet NaCrO$_2$ are investigated by means of quasi-elastic neutron scattering with high energy resolution and wide energy band. Two components with the following features are captured separately. They are pronounced at intermediate temperatures of 20-50 K. One with quite an extended lifetime corresponding to $\sim$$0.001E_{\rm ex}$ ($E_{\rm ex}$ the exchange energy) nearly disappears at low temperature 10 K, and the other with an extended lifetime $\sim$$0.01E_{\rm ex}$ survives there, identified as free $Z_2$ vortex and $Z_2$-vortex pair, respectively, in harmony with the $Z_2$ vortex theory.

cond-mat.str-el↗

arXiv2022

Symmetry-resolved elastic anomalies in spin-crossover cobaltite LaCoO$_3$

Ultrasound velocity measurements of the pseudo-cubic spin-crossover cobaltite LaCoO$_3$ and the lightly Ni-substituted La(Co$_{0.99}$Ni$_{0.01}$)O$_3$ reveal two types of symmetry-resolved elastic anomaly in the insulating paramagnetic state that are commonly observed in these compounds. The temperature dependence of the bulk modulus exhibits Curie-type softening upon cooling below 300 K down to $\sim$70 K, indicating the presence of isostructural lattice instability arising from orbital fluctuations. The temperature dependence of the tetragonal and trigonal shear moduli exhibits unusual hardening upon cooling below 300 K, indicating the occurrence of elasticity crossover arising from the spin crossover. The present study also reveals that the isostructural lattice instability in LaCoO$_3$ is sensitively suppressed with the Ni substitution, indicating the suppression of orbital fluctuations with the light Ni substitution. This Ni substitution effect in LaCoO$_3$ can be explained on the basis that the isostructural lattice instability arises from the coupling of the lattice to the Co spin state fluctuating between the high-spin state and intermediate-spin state.

cond-mat.str-el↗

arXiv2018

Quantum paramagnet near spin-state transition

Spin-state transition, also known as spin crossover, plays a key role in diverse systems, including minerals and biological materials. In theory, the boundary range between the low- and high-spin states is expected to enrich the transition and give rise to unusual physical states. However, no compound that realizes a nearly degenerate critical range as the ground state without requiring special external conditions has yet been experimentally identified. This study reports that, by comprehensive measurements of macroscopic physical properties, X-ray diffractometry, and neutron spectroscopy, the Sc substitution in LaCoO$_3$ destabilizes its nonmagnetic low-spin state and generates an anomalous paramagnetic state accompanied by the enhancement of transport gap and magneto-lattice-expansion as well as the contraction of Co--O distance with the increase of electron site-transfer. These phenomena are not well described by the mixture of conventional low- and high-spin states, but by their quantum superposition occurring on the verge of a spin-state transition. The present study enables us to significantly accelerate the design of new advanced materials without requiring special equipment based on the concept of quantum spin-state criticality.

cond-mat.str-el↗

arXiv2018

Emergent units of itinerant spin-state excitations in LaCoO$_3$

Spin crossover is expected to enrich unusual physical states in various types of condensed matter. Through inelastic neutron scattering, we study the spin-state excitations in the canonical and advanced platform, LaCoO$_3$, and reveal that the spatial correlation robustly maintains the seven-Co-site size below 300 K and the internal Co-$d$ electrons are spatially delocalized. By combining theoretical calculations, this dynamical short-range order is identified as a new collective unit for describing spin-state with dual spin-state nature beyond the conventional one-Co-site classification.

cond-mat.str-el↗

arXiv2018

Emergence of spin-orbit order in the spinel CuCr$_2$O$_4$

We determined the magnetic structure of CuCr$_2$O$_4$ using neutron diffraction and irreducible representation analysis. The measurements identified a new phase between 155 K and 125 K as nearly collinear magnetic ordering in the Cr pyrochlore lattice. Below 125 K, a Cu-Cr ferrimagnetic component develops the noncollinear order. Along with the simultaneously obtained O positions and the quantum effect of spin-orbit coupling, the magnetic structure is understood to involve spin-orbit ordering, accompanied by an appreciably deformed orbital of presumably spin-only Cu and Cr.

cond-mat.str-el↗

arXiv2017

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↗

arXiv2017

Coulomb correlations intertwined with spin and orbital excitations in LaCoO$_3$

We carried out temperature-dependent (20 - 550 K) measurements of resonant inelastic X-ray scattering on LaCoO$_3$ to investigate the evolution of its electronic structure across the spin-state crossover. In combination with charge-transfer multiplet calculations, we accurately quantized the renormalized crystal-field excitation energies and spin-state populations. We show that the screening of the on-site Coulomb interaction of 3d electrons is orbital selective and coupled to the spin-state crossover in LaCoO$_3$. The results establish that the gradual spin-state crossover is associated with a relative change of Coulomb energy versus bandwidth, leading to a Mott-type insulator-to-metal transition.

cond-mat.str-el↗

arXiv2017

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↗

arXiv2014

Development of spin correlations in the geometrically frustrated triangular-lattice Heisenberg antiferromagnet CuCrO2

Magnetic excitations in the triangular-lattice Heisenberg antiferromagnet (TLHA) CuCrO2 were studied using single-crystal inelastic neutron scattering. A diffusive quasielastic component that persisted without developing a correlation length over a wide temperature range both below and above the ordering temperature was observed. Furthermore, characteristic momentum dependence was observed that was reproduced using minimum spin clusters. The robust spin clusters contrast with conventional magnetic ordering and may be universal in TLHAs.

cond-mat.str-el↗

arXiv2014

Spin-orbit fluctuations in frustrated heavy-fermion metal LiV$_2$O$_4$

Spin fluctuations were studied over a wide momentum ($\hbar Q$) and energy ($E$) space in the frustrated $d$-electron heavy-fermion metal LiV$_2$O$_4$ by time-of-flight inelastic neutron scattering. We observed the overall $Q$$-$$E$ evolutions near the characteristic $Q=0.6$ Å$^{-1}$ peak and found another weak broad magnetic peak around 2.4 Å$^{-1}$. The data are described by a simple response function, a highly itinerant magnetic form factor, and antiferromagnetic short-range spatial correlations, indicating that heavy-fermion formation is attributable to spin-orbit fluctuations with orbital hybridization.

cond-mat.str-el↗

arXiv2012

Emergence of highly degenerate excited states in frustrated magnet MgCr$_2$O$_4$

High degeneracy in ground states leads to the generation of exotic zero-energy modes, a representative example of which is the formation of molecular spin liquid-like fluctuations in a frustrated magnet. Here we present single-crystal inelastic neutron scattering results for the frustrated magnet MgCr$_2$O$_4$, which show that a common set of finite-energy molecular spin excitation modes is sustained in both the liquid-like paramagnetic phase and a magnetically ordered phase with an extremely complex structure. Based on this finding, we propose the concept of high degeneracy in excited states, which promotes local resonant elementary excitations. This concept is expected to have ramifications on our understanding of excitations in many complex systems, including not only spin but also atomic liquids, complex order systems, and amorphous systems.

cond-mat.str-el↗

arXiv2012

Modified Cross-Correlation for Efficient White-Beam Inelastic Neutron Scattering Spectroscopy

We describe a method of white-beam inelastic neutron scattering for improved measurement efficiency. The method consists of matrix inversion and selective extraction. The former is to resolve each incident energy component from the white-beam data, and the latter eliminates contamination by elastic components, which produce strong backgrounds that otherwise obfuscate the inelastic scattering components. In this method, the optimal experimental condition to obtain high efficiency will strongly depend on the specific aim of the individual experiments.

cond-mat.mtrl-sci↗

arXiv2012

Emergence of magnetic long-range order in frustrated pyrochlore Nd$_2$Ir$_2$O$_7$ with metal-insulator transition

In this study, we performed powder neutron diffraction and inelastic scattering measurements of frustrated pyrochlore Nd$_2$Ir$_2$O$_7$, which exhibits a metal-insulator transition at a temperature $T_{\rm MI}$ of 33 K. The diffraction measurements revealed that the pyrochlore has an antiferromagnetic long-range structure with propagation vector $\vec{q}_{0}$ of (0,0,0) and that it grows with decreasing temperature below 15 K. This structure was analyzed to be of the all-in all-out type, consisting of highly anisotropic Nd$^{3+}$ magnetic moments of magnitude $2.3\pm0.4$$μ_{\rm B}$, where $μ_{\rm B}$ is the Bohr magneton. The inelastic scattering measurements revealed that the Kramers ground doublet of Nd$^{3+}$ splits below $T_{\rm MI}$. This suggests the appearance of a static internal magnetic field at the Nd sites, which probably originates from a magnetic order consisting of Ir$^{4+}$ magnetic moments. Here, we discuss a magnetic structure model for the Ir order and the relation of the order to the metal-insulator transition in terms of frustration.

cond-mat.str-el↗

arXiv2011

Molecular spin-liquid state in spin-3/2 frustrated spinel HgCr$_2$O$_4$

A hexamer-type spin excitation seen in spinel chromates $A$Cr$_2$O$_4$ ($A$ = Mg, Zn, or Cd) is the representative spin-liquid-like state caused by geometrical frustration. To clarify an origin of the state, we comparatively studied spin excitations in an isomorphic material HgCr$_2$O$_4$ by inelastic neutron scattering, and observed a different molecular-type excitation. Numerical analyses performed using model Hamiltonians suggest that these two types of spin excitations originate from a spin-3/2 molecular singlet hidden in a magnetically ordered phase. The difference between the molecular types is explained by the difference in the kind of exchange interactions occurring in the chromates.

cond-mat.str-el↗

arXiv2011

Molecular spin-orbit excitations in the J_eff = 1/2 frustrated spinel GeCo$_2$O$_4$

We describe powder and single-crystal inelastic neutron scattering experiments on a spinel-type antiferromagnet GeCo$_2$O$_4$, represented by an effective total angular momentum J_eff = 1/2. Several types of non-dispersive short-range magnetic excitations were discovered. The scattering intensity maps in $\vec{Q}$ space are well reproduced by dynamical structure factor analyses using molecular model Hamiltonians. The results of analyses strongly suggest that the molecular excitations below T_N arise from a hidden molecular-singlet ground state, in which ferromagnetic subunits are antiferromagnetically coupled. The quasielastic excitations above T_N are interpreted as its precursor. A combination of frustration and J_eff = 1/2 might induce these quantum phenomena.

cond-mat.str-el↗

arXiv2008

Molecular spin resonance in the geometrically frustrated MgCr2O4 magnet by inelastic neutron scattering

We measured two magnetic modes with finite and discrete energies in an antiferromagnetic ordered phase of a geometrically frustrated magnet MgCr2O4 by single-crystal inelastic neutron scattering, and clarified the spatial spin correlations of the two levels: one is an antiferromagnetic hexamer and the other is an antiferromagnetic heptamer. Since these correlation types are emblematic of quasielastic scattering with geometric frustration, our results indicate instantaneous suppression of lattice distortion in an ordered phase by spin-lattice coupling, probably also supported by orbital and charge. The common features in the two levels, intermolecular independence and discreteness of energy, suggest that the spin molecules are interpreted as quasiparticles (elementary excitations with energy quantum) of highly frustrated spins, in analogy with the Fermi liquid approximation.

cond-mat.str-el↗