arXiv subjects

Keisuke Tomiyasu

Publications and source records attributed to Keisuke Tomiyasu.

13 recordsLinked to original sources

arXiv2022

Prominent electron-hole asymmetry in thermoelectric transport of LaCoO$_3$

We have measured the electrical resistivity and the thermopower of the electron-doped perovskite cobaltites LaCo$_{1-y}$Te$_y$O$_3$. In contrast to the hole-doped systems such as metallic ferromagnets La$_{1-x}M_x$CoO$_3$ ($M$ = Ca, Sr, Ba), the electron-doped samples show an insulating behavior even in a heavily doped range due to a spin-state blockade mechanism that an electron hopping from high-spin Co$^{2+}$ to low-spin Co$^{3+}$ site is energetically suppressed. We find that, despite the electron doping, the thermopower shows relatively large positive values above $y=0.05$, strikingly distinct from the hole-doped case where it comes close to zero with doping. This prominent electron-hole asymmetry seen in the thermopower originates from a bipolar conduction which consists of a slight amount of mobile holes and the main immobile electrons, demonstrating an impact of spin-state blockade on thermoelectric transport.

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arXiv2021

Spin dynamics simulation of the $Z_2$-vortex fluctuations

Motivated by the recent quasi-elastic neutron scattering experiment, we extend the spin-dynamics simulation on the triangular-lattice Heisenberg antiferromagnet, to observe a sharp central peak of its energy width $\sim 0.001J$ ($J$ the exchange coupling) of the $Z_2$-vortex origin, consistently with the experiment.

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arXiv2021

Damping of spinful excitons in LaCoO$_3$ by thermal fluctuations: Theory and experiment

We present Co $L_3$-edge resonant inelastic x-ray scattering (RIXS) of bulk LaCoO$_3$ across the thermally-induced spin-state crossover around 100~K. Owing to a high energy resolution of 25~meV, we observe unambiguously the dispersion of the intermediate-spin (IS) excitations in the low temperature regime. Approaching the intermediate temperature regime, the IS excitations are damped and the bandwidth is reduced. The observed behavior can be well described by a model of mobile IS excitons with strong attractive interaction, which we solve using dynamical mean-field theory for hard-core bosons. Our results provide a detailed mechanism of how high-spin (HS) and IS excitations interact to establish the physical properties of cobaltite perovskites.

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arXiv2020

Emergent spin-$1$ Haldane gap and ferroelectricity in a frustrated spin-$1/2$ ladder

We report experimental and theoretical evidence that Rb$_2$Cu$_2$Mo$_3$O$_{12}$ has a nonmagnetic tetramer ground state of a two-leg ladder comprising antiferromagnetically coupled frustrated spin-$1/2$ chains and exhibits a Haldane spin gap of emergent spin-1 pairs. Three spin excitations split from the spin-1 triplet by a Dzyaloshinskii-Moriya interaction are identified in inelastic neutron-scattering and electron spin resonance spectra. A tiny magnetic field generates ferroelectricity without closing the spin gap, indicating a novel class of ferroelectricity induced by a vector spin chirality order.

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arXiv2018

Excitonic dispersion of the intermediate-spin state in LaCoO$_3$ revealed by resonant inelastic X-ray scattering

More than 50 years ago the electron-hole attraction was proposed to drive narrow gap semiconductors or semimetals to a new phase, the excitonic insulator. The experimental proof of its existence in bulk materials remains elusive. In strongly correlated insulators, the proximity of the excitonic insulator phase is reflected by the presence of dispersive electron-hole excitations with a small gap above a singlet ground state. Recently, such an excitation spectrum was proposed to be realized in perovskite oxide LaCoO$_3$. In this Letter we use Co $L_3$-edge resonant inelastic X-ray scattering to put this proposal to experimental test.

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arXiv2017

Magnetic Properties of One-Dimensional Quantum Spin System Rb2Cu2Mo3O12 Studied by Muon Spin Relaxation

Magnetic properties of a one-dimensional frustrated quantum spin system Rb2Cu2Mo3O12 is investigated by the muon spin relaxation (muSR) technique. Although this system shows an incommensurate spin correlation in neutron scattering, it has not yet been determined whether the ground state reaches to a nonmagnetic spin-singlet state or not. In this study, our zero-field (ZF) muSR result undoubtedly reveals a nonmagnetic ground state, which establishes formation of the nonmagnetic incommensurate spin-singlet state in combination of the previous neutron scattering study. Furthermore, we found that the internal field is slightly enhanced below ~7 K. This temperature dependence resembles that of electric polarization under the magnetic field reported recently, indicating a possibility that a small change occurs even under ZF. In longitudinal-field measurements, a fast fluctuation around a narrowing region is observed. This relaxation is expected to reflect characteristics of formation of the spin-singlet state.

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arXiv2016

Microscopic examinations of Co valences and spin states in electron-doped LaCoO$_{3}$

We studied the Co valences and spin states in electron-doped LaCo$_{1-y}$Te$_{y}$O$_3$ by measuring x-ray absorption spectra and electron spin resonance. The low-temperature insulating state involves the low-spin Co$^{3+}$ ($S=0$) and the high-spin Co$^{2+}$ state, which is described by $g=3.8$ and $j_{\rm eff}=1/2$. The results, in concurrence with the electron-hole asymmetry confirmed in electrical resistivity, coincide with a spin-blockade phenomenon in this system. Further, we discuss the $g$ factor in terms of the strong covalent-bonding nature and consider multiple origins of this phenomenon.

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arXiv2015

Acoustic study for dynamical molecular-spin state without undergoing magnetic phase transition in spin-frustrated ZnFe$_2$O$_4$

Ultrasound velocity measurements were performed on a single crystal of spin-frustrated ferrite spinel ZnFe$_2$O$_4$ from 300 K down to 2 K. In this cubic crystal, all the symmetrically-independent elastic moduli exhibit softening with a characteristic minimum with decreasing temperature below $\sim$100 K. This elastic anomaly suggests a coupling between dynamical lattice deformations and molecular-spin excitations. In contrast, the elastic anomalies, normally driven by the magnetostructural phase transition and its precursor, are absent in ZnFe$_2$O$_4$, suggesting that the spin-lattice coupling cannot play a role in relieving frustration within this compound. The present study infers that, for ZnFe$_2$O$_4$, the dynamical molecular-spin state evolves at low temperatures without undergoing precursor spin-lattice fluctuations and spin-lattice ordering. It is expected that ZnFe$_2$O$_4$ provides the unique dynamical spin-lattice liquid-like system, where not only the spin molecules but also the cubic lattice fluctuate spatially and temporally.

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arXiv2012

Spin-state responses to light impurity doping in low-spin perovskite LaCoO$_{3}$

We studied the spin-state responses to light impurity doping in low-spin perovskite LaCoO$_{3}$ (Co^3+: d^6) through magnetization and X-ray fluorescence measurements of single-crystal LaCo$_{0.99}$$M_{0.01}$O$_{3}$ ($M$ = Cr, Mn, Fe, Ni). In the magnetization curves measured at 1.8 K, a change in the spin-state was not observed for Cr, Mn, or Fe doping but was observed for Ni doping. Strong magnetic anisotropy along the [100] easy axis was also found in the Ni-doped sample. The fluorescence measurements revealed that the valences were roughly estimated to be Cr^3+, Mn^4+, Fe^(3+delta)+, and Ni^3+. From the observed chemical trends, we propose that the chemical potential is a key factor in inducing the change of the low-spin state. By expanding a model of the ferromagnetic spin-state heptamer generated by hole doping, we discuss the emergence of highly anisotropic ferromagnetic spin-state clusters induced by low-spin Ni^3+ with Jahn-Teller activity. We also discuss applicability of the present results to mantle materials and impurity-doped pyrites with Fe (d^6).

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arXiv2012

Observation of elastic anomalies driven by coexisting dynamical spin Jahn-Teller effect and dynamical molecular spin state in paramagnetic phase of the frustrated MgCr$_2$O$_4$$

Ultrasound velocity measurements of magnesium chromite spinel MgCr$_2$O$_4$ reveal elastic anomalies in the paramagnetic phase that are characterized as due to geometrical frustration. The temperature dependence of the tetragonal shear modulus $(C_{11}-C_{12})/2$ exhibits huge Curie-type softening, which should be the precursor to spin Jahn-Teller distortion in the antiferromagnetic phase. The trigonal shear modulus $C_{44}$ exhibits nonmonotonic temperature dependence with a characteristic minimum at $\sim$50 K, indicating a coupling of the lattice to dynamical molecular spin state. These results strongly suggest the coexistence of dynamical spin Jahn-Teller effect and dynamical molecular spin state in the paramagnetic phase, which is compatible with the coexistence of magnetostructural order and dynamical molecular spin state in the antiferromagnetic phase.

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arXiv2012

Neutron scattering study of role of partial disorder-type spin fluctuations in conductivity of frustrated conductor Mn$_3$Pt

The spin-frustrated conductor Mn$_3$Pt exhibits a characteristic magnetic structure called partial disorder in which some spin sites can form magnetic order through the generation of non-ordered sites that locally relieve the frustration. Here we report the results of a single-crystal inelastic neutron scattering study of this compound. The measured momentum $\vec{Q}$ correlations of diffusive magnetic scattering reveal that the paramagnetic phase exhibits short-range spin fluctuations with the same type of partial disorder. Its relation to conductivity is also discussed.

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arXiv2011

Elastic Instabilities within Antiferromagnetically Ordered Phase in the Orbitally-Frustrated Spinel GeCo$_2$O$_4$

Ultrasound velocity measurements of the orbitally-frustrated GeCo$_2$O$_4$ reveal unusual elastic instabilities due to the phonon-spin coupling within the antiferromagnetic phase. Shear moduli exhibit anomalies arising from the coupling to short-range ferromagnetic excitations. Diplike anomalies in the magnetic-field dependence of elastic moduli reveal magnetic-field-induced orbital order-order transitions. These results strongly suggest the presence of geometrical orbital frustration which causes novel orbital phenomena within the antiferromagnetic phase.

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arXiv2011

Spin-orbit coupling inactivity of Co$^{2+}$ ion in geometrically frustrated magnet GeCo$_2$O$_4$

We report single-crystal neutron diffraction studies on a spinel antiferromagnet GeCo$_2$O$_4$, which exhibits magnetic order with a trigonal propagation vector and tetragonal lattice expansion ($c/a\simeq1.001$) below $T_{\rm N}=21$ K. For this inconsistency between spin and lattice in symmetry, magnetic Bragg reflections with a tetragonal propagation vector were discovered below $T_{\rm N}$. We discuss spin and orbital states of Co$^{2+}$ ion underlying the new magnetic component.

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