arXiv subjects

Tadataka Watanabe

Publications and source records attributed to Tadataka Watanabe.

10 recordsLinked to original sources

arXiv2026

Suppression of orbital ordering and emergence of a glassy magnetic state in a high-entropy spinel vanadate

High-entropy oxides provide a unique platform for exploring the interplay between configurational disorder and correlated electronic states. We report on structural, thermodynamic, and magnetic properties of the high-entropy spinel vanadate (Li$_{0.2}$Mg$_{0.2}$Mn$_{0.2}$Co$_{0.2}$Zn$_{0.2}$)V$_2$O$_4$, in which orbital-active V ions occupy the pyrochlore sublattice. X-ray diffraction measurements reveal that the cubic spinel structure is preserved at temperatures down to 5 K without any detectable symmetry lowering. Unlike conventional spinel vanadates exhibiting a symmetry-lowering structural transition driven by orbital ordering, the compound that we study exhibits a suppression of long-range orbital ordering in the high-entropy state. Magnetic susceptibility measurements show glassy magnetic freezing at temperatures below $\sim$20 K, while specific-heat measurements reveal no anomaly associated with long-range ordering down to 3 K. Frequency-dependent ac susceptibility reveals pronounced glassy dynamics. Analyses based on the Mydosh parameter, dynamic scaling law, and Vogel--Fulcher law suggest an intermediate dynamical regime between canonical spin-glass and cluster-glass behavior. Furthermore, Cole--Cole analyses reveal systematic deviations from a single Debye relaxation process, indicating the presence of heterogeneous magnetic relaxation dynamics near the freezing regime. Our results demonstrate that, in a frustrated spinel vanadate, high configurational entropy suppresses long-range orbital ordering and stabilizes a heterogeneous glassy magnetic state, highlighting the combined roles of geometrical frustration, orbital degrees of freedom, and configurational disorder in high-entropy magnets.

cond-mat.str-el↗

arXiv2026

Magnetoelastic effects in the metallic frustrated antiferromagnet CrB$_2$

Hexagonal chromium diboride CrB$_2$ is a metallic frustrated antiferromagnet with a N\'{e}el temperature $T_N \sim$ 88 K. In CrB$_2$, Cr 3$d$ electrons not only give rise to localized magnetic moments but also contribute to metallic conduction. We perform ultrasound velocity measurements on a single crystal of hexagonal CrB$_2$ to determine its elastic properties. The temperature dependence of the $ab$-plane shear elastic modulus exhibits Curie-type softening upon cooling from $\sim$120 K down to $T_N$. This behavior is interpreted as a precursor to a symmetry-lowering lattice distortion at $T_N$, indicating that magnetic frustration is relieved via transverse magnetoelastic coupling. In addition, the $a$-axis and $c$-axis compressive elastic moduli show unusual softness and their suppression upon cooling, which are naturally explained by Fermi-surface nesting and its suppression upon cooling. The present results suggest that, in CrB$_2$, longitudinal magnetoelastic coupling suppresses Fermi-surface nesting and enhances frustrated exchange interactions, while transverse magnetoelastic coupling plays a key role in relieving the frustration.

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arXiv2024

Elastic softness of low-symmetry frustrated $A$Ti$_2$O$_5$ ($A$ = Co, Fe)

Orthorhombic pseudobrookites CoTi$_2$O$_5$ and FeTi$_2$O$_5$ have a low-symmetry crystal structure comprising magnetic Co$^{2+}$/Fe$^{2+}$ ions and nonmagnetic Ti$^{4+}$ ions, where the orbital-nondegenerate Co$^{2+}$/Fe$^{2+}$ ions form one-dimensional chains running along the orthorhombic $a$ axis. These compounds undergo an antiferromagnetic phase transition at $T_N \sim$ 26 K for CoTi$_2$O$_5$ and $T_N \sim$ 40 K for FeTi$_2$O$_5$. Ultrasound velocity measurements on single crystals of CoTi$_2$O$_5$ and FeTi$_2$O$_5$ reveal that CoTi$_2$O$_5$ exhibits unusual elastic softness above $T_N$ in the symmetry-lowering elastic mode of $ac$-plane shear elastic modulus, inconsistent with the structural symmetry breaking caused by antiferromagnetic ordering at $T_N$. This suggests the presence of two distinct types of magnetostructural fluctuations above $T_N$ that should be a precursor to the symmetry-lowering lattice distortion at $T_N$. In contrast, FeTi$_2$O$_5$ exhibits either negligible or smaller elastic softness, indicating weaker spin-lattice coupling. These findings highlight CoTi$_2$O$_5$ and FeTi$_2$O$_5$ as unique spin-latticed-coupled frustrated systems with low crystal symmetry, where, while the exchange interactions are quasi-one-dimensional in nature, the frustration is released by further lowering the crystal symmetry through three-dimensional spin-lattice coupling, which is stronger in CoTi$_2$O$_5$ than in FeTi$_2$O$_5$.

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arXiv2017

A variety of elastic anomalies in orbital-active nearly-itinerant cobalt vanadate spinel

We perform ultrasound velocity measurements on a single crystal of nearly-metallic spinel Co$_{1.21}$V$_{1.79}$O$_4$ which exhibits a ferrimagnetic phase transition at $T_C \sim$ 165 K. The experiments reveal a variety of elastic anomalies in not only the paramagnetic phase above $T_C$ but also the ferrimagnetic phase below $T_C$, which should be driven by the nearly-itinerant character of the orbitally-degenerate V 3$d$ electrons. In the paramagnetic phase above $T_C$, the elastic moduli exhibit elastic-mode-dependent unusual temperature variations, suggesting the existence of a dynamic spin-cluster state. Furthermore, above $T_C$, the sensitive magnetic-field response of the elastic moduli suggests that, with the negative magnetoresistance, the magnetic-field-enhanced nearly-itinerant character of the V 3$d$ electrons emerges from the spin-cluster state. This should be triggered by the inter-V-site interactions acting on the orbitally-degenerate 3$d$ electrons. In the ferrimagnetic phase below $T_C$, the elastic moduli exhibit distinct anomalies at $T_1\sim$ 95 K and $T_2\sim$ 50 K, with a sign change of the magnetoresistance at $T_1$ (positive below $T_1$) and an enhancement of the positive magnetoresistance below $T_2$, respectively. These observations below $T_C$ suggest the successive occurrence of an orbital glassy order at $T_1$ and a structural phase transition at $T_2$, where the rather localized character of the V 3$d$ electrons evolves below $T_1$ and is further enhanced below $T_2$.

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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.

cond-mat.str-el↗

arXiv2014

Multiple lattice instabilities resolved by magnetic-field and disorder sensitivities in cubic paramagnetic phase of the orbital-degenerate frustrated spinel MgV$_2$O$_4$

Ultrasound velocity measurements of the orbital-degenerate frustrated spinel MgV$_2$O$_4$ are performed in the high-purity single crystal which exhibits successive structural and antiferromagnetic phase transitions, and in the disorder-introduced single crystal which exhibits spin-glass-like behavior. The measurements reveal that two-types of unusual temperature dependence of the elastic moduli coexist in the cubic paramagnetic phase, which are resolved by magnetic-field and disorder sensitivities: huge Curie-type softening with decreasing temperature, and concave temperature dependence with a characteristic minimum. These elastic anomalies suggest the coupling of lattice to coexisting orbital fluctuations and orbital-spin-coupled excitations.

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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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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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arXiv2008

Jahn-Teller Inactivity and Magnetic Frustration in GeCo$_2$O$_4$ Probed by Ultrasound Velocity Measurements

Ultrasound velocity measurements of cubic spinel GeCo$_2$O$_4$ in single crystal were performed for the investigation of shear and compression moduli. The shear moduli in the paramagnetic state reveal an absence of Jahn-Teller activity despite the presence of orbital degeneracy in the Co$^{2+}$ ions. Such a Jahn-Teller inactivity indicates that the intersite orbital-orbital interaction is much stronger than the Jahn-Teller coupling. The compression moduli in the paramagnetic state near the N$\acute{e}$el temperature $T_N$ reveal that the most relevant exchange path for the antiferromagnetic transition lies in the [111] direction. This exchange-path anisotropy is consistent with the antiferromagnetic structure with the wave vector $q \parallel$ [111], suggesting the presence of bond frustration due to competition among a direct ferromagnetic and several distant-neighbors antiferromagnetic interactions. In the JT-inactive condition, the bond frustration can be induced by geometrical orbital frustration of $t_{2g}$-$t_{2g}$ interaction between the Co$^{2+}$ ions which can be realized in the pyrochlore lattice of the high spin Co$^{2+}$ with $t_{2g}$-orbital degeneracy. In GeCo$_2$O$_4$, the tetragonal elongation below $T_N$ releases the orbital frustration by quenching the orbital degeneracy.

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