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T. Onimaru

Publications and source records attributed to T. Onimaru.

17 recordsLinked to original sources

Microscopic origin of hard-plane antiferromagnetism in the Kondo lattice Ce2Rh3Ge5

Hard plane antiferromagnetic order where ordered moments lie perpendicular to the single-ion crystal electric field easy axis is rare in Ce-based Kondo lattices and is a subject of active interest. Here we show that Ce$_2$Rh$_3$Ge$_5$ realizes a hard-plane antiferromagnetic state in which partial delocalization of the local moment gives rise to an RKKY exchange that overturns the single-ion easy-axis preference. Neutron diffraction reveals moments in the $ab$ plane, while inelastic neutron scattering and susceptibility establish a magnetic easy axis along $c$ in the paramagnetic regime, highlighting a clear inversion between single-ion and ordered-state anisotropies. In this work, we establish a unified microscopic framework to consistently account for partial $4f$-moment delocalization, enhanced in-plane RKKY exchange, and the resulting hard-plane antiferromagnetic order. Ce$_2$Rh$_3$Ge$_5$ thus provides a benchmark system in which single-ion anisotropy, Kondo screening, and RKKY exchange compete on comparable energy scales, revealing a cooperative route to hard-axis ordering in strongly hybridized Kondo lattices.

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TbPt6Al3: A rare-earth-based g-wave altermagnet with a honeycomb structure

The magnetic properties of the Tb-honeycomb lattice compound TbPt6Al3, which crystallizes in the NdPt6Al3-type trigonal structure, have been studied by the measurements of electrical resistivity, magnetization M(T, B), and specific heat on single-crystalline samples. The magnetic susceptibility, M(T)/B, for B || c = 0.1 T shows a cusp at TN = 3.5 K, which temperature decreases with increasing the magnitude of B || c, while M(T)/B for B || a = 0.1 T remains constant with decreasing temperature below TN. This anisotropic behavior suggests a collinear antiferromagnetic (AFM) order of the Tb3+ moments pointing along the c axis. The data of M(T)/B for T > 10 K on the single crystal and that of inelastic neutron scattering from powdered samples have been simultaneously analyzed using the crystal field model. The analysis reveals the non-Kramers doublet ground state for the Tb3+ ion under the trigonal crystal field. The neutron powder diffraction measurement shows that the collinear AFM structure with a magnetic propagation vector k = [0, 0, 0] is associated with moments of 5.1 {\mu}B/Tb pointing along the c axis. Comparison of the magnetic point group with the nontrivial spin Laue group indicates that TbPt6Al3 is classified into bulk g-wave altermagnets.

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Incommensurate quantum magnet based on 4f-electron in a zigzag spin-1/2 chain of YbCuS$_2$

We performed high-resolution powder neutron diffraction experiments and discovered an elliptic helical incommensurate magnetic structure in the semiconducting rare-earth magnet YbCuS2, featuring effective spin-1/2 Yb$^{3+}$ ions that form a zigzag chain. Upon cooling the sample to 0.2 K, we observed very weak magnetic peaks indexed with an incommensurate propagation vector k = [0, 0.305, 0] along the zigzag chain. The magnitude of the magnetic moment is at least one-third smaller than the expected value for the Yb$^{3+}$ Kramers doublet ground state. In an applied magnetic field, up-up-down magnetic order was observed at 7.5 T, characterized by diffraction peaks indexed with k = [0, 1/3, 0] and substantial uniform magnetic components. These observations agree well with theoretical calculations based on the density matrix renormalization group for a zigzag spin-1/2 model with isotropic Heisenberg interactions and off-diagonal symmetric $\Gamma$-type exchange interactions derived from material parameters. The theory elucidates the quantum mechanical nature of the incommensurate magnetism as remnant off-diagonal spin correlations in a nematic dimer-singlet state.

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Divergent Thermal Expansion and Gr\"uneisen Ratio in a Quadrupolar Kondo Metal

We report on the low-temperature thermal expansion and magnetostriction of the single-impurity quadrupolar Kondo candidate Y$_{1-x}$Pr$_{x}$Ir$_2$Zn$_{20}$. In the dilute limit, we find a quadrupolar strain that possesses a singular dependence on temperature $T$, $\varepsilon_{\mathrm{u}} \sim H^2 \log 1/T$, for a small but finite magnetic field $H$. Together with the previously reported anomalous specific heat $C$, this implies a quadrupolar Gr\"uneisen ratio $\Gamma_u = \partial_T \varepsilon_{\mathrm{u}}/C \sim H^2/(T^2 \log 1/T)$ whose divergence for finite $H$ is consistent with the scenario of a quadrupolar Kondo effect. In addition, we find a singular behavior of the isotropic strain $\varepsilon_{\mathrm{B}}$ in zero magnetic field resulting in a divergence of both the volume thermal expansion and the volume Gr\"uneisen parameter. We speculate that this behavior might be also induced by putative Kondo correlations via elastic anharmonicities or static strain disorder.

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First-Order Antiferromagnetic Transition and Novel Gapless Excitation in a 4f Zigzag Chain Compound YbCuS2

We report on the 63/65Cu-nuclear magnetic resonance and nuclear quadrupole resonance (NQR) studies of trivalent Yb zigzag chain compound YbCuS2. Sharp NQR signals were observed in the paramagnetic (PM) state. Below TO = 0.95 K, the multi peaks induced by the internal magnetic fields arising from the antferromagnetic (AFM) ordered moments appear and coexist with the PM signal down to 0.85 K, evidencing the first-order AFM phase transition at TO. In addition, the nuclear spin-lattice relaxation rate 1/T1 abruptly decreases below TO and shows the T-linear behavior below 0.5 K. The significant large 1/T1T value strongly suggests the presence of the novel gapless spin excitation in low temperature region.

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Antiferromagnetic correlations in strongly valence fluctuating CeIrSn

CeIrSn with a quasikagome Ce lattice in the hexagonal basal plane is a strongly valence fluctuating compound, as we confirm by hard x-ray photoelectron spectroscopy and inelastic neutron scattering, with a high Kondo temperature of $T_{\mathrm{K}}\sim 480$\,K. We report a negative in-plane thermal expansion $\alpha/T$ below 2\,K, which passes through a broad minimum near 0.75\,K. Volume and $a$-axis magnetostriction for $B \parallel a$ are markedly negative at low fields and change sign before a sharp metamagnetic anomaly at 6\,T. These behaviors are unexpected for Ce-based intermediate valence systems, which should feature positive expansivity. Rather they point towards antiferromagnetic correlations at very low temperatures. This is supported by muon spin relaxation measurements down to 0.1\,K, which provide microscopic evidence for a broad distribution of internal magnetic fields. Comparison with isostructural CeRhSn suggests that these antiferromagnetic correlations emerging at $T\ll T_{\mathrm{K}}$ result from geometrical frustration.

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Evidence for the Single-Site Quadrupolar Kondo Effect in the Dilute non-Kramers System Y$_{1-x}$Pr$_x$Ir$_2$Zn$_{20}$

Acoustic signatures of the single-site quadrupolar Kondo effect in Y$_{0.966}$Pr$_{0.034}$Ir$_2$Zn$_{20}$ are presented. The elastic constant ($C_{11}-C_{12}$)/2, corresponding to the $\Gamma_3$(E)-symmetry electric-quadrupolar response, reveals a logarithmic temperature dependence of the quadrupolar susceptibility in the low-magnetic-field region below $\sim$0.3 K. Furthermore, the Curie-type divergence of the elastic constant down to $\sim$1 K indicates that the Pr ions in this diluted system have a non-Kramers ground-state doublet. These observations evidence the single-site quadrupolar Kondo effect, as previously suggested based on specific-heat and electrical resistivity data.

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Single-Site Non-Fermi Liquid Behaviors in a Diluted 4$f^2$ System Y$_{1-x}$Pr$_x$Ir$_2$Zn$_{20}$

Electrical resistivity $\rho(T)$ and specific heat $C(T)$ measurements have been made on the diluted 4$f^2$ system Y(Pr)Ir$_2$Zn$_{20}$. Both data of $\rho$ and magnetic specific heat $C_{\rm m}$ per Pr ion are well scaled as a function of $T/T_{\rm 0}$, where $T_{\rm 0}$ is a characteristic temperature of non-Fermi liquid (NFL) behaviors. Furthermore, the temperature dependences of $\rho$ and $C_{\mathrm{m}}/T$ agree with the NFL behaviors predicted by the two-channel Kondo model for the strong coupling limit. Therefore, we infer that the observed NFL behaviors result from the single-site quadrupole Kondo effect due to the hybridization of the 4$f^2$ states with multi-channel conduction electrons.

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Highly anisotropic strain dependencies in PrIr$_2$Zn$_{20}$

We report thermal expansion and magnetostriction of the cubic non-Kramers system PrIr$_2$Zn$_{20}$ with a non-magnetic $\varGamma_{3}$ ground state doublet. In previous experiments, antiferroquadrupolar order at \hbox{$T_{\mathrm{Q}}=0.11$\,K} and a Fermi liquid state around $B_{\mathrm{c}}\approx5$\,T for \hbox{$\boldsymbol{B}\parallel[001]$}, indicative of possible ferrohastatic order, were discovered. For magnetic fields \hbox{$\boldsymbol{B}\parallel[001]$}, the low temperature longitudinal and transverse thermal expansion and magnetostriction are highly anisotropic. The resulting volume strain is very small, indicating that the Pr valence remains nearly constant as a function of magnetic field. We conclude that the Fermi liquid state around $B_{\mathrm{c}}$ forms through a very little change in c-f hybridization. This result is in sharp contrast to Ce- and Yb-based Kramers Kondo lattices which show significantly larger volume strains due to the high sensitivity of the Kondo temperature to hydrostatic pressure.

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Quadrupole-Driven Non-Fermi Liquid and Magnetic-Field Induced Heavy Fermion States in a Non-Kramers Doublet System

Orbital degrees of freedom in condensed matters could play important roles in forming a variety of exotic electronic states by interacting with conduction electrons. In 4f electron systems, because of strong intra-atomic spin-orbit coupling, an orbitally degenerate state inherently carries quadrupolar degrees of freedom. The present work has focussed on a purely quadrupole-active system PrIr2Zn20 showing superconductivity in the presence of an antiferroquadrupole order at TQ = 0.11 K. We observed non-Fermi liquid (NFL) behaviors emerging in the electrical resistivity and the 4f contribution to the specific heat, C_4f, in the paramagnetic state at T > TQ. Moreover, in magnetic fields below 6 T, all data set of the electrical resistivity and C_4f(T) are well scaled with characteristic temperatures T0's. This is the first observation of the NFL state in the nonmagnetic quadrupole-active system, whose origin is intrinsically different from that observed in the vicinity of the conventional quantum critical point. It implies possible formation of a quadrupole Kondo lattice resulting from hybridization between the quadrupoles and the conduction electrons. Below 0.13 K, the electrical resistivity and C_4f(T) exhibit anomalies as B approaches 5 T. This is the manifestation of a field-induced crossover toward a Fermi-liquid ground state in the quadrupole Kondo lattice.

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Synthesis and physical properties of a new caged compound Ce3Pd20As6 of the C6Cr23-type structure

We have found that Ce3Pd20As6 crystallizes into a cubic C6Cr23-type structure. Combination of electron probe microanalysis of the chemical composition and Rietveld analysis of the powder X-ray diffraction pattern has revealed an inhomogeneous atomic composition of variable stoichiometry. The physical properties of Ce3Pd20As6 were investigated by measuring the magnetization, electrical resistivity and specific heat. The 4f electrons of Ce3+ ions are well localized but do not show phase transition down to 0.5 K. The metallic electrical resistivity shows a weak Kondo screening. The residual resistivity ratio is rather low probably due to the variable stoichiometry. The magnetization curve and magnetic entropy suggest the Gamma_8 quartet crystalline-electric-field ground state at least one of two Ce sites.

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Low-Energy Optical Phonon Modes in the Caged Compound LaRu2Zn20

The caged compound LaRu2Zn20 exhibits a structural transition at TS =150 K, whose driving mechanism remains elusive. We have investigated atomic dynamics by the measurements of specific heat C and inelastic X-ray scattering (IXS). The lattice part of the specific heat Clat divided by T3, Clat/T3, shows a broad peak at around 15 K, which is reproduced by two Einstein modes with characteristic temperatures of 35 K and 82 K, respectively. IXS measurements along the [111] and [110] directions reveal optical phonon modes at 3 meV (35 K) and 7 meV (80 K), respectively, whose values agree with the values of Einstein temperatures. The first principles calculation has assigned the phonon modes at 3 meV as the optical modes of Zn atoms located at the middle of two La atoms. The low-energy vibration of the Zn atom perpendicular to the there-fold axis is thought to lead the structural instability of LaRu2Zn20.

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Simultaneous Superconducting and Antiferroquadrupolar Transitions in PrRh$_{2}$Zn$_{20}$

Superconducting and antiferroquadrupolar (AFQ) transitions in a Pr-based compound PrRh2Zn20 have been found to occur simultaneously at Tc=TQ=0.06 K. The superconducting transition manifests itself by zero resistance and large diamagnetic susceptibility. The specific heat exhibits a Schottky anomaly peaking at 14 K and magnetization curves measured at 2 K show anisotropic behaviors. The analysis of these data indicates that the crystalline electric field (CEF) ground state of the trivalent Pr ion is the non-Kramers Gamma3 doublet with the quadrupolar degrees of freedom. A sharp peak in the specific heat at 0.06 K has been attributed not to the superconducting transition but to the AFQ transition because the ordering temperature TQ decreases in B || [100] but increases in B || [110] and B || [111] with increasing B up to 6 T. This anisotropic behavior of TQ(B) can be well explained by a two-sublattice mean-field calculation, which corroborates the AFQ ordered state below TQ. The entropy release at TQ is only 10% of Rln2 expected for the Gamma3 doublet, suggesting possible interplay between the quadrupolar degrees of freedom and the superconductivity.

cond-mat.str-el

Determination of spin Hamiltonian in the Ni$_4$ magnetic molecule

Magnetic excitations in a Ni$_4$ magnetic molecule were investigated by inelastic neutron scattering and bulk susceptibility ($\chi_\text{bulk}$) techniques. The magnetic excitation spectrum obtained from the inelastic neutron scattering experiments exhibits three modes at energy transfers of $\hbar\omega=0.5$, 1.35, and 1.6 meV. We show that the energy, momentum, and temperature dependences of the inelastic neutron scattering data and $\chi_\text{bulk}$ can be well reproduced by an effective spin Hamiltonian consisted of intra-molecule exchange interactions, a single-ionic anisotropy, biquadratic interactions, and Zeeman term. Under a hydrostatic pressure, the bulk magnetization decreases with increasing pressure, which along with the biquadratic term indicates spin-lattice coupling present in this system.

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A Kondo lattice antiferromagnet CePd5Al2

We report on the electrical resistivity, magnetic susceptibility and heat-capacity measurements on a new intermetallic compound CePd5Al2, crystallizing in the ZrNi2Al5-type tetragonal structure, with lattice parameters a = 4.156 A and c = 14.883 A. The compound presents Kondo lattice behavior and an easy-plane antiferromagnetic ground state with two magnetic transitions at 2.9 K and 3.9 K. The Sommerfeld coefficient is estimated as 60 mJ/mol K^2.

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Easy-plane magnetocrystalline anisotropy in the multi-step metamagnet CeIr3Si2

Highly anisotropic properties of CeIr$_3$Si$_2$ have been observed by the magnetization $M$($B$), electrical resistivity $ρ$, and specific heat measurements on a single-crystalline sample. This compound with an orthorhombic structure having zigzag chains of Ce ions along the a-axis undergos magnetic transitions at 3.9 K and 3.1 K. At 0.3 K, metamagnetic transitions occur at 0.68 T and 1.3 T for $B$$//$$b$ and 0.75 T for $B$$//$$c$. Easy-plane magnetocrystalline anisotropy is manifested as $M$($B//b$) $\cong$ $M$($B//c$) $\cong$ 11$M$($B//a$) at $B$ = 5 T. Electrical resistivity is also anisotropic; $ρ_{b}$ $\cong$ $ρ_{c}$ $\ge$ 2$ρ_{a}$. The magnetic part of $ρ$ exhibits a double-peak structure with maxima at 15 K and 250 K. The magnetic entropy at $T$$\rm_{N1}$ = 3.9 K is a half of $R$ln2. These observations are ascribable to the combination of the Kondo effect with $T$$\rm_{K}$ $\sim$ 20 K and a strong crystal field effect. The analysis of $M$($B$) and paramagnetic susceptibility revealed unusually large energy splitting of 500 K and 1600 K for the two excited doublets, respectively.

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Observation of Modulated Quadrupolar Structures in PrPb3

Neutron diffraction measurements have been performed on the cubic compound PrPb3 in a [001] magnetic field to examine the quadrupolar ordering. Antiferromagnetic components with q=(1/2+-d 1/2 0), (1/2 1/2+-d 0) (d~1/8) are observed below the transition temperature TQ (0.4 K at H=0) whose amplitudes vary linear with H and vanish at zero field, providing the first evidence for a modulated quadrupolar phase. For H<1 T, a non-square modulated state persists even below 100 mK suggesting quadrupole moments associated with a Gamma3 doublet ground state to be partially quenched by hybridization with conduction electrons.

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