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Toshiro Sakakibara

Publications and source records attributed to Toshiro Sakakibara.

At least 19 recordsLinked to original sources

Competition between Geometrical Frustration and the Kondo Effect in CePdAl Revealed by High-Resolution Magnetization

CePdAl is a heavy-fermion compound with a quasi-kagome structure, where geometrical frustration competes with the Kondo effect. Using a high-sensitivity magnetometer, we observe clear first-order metamagnetic transitions without magnetization plateaus in CePdAl at 80 mK, indicating a lifting of frustration through the suppression of the Kondo effect and spin flips of ordered moments under fields. An anomaly in the nonlinear magnetic susceptibility at 4.3 T suggests nondipolar correlations in the polarized paramagnetic state. Furthermore, we found no evidence of non-Fermi-liquid behavior in the high-field region, where the antiferromagnetic order is completely suppressed. These findings establish the essential thermodynamic constraints for understanding the field-induced spin-liquid state in CePdAl.

cond-mat.str-el↗

Designing electronic magnetoelectric matter with organic quantum spin trimers

Magnetoelectric (ME) phenomena are commonly driven by spin-lattice coupling. Here we demonstrate a different route based on frustrated quantum spin trimers that intrinsically intertwine magnetic moments and electric dipoles. Using molecular design principles, we realize a weakly coupled lattice of equilateral $S=1/2$ spin trimers in the organic radical crystal TNN$\cdot$CH$_3$CN. In this material, correlated electronic fluctuations within each trimer generate electric dipoles, while geometrically frustrated intertrimer interactions organize them into collective ME states. Magnetization, thermodynamic, and dielectric measurements reveal multiple magnetic-field-induced phases, including the $1/3$-magnetization plateau marked by pronounced dielectric anomalies. Effective low-energy theories and numerical simulations show that these phenomena are driven by electronically generated trimer dipoles whose collective order is stabilized by frustration relief of the intertrimer interactions, establishing a direct connection between geometric frustration and emergent magnetoelectricity. Our results identify quantum spin trimers as multifunctional building blocks, providing a bottom-up route for designing correlated ME materials from electronically active quantum spin clusters.

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Field-induced anomaly in the anisotropic non-Fermi-liquid normal state of UBe$_{13}$

We report the results of high-resolution dc magnetization and specific-heat measurements at very low temperatures for a single crystal \color{black} of UBe$_{13}$ in magnetic fields applied along the [001] and [111] directions, in both the normal and superconducting states. In the normal state, magnetic susceptibility $χ(T) = M/H$ exhibits a logarithmic temperature dependence over a wide temperature range (1-20 K). However, with increasing field, this non-Fermi-liquid (NFL) behavior of $χ(T) $ at low temperatures is suppressed. Moreover, a susceptibility maximum occurs below 4 T, whereas Fermi-liquid coherence is recovered above 8 T. In addition, thermodynamic anomalies ($T_{\rm A}$ and $H_{\rm A}$) occur in both magnetic susceptibility and specific heat at intermediate fields (6--10 T) along the [111] direction. Furthermore, a nontrivial fifth-order nonlinear susceptibility is observed in the normal-state magnetization of UBe$_{13}$. These results suggest a close relationship between the field-induced multipolar correlations of $5f$-electron degrees of freedom and the Fermi-surface reconstruction accompanying the crossover from the NFL state to the Fermi-liquid state in UBe$_{13}$.

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High-resolution magnetostriction measurements of the Pauli-limited superconductor Sr2RuO4

We performed high-resolution magnetostriction measurements on the Pauli-limited superconductor Sr$_2$RuO$_4$ using high-quality single crystals. A first-order superconducting transition, accompanied by pronounced hysteresis, was observed under in-plane magnetic fields, where the relative length change of the sample, $ΔL/L$, was on the order of $10^{-8}$. To ensure the reliability of the measurements, particular attention was paid to minimizing the influence of magnetic torque, which can significantly affect data under in-plane field configurations, via field-angle-resolved magnetostriction. Within the hysteresis regime, slightly below the Pauli-limited upper critical field, a hump-like anomaly in the magnetostriction coefficient was identified. Furthermore, a characteristic double-peak structure in the field-angle derivative of the magnetostriction provides additional support for this anomaly. Although these findings may reflect a lattice response associated with the emergence of the Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) phase in Sr$_2$RuO$_4$, the possibility of a broadened first-order transition cannot be excluded. Notably, this magnetostriction anomaly qualitatively deviates from the FFLO phase boundary suggested by previous NMR measurements, highlighting the necessity for further experimental and theoretical investigations to elucidate the nature of the FFLO state in this material.

cond-mat.supr-con↗

Multiple magnetic orders discovered in the superconducting state of EuFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$

The interplay between superconductivity and magnetism is an important subject in condensed matter physics. EuFe$_{2}$As$_{2}$-based iron pnictides could offer an interesting plateau to study their relationship that has attracted considerable attention. So far, two magnetic phase transitions were observed in EuFe$_{2}$As$_{2}$-based crystal, which were deemed to originate from the itinerant Fe moments ($\sim$ 190 K) and the localized Eu$^{2+}$ moments ($\sim$ 19 K), respectively. Here, we systematically studied the heat capacity for the EuFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$ crystals with \textit{x} = 0.21 (optimally doped) and \textit{x} = 0.29 (overdoped). We have found two new magnetic orders in the superconducting state (ranging from 0.4 to 1.2 K) in the optimally doped crystal. As more P was introduced into the As site, one of the magnetic orders becomes absent in the overdoped crystal. Additionally, we observed strong field and orientation dependence in heat capacity. The present findings in EuFe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$ have detected the new low-temperature magnetic orders, which may originate from the localized Eu$^{2+}$ spins order or the spin reorientation.

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Anisotropy of the magnetic-field-induced phase pocket in the non-Kramers doublet system PrIr$_2$Zn$_{20}$

We provide thermodynamic evidence for the presence of a magnetic-field-induced small phase pocket near the antiferro-quadrupole (AFQ) phase boundary in the non-Kramers $Γ_3$ doublet system PrIr$_2$Zn$_{20}$. In particular, we measured the specific heat as functions of temperature $T$, magnetic field $B$, and field angle $ϕ_B$, and found a second specific-heat anomaly in a relatively wide field-angle range near $B \parallel [001]$, although fine tuning of the field strength is required. We also investigated the rotational magnetocaloric effect and evaluated an entropy change in this phase pocket. The present findings demonstrate that multipole degrees of freedom give rise to a magnetic-field-induced exotic order in PrIr$_2$Zn$_{20}$, suggesting the possibility of switching between the order parameters or emergence of a multiple-$q$ order of quadrupoles.

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Magnetic Properties of YbBe13 Probed by Neutron Scattering and Thermodynamic Measurements

We examined the magnetic properties of YbBe13, which exhibits an antiferromagnetic order below TN = 1.2 K. Unlike other MBe13 compounds (M = rare earth/actinide elements), based on elastic neutron scattering, we observed an incommensurate magnetic propagation vector τ = (0,0,τz), where τz = 0.5385 is in the reciprocal lattice unit. Additionally, we constructed a precise magnetic phase diagram for YbBe13. We observed non-trivial magnetic anomalies in YbBe13, which cannot be understood based on a simple helical order. Our results for YbBe13 provide an opportunity to reconsider the electron state of UBe13 and present an important step toward a comprehensive understanding of magnetic correlations in MBe13 series.

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Modulation vector of the Fulde-Ferrell-Larkin-Ovchinnikov state in CeCoIn5 revealed by high-resolution magnetostriction measurements

The Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) state is an exotic superconducting phase formed by Cooper pairs with finite center-of-mass momentum $q$. On theoretical grounds, the superconducting order parameter in the FFLO state is spatially modulated along the $q$ vector, and the emergence of an associated anisotropy is expected at the phase transition from the Abrikosov state to the FFLO state. Here, we report the results of high-resolution magnetostriction measurements for a single crystal of CeCoIn$_5$ around $B \parallel c$. We find two anomalies in the magnetostriction along the $c$ axis, parallel to the magnetic-field orientation. In sharp contrast, this $B_{\rm K}$ anomaly disappears in the magnetostriction along the $a$-axis direction, perpendicular to the magnetic-field orientation. To explain this uniaxial expansion, we suggest a possibility that the FFLO transition occurs slightly below the upper critical field, and the FFLO modulation vector parallel to the applied magnetic field gives rise to the anisotropic response.

cond-mat.supr-con↗

One-dimensional magnetism in synthetic Pauflerite, $β$-VOSO$_4$

We have synthesized single-crystal samples of $β$-VOSO$_4$ and fully characterized their magnetic properties. Our magnetic susceptibility, high field magnetization and powder inelastic neutron scattering results are in excellent agreement with theoretical expressions for a one-dimensional spin-1/2 Heisenberg chain with an exchange parameter of $3.83(2)$ meV. Ab initio calculations identify the superexchange pathway, revealing that the spin-chain does not run along the expected crystallographic chain $a$ direction but instead between V$^{4+}$O$_{6}$ octahedra that are linked via SO$_{4}$ tetrahedra along the $b$ axis. We do not detect any phase transition to a long-range magnetic order within our experimental conditions, indicating $β$-VOSO$_4$ is very close to an ideal one-dimensional magnetic system.

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Anisotropic field response of specific heat for a ferromagnetic superconductor UCoGe in magnetic fields

Magnetic-field-angle-resolved specific heat and magnetization measurements were conducted on a ferromagnetic superconductor UCoGe with remarkable anisotropic upper critical field $H_{\rm c2}$. Although $H_{\rm c2}$ reaches a high magnetic field ($\sim 20$~T) along the $b$ axis, it is small ($\sim~0.6$~T) when a magnetic field is applied along the magnetic easy $c$-axis. This study indicates that the specific heat is abruptly suppressed when the magnetic field is applied toward the $c$ axis from the $a$ and $b$ axes in the ferromagnetic state. The field response of density of states (DOS) is anisotropic, relative to the $c$ axis, and its angle dependence is slightly singular. The Ising-type magnetic anisotropy of the ferromagnetic state is dominant even in the anisotropic reinforced superconducting state. These facts indicate that the suppression of DOS may closely relate to the superconducting state. We theoretically analyze these findings together with URhGe and UTe$_2$ by highlighting the common and distinctive features among three compounds.

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SmI3: 4f5 honeycomb magnet with spin-orbital entangled Γ7 Kramers doublet

We report magnetic properties of a 4f-honeycomb iodide SmI3 made up of edge-shared network of SmI6 octahedra. High temperature magnetic susceptibility indicates Γ7 Kramers doublet ground state of Sm3+ (4f5) ions stabilized by the spin-orbit coupling and octahedral crystal electric field, which interact with Sm-I-Sm bond angle nearly 90 degree. Magnetization measurements down to 0.1 K detected antiferromagnetic correlations and an anomaly in the magnetization curve before saturation without a sign of long-range order. Relevance between SmI3 and the antiferromagnetic Kitaev material proposed in the 4f-electron system is discussed.

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Field-angle-resolved landscape of non-Fermi-liquid behavior in the quasi-kagome Kondo Lattice CeRhSn

We have employed a magnetic field angle as a tuning parameter in a comprehensive measurement of the specific heat, magnetocaloric effect, and magnetization for the quasi-kagome Kondo lattice CeRhSn, which is considered to exhibit zero-field quantum criticality driven by geometrical frustration. By constructing the field-angle-resolved landscape of the entropy, we unexpectedly revealed that the non-Fermi-liquid nature survives up to a metamagnetic crossover field of roughly 3 T in the very narrow field-orientation range, close to the direction parallel to the quasi-kagome plane. We propose that spin fluctuations along the hexagonal $c$ axis are the dominant driving force for the non-Fermi-liquid behavior because it is strongly suppressed by a magnetic-field component along the $c$ axis. The multidimensional entropy landscape, which directly reflects the degeneracy of ground states, opens a new route for uncovering the nature of exotic phases in anisotropic systems.

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Thermal Hall Effects of Spins and Phonons in Kagome Antiferromagnet Cd-Kapellasite

We have investigated the thermal-transport properties of the kagome antiferromagnet Cd-kapellasite (Cd-K). We find that a field suppression effect on the longitudinal thermal conductivity k_xx sets in below ~25 K, suggesting a large spin contribution k_xx^sp in k_xx. We also find clear thermal Hall signals in the spin liquid phase in all Cd-K samples. The magnitude of the thermal Hall conductivity k_xy shows a significant dependence on the sample's scattering time. On the other hand, the temperature dependence of k_xy is similar in all Cd-K samples; k_xy shows a peak at almost the same temperature of the peak of the phonon thermal conductivity k_xy^ph which is estimated by k_xx at 15 T. These results indicate the presence of a dominant phonon thermal Hall k_xy^ph at 15 T. In addition to k_xy^ph, we find that the field dependence of k_xy at low fields turns out to be non-linear at low temperatures, concomitantly with the appearance of the field suppression of k_xx, indicating the presence of a spin thermal Hall k_xy^sp at low fields. Remarkably, by assembling the k_xx dependene of k_xy^sp data of other kagome antiferromagnets, we find that, whereas k_xy^sp stays a constant in the low-k_xx region, k_xy^sp starts to increase as k_xx does in the high-k_xx region. This k_xx dependence of k_xy^sp indicates the presence of both intrinsic and extrinsic mechanisms in the spin thermal Hall effect in kagome antiferromagnets. Furthermore, both k_xy^ph and k_xy^sp disappear in the antiferromagnetic ordered phase at low fields, showing that phonons alone do not exhibit the thermal Hall effect. A high field above ~7 T induces k_xy^ph, concomitantly with a field-induced increase of k_xx and the specific heat, suggesting a coupling of the phonons to the field-induced spin excitations as the origin of k_xy^ph.

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Fully gapped superconductivity without sign reversal in the topological superconductor PbTaSe$_2$

We investigate the superconducting gap function of topological superconductor PbTaSe$_2$. Temperature, magnetic field, and three-dimensional (3D) field-angle dependences of the specific heat prove that the superconductivity of PbTaSe$_2$ is fully-gapped, with two isotropic $s$-wave gaps. The pair-breaking effect is probed by systematically increasing non-magnetic disorders through H$^+$-irradiations. The superconducting transition temperature, $T_{\rm{c}}$, is found to be robust against disorders, which suggests that the pairing should be sign-preserved rather than sign-reversed.

cond-mat.supr-con↗

Orientation of point nodes and nonunitary triplet pairing tuned by the easy-axis magnetization in UTe2

The gap structure of a novel uranium-based superconductor UTe$_2$, situated in the vicinity of ferromagnetic quantum criticality, has been investigated via specific-heat $C(T,H,Ω)$ measurements in various field orientations. Its angular $Ω(ϕ,θ)$ variation shows a characteristic shoulder anomaly with a local minimum in $H \parallel a$ at moderate fields rotated within the $ab$ and $ac$ planes. Based on the theoretical calculations, these features can be attributed to the presence of point nodes in the superconducting gap along the $a$ direction. Under the field orientation along the easy-magnetization $a$ axis, an unusual temperature dependence of the upper critical field at low fields together with a convex downward curvature in $C(H)$ were observed. These anomalous behaviors can be explained on the basis of a nonunitary triplet state model with equal-spin pairing whose $T_{\rm c}$ is tuned by the magnetization along the $a$ axis. From these results, the gap symmetry of UTe$_2$ is most likely described by a vector order parameter of $d(k)=(b + ic)(k_b + ik_c)$.

cond-mat.supr-con↗

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.

cond-mat.str-el↗

Field-Orientation Effect on Ferro-Quadrupole Order in PrTi2Al20

Ferro-quadrupole (FQ) order in the non-Kramers $Γ_3$ doublet system PrTi$_2$Al$_{20}$ has been investigated via angle-resolved measurements of the specific heat, rotational magnetocaloric effect, and entropy, under a rotating magnetic field within the $(1\bar{1}0)$ plane. The FQ transition occurring at 2 K is robust when the magnetic field $B$ is applied precisely along the $[111]$ direction. By contrast, the magnetic field of larger than 1 T tilted away from the $[111]$ direction sensitively changes the FQ transition to a crossover. The energy gap between the ground and first-excited states in the FQ order increases remarkably with the magnetic field in $B \parallel [001]$, but hardly depends on the magnetic-field strength, at least up to 5 T, in the field orientation between the $[111]$ and $[110]$ axes. These features can be reproduced by using a phenomenological model for FQ order assuming an anisotropic field-dependent interaction between quadrupoles, which has been recently proposed to explain the field-induced first-order phase transition in PrTi$_2$Al$_{20}$. The present study demonstrates the great potential of the field-angle-resolved measurements for evaluating possible scenarios for multipole orders.

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$^{105}$Pd NMR and NQR study of the cubic heavy fermion system Ce$_3$Pd$_{20}$Si$_6$

We report $^{105}$Pd NMR and NQR measurements on a single crystal of Ce$_3$Pd$_{20}$Si$_6$, where antiferroquadrupolar and antiferromagnetic orders develop at low temperature. From the analysis of NQR and NMR spectra, we have determined the electric field gradient (EFG) tensors and the anisotropic Knight shift ($K$) components for both inequivalent Pd sites - Pd($32f$) and Pd($48h$). The observed EFG values are in excellent agreement with our state-of-the-art DFT calculations. The principal values of the quadrupolar coupling are $(20.37 \pm 0.02)$ MHz and $(5.45 \pm 0.02)$ MHz, for the Pd($32f$) and Pd($48h$) site, respectively, which is large compared to the Larmor frequency defined by the gyromagnetic constant $γ= 1.94838$ MHz/T for $^{105}$Pd. Therefore, the complete knowledge of $K$ and the EFG tensors is crucial to establish the correspondence between NMR spectra and crystallographic sites, which is needed for a complete analysis of the magnetic structure, static spin susceptibility, and the spin-lattice relaxation rate data and a better understanding of the groundstate of Ce$_3$Pd$_{20}$Si$_6$.

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