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K. Kindo

Publications and source records attributed to K. Kindo.

At least 19 recordsLinked to original sources

High-field fate of the Kitaev quantum spin liquid in $\alpha$-RuCl$_3$

Kitaev quantum spin liquids (KQSLs) host fractionalized excitations described by itinerant Majorana quasiparticles and gapped $Z_2$ fluxes (visons), providing a platform for emergent topological matter. Whether such a state survives under strong magnetic fields, however, remains an open question. The layered honeycomb magnet $\alpha$-RuCl$_3$ is a leading candidate material: an in-plane field of $\sim$ 7 T suppresses antiferromagnetic order and induces a quantum-disordered phase exhibiting signatures consistent with Majorana excitations, including an anomalous thermal Hall effect and field-angle-dependent specific heat. At higher fields, the magnetization approaches saturation, suggesting a transition to a spin-polarized state, yet the microscopic evolution between these limits remains unresolved. Here we report high-field specific heat measurements up to 24 T that reveal a distinct crossover at $\mu_0H^*\approx$15 T, beyond which the perturbative Kitaev description breaks down. Above $H^*$, the characteristic six-fold angular modulation of the specific heat collapses and the excitation gap deviates from the predicted $H^3$ scaling. Meanwhile, the gap decreases with increasing field and the in-plane magnetization anisotropy persists up to $\sim$ 24 T, both in sharp contrast to a trivial spin-polarized state, indicating that KQSL signatures are preserved even at $\sim$ 90 % of magnetization saturation. These results reveal that the KQSL in $\alpha$-RuCl$_3$ extends well beyond the perturbative window, persisting as a nonperturbative regime in which the Majorana and vison energy scales merge, before eventually giving way to spin polarization. This thermodynamic roadmap provides a basis for understanding how fractionalized phases evolve under strong magnetic fields.

cond-mat.str-el

Pressure-Tuned Metamagnetism and Emergent Three-Body Interactions in CsFeCl$_3$

We present a combined experimental and theoretical study of the triangular-lattice quantum antiferromagnet CsFeCl$_3$ under high magnetic fields and high pressure. Pulsed-field magnetization for the magnetic field along the symmetric $c$ direction at ambient pressure reveals a magnetization process from a nonmagnetic singlet ground state with a nearly linear increase between 3.7 and 10.7 T, a plateau-like region, and then a sharp stepwise metamagnetic transition near 32 T. Wide frequency--field range electron spin resonance indicates that the low-field regime originates from the $J = 1$ manifold, while the high-field metamagnetic transition suggests a level crossing between the $J = 1$ and $J = 2$ lowest states. Pulsed-field magnetic susceptibilities measured with a proximity detector oscillator under high pressure show that the low-field nonmagnetic singlet phase is gradually suppressed, while the high-field metamagnetic transition evolves into an increasingly rich pattern of fractional steps. While the observations at low to intermediate fields can be understood within the established spin-1 description, the high-field regime requires a new perspective, which we provide through a projected spin-1/2 framework built from Zeeman-selected crystal-field states not related by time reversal. This construction naturally allows emergent three-body interactions on triangular plaquettes and explains the asymmetric evolution of the fractional steps in the magnetization. Our findings reveal that high-field effective spin models in quantum magnets with separated yet accessible crystal-field multiplets are not constrained to even-body couplings, but can naturally host odd-body terms, opening a broader avenue for realizing field-asymmetric magnetization processes and exotic phases beyond conventional even-body physics.

cond-mat.mtrl-sci

High-field NMR study of field-induced states in Pb(TiO)Cu$_4$(PO$_4$)$_4$

The square cupola antiferromagnet Pb(TiO)Cu$_4$(PO$_4$)$_4$ exhibits the intriguing magnetoelectric responses arising from the consecutive change in the magnetic quadrupolar-type configuration of magnetic moments under external magnetic fields higher than 15 T. To clarify the high-field magnetic structures in Pb(TiO)Cu$_4$(PO$_4$)$_4$, an NMR measurement was performed in pulsed fields up to 32.2 T significantly extending the field range accessible by superconducting magnets. The double-peak structure of NMR spectra emerging above 29 T applied along the [001] direction evidences the successive magnetic transitions. The field dependence of NMR spectra was analyzed on the basis of cluster mean-field theory, which allows us to propose possible magnetic structures for the high-field magnetic states.

cond-mat.str-el

Evidence of random spin-singlet state in a three-dimensional quantum spin liquid candidate Sr$_3$CuNb$_2$O$_9$

Disorder is ubiquitous in any quantum many-body system and is usually considered to be an obstacle to the elucidation of the underlying physics of complex systems, but its presence can often introduce exotic phases of matter that cannot generally be realized in a clean system. We report here a detailed experimental and theoretical study of magnetic properties of highly disordered Sr$_3$CuNb$_2$O$_9$ material which exhibits random site mixing between Cu and Nb. The magnetic moments (Cu$^{2+}$) are arranged in a quasi-cubic (three-dimensional) manner, leading to a high degree of frustration with a Curie-Weiss temperature ($\theta_{CW}$) of about -60 K without any long-range magnetic ordering down to 466 mK. These observations suggest that Sr$_3$CuNb$_2$O$_9$ is a candidate for a quantum spin liquid. More interestingly, the susceptibility ($\chi = M/\mu_0H$) and the $C_m/T$ ($C_m$ is the magnetic part of the heat capacity) follow a power-law behavior with decreasing temperature. In addition, $M(T,\mu_0H)$ and $C_m(T,\mu_0H)/T$ show scaling relationships over a wide temperature and field range. This unusual behavior with respect to the conventional behavior of a QSL can be discussed qualitatively as the coexistence of a disorder-induced random spin singlet (RSS) state and a QSL state. A quantitative description has been given by numerical calculations considering a power-law probability distribution $P(J) \propto J^{-\gamma}$ ($J$ is the exchange interaction) of random spin singlets. The parameters extracted from the numerical calculations are in excellent agreement with the experimental data. Furthermore, the analytical results are also consistent with the power-law and scaling behavior of $\chi$ and $C_m(T,\mu_0H)/T$ as a whole. Thus, our comprehensive experimental and theoretical analysis provides evidence for the stabilization of the RSS state in a three-dimensional lattice.

cond-mat.str-el

Emergent topological magnetism in Hund's excitonic insulator

Analogous to the charged electron-electron pair condensation in superconductors, an excitonic insulator (EI) represents Fermi surface instability due to spontaneous formation and condensation of charge-neutral electron-hole pair (exciton). Unlike in superconductors, however, the charge-neutral nature of exciton makes probing emergent EI phase via macroscopic physical properties generally difficult. Here, we propose a van der Waals coupled antiferromagnetic semiconductor GdGaI (GGI) as a new material category leading to emergent multi-q magnet intertwined with spontaneous exciton formation/condensation. Before excitonic band hybridization, a simple picture for the parent electronic state consists of electron (Gd-derived 5d) and hole (Ga-derived 4p) delocalized bands, together with Gd-derived 4f localized antiferromagnets with S = 7/2 classical nature. Through intra Gd atom 4f-5d Hund's coupling, a notable finding is the emergent minimum length scale (2a) Skyrmion-like spin texture resulting from spontaneous condensation/formation of spin-polarized exciton with BCS-BEC crossover phenomenology. This discovered platform is promising for realizing valuable quantum matter on the nanoscale; our finding will provide significant insight into designing the atomic scale topological magnetism out of itinerant systems.

cond-mat.str-el

Rhenium oxyhalides: a showcase for anisotropic-triangular-lattice quantum antiferromagnets

The spin-1/2 Heisenberg antiferromagnet on an anisotropic triangular lattice (ATL) is an archetypal spin system hosting exotic quantum magnetism and dimensional crossover. However, the progress in experimental research on this field has been limited due to the scarcity of ideal model materials. Here, we show that rhenium oxyhalides $A_{3}$ReO$_{5}X_{2}$, where spin-1/2 Re$^{6+}$ ions form a layered structure of ATLs, allow for flexible chemical substitution in both cation $A^{2+}$ ($A$ = Ca, Sr, Ba, Pb) and anion $X^{-}$ ($X$ = Cl, Br) sites, leading to seven synthesizable compounds. By combining magnetic susceptibility and high-field magnetization measurements with theoretical calculations using the orthogonalized finite-temperature Lanczos method, we find that the anisotropy $J'/J$ ranges from 0.25 to 0.45 depending on the chemical composition. Our findings demonstrate that $A_{3}$ReO$_{5}X_{2}$ is an excellent platform for realizing diverse effective spin Hamiltonians that differ in the strength of the anisotropy $J'/J$ as well as the relevance of perturbation terms such as the Dzyaloshinskii-Moriya interaction and interlayer exchange coupling.

cond-mat.mtrl-sci

Breathing pyrochlore magnet CuGaCr$_{4}$S$_{8}$: Magnetic, thermodynamic, and dielectric properties

We investigate the crystallographic and magnetic properties of a chromium-based thiospinel CuGaCr$_{4}$S$_{8}$. From a synchrotron x-ray diffraction experiment and structural refinement, Cu and Ga atoms are found to occupy the tetrahedral $A$-sites in an alternate way, yielding breathing pyrochlore Cr network. CuGaCr$_{4}$S$_{8}$ undergoes a magnetic transition associated with a structural distortion at 31 K in zero magnetic field, indicating that the spin-lattice coupling is responsible for relieving the geometrical frustration. When applying a pulsed high magnetic field, a sharp metamagnetic transition takes place at 40 T, followed by a 1/2-magnetization plateau up to 103 T. These phase transitions accompany dielectric anomalies, suggesting the presence of helical spin correlations in low-field phases. The density-functional-theory calculation reveals that CuGaCr$_{4}$S$_{8}$ is dominated by antiferromagnetic and ferromagnetic exchange couplings within small and large tetrahedra, respectively, in analogy with CuInCr$_{4}$S$_{8}$. We argue that $A$-site-ordered Cr thiospinels serve as an excellent platform to explore diverse magnetic phases along with pronounced magnetoelastic and magnetodielectric responses.

cond-mat.mtrl-sci

Signatures of a magnetic superstructure phase induced by ultrahigh magnetic fields in a breathing pyrochlore antiferromagnet

The mutual coupling of spin and lattice degrees of freedom is ubiquitous in magnetic materials and potentially creates exotic magnetic states in response to the external magnetic field. Particularly, geometrically frustrated magnets serve as a fertile playground for realizing magnetic superstructure phases. Here, we observe an unconventional two-step magnetostructural transition prior to a half-magnetization plateau in a breathing pyrochlore chromium spinel by means of state-of-the-art magnetization and magnetostriction measurements in ultrahigh magnetic fields available up to 600 T. Considering a microscopic magnetoelastic theory, the intermediate-field phase can be assigned to a magnetic superstructure with a three-dimensional periodic array of 3-up-1-down and canted 2-up-2-down spin molecules. We attribute the emergence of the magnetic superstructure to a unique combination of the strong spin-lattice coupling and large breathing anisotropy.

cond-mat.mtrl-sci

Observation of field-induced single-ion magnetic anisotropy in a multiorbital Kondo alloy $\mathrm{(Lu,Yb)}\mathrm{Rh}_{2}\mathrm{Zn}_{20}$

We demonstrate field-induced single-ion magnetic anisotropy resulting from the multiorbital Kondo effect on the diluted ytterbium alloy $(\mathrm{Lu}_{1-x}\mathrm{Yb}_x)\mathrm{Rh}_2\mathrm{Zn}_{20}$. Single-ion anisotropic metamagnetic behavior is revealed in low-temperature regions where the local Fermi-liquid state is formed. Specific hea, low-field magnetic susceptibility, and resistivity indicate reproduction of the ground-state properties by the $\mathrm{SU}(N = 8)$ Kondo model with a relatively large $c$-$f$ hybridization of $T_{\mathrm{K}} = 60.9 \ \mathrm{K}$. Dynamical susceptibility measurements on $\mathrm{Yb}\mathrm{Rh}_2\mathrm{Zn}_{20}$ support realizing the multiorbital Kondo ground state in $(\mathrm{Lu}_{1-x}\mathrm{Yb}_x)\mathrm{Rh}_2\mathrm{Zn}_{20}$. The single-ion magnetic anisotropy becomes evident above $\sim5 \ \mathrm{T}$, which is lower than the isotropic Kondo crossover field of 22.7 T, verifying blurred low-lying crystal field states through the multiorbital Kondo effect.

cond-mat.str-el

Quantum oscillations in a centrosymmetric skyrmion-hosting magnet GdRu2Si2

We have performed magnetic torque and resistivity measurements on a centrosymmetric skyrmion-host GdRu2Si2, in which the dominant magnetic interaction leading to skyrmion formation is under debate. We observe both the de Haas-van Alphen and Shubnikov-de Haas oscillations in the forced ferromagnetic phase. The angular dependence of the quantum oscillation frequencies can be reproduced by the ab-initio calculation. The de Haas-van Alphen oscillation is also observed in the double-Q phase with a different frequency to that in the forced ferromagnetic phase, indicating a Fermi surface reconstruction due to the coupling between localized spins and conduction electrons. Based on these experimental findings, the magnetic interactions in this system are discussed.

cond-mat.str-el

Dimensional reduction and incommensurate dynamic correlations in the $S=\frac{1}{2}$ triangular-lattice antiferromagnet Ca$_3$ReO$_5$Cl$_2$

The observation of spinon excitations in the $S=\frac{1}{2}$ triangular antiferromagnet Ca$_3$ReO$_5$Cl$_2$ reveals a quasi-one-dimensional (1D) nature of magnetic correlations, in spite of the nominally 2D magnetic structure. This phenomenon is known as frustration-induced dimensional reduction. Here, we present high-field electron spin resonance spectroscopy and magnetization studies of Ca$_3$ReO$_5$Cl$_2$, allowing us not only to refine spin-Hamiltonian parameters, but also to investigate peculiarities of its low-energy spin dynamics. We argue that the presence of the uniform Dzyaloshinskii-Moriya interaction (DMI) shifts the spinon continuum in momentum space and, as a result, opens a zero-field gap at the $\Gamma$ point. We observed this gap directly. The shift is found to be consistent with the structural modulation in the ordered state, suggesting this material as a perfect model triangular-lattice system, where a pure DMI-spiral ground state can be realized.

cond-mat.str-el

Magnetic-field and pressure phase diagram of the triangular lattice antiferromagnet CsCuCl$_3$ clarified by magnetic susceptibility measured with a proximity detector oscillator

The effect of pressure ($P$) on magnetic susceptibility of CsCuCl$_3$ was examined in magnetic fields ($\rm \mu_0$$H$) of up to 51 T using a proximity detector oscillator (PDO), and the $H$-$P$ phase diagram of CsCuCl$_3$ was constructed over the saturation field ($H_{\rm sat}$). We found that, with increasing $P$, $H_{\rm sat}$ increases and the uud-phase that appeared at $P$ = 0.7 GPa widened. Based on comparison between the experimental and calculated $H$-$P$ phase diagrams, the Y-phase was predicted to appear above 1.7 GPa. The interchain antiferromagnetic exchange interaction in the $ab$-plane was evaluated and found to increase with increasing $P$, which is consistent with a previous study under high pressure [D. Yamamoto {\it et al.}, Nat. Commun. {\bf 12}, 4263 (2021).]. Moreover, an anomaly was observed below $P$ = 0.6 GPa just below $H_{\rm sat}$ and might be a new phase transition derived from nonlinear response caused by the PDO technique.

cond-mat.mtrl-sci

Enhanced superconducting pairing strength near a nonmagnetic nematic quantum critical point

The quest for high-temperature superconductivity at ambient pressure is a central issue in physics. In this regard, the relationship between unconventional superconductivity and the quantum critical point (QCP) associated with the suppression of some form of symmetry-breaking order to zero temperature has received particular attention. The key question is how the strength of the electron pairs changes near the QCP, and this can be verified by high-field experiments. However, such studies are limited mainly to superconductors with magnetic QCPs, and the possibility of unconventional mechanisms by which nonmagnetic QCP promotes strong pairing remains a nontrivial issue. Here, we report systematic measurements of the upper critical field $H_{{\rm c2}}$ in nonmagnetic FeSe$_{1-x}$Te$_{x}$ superconductors, which exhibit a QCP of electronic nematicity characterized by spontaneous rotational-symmetry breaking. As the magnetic field increases, the superconducting phase of FeSe$_{1-x}$Te$_{x}$ shrinks to a narrower dome surrounding the nematic QCP. The analysis of $H_{{\rm c2}}$ reveals that the Pauli-limiting field is enhanced toward the QCP, implying that the pairing interaction is significantly strengthened via nematic fluctuations emanated from the QCP. Remarkably, this nonmagnetic nematic QCP is not accompanied by a divergent effective mass, distinct from the magnetically mediated pairing. Our observation opens up a nonmagnetic route to high-temperature superconductivity.

cond-mat.supr-con

Complex magnetic phase diagram with a small phase pocket in a three-dimensional frustrated magnet CuInCr$_{4}$S$_{8}$

Frustrated magnets with a strong spin-lattice coupling can show rich magnetic phases and the associated fascinating phenomena. A promising platform is the breathing pyrochlore magnet CuInCr$_{4}$S$_{8}$ with localized $S=3/2$ Cr$^{3+}$ ions, which is proposed to be effectively viewed as an $S=6$ Heisenberg antiferromagnet on the face-centered-cubic lattice. Here, we unveil that CuInCr$_{4}$S$_{8}$ exhibits a complex magnetic phase diagram with a small phase pocket ($A$ phase) by means of magnetization, magnetostriction, magnetocapacitance, and magnetocaloric-effect measurements in pulsed high magnetic fields of up to 60 T. Remarkably, the appearance of $A$ phase is accompanied by anomalous magnetostrictive and magnetocapacitive responses, suggesting the emergence of helimagnetism in contrast to the neighboring commensurate magnetic phases. Besides, the high-entropy nature is confirmed in the high-temperature side of $A$ phase. These features are potentially related to a thermal fluctuation-driven multiple-$q$ state caused by the magnetic frustration, which has been theoretically predicted but yet experimentally undiscovered.

cond-mat.str-el

Gradual charge order melting in Bi0.5Ca0.5MnO3 induced by ultrahigh magnetic field

We have investigated the magnetic properties of Bi0.5Ca0.5MnO3 under ultrahigh magnetic fields by magnetization measurements. This compound shows the metamagnetic transition which indicates the magnetic field induced charge order melting at the room temperature T = 293 K. We reveled that the temperature dependence of the critical field, where the highest critical field is higher than 100 T. At low temperatures, it has been found that the metamagnetic transitions become broad and vanish in the field ascending process below 70 K. On the other hand, in the field descending process, a clear metamagnetic transition is observed even below 70 K. This unusual behavior can be understood as the gradual charge order melting by magnetic field, and its simultaneous reformation. A coexistence of multiple order parameters can account for the observed characteristic dynamics of the first order phase transition. Finally, we constructed the B-T phase diagram with the unusual critical feature at ultrahigh magnetic fields.

cond-mat.str-el

Physical properties of liquid oxygen under ultrahigh magnetic fields

We studied the acoustic properties of liquid oxygen up to 90 T by means of ultrasound measurements. We observed a monotonic decrease of the sound velocity and an asymptotic increase of the sound attenuation when applying magnetic fields. The unusual attenuation, twenty times as large as the zero-field value, suggests strong fluctuations of the local molecular arrangement. We point out that the observed fluctuations are related to a liquid-liquid transition or crossover, from a small-magnetization to a large-magnetization liquid, which is characterized by a local-structure rearrangement. To investigate higher-field properties of liquid oxygen, we performed single-turn-coil experiments up to 180 T by means of the acoustic, dilatometric, magnetic, and optical techniques. We observed only monotonic changes of these properties, reflecting the absence of the proposed liquid-liquid transition in our experimental conditions.

cond-mat.soft

Normal state specific heat in the cuprates La$_{2-x}$Sr$_x$CuO$_4$ and Bi$_{2+y}$Sr$_{2-x-y}$La$_x$CuO$_{6+\delta}$ near the critical point of the pseudogap phase

The specific heat $C$ of the cuprate superconductors La$_{2-x}$Sr$_x$CuO$_4$ and Bi$_{2+y}$Sr$_{2-x-y}$La$_x$CuO$_{6+\delta}$ was measured at low temperature (down to $0.5~{\rm K}$), for dopings $p$ close to $p^\star$, the critical doping for the onset of the pseudogap phase. A magnetic field up to $35~{\rm T}$ was applied to suppress superconductivity, giving direct access to the normal state at low temperature, and enabling a determination of $C_e$, the electronic contribution to the normal-state specific heat, at $T \to 0$. In La$_{2-x}$Sr$_x$CuO$_4$ at $x=p = 0.22$, $0.24$ and $0.25$, $C_e / T = 15-16~{\rm mJmol}^{-1}{\rm K}^{-2}$ at $T = 2~{\rm K}$, values that are twice as large as those measured at higher doping ($p > 0.3$) and lower doping ($p < 0.15$). This confirms the presence of a broad peak in the doping dependence of $C_e$ at $p^\star\simeq 0.19$, as previously reported for samples in which superconductivity was destroyed by Zn impurities. Moreover, at those three dopings, we find a logarithmic growth as $T \to 0$, such that $C_e / T \sim {\rm B}\ln(T_0/T)$. The peak vs $p$ and the logarithmic dependence vs $T$ are the two typical thermodynamic signatures of quantum criticality. In the very different cuprate Bi$_{2+y}$Sr$_{2-x-y}$La$_x$CuO$_{6+\delta}$, we again find that $C_e / T \sim {\rm B}\ln(T_0/T$) at $p \simeq p^\star$, strong evidence that this $\ln(1/T)$ dependence - first discovered in the cuprates La$_{1.8-x}$Eu$_{0.2}$Sr$_x$CuO$_4$ and La$_{1.6-x}$Nd$_{0.4}$Sr$_x$CuO$_4$ - is a universal property of the pseudogap critical point. All four materials display similar values of the $\rm B$ coefficient, indicating that they all belong to the same universality class.

cond-mat.supr-con

Magnetic structure and high-field magnetization of the distorted kagome lattice antiferromagnet Cs$_2$Cu$_3$SnF$_{12}$

High-resolution time-of-flight powder neutron diffraction and high-field magnetization were measured to investigate the magnetic structure and existence of a field-induced magnetic phase transition in the distorted kagome antiferromagnet Cs$_2$Cu$_3$SnF$_{12}$. Upon cooling from room temperature, the compound undergoes a structural phase transition at $T_\textrm{t}=185$ K from the rhombohedral space group $R\bar{3}m$ with the perfect kagome spin network to the monoclinic space group $P2_1/n$ with the distorted kagome planes. The distortion results in three inequivalent exchange interactions among the $S=1/2$ Cu$^{2+}$ spins that magnetically order below $T_\textrm{N}=20.2$ K. Magnetization measured with a magnetic field applied within the kagome plane reveals small in-plane ferromagnetism resulting from spin canting. On the other hand, the out-of-plane magnetization does not show a clear hysteresis loop of the ferromagnetic component nor a prominent anomaly up to 170 T, with the exception of the subtle knee-like bend around 90 T, which could indicate the 1/3 magnetization plateau. The combined analysis using the irreducible representations of the magnetic space groups and magnetic structure refinement on the neutron powder diffraction data suggests that the magnetic moments order in the magnetic space group $P2_1'/n'$ with the all-in-all-out spin structure, which by symmetry allows for the in-plane canting, consistent with the in-plane ferromagnetism observed in the magnetization.

cond-mat.str-el