arXiv subjects

Masashi Takigawa

Publications and source records attributed to Masashi Takigawa.

At least 19 recordsLinked to original sources

arXiv2026

Pinwheel-shaped bound triplet pairs in the magnetization plateaus of SrCu$_2$(BO$_3$)$_2$

The sequence of magnetization plateaus at 1/8, 2/15, 1/6, 1/4, 1/3, 2/5, and 1/2 of the saturation observed in SrCu$_2$(BO$_3$)$_2$ remained a puzzle until tensor-networks-based numerical simulations suggested that the low-magnetization plateaus are stabilized as Wigner crystals of spin-2 bound states, and not as one of the standard configurations (semiclassical up-down, or crystals of triplets). We report on $^{63,65}$Cu nuclear magnetic resonance spectra up to 41.9 T: Based on constraints deduced from the 1/3 plateau, we show that the spectra in the 1/8 and 2/15 plateaus indeed agree with the prediction for the spin-2 bound states, while being incompatible with a crystal of triplets. This adds the formation of Wigner crystals of bound states as an alternative fundamental paradigm in the theory of magnetization plateaus.

cond-mat.str-el↗

arXiv2024

Properties of an organic model $S=1$ Haldane chain system

We present the properties of a new organic $S=1$ antiferromagnetic chain system $m$-NO$_2$PhBNO (abbreviated BoNO). In this biradical system two unpaired electrons from aminoxyl groups are strongly ferromagnetically coupled ($|J_\text{FM}| /k_B \gtrsim 500$ K) which leads to the formation of an effective $S=1$ state for each molecule. The chains of BoNO biradicals propagate along the crystallographic $a$ axis. Temperature dependence of the $g$ factor and electron paramagnetic resonance (EPR) linewidth are consistent with a low-dimensional system with antiferromagnetic interactions. The EPR data further suggest that BoNO is the first known Haldane system with an almost isotropic $g$ factor ($2.0023 \pm 2 \unicode{x2030}$). The magnetization measurements in magnetic fields up to $40$ T and low-field susceptibility, together with $^1$H nuclear magnetic resonance (NMR) spectra, reveal a dominant intrachain antiferromagnetic exchange coupling of $J_\text{1D}/k_B = (11.3\pm0.1)$ K, and attainable critical magnetic fields of $μ_0 H_\text{c1} \approx 2$ T and $μ_0 H_\text{c2} \approx 33$ T. These measurements therefore suggest that BoNO is a unique Haldane system with extremely small magnetic anisotropy. Present results are crucial for a future in-depth NMR study of the low-temperature Tomonaga-Luttinger liquid (TLL) and magnetic field-induced phases, which can be performed in the entire phase space.

cond-mat.str-el↗

arXiv2024

Magnetic structure of polar magnet GaV$_4$Se$_8$ with Néel-type skyrmion lattice probed by $^{51}$V NMR

We report the magnetization and the $^{51}$V NMR measurements in the polar magnet GaV$_4$Se$_8$ in which a magnetic skyrmion lattice appears in the structural domain with the polar axis parallel to the magnetic field. Although we successfully separate the $^{51}$V NMR signals in the domain from those in the other structural domains, only the high-frequency region of NMR spectrum is observed due to a significant increase of the spin-echo decay rate in the low-frequency region. In $B_{\rm{ext}}\parallel[111]$, we find the NMR signals from the supermagnetized cycloidal state in the parallel domains as well as from the conical state in domains where the polar axis is tilted from the magnetic field. No NMR signal from the skyrmion lattice state is observed, suggesting a significant increase of the decay rate by additional low-energy excitations caused by dynamics of the skyrmions. In $B_{\rm{ext}}\parallel[001]$, where all the structural domains are magnetically equivalent, multiple NMR peaks converge into one peak at the saturation magnetic field. This field dependence is explained by the closing of magnetic cones as approaching the forced-ferromagnetic state.

cond-mat.str-el↗

arXiv2023

Extremely Large Magnetoresistance and Anisotropic Transport in Multipolar Kondo System PrTi$_{2}$Al$_{20}$

Multipolar Kondo systems offer unprecedented opportunities for designing astonishing quantum phases and functionalities beyond spin-only descriptions. A model material platform of this kind is the cubic heavy-fermion system Pr$Tr_{2}$Al$_{20}$ ($Tr=$ Ti, V), which hosts a nonmagnetic crystal-electric-field (CEF) ground state and substantial Kondo entanglement of the local quadrupolar and octopolar moments with the conduction electron sea. Here, we explore magnetoresistance (MR) and Hall effect of PrTi$_{2}$Al$_{20}$ that develops ferroquadrupolar (FQ) order below $T_{Q} \sim 2$ K and compare its behavior with that of the non-4$f$ analog, LaTi$_{2}$Al$_{20}$. In the FQ ordered phase, PrTi$_{2}$Al$_{20}$ displays extremely large magnetoresistance (XMR) of $\sim 10^{3}\%$. The unsaturated, quasi-linear field ($B$) dependence of the XMR violates the conventional Kohler's scaling and defies description based on carrier compensation alone. By comparing the MR and the Hall effect observed in PrTi$_{2}$Al$_{20}$ and LaTi$_{2}$Al$_{20}$, we conclude that the open-orbit topology on the electron-type Fermi surface (FS) sheet is key for the observed XMR. The low-temperature MR and the Hall resistivity in PrTi$_{2}$Al$_{20}$ display pronounced anisotropy in the [111] and [001] magnetic fields, which is absent in LaTi$_{2}$Al$_{20}$, suggesting that the transport anisotropy ties in with the anisotropic magnetic-field response of the quadrupolar order parameter.

cond-mat.str-el↗

arXiv2023

Inelastic Neutron Scattering Study of the Spin Dynamics in the Breathing Pyrochlore System LiGa0.95In0.05Cr4O8

The A-site ordered chromate spinels LiGa1-xInxCr4O8 host a network of size-alternating spin-3/2 Cr3+ tetrahedra known as a 'breathing' pyrochlore lattice. For the x=0.05 composition, the complex magneto-structural ordering observed in the parent x=0 material is replaced by a single transition at Tf=11 K, ascribed to the collinear nematic order caused by strong spin-lattice coupling. We present here an inelastic neutron scattering study of the spin dynamics in this composition. Above Tf , the dynamical scattering function S(Q,E) is ungapped and quasi-elastic, similar to undoped LiGaCr4O8. Below Tf , the spectral weight splits between a broad inelastic feature at 5.8 meV and toward the elastic line. The former feature can be ascribed to spin precessions within antiferromagnetic loops, lifted to finite energy by the effective biquadratic spin-lattice term in the spin Hamiltonian.

cond-mat.str-el↗

arXiv2021

Magnetic field-driven transition between valence bond solid and antiferromagnetic order in distorted triangular lattice

A molecular Mott insulator $κ$-(ET)$_2$B(CN)$_4$ [ET = bis(ethylenedithio)tetrathiafulvalene] with a distorted triangular lattice exhibits a quantum disordered state with gapped spin excitation in the ground state. $^{13}$C nuclear magnetic resonance, magnetization, and magnetic torque measurements reveal that magnetic field suppresses valence bond order and induces long-range magnetic order above a critical field $\sim 8$ T. The nuclear spin-lattice relaxation rate $1/T_1$ shows persistent evolution of antiferromagnetic correlation above the transition temperature, highlighting a quantum spin liquid state with fractional excitations. The field-induced transition as observed in the spin-Peierls phase suggests that the valence bond order transition is driven through renormalized one-dimensionality and spin-lattice coupling.

cond-mat.str-el↗

arXiv2021

Pressure-induced phase transition in the $J_1$-$J_2$ square lattice antiferromagnet RbMoOPO$_4$Cl

We report results of magnetization and $^{31}$P NMR measurements under high pressure up to 6.4~GPa on RbMoOPO$_4$Cl, which is a frustrated square-lattice antiferromagnet with competing nearest-neighbor and next-nearest-neighbor interactions. Anomalies in the pressure dependences of the NMR shift and the transferred hyperfine coupling constants indicate a structural phase transition at 2.6~GPa, which is likely to break mirror symmetry and triggers significant change of the exchange interactions. In fact, the NMR spectra in magnetically ordered states reveal a change from the columnar antiferromagnetic (CAF) order below 3.3~GPa to the Néel antiferromagnetic (NAF) order above 3.9~GPa. The spin lattice relaxation rate $1/T_1$ also indicates a change of dominant magnetic fluctuations from CAF-type to NAF-type with pressure. Although the NMR spectra in the intermediate pressure region between 3.3 and 3.9 GPa show coexistence of the CAF and NAF phases, a certain component of $1/T_1$ shows paramagnetic behavior with persistent spin fluctuations, leaving possibility for a quantum disordered phase. The easy-plane anisotropy of spin fluctuations with unusual nonmonotonic temperature dependence at ambient pressure gets reversed to the Ising anisotropy at high pressures. This unexpected anisotropic behavior for a spin 1/2 system may be ascribed to the strong spin-orbit coupling of Mo-4$d$ electrons.

cond-mat.str-el↗

arXiv2020

Dynamic Spin Fluctuations in the Frustrated A-site Spinel CuAl2O4

We performed nuclear magnetic resonance (NMR) and muon spin relaxation (μSR) experiments to identify the magnetic ground state of the frustrated quantum A-site spinel, CuAl2O4. Our results verify that the ground state does not exhibit a long-range magnetic ordering, but a glass-like transition manifests at T*=2.3 K. However, the Gaussian shape and the weak longitudinal field dependence of μSR spectra below T* show that the ground state has dynamic spin fluctuations, distinct from those of conventional spin-glasses.

cond-mat.str-el↗

arXiv2020

Regular-Triangle Trimer and Charge Order Preserving the Anderson Condition in the Pyrochlore Structure of CsW$_2$O$_6$

Since the discovery of the Verwey transition in magnetite, transition metal compounds with pyrochlore structures have been intensively studied as a platform for realizing remarkable electronic phase transitions. We report the discovery of a unique phase transition that preserves the cubic symmetry of the beta-pyrochlore oxide CsW$_2$O$_6$, where each of W 5d electrons are confined in regular-triangle W3 trimers. This trimer formation is an unprecedented self-organization of d electrons, which can be resolved into a charge order satisfying the Anderson condition in a nontrivial way, orbital order caused by the distortion of WO6 octahedra, and the formation of a spin-singlet pair in a regular-triangle trimer. Electronic instability due to the unusual three-dimensional nesting of Fermi surfaces and the localized nature of the 5d electrons characteristic of the pyrochlore oxides were found to play important roles in this unique charge-orbital-spin coupled phenomenon.

cond-mat.mtrl-sci↗

arXiv2020

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.

cond-mat.str-el↗

arXiv2019

Field-Induced Switching of Ferro-Quadrupole Order Parameter in PrTi2Al20

We report magnetic-field-induced first-order phase transitions in the ferro-quadrupole (FQ) ordered state of PrTi2Al20, in which non-Kramers Pr3+ ions with two 4f electrons have a non-magnetic Gamma3 doublet ground state in the cubic Td crystalline electric field. For magnetic fields along [111], 27Al-NMR and magnetization experiments reveal Qz \propto 3z2-r2 type FQ order below 2 K independent of field strength. Magnetic fields along [001] or [110], however, induce discontinuous switching of order parameters within the two dimensional space spanned by Qz and Qx \propto x2-y2 at small field values less than a few tesla. A symmetry-based theoretical analysis shows that the transitions can be caused by competition between the magnetic Zeeman interaction and anisotropy in the quadrupole-quadrupole interactions, if the latter dominates over the former in low fields and vice versa in high fields. Furthermore, striking violation of proportionality between NMR Knight shift and magnetic susceptibility is observed in the symmetry-broken FQ phases, indicating significant influence of FQ order on the hybridization between conduction and f electrons, which in turn mediates the RKKY-type quadrupole interaction causing the FQ order. This feedback effect may be a specific feature of quadrupole orders not commonly observed in magnetic phase transitions and play a key role for inducing the discontinuous transitions.

cond-mat.str-el↗

arXiv2019

Quantum critical behaviour and Lifshitz transition in intermediate valence $α$-YbAlB$_4$

Intermetallic compounds containing $f$-electron elements have been prototypical materials for investigating strong electron correlations and quantum criticality (QC). Their heavy fermion ground state evoked by the magnetic $f$-electrons is susceptible to the onset of quantum phases, such as magnetism or superconductivity, due to the enhanced effective mass ($m^{*}$) and a corresponding decrease of the Fermi temperature. However, the presence of $f$-electron valence fluctuations to a non-magnetic state is regarded an anathema to QC, as it usually generates a paramagnetic Fermi-liquid state with quasiparticles of moderate $m^{*}$. Such systems are typically isotropic, with a characteristic energy scale $T_0$ of the order of hundreds of kelvins that require large magnetic fields or pressures to promote a valence or magnetic instability. Here we show that the intermediate valence compound $α$-YbAlB$_4$ surprisingly exhibits both quantum critical behaviour and a Lifshitz transition under low magnetic field, which is attributed to the anisotropy of the hybridization between the conduction and localized $f$-electrons. These findings suggest a new route to bypass the large valence energy scale in developing the QC.

cond-mat.str-el↗

arXiv2017

Collinear Spin-density-wave Order and Anisotropic Spin Fluctuations in the Frustrated $J_1$--$J_2$ Chain Magnet NaCuMoO$_4$(OH)

The phase diagram of the quasi-one-dimensional magnet NaCuMoO$_4$(OH) is established through single-crystal NMR and heat-capacity measurements. The $^{23}$Na and $^1$H NMR experiments indicate a spiral and a collinear spin-density-wave (SDW) order below and above $B_c$ = 1.5-1.8 T, respectively. Moreover, in the paramagnetic state above the SDW transition temperature, the nuclear spin-lattice relaxation rate $1/T_1$ indicates anisotropic spin fluctuations that have gapped excitations in the transverse spectrum but gapless ones in the longitudinal spectrum. These static and dynamic properties are well described by a theoretical model assuming quasi-one-dimensional chains with competing ferromagnetic nearest-neighbor interactions $J_1$ and antiferromagnetic next-nearest-neighbor interactions $J_2$ ($J_1$-$J_2$ chains). Because of the excellent crystal quality and good one dimensionality, NaCuMoO$_4$(OH) is a promising compound to elucidate the unique physics of the frustrated $J_1$-$J_2$ chain.

cond-mat.str-el↗

arXiv2017

Dynamics of Bound Magnon Pairs in the Quasi-One-Dimensional Frustrated Magnet LiCuVO_4

We report on the dynamics of the spin-1/2 quasi-one-dimensional frustrated magnet LiCuVO$\mathrm{_4}$ measured by nuclear spin relaxation in high magnetic fields 10--34 T, in which the ground state has spin-density-wave order. The spin fluctuations in the paramagnetic phase exhibit striking anisotropy with respect to the magnetic field. The transverse excitation spectrum probed by $^{51}$V nuclei has an excitation gap, which increases with field. On the other hand, the gapless longitudinal fluctuations sensed by $^7$Li nuclei grow with lowering temperature, but tend to be suppressed with increasing field. Such anisotropic spin dynamics and its field dependence agree with the theoretical predictions and are ascribed to the formation of bound magnon pairs, a remarkable consequence of the frustration between ferromagnetic nearest neighbor and antiferromagnetic next-nearest-neighbor interactions.

cond-mat.str-el↗

arXiv2017

$J_1-J_2$ Square-Lattice Heisenberg Antiferromagnets with 4$d^1$ spins: AMoOPO$_4$Cl (A = K, Rb)

Magnetic properties of AMoOPO$_4$Cl (A = K, Rb) with Mo$^{5+}$ ions in the 4$d^1$ electronic configuration are investigated by magnetization, heat capacity and NMR measurements on single crystals, combined with powder neutron diffraction experiments. The magnetization measurements reveal that they are good model compounds for the spin-1/2 $J_1-J_2$ square lattice magnet with the first and second nearest-neighbor interactions. Magnetic transitions are observed at around 6 and 8 K in the K and Rb compounds, respectively. In contrast to the normal Néel-type antiferromagnetic order, the NMR and neutron diffraction experiments find a columnar antiferromagnetic order for each compound, which is stabilized by a dominant antiferromagnetic $J_2$. Both compounds realize the unusual case of two interpenetrating $J_2$ square lattices weakly coupled to each other by $J_1$.

cond-mat.str-el↗

arXiv2016

NMR Observation of Ferro-quadrupole Order in PrTi2Al20

We report the results of 27Al-NMR measurements on a single crystal of PrTi2Al20. This compound shows a phase transition near 2 K associated with the quadrupole degree of freedom of Pr ions, for which the ground state of the crystalline electric field is a nonmagnetic doublet. When a magnetic field is applied along the <111> direction, the NMR lines split upon entering the low-temperature phase, indicating the breaking of the three fold rotation symmetry due to the field-induced magnetic dipole perpendicular to the field. This provides microscopic evidence for a ferro order of the O20 quadrupole. Although a first-order transition is expected theoretically, the line splitting evolves continuously within the experimental resolution.

cond-mat.str-el↗

arXiv2016

Pressure-Tuned Exchange Coupling of a Quantum Spin Liquid in the Molecular Triangular Lattice $κ$-(ET)$_2$Ag$_2$(CN)$_3$

The effects of pressure on a quantum spin liquid are investigated in an organic Mott insulator $κ$-(ET)$_2$Ag$_2$(CN)$_3$ with a spin-1/2 triangular lattice. The application of negative chemical pressure to $κ$-(ET)$_2$Cu$_2$(CN)$_3$, which is a well-known sister Mott insulator, allows for extensive tuning of antiferromagnetic exchange coupling, with $J/k_{\rm B} = 175 - 310$ K, under hydrostatic pressure. Based on $^{13}$C nuclear magnetic resonance measurements under pressure, we uncover universal scaling in the static and dynamic spin susceptibilities down to low temperatures $\sim 0.1k_{\rm B}T/J$. The persistent fluctuations and residual specific heat coefficient are consistent with the presence of gapless low-lying excitations. Our results thus demonstrate fundamental finite-temperature properties of quantum spin liquid in a wide parameter range.

cond-mat.str-el↗

arXiv2015

Structural anomalies and short-range magnetic correlations in the orbitally degenerated system Sr$_2$VO$_4$

We report on the electronic ground state of a layered perovskite vanadium oxide Sr$_2$VO$_4$ studied by the combined use of synchrotron radiation x-ray diffraction (SR-XRD) and muon spin rotation/relaxation ($μ$SR) techniques, where $μ$SR measurements were extended down to 30 mK. We found an intermediate orthorhombic phase between $T_{\rm c2} \sim$~130 K and $T_{\rm c1} \sim$~100 K, whereas a tetragonal phase appears for $T > T_{\rm c2}$ and $T < T_{\rm c1}$. The absence of long-range magnetic order was confirmed by $μ$SR at the reentrant tetragonal phase below $T_{\rm c1}$, where the relative enhancement in the $c$-axis length versus that of the $a$-axis length was observed. However, no clear indication of the lowering of the tetragonal lattice symmetry with superlattice modulation, which is expected in the orbital order state with superstructure of $d_{yz}$ and $d_{zx}$ orbitals, was observed by SR-XRD below $T_{\rm c1}$. Instead, it was inferred from $μ$SR that a magnetic state developed below $T_{\rm c0} \sim$~10 K, which was characterized by the highly inhomogeneous and fluctuating local magnetic fields down to 30 mK. We argue that the anomalous magnetic ground state below $T_{\rm c0}$ originates from the coexistence of ferromagnetic and antiferromagnetic correlations.

cond-mat.str-el↗