arXiv subjects

Tokuro Shimokawa

Publications and source records attributed to Tokuro Shimokawa.

At least 19 recordsLinked to original sources

arXiv2025

Magnetic excitations from the hexagonal spin clusters in the S = 1/2 distorted honeycomb lattice antiferromagnet Cu2(pymca)3(ClO4)

Cu2(pymca)3(ClO4) (pymca: pyrimidine-2-carboxylate) consists of a slightly distorted honeycomb lattice of Cu2+ spins, which shows no long-range magnetic order down to 0.6 K. A magnetization study revealed 1/3 and 2/3 plateau phases [A. Okutani et al., J. Phys. Soc. Jpn. 88, 013703 (2019)], which is not expected for regular honeycomb antiferromagnets. Inelastic neutron scattering experiments were performed using a powder sample to investigate the exchange interactions of this material. The spin excitations from the singlet ground state to the first three triplet states, predicted from the antiferromagnetic hexagonal spin cluster interacting with 3.9 meV, were observed. Using the exact diagonalization mothods, the intercluster coupling was estimated from the excitation peak width to be about 20% of the intracluster interaction, which is consistent with the previously reported value. Our exchange path model explains the anisotropic exchange interactions in the distorted honeycomb plane.

cond-mat.str-el↗

arXiv2025

Can experimentally-accessible measures of entanglement distinguish quantum spin liquids from disorder-driven "random singlet" phases ?

At the theoretical level, quantum spin liquids are distinguished from other phases of matter by their entanglement properties. However, since the usual measure of entanglement, entanglement entropy, cannot accessed in experiment, indentifying quantum spin liquids in candidate materials remains an acute problem. Here we show other, experimentally-accessible, measures of entanglement can be used to distinguish a quantum spin liquid from a competing disorder-driven "random singlet" phase, in a model of a disordered antiferromagnet on a triangular lattice. The application of these results to the triangular-lattice systems YbZnGaO$_4$, YbZn$_2$GaO$_5$ and KYbSe$_2$ is discussed.

cond-mat.str-el↗

arXiv2025

Witnessing Disorder in Quantum Magnets

There are no clean samples in nature. Therefore, when we come to discuss the entanglement properties of quantum materials, the effects of disorder must be taken into account. This question is of particular interest for high-entangled phases, such as quantum spin liquids, which lie outside the Landau paradigm for classifying phases of matter. In this work, we explore what experimentally-accessible measures, in the form of concurrence, residual tangle and quantum Fisher information, can teach us about the entanglement in the presence of disorder. As a representative example, we consider the Tomonaga-Luttinger liquids (TLL) and disorder-driven random singlet (RS) phases found in antiferromagnetic quantum spin chains. Using quantum Fisher information and residual tangle, we demonstrate that both TLL and RS phases exhibit multi-partite entanglement. In the case of the RS phase, we attribute this to entanglement localized below a crossover length scale. We further show that the order of disorder average matters in calculating measures like concurrence, and that this can lead to false inferences when interpreting experiment. Nonetheless, correctly interpreted, these witnesses provide useful information about the effects of disorder. We explore how information about the central charge of the TLL can be extracted from the low-temperature behavior of concurrence, and conjecture that this analysis can be extended to the effective central charge of the RS phase. Finally, we establish how RS and TLL phases can be distinguished through the growth of multi-partite entanglement, as witnessed by the equal-time structure factor. These results establish that, used carefully, experiments based on entanglement witnesses can provide important information about quantum spin systems in the presence of disorder.

cond-mat.str-el↗

arXiv2022

Quantum paramagnetic states in the spin-1/2 distorted honeycomb-lattice Heisenberg antiferromagnet -- application to Cu$_2$(pymca)$_3$(ClO$_4$)

We investigate the ground-state phase diagram of a spin-1/2 honeycomb-lattice antiferromagnetic (AF) Heisenberg model with three exchange interactions, $J_{\rm A}$, $J_{\rm B}$, and $J_{\rm C}$ that is realized in a distorted honeycomb-lattice antiferromagnet ${\rm Cu_2 (pymca)_3 (ClO_4)}$. We remeasured the magnetic susceptibility of its polycrystalline sample with special care, and determined the exchange parameters of this material through the comparison with numerical results based on a quantum Monte Carlo (QMC) method. The QMC method also provides a ground-state phase diagram in the $J_{\rm A}/J_{\rm C}$-$J_{\rm B}/J_{\rm C}$ plane. The phase diagram consists of a small N${\rm \acute{e}}$el phase and a gapped quantum paramagnetic phase surrounding the N${\rm \acute{e}}$el phase. The latter includes six regimes of hexagonal-singlet-type states and dimer-singlet-type states alternatingly without boundaries closing the spin gap. We further calculate the equal-time spin structure factor in each phase using the QMC method. The computed spin dynamics by the exact diagonalization method exhibits continuums near and in the AF phase. Characteristic four energy band structures in the state with strong hexagonal-singlet-type correlations are informative to clarify the ground-state of ${\rm Cu_2 (pymca)_3 (ClO_4)}$ by future neutron scattering measurements.

cond-mat.str-el↗

arXiv2021

Quantum spin solver near saturation: QS$^3_{~}$

We develop a program package named QS$^{3}$ [\textipa{kjú:-és-kjú:b}] based on the (thick-restart) Lanczos method for analyzing spin-1/2 XXZ-type quantum spin models on spatially uniform/non-uniform lattices near fully polarized states, which can be mapped to dilute hardcore Bose systems. All calculations in QS$^{3}$, including eigenvalue problems, expectation values for one/two-point spin operators, and static/dynamical spin structure factors, are performed in the symmetry-adapted bases specified by the number $N_{\downarrow}$ of down spins and the wave number $\boldsymbol{k}$ associated with the translational symmetry without using the bit representation for specifying spin configurations. Because of these treatments, QS$^{3}$ can support large-scale quantum systems containing more than 1000 sites with dilute $N_{\downarrow}$. We show the benchmark results of QS$^{3}$ for the low-energy excitation dispersion of the isotropic Heisenberg model on the $10\times10\times10$ cubic lattice, the static and dynamical spin structure factors of the isotropic Heisenberg model on the $10\times10$ square lattice, and the open-MP parallelization efficiency on the supercomputer (Ohtaka) based on AMD Epyc 7702 installed at the Institute for the Solid State Physics (ISSP). Theoretical backgrounds and the user interface of QS$^{3}$ are also described.

physics.comp-ph↗

arXiv2021

Signatures of the finite-temperature mirror symmetry breaking in the $S$=1/2 Shastry-Sutherland model

We investigate the finite-temperature properties of the $S$=1/2 Shastry-Sutherland Heisenberg model using a quantum typicality method. In the intermediate plaquette state region, we naturally expect to realize the finite-temperature phase transition associated with breaking the mirror symmetry of this model. We reveal some signatures of the spontaneous phase transition within a two-point correlation level at moderate temperatures since the constructed typical state can sense the existence of the degenerated excited states depending on the initial random state. We also confirm that the local mirror order parameter shows the intriguing recovering phenomenon of the mirror symmetry in very low-temperatures, which could be understood from the nature of the ground and excited states of the finite-size systems. We expect that this recovering feature disappears; instead, a saturated behavior appears in the local mirror order parameter in the thermodynamic limit. We discuss the relationship to the recent experimental results on ${\rm SrCu_2(BO_3)_2}$ under high pressures.

cond-mat.str-el↗

arXiv2019

Multiple-$q$ states of the $J_1$-$J_2$ classical honeycomb-lattice Heisenberg antiferromagnet under magnetic fields

Motivated by the recent theoretical study by Okubo $et \ al$ [Phys. Rev. Lett. ${\bf 108}$, 017206 (2012)] on the possible realization of the frustration-induced $ symmetric$ skyrmion-lattice state in the $J_1$-$J_2$ (or $J_1$-$J_3$) triangular-lattice Heisenberg model without the Dzyaloshinskii-Moriya interaction, we investigate the ordering of the classical $J_1$-$J_2$ honeycomb-lattice Heisenberg antiferromagnet under magnetic fields by means of a Monte Carlo simulation, a mean-field analysis and a low-temperature expansion. The model has been known to have an infinite ring-like degeneracy in the wavevector space in its ground state for $1/6<J_2/J_1<0.5$, in distinction with the triangular-lattice model. As reported by Okumura $et \ al$ [J. Phys. Soc. Jpn. ${\bf 79}$, 114705 (2010)], such a ring-like degeneracy gives rise to exotic spin liquid states in zero field, $e.g$, the "ring-liquid" state and the "pancake-liquid" state. In this paper, we study the in-field ordering properties of the model paying attention to the possible appearance of exotic multiple-$q$ states. Main focus is made on the $J_2/J_1=0.3$ case, where we observe a rich variety of multiple-$q$ states including the single-$q$, double-$q$ and triple-$q$ states. While the skyrmion-lattice triple-$q$ state observed in the triangular-lattice model is not realized, we instead observe an exotic double-$q$ state consisting of meron/antimeron lattice textures.

cond-mat.str-el↗

arXiv2019

Ripple state in the frustrated honeycomb-lattice antiferromagnet

We discover a new type of multiple-$q$ state, "ripple state", in a frustrated honeycomb-lattice Heisenberg antiferromagnet under magnetic fields. The ground state has an infinite ring-like degeneracy in the wavevector space, exhibiting a cooperative paramagnetic state, "ring-liquid" state. We elucidate that the system exhibits the ripple state as a new low-temperature thermodynamic phase via a second-order phase transition from the ring-liquid state, keeping the ring-like spin structure factor. The spin texture in real space looks like a "water ripple" and can induce a giant electric polarization vortex. Possible relationship to the honeycomb-lattice compound, ${\rm Bi_{3}Mn_{4}O_{12}(NO_{3})}$, is discussed.

cond-mat.str-el↗

arXiv2018

High-field Magnetism of the Honeycomb-lattice Antiferromagnet Cu$_2$(pymca)$_3$(ClO$_4$)

We report on the experimental results of magnetic susceptibility, specific heat, electron spin resonance (ESR), and high-field magnetization measurements on a polycrystalline sample of the spin-$1/2$ distorted honeycomb-lattice antiferromagnet Cu$_2$(pymca)$_3$(ClO$_4$). Magnetic susceptibility shows a broad peak at about 25~K, which is typical of a low dimensional antiferromagnet, and no long range magnetic order is observed down to 0.6~K in the specific heat measurements. Magnetization curve up to 70~T at 1.4~K shows triple stepwise jumps. Assuming three different exchange bonds $J_{\rm A}$, $J_{\rm B}$ and $J_{\rm C}$ from the structure, the calculated magnetization curve reproduces the observed one when $J_{\rm A}/k_{\rm B} = 43.7~{\rm K}$, $J_{\rm B}/J_{\rm A} = 1$ and $J_{\rm C}/J_{\rm A} = 0.2$ except the magnetization near 70~T, where the observed magnetization indicates another step while the calculated magnetization becomes saturated. The relationship between magnetization plateaus and exchange bonds is discussed based on the numerical calculations.

cond-mat.str-el↗

arXiv2017

Exact diagonalization and cluster mean-field study of triangular-lattice XXZ antiferromagnets near saturation

Quantum magnetic phases near the magnetic saturation of triangular-lattice antiferromagnets with XXZ anisotropy have been attracting renewed interest since it has been suggested that a nontrivial coplanar phase, called the $π$-coplanar or $Ψ$ phase, could be stabilized by quantum effects in a certain range of anisotropy parameter $J/J_z$ besides the well-known 0-coplanar (known also as $V$) and umbrella phases. Recently, Sellmann $et$ $al$. [Phys. Rev. B {\bf 91}, 081104(R) (2015)] claimed that the $π$-coplanar phase is absent for $S=1/2$ from an exact-diagonalization analysis in the sector of the Hilbert space with only three down-spins (three magnons). We first reconsider and improve this analysis by taking into account several low-lying eigenvalues and the associated eigenstates as a function of $J/J_z$ and by sensibly increasing the system sizes (up to 1296 spins). A careful identification analysis shows that the lowest eigenstate is a chirally antisymmetric combination of finite-size umbrella states for $J/J_z\gtrsim 2.218$ while it corresponds to a coplanar phase for $J/J_z\lesssim 2.218$. However, we demonstrate that the distinction between 0-coplanar and $π$-coplanar phases in the latter region is fundamentally impossible from the symmetry-preserving finite-size calculations with fixed magnon number.} Therefore, we also perform a cluster mean-field plus scaling analysis for small spins $S\leq 3/2$. The obtained results, together with the previous large-$S$ analysis, indicate that the $π$-coplanar phase exists for any $S$ except for the classical limit ($S\rightarrow \infty$) and the existence range in $J/J_z$ is largest in the most quantum case of $S=1/2$.

cond-mat.str-el↗

arXiv2016

Dzyaloshinsky-Moriya interaction and the ground state in S=3/2 perfect kagome lattice antiferromagnet $\mathbf{KCr_3(OH)_6(SO_4)_2}$ (Cr-jarosite) studied by X-band and high-frequency ESR

A single crystal S=3/2 perfect kagome lattice antiferromagnet $\mathrm{KCr_3(OH)_6(SO_4)_2}$ (Cr-jarosite) has been studied by X-band and high-frequency electron spin resonance (ESR). The g-values perpendicular to the kagome plane (c-axis) and in the plane are determined to be $g_c=1.9704 \pm 0.0002$ and $g_ξ=1.9720 \pm 0.0003$, respectively, by high-frequency ESR observed at 265 K. Antiferromagnetic resonances (AFMR) with the antiferromagnetic gap of 120 GHz are observed at 1.9 K, which is below $T_N$=4.5 K. The analysis of AFMR modes by the conventional molecular field theory shows $d_p=0.27$ K and $d_z=0.07$ K, where $d_p$ and $d_z$ are in-plane and out-of-plane components of DM d vector, respectively. From these results and the estimated exchange interaction J=6.15 K by Okuta et al., the ground state of Cr-jarosite is discussed in connection with the Monte Carlo simulations result with classical Heisenberg spins on the kagome lattice by Elhajal et al. Finally, the angular dependence of linewidth and the lineshape observed at 296 K by X-band ESR show typical behavior of a two-dimensional Heisenberg antiferromagnet, suggesting a good two-dimensionality of Cr-jarosite.

cond-mat.str-el↗

arXiv2016

Finite-temperature crossover phenomenon in the $S=1/2$ antiferromagnetic Heisenberg model on the kagome lattice

Thermal properties of the $S=1/2$ kagome Heisenberg antiferromagnet at low temperatures are investigated by means of the Hams-de Raedt method for clusters of up to 36 sites possessing a full symmetry of the lattice. The specific heat exhibits, in addition to the double peaks, the third and the forth peaks at lower temperatures. With decreasing the temperature, the type of the magnetic short-range order (SRO) changes around the third-peak temperature from the $\sqrt{3} \times \sqrt{3}$ to the $q$=0 states, suggesting that the third peak of the specific heat is associated with a crossover phenomenon between the spin-liquid states with distinct magnetic SRO. Experimental implications are discussed.

cond-mat.str-el↗

arXiv2015

Static and dynamical spin correlations of the S=1/2 random-bond antiferromagnetic Heisenberg model on the triangular and the kagome lattices

Inspired by the recent theoretical suggestion that the random-bond $S=1/2$ antiferromagnetic Heisenberg model on the triangular and the kagome lattices might exhibit a randomness-induced quantum spin liquid (QSL) behavior when the strength of the randomness exceeds a critical value, and that this "random-singlet state" might be relevant to the QSL behaviors experimentally observed in triangular organic salts $κ{\rm -(ET)_2 Cu_2 (CN)_3}$and ${\rm EtMe_3 Sb[Pd(dmit)_2]_2}$ and in kagome herbertsmithite ${\rm CuZn_3(OH)_6Cl_2}$, we further investigate the nature of the static and the dynamical spin correlations of these models. We compute the static and the dynamical spin structure factors, $S({\bf q})$ and $S({\bf q},ω)$, by means of an exact diagonalization method. In both triangular and kagome models, the computed $S({\bf q},ω)$ in the random-singlet state depends on the wavevector ${\bf q}$ only weakly, robustly exhibiting gapless behaviors accompnied by the broad distribution extending to higher energy $ω$. Especially in the strongly random kagome model, $S({\bf q},ω)$ hardly depends on ${\bf q}$, and exhibits an almost flat distribution for a wide range of $ω$, together with a $ω=0$ peak. These features agree semi-quantitatively with the recent neutron-scattering data on a single-crystal herbertsmithite, suggesting that the QSL state observed in herbersmithite might indeed be the randomness-induced QSL state, {\it i.e.\/}, the random-singlet state.

cond-mat.str-el↗

arXiv2015

$S$ = 1/2 ferromagnetic-antiferromagnetic alternating Heisenberg chain in a zinc-verdazyl complex

We successfully synthesized the zinc-verdazyl complex [Zn(hfac)$_2$]$\cdot$($o$-Py-V) [hfac = 1,1,1,5,5,5-hexafluoroacetylacetonate; $o$-Py-V = 3-(2-pyridyl)-1,5-diphenylverdazyl], which is an ideal model compound with an $S$ = 1/2 ferromagnetic-antiferromagnetic alternating Heisenberg chain (F-AF AHC). $Ab$ $initio$ molecular orbital (MO) calculations indicate that two dominant interactions $J_{\rm{F}}$ and $J_{\rm{AF}}$ form the $S=1/2$ F-AF AHC in this compound. The magnetic susceptibility and magnetic specific heat of the compound exhibit thermally activated behavior below approximately 1 K. Furthermore, its magnetization curve is observed up to the saturation field and directly indicates a zero-field excitation gap of 0.5 T. These experimental results provide evidence for the existence of a Haldane gap. We successfully explain the results in terms of the $S=1/2$ F-AF AHC through quantum Monte Carlo calculations with $|J_{\rm{AF}}/J_{\rm{F}}|$ = 0.22. The $ab$ $initio$ MO calculations also indicate a weak AF interchain interaction $J'$ and that the coupled F-AF AHCs form a honeycomb lattice. The $J'$ dependence of the Haldane gap is calculated, and the actual value of $J'$ is determined to be less than 0.01$|J_{\rm{F}}|$.

cond-mat.str-el↗

arXiv2015

Microscopic properties of degradation-free capped GdN thin films studied by Electron Spin Resonance

The microscopic magnetic properties of high-quality GdN thin films have been investigated by electron spin resonance (ESR) and ferromagnetic resonance (FMR) measurements. Detailed temperature dependence ESR measurements have shown the existence of two ferromagnetic components at lower temperatures which was not clear from the previous magnetization measurements. The temperature, where the resonance shift occurs for the major ferromagnetic component, seems to be consistent with the Curie temperature obtained from the previous magnetization measurement. On the other hand, the divergence of line width is observed around 57 K for the minor ferromagnetic component. The magnetic anisotropies of GdN thin films have been obtained by the analysis of FMR angular dependence observed at 4.2 K. Combining the X-ray diffraction results, the correlation between the magnetic anisotropies and the lattice constants is discussed.

cond-mat.mtrl-sci↗

arXiv2014

Quantum spin-liquid behavior in the spin-1/2 random-bond Heisenberg antiferromagnet on the kagome lattice

The effect of the quenched bond-randomness on the ordering of the $S=1/2$ antiferromagnetic Heisenberg model on the kagome lattice is investigated by means of an exact-diagonalization method. When the randomness exceeds a critical value, the ground state of the model exhibits a transition within the non-magnetic state into the randomness-relevant gapless spin-liquid state. Implications to the S=1/2 kagome-lattice antiferromagnet herbertsmithite is discussed.

cond-mat.str-el↗

arXiv2014

Fine-Tuning of Magnetic Interactions in Organic Spin Ladders

We have succeeded in synthesizing two types of new organic radical crystals 3-I-V [= 3- (3-iodophenyl)-1,5-diphenylverdazyl] and 3-Br-4-F-V [= 3-(3-bromo-4-fluorophenyl)-1,5- diphenylverdazyl]. Their crystal strucutures are found to be isomorphous to that of previously reported spin ladder 3-Cl-4-F-V. Through the quantitative analysis of their molecular arrangements and magnetic properties, we confirm that these materials form ferromagnetic chain-based spin ladders with slightly modulated magnetic interactions. These results present the first quantitative demonstration of the fine-tuning of magnetic interactions in the molecular- based materials.

cond-mat.str-el↗

arXiv2012

Nontrivial ferrimagnetism of the Heisenberg model on the Union Jack strip lattice

We study the ground-state properties of the S=1/2 antiferromagnetic Heisenberg model on the Union Jack strip lattice by using the exact-diagonalization and density matrix renormalization group methods. We confirm a region of the intermediate-magnetization state between the Neel-like spin liquid state and the conventional ferrimagnetic state of Lieb-Mattis type. In the intermediate-state, we find that the spontaneous magnetization changes gradually with respect to the strength of the inner interaction. In addition, the local magnetization clearly shows an incommensurate modulation with long-distance periodicity in the intermediate-magnetization state. These characteristic behaviors lead to the conclusion that the intermediate-magnetization state is the non-Lieb-Mattis ferrimagnetic one. We also discuss the relationship between the ground-state properties of the S=1/2 antiferromagnetic Heisenberg model on the original Union Jack lattice and those on our strip lattice.

cond-mat.str-el↗