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Toshio Ono

Publications and source records attributed to Toshio Ono.

17 recordsLinked to original sources
arXiv2026

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.

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↗
arXiv2017

Spin Dynamics in a Stripe-ordered Buckled Honeycomb Lattice Antiferromagnet Ba$_{2}$NiTeO$_{6}$

We carried out inelastic neutron scattering experiments on a buckled honeycomb lattice antiferromagnet Ba$_{2}$NiTeO$_{6}$ exhibiting a stripe structure at a low temperature. Magnetic excitations are observed in the energy range of $\hbar ω\lesssim 10$ meV having an anisotropy gap of 2 meV at 2 K. We perform spin-wave calculations to identify the spin model. The obtained microscopic parameters are consistent with the location of the stripe structure in the classical phase diagram. Furthermore, the Weiss temperature independently estimated from a bulk magnetic susceptibility is consistent with the microscopic parameters. The results reveal that a competition between the NN and NNN interactions that together with a relatively large single ion magnetic anisotropy stabilize the stripe magnetic structure.

cond-mat.str-el↗
arXiv2017

Magnetization process of the S = 1/2 two-leg organic spin-ladder compound BIP-BNO

We have measured the magnetization of the organic compound BIP-BNO (3,5'-bis(N-tert-butylaminoxyl)-3',5-dibromobiphenyl) up to 76 T where the magnetization is saturated. The S = 1/2 antiferromagnetic Heisenberg two-leg spin-ladder model accounts for the obtained experimental data regarding the magnetization curve, which is clarified using the quantum Monte Carlo method. The exchange constants on the rung and the side rail of the ladder are estimated to be J(rung)/kB = 65.7 K and J(leg)/kB = 14.1 K, respectively, deeply in the strong coupling region: J(rung)/J(leg) > 1.

cond-mat.str-el↗
arXiv2015

Spinon, soliton and breather in the spin-1/2 antiferromagnetic chain KCuGaF$_6$

Elementary excitations of the S=1/2 one-dimensional antiferromagnet KCuGaF_6 were investigated by inelastic neutron scattering in zero and finite magnetic fields perpendicular to the (1, 1, 0) plane combined with specific heat measurements. KCuGaF$_6$ exhibits no long-range magnetic ordering down to 50 mK despite the large exchange interaction J/k_B=103 K. At zero magnetic field, well-defined spinon excitations were observed. The energy of the des Cloizeaux and Pearson mode of the spinon excitations is somewhat larger than that calculated with the above exchange constant. This discrepancy is mostly ascribed to the effective XY anisotropy arising from the large Dzyaloshinsky-Moriya interaction with an alternating D vector. KCuGaF_6 in a magnetic field is represented by the quantum sine-Gordon model, for which low-energy elementary excitations are composed of solitons, antisolitons and their bound states called breathers. Unlike the theoretical prediction, it was found that the energy of a soliton is smaller than that of the first breather, although the energy of the first breather coincides with that observed in a previous ESR measurement.

cond-mat.str-el↗
arXiv2015

Successive magnetic phase transitions in $\bmα$-RuCl$_3$: XY-like frustrated magnet on the honeycomb lattice

The layered compound $α$-RuCl$_3$ is composed of a honeycomb lattice of magnetic Ru$^{3+}$ ions with the $4d^5$ electronic state. We have investigated the magnetic properties of $α$-RuCl$_3$ via magnetization and specific heat measurements using single crystals. It was observed that $α$-RuCl$_3$ undergoes a structural phase transition at $T_{t}\,{\simeq}\,150$ K accompanied by fairly large hysteresis. This structural phase transition is expected to be similar to that observed in closely related CrCl$_3$. The magnetizations and magnetic susceptibilities are strongly anisotropic, which mainly arise from the anisotropic $g$-factors, i.e., $g_{ab}\,{\simeq}\,2.5$ and $g_c\,{\simeq}\,0.4$ for magnetic fields parallel and perpendicular to the $ab$ plane, respectively. These $g$-factors and the obtained entropy indicate that the effective spin of Ru$^{3+}$ is one-half, which results from the low-spin state. Specific heat data show that magnetic ordering occurs in four steps at zero magnetic field. The successive magnetic phase transitions should be ascribed to the competition among exchange interactions. The magnetic phase diagram for $H\,{\parallel}\,ab$ is obtained. We discuss the strongly anisotropic $g$-factors in $α$-RuCl$_3$ and deduce that the exchange interaction is strongly XY-like. $α$-RuCl$_3$ is magnetically described as a three-dimensionally coupled XY-like frustrated magnet on a honeycomb lattice.

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↗
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

Ferromagnetism induced in anisotropic stacked kagome-lattice antiferromagnet Cs$_2$Cu$_3$CeF$_{12}$

The magnetic properties of Cs$_2$Cu$_3$CeF$_{12}$ were investigated through magnetization and specific heat measurements. Cs$_2$Cu$_3$CeF$_{12}$ is composed of a buckled kagome lattice of Cu$^{2+}$, which is stacked along the b axis. The exchange network in the buckled kagome lattice is strongly anisotropic. Consequently, Cs$_2$Cu$_3$CeF$_{12}$ can be divided into two subsystems: alternating Heisenberg chains with strong antiferromagnetic exchange interactions and dangling spins. The dangling spins couple with one another via effective exchange interactions, which are mediated by chain spins. The dangling spins are further divided into two subsystems, DS1 and DS2. The dangling spins in DS1 undergo three-dimensional ferromagnetic ordering at 3.14 K, while those in DS2 remain paramagnetic down to 0.35 K. The effective interaction between the DS1 spins is approximately expressed by the ferromagnetic $XXZ$ model with the $z$ direction parallel to the crystallographic c axis. A magnetic phase diagram for $H {\parallel} c$ was obtained and was analyzed within the framework of the molecular field approximation. With increasing magnetic field, the dangling spins are polarized and the magnetization curve exhibits a wide plateau at one-third of the saturation magnetization.

cond-mat.str-el↗
arXiv2011

Thermodynamic properties of quantum sine-Gordon spin chain system KCuGaF6

We investigated the thermodynamic properties of the spin-1/2 one-dimensional Heisenberg antiferromagnet KCuGaF6 by measuring the specific heat in magnetic fields. When this compound is subjected to a uniform magnetic field H a transverse staggered magnetic field h is induced in this compound owing to the staggered component of the g tensor and the Dzyaloshinskii-Moriya interaction with an alternating D vector. Consequently, the quantum sine-Gordon (SG) model is an effective model of this compound in a uniform magnetic field. In three different field directions, we observed a magnetic-field-induced gap, which increases with H. We analyzed experimental results using specific heat theory based on quantum SG theory. The thermodynamic property for H // c is very well described in terms of the elementary excitations characteristic of the quantum SG model, while for the other field directions, significant contributions from other excitation modes beyond the framework of the quantum SG model were observed. For H // b, a quantum phase transition between gapless and gapped ground states was observed.

cond-mat.str-el↗
arXiv2011

Quantum Magnetization Plateau in Spin-1 Triangular-Lattice Antiferromagnet Ba$_3$NiSb$_2$O$_9$

We report the results of magnetization and specific heat measurements on Ba$_3$NiSb$_2$O$_9$, which is a quasi-two-dimensional spin-1 triangular-lattice antiferromagnet. We observed a nonclassical magnetization plateau at one-third of the saturation magnetization that is driven by spin frustration and quantum fluctuation. Exact diagonalization for a 21-site rhombic cluster was performed to analyze the magnetization process. Experimental and calculated results agree well.

cond-mat.str-el↗
arXiv2010

Bose Glass-BEC Transition of Magnons in Tl$_{1-x}$K$_x$CuCl$_3$

We report the magnetic-field induced Bose glass$-$BEC transition of magnons in Tl$_{1-x}$K$_x$CuCl$_3$ and its critical behavior investigated through specific heat and ESR measurements. The field dependence of the BEC transition temperature $T_{\rm N}$ can be described by the power law $\left[H\,{-}\,H_{\rm c}\right]\,{\propto}\,T_{\rm N}^ϕ$ near the quantum critical point $H_{\rm c}\,{\sim}\,3.5$ T. The critical exponent $ϕ$ tends to reach a value smaller than 1/2 with decreasing fitting window in contrast with $ϕ\rightarrow 3/2$ for the standard BEC in pure system. At sufficiently low temperatures, the ESR line shape for $H\,{\simeq}\,H_{\rm c}$ is intermediate between Gaussian and Lorentzian. This indicates the localization of magnons for $H\,{<}H_{\rm c}$ at T=0.

cond-mat.str-el↗
arXiv2009

Elementary excitations of S=1/2 one-dimensional antiferromagnet KCuGaF6 in magnetic field and quantum sine-Gordon model

Elementary excitations of the S=1/2 one-dimensional Heisenberg antiferromagnet KCuGaF$_6$ with exchange constant $J/k_B$=103 K were investigated by high-frequency ESR measurements combined with a pulsed high magnetic field. When an external magnetic field H is applied in KCuGaF$_6$, a staggered magnetic field h is induced perpendicular to H owing to the staggered g tensor and the Dzyaloshinsky-Moriya (DM) interaction with an alternating D vector. Consequently, KCuGaF$_6$ in a magnetic field is represented by the quantum sine-Gordon (SG) model. We observed many resonance modes including a soliton resonance, breathers, interbreather transitions and two-breather excitation. Their resonance conditions are beautifully described by the quantum SG field theory with one adjustable parameter $c_ s=h/H$. To investigate the relationship between the Curie term due to the DM interaction and the proportional coefficient $c_s$, magnetic susceptibility measurements were also performed varying the external field direction.

cond-mat.str-el↗
arXiv2007

Magnetic-Field Induced Bose-Einstein Condensation of Magnons and Critical Behavior in Interacting Spin Dimer System TlCuCl$_3$

Magnetization measurements were performed to investigate the critical behavior of the field-induced magnetic ordering in gapped spin system TlCuCl$_3$. The critical density of the magnons was obtained as a function of temperature and the magnon-magnon interaction constant was evaluated. The experimental phase boundary for $T < 5$ K agrees almost perfectly with the magnon BEC theory based on the Hartree-Fock approximation with realistic dispersion relations. The phase boundary can be described by the power law $[H_{N}(T)-H_{c}] propto T^{phi}$. With decreasing fitting temperature range, the critical exponent ${phi}$ decreases and converges at $phi_{BEC} =3/2$ predicted by the magnon BEC theory.

cond-mat.str-el↗
arXiv2007

Thermodynamic Properties and Elementary Excitations in Quantum Sine-Gordon Spin System KCuGaF6

Thermodynamic properties and elementary excitations in $S=1/2$ one-dimensional Heisenberg antiferromagnet KCuGaF$_6$ were investigated by magnetic susceptibility, specific heat and ESR measurements. Due to the Dzyaloshinsky-Moriya interaction with alternating $D$-vectors and/or the staggered $g$-tensor, the staggered magnetic field is induced when subjected to external magnetic field. Specific heat in magnetic field clearly shows the formation of excitation gap, which is attributed to the staggered magnetic field. The specific heat data was analyzed on the basis of the quantum sine-Gordon (SG) model. We observed many ESR modes including one soliton and three breather excitations characteristic of the quantum SG model.

cond-mat.str-el↗
arXiv2004

Pressure-Induced Magnetic Quantum Phase Transitions from Gapped Ground State in TlCuCl3

Magnetization maesurements under hydrostatic pressure were performed on an S=1/2 coupled spin system TlCuCl3 with a gapped ground state under magnetic field H parallel to the [2,0,1] direction. With increasing applied pressure P, the gap decreases and closes completely at Pc=0.42 kbar. For P>Pc, TlCuCl3 undergoes antiferromagnetic ordering. A spin-flop transition was observed at Hsf=0.7T. The spin-flop field is approximately independent of pressure, although the sublattice magnetization increases with pressure. The gap and Neel temperature are presented as function is attributed to to the relative enhancement of the interdimer exchange interactions compared with the intradimer exchange interaction.

cond-mat.stat-mech↗