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Koji Araki

Publications and source records attributed to Koji Araki.

11 recordsLinked to original sources

Search for magnetoacoustic quantum oscillations in the insulating phase of YbB$_{12}$

A highly exotic phenomenon in solid-state physics is the observation of magnetic quantum oscillations in insulators. For instance, in the Kondo insulator YbB$_{12}$ various groups reported the observation of such oscillations seemingly originating from Fermi surfaces, though this contradicts the concept of an insulator having no charged quasiparticles. In this study, we searched for quantum oscillations in YbB$_{12}$ by using bulk-sensitive ultrasonic experiments in high magnetic fields up to 65 T and down to 485 mK. For that, we utilized an YbB$_{12}$ single crystal that, in previous experiments, revealed oscillations in the magnetoresistance in the insulating state. We confirmed oscillation-like behavior of the magnetoresistance as well as field-dependent oscillations in the magnetocaloric effect. However, we could not observe magnetoacoustic quantum oscillations in the insulating state, only in the field-induced metallic state. In the insulating state, we found some anomalies in our ultrasound data, the origin of which remains elusive. Our findings provide further information on the puzzling behavior of the insulating state of YbB$_{12}$.

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Emergence of Kondo-assisted Néel order in a Kondo necklace model

The interplay between Kondo screening and magnetic order has long been a central issue in the physics of strongly correlated systems. While the Kondo effect has traditionally been understood to suppress magnetism through the formation of local singlets, recent studies suggest that Kondo interactions may enhance magnetic order under certain conditions. However, these scenarios often rely on complex electronic structures, including orbital and charge degrees of freedom, making the essential mechanisms difficult to isolate. Here we report the realization of a spin-(1/2,1) Kondo necklace model in a Ni-based complex-a minimal spin-only analog of the Kondo lattice that isolates quantum spin correlations by eliminating charge degrees of freedom. Thermodynamic measurements identify a magnetic phase transition and a field-induced quantum phase transition. Perturbative analysis reveals that the Kondo coupling mediates effective antiferromagnetic interactions between the spin-1 sites, stabilizing the Néel order across the entire chain. Our results establish a universal boundary in Kondo physics, where coupling to spin-1/2 moments yields singlets, but to spin-1 and higher stabilizes magnetic order.

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Realization of a triangular spin necklace in a verdazyl-based Ni complex

We successfully synthesized a verdazyl-based complex, ($m$-Py-V)$_3$[Ni(NO$_3$)$_2$], in which Ni$^{2+}$ ions and verdazyl radicals form a one-dimensional, triangular spin necklace consisting of spin-1/2 and spin-1 units. Molecular orbital calculations reveal strong antiferromagnetic (AF) interactions between inversion-related radical pairs that form spin-1/2 singlet dimers. The remaining verdazyl and Ni$^{2+}$ spins form frustrated triangular units, creating a distinctive spin network. Magnetic susceptibility and specific heat measurements identify a phase transition to an AF order. The application of magnetic fields suppresses the phase transition signal, suggesting field-induced decoupling of the spin-1 moments. Electron spin resonance measurements are used to evaluate the easy-axis anisotropy of spin-1, which may promote the AF order. This work provides a rare example of a geometrically frustrated quantum spin chain realized via molecular design, thereby offering a platform for exploring frustration-driven quantum phases in low-dimensional materials.

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Experimental benchmark of the quantum-classical crossover in a spin ladder

We report a spin-(1/2, 5/2) three-leg ladder realized in a radical-Mn polymer, exhibiting an antiferromagnetic transition and magnetization curves accurately described by classical mean-field theory. Although the underlying spin model intrinsically supports strong quantum fluctuations, as confirmed by quantum Monte Carlo simulations, the real system shows an anomalously complete suppression of quantum behavior. These findings provide a key experimental benchmark for the quantum-classical crossover and suggest that lattice topology can play a crucial role in tuning the balance between quantum and classical physics in strongly correlated systems.

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Realization of a Spin-1/2 Hexagonal-Plaquette Chain with Ising-Like Anisotropy

We present the realization of a spin-1/2 hexagonal-plaquette chain with Ising anisotropy, an unexplored quantum spin model that serves as a platform for investigating anisotropic quantum magnetism. Specific heat at zero field reveals a sharp peak at $T_{\rm{N}}$ = 1.0 K, indicating a phase transition to a N$\acute{\rm{e}}$el order stabilized by interchain couplings. A perturbative analysis maps the system onto an effective spin-1/2 Ising-like chain, supporting the presence of an anisotropy-induced excitation gap. Furthermore, the interchain interactions may induce discrete excitations in the spinon continuum, reminiscent of Zeeman ladder physics observed in related 1D Ising-like systems. These results establish a well-defined model system for correlated spin phenomena in anisotropic magnets and highlight a route for engineering Ising-like quantum states in molecular-based frameworks.

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Gapless behavior in a two-leg spin ladder with bond randomness

We successfully synthesized [Cu$_2$(AcO)$_4$($p$-Py-V-$p$-F)$_2$]$\cdot$4CHCl$_3$, a verdazyl-based complex with a paddlewheel structure comprising two Cu atoms, which induces strong antiferromagnetic (AF) exchange interactions between Cu spins, generating a nonmagnetic singlet state at low temperatures. Two primary exchange interactions between radical spins generate a spin-1/2 AF two-leg ladder. In addition, two possible positional configurations of the F atom in the complex create four different overlap patterns of molecular orbitals, introducing bond randomness in the spin ladder. The observed experimental behaviors, such as the Curie tail in the magnetic susceptibility and the gapless gradual increase in the magnetization curve, are attributed to a broad distribution of excitation energies and a few orphan spins in the random-singlet (RS) state that are stabilized by bond randomness. The low-temperature specific heat exhibits a temperature dependence with $\propto 1/|{\rm{ln}}T|^3$, demonstrating the formation of the RS state in unfrustrated systems. We also consider the effect of restricted patterns of exchange interactions and one-dimensional nature of the system on the RS state.

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Quantum gapped state in a spin-1/2 distorted honeycomb-based lattice with frustration

We successfully synthesized ($p$-Py-V)[Cu(hfac)$_2$], a verdazyl-based complex. Molecular orbital calculations revealed five types of intermolecular interactions between the radical spins and two types of intramolecular interactions between the radical and the Cu spins, resulting in a spin-1/2 distorted honeycomb-based lattice. Additionally, competing ferromagnetic and antiferromagnetic (AF) interactions induce frustration. The magnetization curve displayed a multistage increase, including a zero-field energy gap. Considering the stronger AF interactions that form dimers and tetramers, the magnetic susceptibility and magnetization curves were qualitatively explained. These findings demonstrated that the quantum state, based on the dominant AF interactions, was stabilized due to the effects of frustration in the lattice. Hence, the exchange interactions forming two-dimensional couplings decoupled, reducing energy loss caused by frustration and leading to frustration-induced dimensional reduction.

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Field-induced quantum phase in a frustrated zigzag-square lattice

This study presents the experimental realization of a spin-1/2 zigzag-square lattice in a verdazyl-based complex, namely ($m$-Py-V-2,6-F$_2$)$[$Cu(hfac)$_2]$. Molecular orbital calculations suggest the presence of five types of frustrated exchange couplings. Our observations reveal an incremental increase in the magnetization curve beyond a critical field, signifying a phase transition from the antiferromagnetic ordered state to a quantum state characterized by a 1/2 plateau. This intriguing behavior arises from the effective stabilization of a zigzag chain by the external fields. These results provide evidence for field-induced dimensional reduction in a zigzag-square lattice attributed to the effects of frustration.

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Giant Anisotropic Magnetoresistance due to Purely Orbital Rearrangement in the Quadrupolar Heavy Fermion Superconductor PrV$_2$Al$_{20}$

We report the discovery of giant and anisotropic magnetoresistance due to the orbital rearrangement in a non-magnetic correlated metal. In particular, we measured the magnetoresistance under fields up to 31.4 T in the cubic Pr-based heavy fermion superconductor PrV$_2$Al$_{20}$ with a non-magnetic $Γ_3$ doublet ground state, exhibiting antiferro-quadrupole ordering below 0.7 K. For the [100] direction, we find that the high-field phase appears between 12 T and 25 T, accompanied by a large jump at 12 T in the magnetoresistance ($ΔMR \sim $ 100 $\% $) and in the anisotropic magnetoresistivity (AMR) ratio by $\sim $ 20 $\% $. These observations indicate that the strong hybridization between the conduction electrons and anisotropic quadrupole moments leads to the Fermi surface reconstruction upon crossing the field-induced antiferro-quadrupole (orbital) rearrangement.

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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.

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Magnetic-Field-Independent Ultrasonic Dispersions in the Magnetically Robust Heavy Fermion System SmOs4Sb12

Elastic properties of the filled skutterudite compound SmOs$_4$Sb$_{12}$ have been investigated by ultrasonic measurements. The elastic constant $C_{11}(ω)$ shows two ultrasonic dispersions at $\sim$15 K and $\sim$53 K for frequencies $ω$ between 33 and 316 MHz, which follow a Debye-type formula with Arrhenius-type temperature-dependent relaxation times, and remain unchanged even with applied magnetic fields up to 10 T. The corresponding activation energies were estimated to be $E_2$ = 105 K and $E_1$ = 409 K, respectively. The latter, $E_1$, is the highest value reported so far in the Sb-based filled skutterudites. The presence of magnetically robust ultrasonic dispersions in SmOs$_4$Sb$_{12}$ implies a possibility that an emergence of a magnetically insensitive heavy fermion state in this system is associated with a novel local charge degree of freedom which causes the ultrasonic dispersion.

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