arXiv subjects

H. Taniguchi

Publications and source records attributed to H. Taniguchi.

At least 19 recordsLinked to original sources

arXiv2026

Giant dielectric permittivity in Nb-doped rutile crystals

Dielectric properties of Nb-doped (~1.5 at%) rutile single crystals were studied in the 10-300 K temperature range (at frequencies below the MHz range down to 0.3 K) in a broad frequency range, up to terahertz and infrared range, to understand the origin of its giant permittivity. The results were fitted, modelled and compared with those of the undoped rutile crystal measured in the terahertz and infrared ranges. The primary effect originates from the near-electrode depletion layer of lower conductivity compared to the bulk (surface barrier-layer capacitor effect), which causes a strong thermally activated relaxation in the MHz dielectric spectra. In the higher frequency range, the main difference between doped and undoped crystals is the presence of an overdamped microwave excitation (central mode) in the doped crystal for both polarizations, persisting down to 10 K and not thermally activated. This accounts for the previously reported permittivity increase, even at 2 K - where all lower-frequency relaxations are frozen - compared to undoped crystals. It also explains why our low-frequency permittivity at 0.3K exceeds the THz value. The origin of this excitation remains unclear and requires further investigations. Doping affects polar phonons only by slightly increasing their damping.

cond-mat.mtrl-sci↗

arXiv2025

Photoinduced Frustration Modulation in $\kappa$-type Quantum Spin Liquid Candidates

Geometric frustration is a key parameter controlling electronic and magnetic properties of quantum spin liquid systems, yet remains challenging to tune. Here, we coherently drive molecular vibrations with midinfrared pulses in two organic quantum spin liquid candidates, the insulating $\kappa$-(BEDT-TTF)$_2$Cu$_2$(CN)$_3$ and the metallic $\kappa$-(BEDT-TTF)$_4$Hg$_{2.89}$Br$_8$, and probe their electronic response through ultrafast reflectivity measurements. We observe a nonlinear coupling between local molecular vibrations and nonlocal phonons, which is expected to directly modulate the geometric frustration of their triangular lattice. Our findings establish a promising route to dynamically control frustration in nonbipartite quantum materials.

cond-mat.str-el↗

arXiv2025

Pressure-induced topological changes in Fermi surface of two-dimensional molecular conductor

We demonstrated X-ray structural analysis of the pressure-induced superconductor, $\beta'$-ET$_2$ICl$_2$ under extremely high-pressure conditions, where ET denotes bis(ethylenedithio)tetrathiafulvalene. This material has been known as the highest transition temperature ($T_c$) superconductor among organic superconductors ($T_c=14.2$ K at $8.2$ GPa). On the basis of the experimental results, ab-initio models were derived using the constrained random phase approximation. We revealed that the Lifshitz transition exists behind the Mott insulator-metal transition and found that the value of the on-site Coulomb interaction was halved to around $10$ GPa compared to that at ambient pressure. This study clarifies the enigmatic origins of high $T_{\rm c}$, and concurrently, provides a new understanding of the impacts of structural alterations in organic materials under high pressure on their electronic properties and the superconductivity process.

cond-mat.supr-con↗

arXiv2022

Dynamics of ethylene groups and hyperfine interactions between donor and anion molecules in $\lambda$-type organic conductors studied by $^{69,71}$Ga-NMR spectroscopy

We present the results of $^{69,71}$Ga-NMR measurements on an organic antiferromagnet $\lambda$-(BEDSe-TTF)$_2$GaCl$_4$ [BEDSe-TTF=bis(ethylenediseleno)tetrathiafulvalene], with comparison to reports on $\lambda$-(BETS)$_2$GaCl$_4$ [BETS=bis(ethylenedithio)tetraselenafulvalene] [T. Kobayashi et al., Phys. Rev. B 102, 235131 (2020)]. We found that the dynamics of two crystallographically independent ethylene groups induce two types of quadrupolar relaxation in the high-temperature region. As the ethylene motion freezes, hyperfine (HF) interactions develop between $\pi$ spin and Ga nuclear spin below 100 K, and thereby magnetic fluctuations of the $\pi$-spin system are detected even from the Ga site. The HF interaction in $\lambda$-(BETS)$_2$GaCl$_4$ was more than twice as large as in $\lambda$-(BEDSe-TTF)$_2$GaCl$_4$, implying that the short contacts between Cl atoms and the chalcogens of fulvalene part are essential for the transferred HF interaction. We propose that NMR using nuclei in anion layers is useful for studying interlayer interactions in organic conductors, which have not been studied experimentally. In addition, because the mechanism of the transferred HF interaction is considered to be the same as $\pi$-$d$ interaction in isostructural Fe-containing $\lambda$-type salts, our findings aid in the understanding of their physical properties.

cond-mat.str-el↗

arXiv2022

Role of hydrogen bonding in charge-ordered organic conductor $\alpha$-(BEDT-TTF)$_2$I$_3$ probed by $^{127}$I nuclear quadrupole resonance

We present $^{127}$I nuclear quadrupole resonance spectra and nuclear relaxation of $\alpha$-(BEDT-TTF)$_2$I$_3$ that undergoes a charge-ordering transition. Only one of the two I$_3$ anion sites shows a significant differentiation in the electric field gradients across the first-order transition. The charge modulation only in the BEDT-TTF layers can not reproduce; instead, an anion-donor interaction accompanied by hydrogen bonding is necessary. The dominating source for the nuclear relaxation is the local libration of the I$_3$ anions, but an anomalous peak is detected just below the transition, as observed by $^{13}$C NMR.

cond-mat.str-el↗

arXiv2022

Reduced superfluid density in a doped spin liquid candidate

A quantum spin liquid (QSL) would be an exotic stage for superconductivity. A promising candidate for a doped QSL is the organic triangular-lattice system, kappa-(BEDT-TTF)4Hg2:89Br8, which hosts a non-Fermi liquid and magnetism of a QSL nature and shows superconductivity upon cooling. Here, we report that its superfluid density is anomalously reduced, indicating the existence of substantial incoherent spectral weight and weak superconducting phase stiffness. Moreover, the ratio of the superconducting transition temperature to the nominal Fermi temperature is as large as 0.1, orders of magnitude beyond typical BCS values. These observations in a system free from competing orders that complicate the similar issue in underdoped cuprates give a clue to the enigmatic missing superfluid density in doped Mott insulators.

cond-mat.supr-con↗

arXiv2022

Thermoelectric signature of quantum critical phase in a doped spin liquid candidate

Quantum spin liquid is a nontrivial magnetic state of longstanding interest, in which spins are strongly correlated and entangled but do not order1, 2; further intriguing is its doped version, which possibly hosts strange metal and unconventional superconductivity3. Promising and currently the only candidate of the doped spin liquid is a triangular-lattice organic conductor, kappa-(BEDT-TTF)4Hg2.89Br8, recently found to hold metallicity, spin-liquid-like magnetism and BEC-like superconductivity4-6. The nature of the metallic state with the spin-liquid behaviour is awaiting to be further clarified. Here, we report the thermoelectric signature that mobile holes in the spin liquid background is in a quantum critical state and it pertains to the BEC-like superconductivity. The Seebeck coefficient divided by temperature, S/T, is enhanced on cooling with logarithmic divergence indicative of quantum criticality. Furthermore, the logarithmic enhancement is correlated with the superconducting transition temperature under pressure variation, and the temperature and magnetic field profile of S/T upon the superconducting transition change with pressure in a consistent way with the previously suggested BEC-BCS crossover. The present results reveal that the quantum criticality in a doped spin liquid emerges in a phase, not at a point, and is involved in the unconventional BEC-like nature.

cond-mat.str-el↗

arXiv2022

Mott-driven BEC-BCS crossover in a doped spin liquid candidate, kappa-(BEDT-TTF)4Hg2.89Br8

The pairing of interacting fermions leading to superfluidity has two limiting regimes: the Bardeen-Cooper-Schrieffer (BCS) scheme for weakly interacting degenerate fermions and the Bose-Einstein condensation (BEC) of bosonic pairs of strongly interacting fermions. While the superconductivity that emerges in most metallic systems is the BCS-like electron pairing, strongly correlated electrons with poor Fermi liquidity can condense into the unconventional BEC-like pairs. Quantum spin liquids harbor extraordinary spin correlation free from order and the superconductivity that possibly emerges by carrier doping of the spin liquids is expected to have a peculiar pairing nature. The present study experimentally explores the nature of the pairing condensate in a doped spin-liquid candidate material and under varying pressure, which changes the electron-electron Coulombic interactions across the Mott critical value in the system. The transport measurements reveal that the superconductivity at low pressures is a BEC-like condensate from a non-Fermi liquid and crosses over to a BCS-like condensate from a Fermi liquid at high pressures. The Nernst-effect measurements distinctively illustrate the two regimes of the pairing in terms of its robustness to the magnetic field. The present Mott tuning of the BEC-BCS crossover can be compared to the Feshbach tuning of the BEC-BCS crossover of fermionic cold atoms.

cond-mat.supr-con↗

arXiv2021

Antiferromagnetic ordering of organic Mott insulator $\lambda$-(BEDSe-TTF)$_2$GaCl$_4$

The band structure and magnetic properties of organic charge-transfer salt $\lambda$-(BEDSe-TTF)$_2$GaCl$_4$ (BEDSe-TTF: bis(ethylenediseleno)tetrathiafulvalene; abbreviated as $\lambda$-BEDSe) are investigated. The reported crystal structure is confirmed using X-ray diffraction measurements, and the transfer integrals are calculated. The degree of electron correlation $U/W$ ($U$: on-site Coulomb repulsion, $W$: bandwidth) of $\lambda$-BEDSe is larger than one and comparable to that of the isostructural Mott insulator $\lambda$-(ET)$_2$GaCl$_4$ (ET: bis(ethylenedithio)tetrathiafulvalene, abbreviated as $\lambda$-ET), whereas the $U/W$ of the superconducting salt $\lambda$-(BETS)$_2$GaCl$_4$ (BETS: bis(ethylenedithio)tetraselenafulvalene) is smaller than one. $^{13}$C-NMR and $\mu$SR measurements revealed that $\lambda$-BEDSe undergoes an antiferromagnetic (AF) ordering below $T_{\rm N} = 22$~K. In the AF state, discrete $^{13}$C-NMR spectra with a remaining central peak are observed, indicating the commensurate AF spin structure also observed in $\lambda$-ET. The similarity between the structural and magnetic properties of $\lambda$-BEDSe and $\lambda$-ET suggests that both salts are in the same electronic phase, i.e., the physical properties of $\lambda$-BEDSe can be understood by the universal phase diagram of bandwidth-controlled $\lambda$-type organic conductors obtained by donor molecule substitution.

cond-mat.str-el↗

arXiv2020

Charge disproportionation in the spin-liquid candidate $κ$-(ET)$_2$Cu$_2$(CN)$_3$ at 6 K revealed by $^{63}$Cu NQR measurements

The spin-liquid candidate $κ$-(ET)$_2$Cu$_2$(CN)$_3$ [ET: bis(ethylenedithio)tetrathiafulvalene] does not exhibit magnetic ordering down to a very low temperature, but shows a mysterious anomaly at 6 K. The origin of the so-called 6 K anomaly is still under debate. We carried out nuclear quadrupole resonance (NQR) measurements on the copper sites of the insulating layers, which are sensitive to the charge dynamics unlike the conventional spin-1/2 nuclear magnetic resonance (NMR). The main finding of this study is that the observation of a sharp peak behavior in the nuclear spin-lattice relaxation rate $T_1^{-1}$ of $^{63}$Cu NQR at 6 K while $T_1^{-1}$ of both $^{13}$C and $^{1}$H NMR show no clear anomaly. This behavior can be understood as a second-order phase transition related to charge disproportionation in the ET layers.

cond-mat.str-el↗

arXiv2020

Structural, physical and photocatalytic properties of mixed-valence double-perovskite Ba$_{2}$Pr(Bi,Sb)O$_{6}$ semiconductor synthesized by citrate pyrolysis technique

We demonstrated crystal structures, magnetic, optical, and photocatalytic properties of the B-site substituted double perovskite Ba$_{2}$Pr(Bi$_{1-x}$Sb$_{x}$)O$_{6}$ ($x$=0, 0.1, 0.2, 0.5 and 1.0) synthesized by the citrate pyrolysis method. The single-phase polycrystalline samples with the light Sb substitution crystallized in a monoclinic structure ($I2/m$). Magnetization measurements on all the samples showed that the effective magnetic moments are located around 3 $μ_{B}$ , indicating the valence mixing states between Pr$^{3+}$ and Pr$^{4+}$.The magnitudes of band gap energy for the two end member samples were estimated from the optical measurements to be $E_{g}$ =1.06 eV at $x$=0 and 2.71 eV at $x$=1.0. The Ba$_{2}$Pr(Bi$_{1-x}$Sb$_{x}$)O$_{6}$ ($x$=0, and 0.1) powders obtained by the present technique exhibited enhanced photocatalytic activities when compared to the same compounds prepared by the conventional solid state method. Our findings suggest that the higher photocatalytic activities strongly depend on powder preparation method as well as the band gaps and charge separation.

cond-mat.mtrl-sci↗

arXiv2018

Spectroscopic signature of trimer Mott insulator and charge disproportionation in BaIrO$_3$

We have measured the reflectivity spectra of the barium iridate $9R$ BaIrO$_3$, the crystal structure of which consists of characteristic Ir$_3$O$_{12}$ trimers. In the high-temperature phase above the transition temperature $T_c\simeq180$ K, we find that the optical conductivity involves two temperature-dependent optical transitions with an ill-defined Drude response. These features are reminiscent of the optical spectra in the organic dimer Mott insulators, implying a possible emergence of an unusual electronic state named trimer Mott insulator in BaIrO$_3$, where the carrier is localized on the trimer owing to the strong Coulomb repulsion. Along with a pronounced splitting of the phonon peak observed below $T_c$, which is a hallmark of charge disproportionation, we discuss a possible phase transition from the trimer Mott insulator to a charge-ordered insulating phase in BaIrO$_3$.

cond-mat.str-el↗

arXiv2017

Dimer-Mott and charge-ordered insulating states in the quasi-one-dimensional organic conductors $δ'_{P}$- and $δ'_{C}$-(BPDT-TTF)$_2$ICl$_2$

We investigated the electronic states of the quasi-one-dimensional organic conductors $δ'_{P}$-(BPDT-TTF)$_2$ICl$_2$ and $δ'_{C}$-(BPDT-TTF)$_2$ICl$_2$, both of which are insulating at room temperature owing to strong electron correlations. Through measurements of electrical resistivity, optical conductivity, and magnetic susceptibility, as well as band-structure calculations, we have revealed that the two materials possess completely different ground states, even though they have the same chemical composition and stacking configuration of the donor molecules. We have found that the $δ_P'$-type salt with an effective half-filled band behaves as a dimer-Mott (DM) insulator and exhibits a nonmagnetic transition at 25 K, whereas the $δ'_C$-type salt with a 3/4-filled band shows a charge ordering (CO) transition just above room temperature and becomes nonmagnetic below 20 K. The optical spectra of the $δ_P'$-type salt are composed of two characteristic bands due to intra- and interdimer charge transfers, supporting the DM insulating behavior arising from the strong on-site Coulomb interaction. By contrast, in the $δ'_C$-type salt, a single band characterizing the formation of CO arising from the off-site Coulomb interactions is observed. Upon lowering the temperature, the shape of the optical spectra in the $δ_C'$-type salt becomes asymmetric and shifts to much lower frequencies, suggesting the emergence of domain-wall excitations with fractional charges expected in a one-dimensional CO chain. The temperature dependence of the magnetic susceptibility of the $δ_P'$-type salt is well described by a 2D spin-1/2 Heisenberg AFM model on an anisotropic square lattice in the dimerized picture, while in the $δ_C'$-type salt, it can be explained by a 2D spin-1/2 Heisenberg AFM model on an anisotropic honeycomb lattice formed in the CO state.

cond-mat.str-el↗

arXiv2016

Spin-charge-entangled non-Fermi liquid in a candidate material for a doped spin liquid

Quantum spin liquids are exotic Mott insulators that carry extraordinary spin excitations and thus, when doped, expected to afford novel metallic states coupled to the unconventional magnetic excitations. The organic triangular-lattice system k-(ET)4Hg2.89Br8 is a promising candidate for the doped spin-liquid and hosts a non-Fermi liquid at low pressures. We show that, in the non-Fermi liquid regime, the charge transport confined in the layer gets deconfined sharply at low temperatures, coinciding with the entrance of spins into a quantum regime as signified by a steep decrease in spin susceptibility behaving like the triangular-lattice Heisenberg model indicative of spin-charge separation at high temperatures. This suggests a new type of non-Fermi liquid, where interlayer charge-deconfimement is associated with spin-charge entanglement.

cond-mat.str-el↗

arXiv2015

An Unconventional Phase Transition in BaAl2O4 Driven by Two Competing Soft Modes

We investigated the temperature dependence of the superlattice intensity and thermal diffuse scattering intensity of BaAl2O4, which has a network structure with corner-sharing AlO4 tetrahedra, via synchrotron X-ray diffraction experiments. The temperature variation of the superlattice intensity revealed that the structural phase transition occurs at TC = 451.4 K from the P6322 parent crystal structure to the low-temperature superstructure with a cell volume of 2a x 2b x c. BaAl2O4 exhibits an unconventional structural phase transition driven by two competing soft modes, q1/2 ~ (1/2, 1/2, 0) and q1/3 ~ (1/3, 1/3, 0). When approaching the TC from above, the soft mode with q1/3 appeared first and was followed by the q1/2 soft mode. The thermal diffuse scattering intensities from both soft modes increased sharply at TC; therefore, both modes condensed simultaneously. The first principles calculation revealed that structural instabilities exist at the M- and K-points, at which the calculated imaginary frequencies are similar. The small energy difference of these structural instabilities generates the two competing soft modes and determines the eventual low-temperature crystal structure.

cond-mat.mtrl-sci↗

arXiv2015

Emergence of charge degrees of freedom under high pressure in an organic dimer-Mott insulator $β^{\prime}$-(BEDT-TTF)$_2$ICl$_2$

To elucidate the pressure evolution of the electronic structure in an antiferromagnetic dimer-Mott (DM) insulator $β^{\prime}$-(BEDT-TTF)$_2$ICl$_2$, which exhibits superconductivity at 14.2 K under 8 GPa, we measured the polarized infrared (IR) optical spectra under high pressure. At ambient pressure, two characteristic bands due to intra- and interdimer charge transfers have been observed in the IR spectra, supporting that this salt is a typical half-filled DM insulator at ambient pressure. With increasing pressure, however, the intradimer charge transfer excitation shifts to much lower energies, indicating that the effective electronic state changes from half-filled to 3/4-filled as a result of weakening of dimerization. This implies that the system approaches a charge-ordered state under high pressure, in which charge degrees of freedom emerge as an important factor. The present results suggest that charge fluctuation inside of dimers plays an important role in the high-temperature superconductivity.

cond-mat.str-el↗

arXiv2014

Mottness in a doped organic superconductor

We report the pressure study of a doped organic superconductor with Hall coefficient and conductivity measurements. We find that maximally enhanced superconductivity and a non-Fermi liquid appear around a certain pressure where mobile carriers increase critically, suggesting a possible quantum phase transition between strongly and weakly correlated regimes. Our description extends the conventional picture of a Mott metal-insulator transition at half filling to the case of a doped Mott insulator with tunable correlation.

cond-mat.mtrl-sci↗

arXiv2013

Photo-Seebeck effect in tetragonal PbO single crystals

We report the observation of photo-Seebeck effect in tetragonal PbO crystals. The photo-induced carriers contribute to the transport phenomena, and consequently the electrical conductivity increases and the Seebeck coefficient decreases with increasing photon flux density. A parallel-circuit model is used to evaluate the actual contributions of photo-excited carriers from the measured transport data. The photo-induced carrier concentration estimated from the Seebeck coefficient increases almost linearly with increasing photon flux density, indicating a successful photo-doping effect on the thermoelectric property. The mobility decreases by illumination but the reduction rate strongly depends on the illuminated photon energy. Possible mechanisms of such photon-energy-dependent mobility are discussed.

cond-mat.mtrl-sci↗