arXiv subjects

Ichiro Terasaki

Publications and source records attributed to Ichiro Terasaki.

At least 19 recordsLinked to original sources

arXiv2025

Band-selective Plasmonic Polaron in Thermoelectric Semimetal Ta$_2$PdSe$_6$ with ultra-high power factor

We report the electronic structure of the thermoelectric semimetal Ta$_2$PdSe$_6$ with a large thermoelectric power factor and giant Peltier conductivity by means of angle-resolved photoemission spectroscopy (ARPES). The ARPES spectra reveal the coexistence of a sharp hole band with a light electron mass and a broad electron band with a relatively heavy electron mass, which originate from different quasi-one-dimensional (Q1D) chains in Ta$_2$PdSe$_6$. Moreover, the electron band around the Brillouin-zone (BZ) boundary shows a replica structure with respect to the energy originating from plasmonic polarons due to electron-plasmon interactions. The different scattering effects and interactions in each atomic chain lead to asymmetric transport lifetimes of carriers: a large Seebeck coefficient can be realized even in a semimetal. Our findings pave the way for exploring the thermoelectric materials in previously overlooked semimetals and provide a new platform for low-temperature thermoelectric physics, which has been challenging with semiconductors.

cond-mat.mtrl-sci↗

arXiv2025

Current-induced successive structural phase transitions beyond thermal equilibrium in single-crystal VO2

Nonequilibrium systems driven by external energy sources host unexplored physics; yet phase transitions beyond thermal equilibrium remain elusive. Here, we demonstrate that electric current induces structural phase transitions in single-crystal VO2, a prototypical strongly correlated material. At room temperature, synchrotron X-ray diffraction shows that a current density of 6.5 A/cm2 disrupts V-V dimers, driving a monoclinic-to-tetragonal insulator-to-metal transition, independent of Joule heating. Increasing the current to 10 A/cm2 triggers a discontinuous isotropic lattice expansion, stabilizing a novel tetragonal structure that does not exist in thermal equilibrium. Optical microscopy and microscopic Raman spectroscopy reveal dynamic domain motion and metastable phases, reminiscent of dissipative structures. These findings establish direct pathways to access hidden phases and symmetry changes beyond thermal equilibrium, broadening the frontiers of nonequilibrium thermodynamics.

cond-mat.str-el↗

arXiv2025

Current-induced Nonequilibrium Phase Transition Accompanied by Giant Gap Reduction in Vanadium Dioxide

We investigated nonlinear conduction in bulk single crystals of VO2 with precise temperature control. Two distinct nonequilibrium phenomena were identified: a gradual reduction of the charge gap and a current-induced insulator-metal transition. The electric field required to drive the nonlinear conduction is two to three orders of magnitude smaller than that reported for VO2 thin films or nanobeams, strongly indicating an intrinsic electronic origin rather than a temperature increase due to self heating. Notably, our results suggest that the application of a steady current to the frozen insulating state can induce a nonequilibrium steady-state metallic phase -- effectively melting the electronic ice. This highlights a novel route to controlling electronic states via nonthermal, current-driven mechanisms.

cond-mat.str-el↗

arXiv2024

Pressure-induced anomalous enhancement in superconducting critical temperature of transition-metal chalcogenide Ta$_2$PdS$_6$ and Ta$_2$PdSe$_6$

The emergence of a second dome in the superconducting phase through pressure-driven manipulation of crystal structures in materials has attracted considerable attention. Transition metal chalcogenides (TMCs) represent a highly promising platform, as the second dome has been observed in several binary compounds. Recently, ternary TMCs such as Ta$_2$PdS$_6$ and Ta$_2$PdSe$_6$ have exhibited pressure-induced superconducting domes. In this study, we perform electrical transport measurements of Ta$_2$PdS$_6$ and Ta$_2$PdSe$_6$ under extremely high pressures exceeding 100 GPa, namely uninvestigated regions in previous reports, to reveal the emergence of the second dome. The superconducting critical temperatures (T$_c$) in both Ta$_2$PdS$_6$ and Ta$_2$PdSe$_6$ initially decrease with increasing pressure. Subsequently, the Tcs tend to enhance drastically above 100 GPa. Notably, the maximum T$_c$ in Ta$_2$PdS$_6$ is 11.2 K at 130.0 GPa, which is a relatively high record among the TMCs. The emergence of the second dome in Ta$_2$PdS$_6$ and Ta$_2$PdSe$_6$ opens further motivation for the investigation under extreme conditions beyond the first dome to find hidden ordered phases.

cond-mat.supr-con↗

arXiv2024

Molecular orbital formation and metastable short-range ordered structure in VO$_2$

The metal-insulator transition (MIT) in vanadium dioxide VO$_2$ due to V-V dimerization has been extensively discussed for decades. While it is widely acknowledged that electron correlations, Peierls instabilities, and molecular orbital formations are crucial for understanding the MIT of VO$_2$, the primary origin of the MIT remains controversial. In this study, we delve into the crystal structure and orbital state of VO$_2$ through synchrotron x-ray diffraction experiments. The molecular orbital formation corresponding to the V-V dimerization is directly observed in the low-temperature insulating monoclinic phase, called the M1 phase, as indicated by the valence electron density distribution. Moreover, diffuse scattering observed in the high-temperature metal phase of rutile structure suggests the presence of short-range correlation of V displacements, which is not directly attributed to the structural fluctuation of the M1 phase. The short-range order in the rutile phase will be the key to understanding the MIT in this system.

cond-mat.str-el↗

arXiv2023

Antiferromagnetic order and consequences on the transport properties of Ba$_{4}$Ru$_{3}$O$_{10}$

Barium ruthenate Ba$_{4}$Ru$_{3}$O$_{10}$, in which Ru$_{3}$O$_{12}$ trimers are connected together to form a chequered two-dimensional framework, has been synthesised and its structural, magnetic and transport properties studied between 300 K and 2 K. The paramagnetic to antiferromagnetic transition at $T_N \sim 105$ K evidenced on the susceptibility curve coincides with an increase of electron localization in transport measurements. Thermoelectric power and Hall coefficient measurements both exhibit dramatic changes at $T_N$, characteristic of a reconstruction of the bands structure near the Fermi level. No pronounced structural changes are observed at TN in this compound. The magnetic scattering signal on the neutron powder diffraction patterns below $T_N$ is weak, but can be tentatively modelled with an antiferromagnetic ordering of the spins at both ends of a trimer, the spin of the more symmetric Ru site remaining idle. Crystal field and strong spin-orbit coupling at the Ru$^{4+}$ site seem to be the key parameters to understand the magnetic state of Ba$_{4}$Ru$_{3}$O$_{10}$.

cond-mat.str-el↗

arXiv2021

Giant Peltier Conductivity in an Uncompensated Semimetal Ta2PdSe6

Thermoelectric properties of single crystal Ta2PdSe6 is investigated by means of transport measurements, and a density functional calculation. We found a giant Peltier conductivity of 100 Acm-1K-1 at 10 K and successfully explained it by means of conventional semiconductor theory. We concluded that an uncompensated semimetal, high mobility, and heavy effective mass are responsible for the giant Peltier conductivity. Our finding opens a new ground in the field of thermoelectrics to explore much better semimetals for a new possible application such as an electric current generator for a superconducting magnet.

cond-mat.mtrl-sci↗

arXiv2021

Room Temperature Thermoelectric Properties of Isostructural Selenides Ta2PdS6 and Ta2PdSe6

We have measured thermoelectric properties of Ta2PdX6 (X=S, Se) around room temperature using single crystal samples. We find that the power factor of Ta2PdX6 is relatively high from middle-low to room temperatures, and notably Ta2PdSe6 shows the largest power factor among thermoelectric materials with an electrical conductivity of 10-2 Ωcm at 300 K. Ta2PdS6 will be a possible candidate for a Peltier cooling material if the lattice thermal conductivity is reduced by chemical substitution.

cond-mat.mtrl-sci↗

arXiv2019

Weak Ferroelectricity in n = 2 pseudo Ruddlesden-Popper-type niobate Li2SrNb2O7

Li2SrNb2O7 (LSNO) crystallizes in a structure closely related to n = 2 Ruddlesden-Popper-type compounds, which is gen-erally formed by intergrowth of 2-dimensional perovskite-type blocks and rocksalt-type layers. The present study demonstrates a coexistence of spontaneous polarization and anti-ferroelectric-like nonlinear response in LSNO at 80 K, suggesting a weak ferroelectricity below the phase transition temperature of 217 K. A combination of first-principles cal-culations and single crystal x-ray diffractions clarifies a polar P21cn structure for the ground state of LSNO, where an in-plane anti-ferroelectric displacement and an out-of-plane polar shift simultaneously take place. The present study offers a new perspective to design ferroelectric and antiferroelectric materials with Ruddlesden-Popper-type compounds.

cond-mat.mtrl-sci↗

arXiv2018

Dynamical coupling of dilute magnetic impurities with quantum spin liquid state in the S = 3/2 dimer compound Ba3ZnRu2O9

We have investigated the dilute magnetic impurity effect on the magnetic properties of a quantum spin liquid candidate Ba3ZnRu2O9 and a spin gapped compound Ba3CaRu2O9. The magnetic ground state of each compound stands against 2% substitution of magnetic impurities for Zn or Ca. We have found that the magnetic response of these impurities, which behave as paramagnetic spins, depends on the host materials and the difference of the two manifests itself in the Weiss temperature, which can hardly be explained by the dilute magnetic impurities alone in the case of Ba3ZnRu2O9. We consider a contribution from the Ru5+ ions which would appear only in the substituted Ba3ZnRu2O9 and discuss a possible physical meaning of the observed Weiss temperature.

cond-mat.str-el↗

arXiv2018

Enhanced thermopower via spin-state modification

We investigated the effect of pressure on the magnetic and thermoelectric properties of Sr$_{3.1}$Y$_{0.9}$Co$_{4}$O$_{10+δ}$. The magnetization is reduced with the application of pressure, reflecting the spin-state modification of the Co$^{3+}$ ions into the nonmagnetic low-spin state. Accordingly, with increasing pressure, the Seebeck coefficient is enhanced, especially at low temperatures, at which the effect of pressure on the spin state becomes significant. These results indicate that the spin-orbital entropy is a key valuable for the thermoelectric properties of the strongly correlated cobalt oxides.

cond-mat.str-el↗

arXiv2017

Anomalous Thermoelectric Response in an Orbital-Ordered Oxide Near and Far from Equilibrium

We report the thermoelectric transport properties in the orbital-ordered Mott insulating phase of Ca$_2$RuO$_4$ close to and far from equilibrium. Near equilibrium conditions where the temperature gradient is only applied to the sample, an insulating but non-monotonic temperature variation of the Seebeck coefficient is observed, which is accounted for in terms of a temperature-induced suppression of the orbital order. In non-equilibrium conditions where we have applied high electrical currents, we find that the Seebeck coefficient is anomalously increased in magnitude with increasing external current. The present result clearly demonstrates a non-thermal effect since the heating simply causes a decrease of the Seebeck coefficient, implying a non-trivial non-equilibrium effect such as a modification of the spin and orbital state in currents.

cond-mat.str-el↗

arXiv2017

Magneto-thermopower in the Weak Ferromagnetic Oxide CaRu0.8Sc0.2O3: An Experimental Test for the Kelvin Formula in a Magnetic Material

We have measured the resistivity, the thermopower, and the specific heat of the weak ferromagnetic oxide CaRu0.8Sc0.2O3 in external magnetic fields up to 140 kOe below 80 K. We have observed that the thermopower Q is significantly suppressed by magnetic fields at around the ferromagnetic transition temperature of 30 K, and have further found that the magneto-thermopower ΔQ(H, T) = Q(H, T) - Q(0, T) is roughly proportional to the magneto-entropy ΔS(H, T) = S(H, T)-S(0, T).We discuss this relationship between the two quantities in terms of the Kelvin formula, and find that the observed ΔQ is quantitatively consistent with the values expected from the Kelvin formula, a possible physical meaning of which is discussed.

cond-mat.str-el↗

arXiv2017

Absence of magnetic long range order in Ba$_3$ZnRu$_2$O$_9$: A spin-liquid candidate in the $S=3/2$ dimer lattice

We have discovered a novel candidate for a spin liquid state in a ruthenium oxide composed of dimers of $S = $ 3/2 spins of Ru$^{5+}$,Ba$_3$ZnRu$_2$O$_9$. This compound lacks a long range order down to 37 mK, which is a temperature 5000-times lower than the magnetic interaction scale of around 200 K. Partial substitution for Zn can continuously vary the magnetic ground state from an antiferromagnetic order to a spin-gapped state through the liquid state. This indicates that the spin-liquid state emerges from a delicate balance of inter- and intra-dimer interactions, and the spin state of the dimer plays a vital role. This unique feature should realize a new type of quantum magnetism.

cond-mat.str-el↗

arXiv2016

Intrinsic Enhancement of Dielectric Permittivity in (Nb + In) co-doped TiO2 single crystals

The development of dielectric materials with colossal permittivity is important for the miniaturization of electronic devices and fabrication of high-density energy-storage devices. The electron-pinned defect-dipoles has been recently proposed to boost the permittivity of (Nb + In) co-doped TiO2 to 105. However, the follow-up studies suggest an extrinsic contribution to the colossal permittivity from thermally excited carriers. Herein, we demonstrate a marked enhancement in the permittivity of (Nb + In) co-doped TiO2 single crystals at sufficiently low temperatures such that the thermally excited carriers are frozen out and exert no influence on the dielectric response. The results indicate that the permittivity attains quadruple of that for pure TiO2. This finding suggests that the electron-pinned defect-dipoles add an extra dielectric response to that of the TiO2 host matrix. The results offer a novel approach for the development of functional dielectric materials with large permittivity by engineering complex defects into bulk materials.

cond-mat.mtrl-sci↗

arXiv2016

Improper ferroelectricity in stuffed aluminate sodalites for pyroelectric energy harvesting

Ferroelectricity in stuffed aluminate sodalites is demonstrated in the present study. The present results indicate that stuffed aluminate sodalites exhibit excellent performance as a pyroelectric energy harvester, suggesting that they exhibit great promise as a class of materials for highly efficient energy harvesting devices. (See manuscript for the full abstract)

cond-mat.mtrl-sci↗

arXiv2016

Novel Charge Ordering in the Trimer Iridium Oxide BaIrO3

We have prepared polycrystalline samples of the trimer Ir oxide BaIrO3 with face-shared Ir3O12 trimers, and have investigated the origin of the phase transition at 182 K by measuring resistivity, thermopower, magnetization and synchrotron x-ray diffraction. We propose a possible electronic model and transition mechanism, starting from a localized electron picture on the basis of the Rietveld refinement. Within this model, BaIrO3 can be basically regarded as a Mott insulator, when the Ir3O12 trimer is identified to one pseudo-atom or one lattice site. The transition can be viewed as a transition from the Mott insulator phase to a kind of charge ordered insulator phase.

cond-mat.str-el↗

arXiv2016

Ferromagnetic Cluster Glass Phase Embedded in a Paramagnetic and Metallic Host in Non-uniform Magnetic System CaRu_{1-x}Sc_{x}O_{3}

We have investigated both static and dynamic magnetic properties of polycrystalline CaRu$_{1-x}$Sc$_{x}$O$_{3}$ system in order to clarify the role of Sc ions as a disorder for magnetic ordering. We have observed typical features of a ferromagnetic cluster glass state below around 40 K: (i) a broad, frequency-dependent peak in the ac magnetic susceptibility, (ii) a slow relaxation of the magnetization, and (iii) a continuous increase in the dc magnetic susceptibility in field cooling process. The composition dependence of characteristic parameters for the cluster glass state suggests that chemical segregation can hardly explain the clustering mechanism. We propose a possible picture that the ferromagnetic clusters are distributed uniformly and form the glassy state embedded in the paramagnetic and metallic host of CaRuO$_{3}$.

cond-mat.str-el↗