arXiv subjects

Naoyuki Katayama

Publications and source records attributed to Naoyuki Katayama.

At least 19 recordsLinked to original sources

arXiv2026

Observation of complex orbital order in MnV2O4

Orbital ordering in vanadium spinel oxides with a geometrically frustrated pyrochlore structure has been a subject of controversy, owing to competing theoretical models and the absence of direct experimental evidence. Here we combine high-precision single-crystal synchrotron x-ray diffraction with core differential fourier synthesis to visualize the valence electron density (VED) of the orbital-ordered ground state in real space. By carefully investigating multiple-scattering artifacts, we identify the low-temperature structure as belonging to the I41/amd space group. The reconstructed VED around the V sites reveals an orbital-ordered state distinct from both previously proposed real- and complex-orbital models. Our results resolve the long-standing controversy in MnV2O4 and establish a route to identifying orbital states in frustrated spin-orbital systems.

cond-mat.str-el↗

arXiv2026

Real-space determination of orbital states driving successive phase transitions in FeV2O4

Direct experimental access to orbital states in strongly correlated materials remains a major challenge, despite their central role in driving coupled structural and magnetic phase transitions. In systems where electronic correlations, electron-lattice coupling, and relativistic spin-orbit interactions compete on comparable energy scales, even first-principles calculations often yield multiple metastable solutions, hindering the unambiguous identification of the ground state. Here, we demonstrate that the orbital states of the spinel oxide FeV2O4, which possesses active orbital degrees of freedom on both Fe and V ions, are uniquely resolved by combining valence electron density (VED) analysis based on state-of-the-art synchrotron x-ray diffraction with spin-polarized density-functional-theory calculations. Our results reveal that temperature-dependent rearrangements of orbital occupations drive successive structural transitions that accompany collinear and noncoplanar ferrimagnetic orders, establishing a direct correspondence between orbital anisotropy and spin structure. More broadly, this work shows that experimentally determined VED provides a decisive real-space constraint on competing theoretical solutions, offering a powerful and broadly applicable framework for elucidating the microscopic mechanisms of complex phase transitions in strongly correlated electron systems.

cond-mat.str-el↗

arXiv2025

Superconductivity in High-Entropy Antimonide M$_{1-x}$Pt$_x$Sb (M = equimolar Ru, Rh, Pd, and Ir)

The high-entropy concept was applied to the synthesis of transition-metal antimonides, M1-xPtxSb (M = equimolar Ru, Rh, Pd, and Ir). High-entropy antimonide samples crystallized in a pseudo-hexagonal NiAs-type crystal structure with a P63/mmc space group were successfully synthesized through a conventional solid-state reaction and subsequent quenching. A detailed investigation of the composition and equilibration conditions confirmed the reversible phase transition between a multi-phase state at low temperature and an entropy-driven single-phase solid solution at high temperatures. Electrical resistivity, magnetization, and heat capacity measurements of single-phase M1-xPtxSb (x = 0.2) samples revealed a bulk superconducting transition at 2.15(2) K. This study demonstrates that the high-entropy concept provides numerous opportunities for the discovery of new functional materials such as superconductors.

cond-mat.supr-con↗

arXiv2025

Topological Electronic Structure and Transport Properties of the Distorted Rutile-type WO$_2$

We elucidate the transport properties and electronic structures of distorted rutile-type WO2. Electrical resistivity and Hall effect measurements of high-quality single crystals revealed the transport property characteristics of topological materials; these characteristics included an extremely large magnetoresistance of 13,200% (2 K and 9 T) and a very high carrier mobility of 25,700 cm2 V-1 s-1 (5 K). First-principles calculations revealed Dirac nodal lines (DNL) near the Fermi energy in the electronic structure when spin-orbit interactions (SOIs) were absent. Although these DNLs mostly disappeared in the presence of SOIs, band crossings at high-symmetry points in the reciprocal space existed as Dirac points. Furthermore, DNLs protected by nonsymmorphic symmetry persisted on the ky = π/b plane. The unique transport properties originating from the topological electronic structure of chemically and thermally stable WO2 could represent an opportunity to investigate the potential electronic applications of the material.

cond-mat.mtrl-sci↗

arXiv2024

Odd-parity multipole order in the spin-orbit coupled metallic pyrochlore Pb$_2$Re$_2$O$_{7-δ}$

The pyrochlore oxide Pb2Re2O7-δ (PRO) is a candidate spin-orbit-coupled metal (SOCM) that exhibits a structural phase transition with inversion symmetry breaking. In this study, we report the results of detailed X-ray diffraction (XRD) measurements on single crystals of PRO to clarify the crystal structure below the phase transition temperature at Ts = 300 K. In the XRD patterns, a clear peak splitting is observed below Ts, indicating a cubic to tetragonal transition. Based on the group-subgroup relationship and the observed reflection conditions, the space group of the low-temperature phase is proposed to be I4122, which agrees with optical second harmonic generation measurements. This space group is the same as that of the lowest temperature structure of the analogous SOCM Cd2Re2O7 (CRO), which is realized by the emergence of odd-parity multipole order. The comparison between PRO and CRO allows for advancing our understanding on the symmetry-lowering complex order exhibited by SOCMs.

cond-mat.str-el↗

arXiv2023

Fermi surface and light quasi particles in hourglass nodal chain metal \b{eta}-ReO2

Quantum oscillations in magnetic torque and electrical resistivity were measured to investigate the electronic structure of \b{eta}-ReO2, a candidate hourglass nodal chain metal (Dirac loop chain metal). All the de Haas-van Alphen oscillation branches measured at 30 mK in magnetic fields of up to 17.5 T were consistent with first-principles calculations predicting four Fermi surfaces (FSs). The small-electron FS of the four FSs exhibited a very small cyclotron mass, 0.059 times that of the free electrons, which is likely to be related to the linear dispersion of the energy band. The consistency between the quantum oscillation results and band calculations indicates the presence of the hourglass nodal chain predicted for \b{eta}-ReO2 in the vicinity of the Fermi energy.

cond-mat.str-el↗

arXiv2023

Linear Trimer Formation by Three-Center-Four-Electron Bonding in RuP

In molecules like hydrogen, most chemical bonds are formed by sharing two electrons from each atom in the bonding molecular orbital (two-center-two-electron (2c2e) bonding). There are, however, different kinds of chemical bonding. The I3- molecule, for example, is noteworthy because three iodine atoms are linearly united by sharing four electrons (three-center-four-electron (3c4e) bonding). Some inorganic solids undergo phase transitions that result in the formation of "molecules" in their crystalline frameworks, which are often accompanied by dramatic changes in physical properties; the metal-to-insulator transition (MIT) in vanadium dioxide, for example, occurs with the formation of dimer molecules with 2c2e bonding. We repot the creation of a linear ruthenium trimer with 3c4e bonding in ruthenium monopnictide at its MIT. Charge transfer from polymerized phosphorous to ruthenium produces this unusual molecule, with all conduction electrons trapped by the bonding molecular orbital. Our results demonstrate that molecules are crucial even in solid crystals as they impact their electronic properties.

cond-mat.str-el↗

arXiv2023

Structural and Electronic Properties of a Triangular Lattice Magnet NaPrTe$_2$ Compared with NaNdTe$_2$ and NaTbTe$_2$

NaPrTe2, NaNdTe2, and NaTbTe2 are found to be triangular lattice magnets with the alpha-NaFeO2 structure, where lanthanoid atoms with 4f electrons form a triangular lattice, based on the structural analysis and physical property measurements of synthesized polycrystalline samples. The alpha-NaFeO2 structure is a new polymorph of NaPrTe2, which has been reported to crystallize in the cubic LiTiO2 structure. Polytypism in NaPrTe2 was discussed based on the structural parameters determined by the Rietveld analysis. NaPrTe2 is suggested to be in the proximity of the phase boundary between the LiTiO2 and alpha-NaFeO2 types, as compared to NaNdTe2 and NaTbTe2, indicating that this compound might be interesting from the perspectives of the dimensional control of geometrically frustrated lattices. The magnetic susceptibility and heat capacity data indicated that NaPrTe2 do not show long-range magnetic order or a spin-glass transition above 2 K.

cond-mat.mtrl-sci↗

arXiv2021

Charge-ordered state satisfying the Anderson condition in LiRh2O4 arising from local dimer order

We report on the charge-ordered structure of LiRh2O4 arising below the metal-insulator transition at 170 K. Structural studies using synchrotron X-rays have revealed that the charge-ordered states of Rh3+ and Rh4+ with dimerization are realized in the low-temperature phase below 170 K. Although the low-temperature ground state resembles that of CuIr2S4, a charge ordering pattern satisfying the Anderson condition is realized in LiRh2O4. Based on structural information such as the short-range order of dimers appearing above the transition temperature and the weakening of the correlation between rhodium one-dimensional chains appearing in the crystal structure, we argue that the Coulomb interaction plays an important role in determining the charge ordering patterns.

cond-mat.str-el↗

arXiv2021

Hybridization-gap Formation and Superconductivity in the Pressure-induced Semimetallic Phase of the Excitonic Insulator Ta$_2$NiSe$_5$

The excitonic insulator Ta$_2$NiSe$_5$ experiences a first-order structural transition under pressure from rippled to flat layer-structure at Ps = 3 GPa, which drives the system from an almost zero-gap semiconductor to a semimetal. The pressure-induced semimetal, with lowering temperature, experiences a transition to another semimetal with a partial-gap of 0.1-0.2 eV, accompanied with a monoclinic distortion analogous to that occurs at the excitonic transition below Ps. We argue that the partial-gap originates primarily from a symmetry-allowed hybridization of Ta-conduction and Ni-valence bands due to the lattice distortion, indicative of the importance of electron-lattice coupling. The transition is suppressed with increasing pressure to Pc = 8 GPa. Superconductivity with a maximum Tsc = 1.2 K emerges around Pc, likely mediated by strongly electron-coupled soft phonons. The electron-lattice coupling is as important ingredient as the excitonic instability in Ta2NiSe5.

cond-mat.str-el↗

arXiv2021

Slow dynamics of disordered zigzag chain molecules in layered LiVS2 under electron irradiation

Electronic instabilities in transition metal compounds often spontaneously form orbital molecules, which consist of orbital-coupled metal ions at low temperature. Recent local structural studies utilizing the pair distribution function revealed that preformed orbital molecules appear disordered even in the high-temperature paramagnetic phase. However, it is unclear whether preformed orbital molecules are dynamic or static. Here, we provide clear experimental evidence of the slow dynamics of disordered orbital molecules realized in the high-temperature paramagnetic phase of LiVS2, which exhibits vanadium trimerization upon cooling below 314 K. Unexpectedly, the preformed orbital molecules appear as a disordered zigzag chain that fluctuate in both time and space under electron irradiation. Our findings should advance studies on soft matter physics realized in an inorganic material due to disordered orbital molecules.

cond-mat.str-el↗

arXiv2021

Ambient pressure Dirac electron system in quasi-two-dimensional molecular conductor $α$-(BETS)$_2$I$_3$

We investigated the precise crystal structures and electronic states in a quasi-two-dimensional molecular conductor $α$-(BETS)$_2$I$_3$ at ambient pressure. The electronic resistivity of this molecular solid shows metal-to-insulator (MI) crossover at $T_{MI}$=50 K. Our x-ray diffraction and $^{13}$C nuclear magnetic resonance experiments revealed that $α$-(BETS)$_2$I$_3$ maintains the inversion symmetry below $T_{MI}$. First-principles calculations found a pair of anisotropic Dirac cones at a general k-point, with the degenerate contact points at the Fermi level. The origin of the insulating state in this system is a small energy gap of ~2 meV opened by the spin-orbit interaction. The Z$_2$ topological invariants indicate that this system is a weak topological insulator. Our results suggest that $α$-(BETS)$_2$I$_3$ is a promising material for studying the bulk Dirac electron system in two dimensions.

cond-mat.str-el↗

arXiv2020

High-Mobility Carriers Induced by Chemical Doping in the Candidate Nodal-Line Semimetal CaAgP

We report the electronic properties of single crystals of candidate nodal-line semimetal CaAgP. The transport properties of CaAgP are understood within the framework of a hole-doped nodal-line semimetal. In contrast, Pd-doped CaAgP shows a drastic increase of magnetoresistance at low magnetic fields and a strong decrease of electrical resistivity at low temperatures probably due to weak antilocalization. Hall conductivity data indicated that the Pd-doped CaAgP has not only hole carriers induced by the Pd doping, but also high-mobility electron carriers in proximity of the Dirac point. Electrical resistivity of Pd-doped CaAgP also showed a superconducting transition with onset temperature of 1.7-1.8 K.

cond-mat.mtrl-sci↗

arXiv2020

Detecting electron-phonon couplings during photo-induced phase transition

Photo-induced phase transitions have been intensively studied owing to the ability to control a material of interest in the ultrafast manner, which can induce exotic phases unable to be attained at equilibrium. However, the key mechanisms are still under debate, and it has currently been a central issue how the couplings between the electron, lattice, and spin degrees of freedom are evolving during photo-induced phase transitions. Here, we develop a new analysis method, frequency-domain angle-resolved photoemission spectroscopy, to gain precise insight into electron-phonon couplings during photo-induced insulator-to-metal transitions for Ta$_2$NiSe$_5$. We demonstrate that multiple coherent phonons generated by displacive excitations show band-selective coupling to the electrons. Furthermore, we find that the lattice modulation corresponding to the 2 THz phonon mode, where Ta lattice is sheared along the a-axis, is the most relevant for the photo-induced semimetallic state.

cond-mat.str-el↗

arXiv2020

Regular-Triangle Trimer and Charge Order Preserving the Anderson Condition in the Pyrochlore Structure of CsW$_2$O$_6$

Since the discovery of the Verwey transition in magnetite, transition metal compounds with pyrochlore structures have been intensively studied as a platform for realizing remarkable electronic phase transitions. We report the discovery of a unique phase transition that preserves the cubic symmetry of the beta-pyrochlore oxide CsW$_2$O$_6$, where each of W 5d electrons are confined in regular-triangle W3 trimers. This trimer formation is an unprecedented self-organization of d electrons, which can be resolved into a charge order satisfying the Anderson condition in a nontrivial way, orbital order caused by the distortion of WO6 octahedra, and the formation of a spin-singlet pair in a regular-triangle trimer. Electronic instability due to the unusual three-dimensional nesting of Fermi surfaces and the localized nature of the 5d electrons characteristic of the pyrochlore oxides were found to play important roles in this unique charge-orbital-spin coupled phenomenon.

cond-mat.mtrl-sci↗

arXiv2019

Effect of Cu intercalation and pressure on excitonic interaction in 1T-TiSe2

1T-TiSe2 has a semimetallic band structure at room temperature and undergoes phase transition to a triple-q charge density wave (CDW) state with a commensurate superlattice structure (2a * 2a * 2c) below Tc ~ 200 K at ambient pressure. This phase transition is caused by cooperative phenomena involving electron-phonon and electron-hole (excitonic) interactions, and cannot be described by a standard CDW framework. By Cu intercalation or the application of pressure, this phase transition temperature is suppressed and superconductivity (SC) appears. However, it is not clear what kind of order parameters are affected by these two procedures. We investigated the crystal structure of CuxTiSe2 and pressurized 1T-TiSe2 around the SC state by synchrotron x-ray diffraction on single crystals. In the high-temperature phase, the variation of structural parameters for the case of Cu intercalation and application of pressure are considerably different. Moreover, the relationship between the critical points of the CDW phase transition and the SC dome are also different for the two cases. The excitonic interaction appears to play an important role in the P-T phase diagram of 1T-TiSe2, but not in the x-T phase diagram.

cond-mat.str-el↗

arXiv2018

Photo-induced semimetallic states realised in electron-hole coupled insulators

Using light to manipulate materials into desired states is one of the goals in condensed matter physics, since light control can provide ultrafast and environmentally-friendly photonics devices. However, it is generally difficult to realise a photo-induced phase which is not merely a higher entropy phase corresponding to a high-temperature phase at equilibrium. Here, we report realization of photo-induced insulator-to-metal transitions in Ta2Ni(Se1-xSx)5 including the excitonic insulator phase using time- and angle-resolved photoemission spectroscopy. From the dynamic properties of the system, we determine that screening of excitonic correlations plays a key role in the timescale of the transition to the metallic phase, which supports the existence of an excitonic-insulator phase at equilibrium. The non-equilibrium metallic state observed unexpectedly in the direct-gap excitonic insulator opens up a new avenue to optical band engineering in electron-hole coupled systems.

cond-mat.mtrl-sci↗

arXiv2018

Inhibition of the photoinduced structural phase transition in the excitonic insulator Ta$_2$NiSe$_5$

Femtosecond time-resolved mid-infrared reflectivity is used to investigate the electron and phonon dynamics occurring at the direct band gap of the excitonic insulator Ta$_2$NiSe$_5$ below the critical temperature of its structural phase transition. We find that the phonon dynamics show a strong coupling to the excitation of free carriers at the Γ point of the Brillouin zone. The optical response saturates at a critical excitation fluence $F_C = 0.30~\pm~0.08$~mJ/cm$^2$ due to optical absorption saturation. This limits the optical excitation density in Ta$_2$NiSe$_5$ so that the system cannot be pumped sufficiently strongly to undergo the structural change to the high-temperature phase. We thereby demonstrate that Ta$_2$NiSe$_5$ exhibits a blocking mechanism when pumped in the near-infrared regime, preventing a nonthermal structural phase transition.

cond-mat.str-el↗