arXiv subjects

Hidetomo Usui

Publications and source records attributed to Hidetomo Usui.

At least 19 recordsLinked to original sources

arXiv2026

Ideal band structures for high-performance thermoelectric materials with band convergence

We investigate optimal band structures in band-converged systems to achieve high zT using numerical calculations based on a virtual spectral conductivity model. We consider a two parabolic band system, in which multiple band parameters can be independently controlled. Despite its simplicity, this model provides theoretical validation of empirical trends observed in thermoelectric materials. Our results provide a physically transparent set of design principles for band-structure engineering, offering quantitative design guidelines for the development of a wide range of thermoelectric materials. The main conclusions are as follows: (i) When a band does not cross the chemical potential and |μ-E_edge |>5k_B T, the contribution of the band to zT is negligibly small; (ii) To suppress the bipolar effect, a band gap E_g satisfying E_g>5k_B T_op, where T_op is the operating temperature, is required; (iii) In band-converged systems, the energy separation between the band edge ΔE should satisfy ΔE~0 to maximize zT when interband scattering is insignificant; (iv) Achieving high spectral conductivity Σ (high band degeneracy N, density of states effective mass m_DOS^*, and relaxation time τ) near the band edge is essential for achieving high zT.

cond-mat.mtrl-sci↗

arXiv2025

Theoretical study on the possibility of high $T_c$ s$\pm$-wave superconductivity in the heavily hole-doped infinite layer nickelates

We theoretically propose a possibility of realizing high $T_c$ superconductivity having $s\pm$-wave symmetry in the heavily hole-doped infinite layer nickelates La$_{1-x}$Sr$_x$NiO$_2$. We consider situations where the original $P4/mmm$ symmetry of LaNiO$_2$ is maintained even for a significant amount of Sr substitution by growing thin films on substrates having tetragonal symmetry. Considering such cases is indeed justified by our phonon calculations. For electron configurations somewhat close to $d^8$, the interaction between the $d_{x^2-y^2}$ band and the other $3d$ bands that lie just below the Fermi level results in an enhancement of superconductivity where the sign of the gap function is reversed between the former and the latter bands. The strong enhancement of superconductivity can be attributed to the large energy level offset between $d_{x^2-y^2}$ and other orbitals due to the absence of the apical oxygens, as has been pointed out in previous studies.

cond-mat.supr-con↗

arXiv2025

Theoretical study of the crystal structure of the bilayer nickel oxychloride Sr$_3$Ni$_2$O$_5$Cl$_2$ and analysis of possible unconventional superconductivity

The discovery of superconductivity under high pressure with $T_c$ exceeding 80 K in a bilayer nickelate La$_3$Ni$_2$O$_7$ has led to a strong desire to realize similar high $T_c$ phenomena at ambient pressure. As one possible path toward realizing superconductivity at ambient pressure, we here propose to consider Sr$_3$Ni$_2$O$_5$Cl$_2$ as a possible candidate. In this study, we theoretically investigate the electronic structure of Sr$_3$Ni$_2$O$_5$Cl$_2$ and its structural stability. Our phonon calculation shows that this compound with the $I4/mmm$ tetragonal structure is dynamically stable even at ambient pressure. The characteristic crystal field in this compound lowers the Ni-$d_{3z^2-r^2}$ orbital energy, by which the Ni-$d_{3z^2-r^2}$ orbital becomes rather closer to the half-filling in Sr$_3$Ni$_2$O$_5$Cl$_2$ than La$_3$Ni$_2$O$_7$. As a result, we find that superconductivity is enhanced even though a relatively strong orbital hybridization between the $t_{2g}$ and $e_g$ orbitals is somewhat detrimental for superconductivity. We also check the formation enthalpy, which shows that the high-pressure synthesis can be a good way to actually produce Sr$_3$Ni$_2$O$_5$Cl$_2$. We find that Sr$_3$Ni$_2$O$_5$Cl$_2$ is a promising new candidate of bilayer-nickelate superconductors, which can possess even higher $T_c$ than pressurized La$_3$Ni$_2$O$_7$, at ambient pressure.

cond-mat.supr-con↗

arXiv2023

Pressure-induced volumetric negative thermal expansion in CoZr2 superconductor

We investigate the thermal expansion and superconducting properties of a CuAl2-type (tetragonal) superconductor CoZr2 under high pressures. We perform high-pressure synchrotron X-ray diffraction in a pressure range of 2.9 GPa < P < 10.4 GPa and discover that CoZr2 exhibits volumetric negative thermal expansion under high pressures. Although the uniaxial positive thermal expansion (PTE) along the a-axis is observed under ambient pressure, that is suppressed by pressure, while the large uniaxial negative thermal expansion (NTE) along the c-axis is maintained under the pressure regime. As a result of a combination of the suppressed uniaxial PTE along the a-axis and uniaxial NTE along the c-axis, volumetric negative thermal expansion is achieved under high pressure in CoZr2. The mechanisms of volumetric NTE would be based on the flexible crystal structure caused by the soft Co-Co bond as seen in the iso-structural compound FeZr2, which exhibits uniaxial NTE along the c-axis. We also perform high-pressure electrical resistance measurements of CoZr2 to confirm the presence of superconductivity under the examined pressure regime in the range of 0.03 GPa < P < 41.9 GPa. We confirm the presence of superconductivity under all pressures and observe dome-like shape pressure dependence of superconducting transition temperature. Because of the coexistence of two phenomena, which are volumetric NTE and superconductivity, in CoZr2 under high pressure, the coexistence would be achievable under ambient pressure by tuning chemical compositions after our present observation.

cond-mat.mtrl-sci↗

arXiv2022

Sign change in c-axis thermal expansion and lattice collapse by Ni substitution in Co1-xNixZr2 superconductors

We investigated the structural, electronic, and superconducting properties of Co1-xNixZr2, in which c-axis thermal expansion is systematically controlled. At x (smaller than) 0.3, c-axis negative thermal expansion (NTE) was observed, and the thermal expansion constant αc approached zero with increasing x. At x = 0.4-0.6, zero thermal expansion was observed, and positive thermal expansion (PTE) appeared for x (greater than) 0.7. By analyzing the c/a ratio, we observed a possible collapsed transition in the tetragonal lattice at around x = 0.6-0.8. The lattice collapse results in c-axis PTE and the suppression of bulk superconductivity.

cond-mat.supr-con↗

arXiv2022

Glassy atomic vibrations and blurry electronic structures created by local structural disorders in high-entropy metal telluride superconductors

The motivation of this work is our recent observation of the robustness of superconductivity in a High-entropy (HE) superconductor Ag0.2In0.2Sn0.2Pb0.2Bi0.2Te (CsCl-type) to external pressure. The superconducting transition temperature (Tc) of Ag0.2In0.2Sn0.2Pb0.2Bi0.2Te is almost constant with pressure, described as robustness of superconductivity to pressure, whereas the PbTe with zero configurational entropy of mixing exhibits a clear decrease in Tc with pressure. Here, we investigated the atomic displacement parameters (Uiso), the atomic-vibration characteristics, and the electronic states of metal tellurides (MTe) with various configurational entropy of mixing (DSmix) at the M site. The Uiso for the M site is clearly increased by M-site alloying with DSmix > 1.1R, which is the evidence of local disorder introduced by the increase in DSmix via the solution of three or more M elements. The revealed vibrational density of states (DOS) shows a remarkable broadening with DSmix > 1.1R, which indicates glassy characteristics of atomic vibration in HE MTe with a NaCl-type structure (low-pressure phase). On the electronic states of the CsCl-type (high-pressure) phases, where the robustness of Tc is observed, blurry electronic band structure appears with increasing DSmix, which indicates the evolution of blurry (glassy) electronic states in HE MTe with the CsCl-type structure. The estimated electronic DOS at Fermi energy cannot explain the changes in Tc for HE MTe when assuming conventional electron-phonon superconductivity, but the conventional explanation seems to work for PbTe. Therefore, the pairing mechanisms in MTe with DSmix > 1.1R are affected by glassy phonon and/or blurry electronic states in MTe, and the robustness of superconductivity would be originating from unique electron-phonon coupling.

cond-mat.supr-con↗

arXiv2021

Superconductivity in In-doped AgSnBiTe3 with possible band inversion

We investigated the chemical pressure effects on structural and electronic properties of SnTe-based material using partial substitution of Sn by Ag0.5Bi0.5, which results in lattice shrinkage. For Sn1-2x(AgBi)xTe, single-phase polycrystalline samples were obtained with a wide range of x. On the basis of band calculations, we confirmed that the Sn1-2x(AgBi)xTe system is basically possessing band inversion and topologically preserved electronic states. To explore new superconducting phases related to the topological electronic states, we investigated the In-doping effects on structural and superconducting properties for x = 0.33 (AgSnBiTe3). For (AgSnBi)(1-y)/3InyTe, single-phase polycrystalline samples were obtained for y = 0-0.5 by high-pressure synthesis. Superconductivity was observed for y = 0.2-0.5. For y = 0.4, the transition temperature estimated from zero-resistivity state was 2.4 K, and the specific heat investigation confirmed the emergence of bulk superconductivity. Because the presence of band inversion was theoretically predicted, and the parameters obtained from specific heat analyses were comparable to In-doped SnTe, we expect that the (AgSnBi)(1-y)/3InyTe and other (Ag,In,Sn,Bi)Te phases are candidate systems for studying topological superconductivity.

cond-mat.supr-con↗

arXiv2020

Possible pairing mechanism switching driven by structural symmetry breaking in BiS2-based layered superconductors

Investigation of isotope effects on superconducting transition temperature (Tc) is one of the useful methods to examine whether electron-phonon interaction is essential for pairing mechanisms. The layered BiCh2-based (Ch: S, Se) superconductor family is a candidate for unconventional superconductors, because unconventional isotope effects have previously been observed in La(O,F)BiSSe and Bi4O4S3. In this study, we investigated the isotope effects of 32S and 34S in the high-pressure phase of (Sr,La)FBiS2, which has a monoclinic crystal structure and a higher Tc of 10 K under high pressures, and observed conventional-type isotope shifts in Tc. The conventional-type isotope effects in the monoclinic phase of (Sr,La)FBiS2 are different from the unconventional isotope effects observed in La(O,F)BiSSe and Bi4O4S3, which have a tetragonal structure. The obtained results suggest that the pairing mechanisms of BiCh2-based superconductors could be switched by a structural-symmetry change in the superconducting layers induced by pressure effects.

cond-mat.supr-con↗

arXiv2020

First principles study on the thermoelectric performance of CaAl$_2$Si$_2$-type Zintl phase compounds

We investigate the thermoelectric properties of CaAl$_2$Si$_2$-type Zintl phase compounds $AB_2X_2$ ($A$ = Mg, Ca, Sr, Ba, $B$ = Mg, Zn, Cd, and $X$ = P, As, Sb) using first principles band calculations within the Boltzmann transport theory assuming the constant relaxation time approximation. We introduce the effective degree of valley degeneracy $n_{TE}$ to focus on the relationship between the thermoelectric properties and the multivalley character of the electronic band structure around the Fermi level. We also introduce a quantity $γ_{TE}$, which takes into account $n_{TE}$ and anisotropy of the valley structure, and it is found that $γ_{TE}$ enables us to well understand the overall trend of the material dependence of the power factor. We finally suggest promising thermoelectric materials, e.g. BaMg$_2$P$_2$ for PF $\sim 20μ$W/cmK$^2$ and $ZT > 0.2$ at 300K and SrZn$_2$As$_2$ for PF $\sim 35μ$W/cmK$^2$ and $ZT > 0.35$ at 300K assuming a relaxation time of 10 fs and a lattice thermal conductivity value of 2 W/mK.

cond-mat.mtrl-sci↗

arXiv2020

Electronic Structure of $\mathrm{Sr}_{1-y}\mathrm{Ca}_{y}\mathrm{Fe_{2}}(\mathrm{As}_{1-x}\mathrm{P}_{x}\mathrm{)_{2}}$ ($x$ = 0.25, $y$ = 0.08) Revealed by Angle-Resolved Photoemission Spectroscopy

We have investigated the electronic structure of $\mathrm{Sr}_{1-y}\mathrm{Ca}_{y}\mathrm{Fe_{2}}(\mathrm{As}_{1-x}\mathrm{P}_{x}\mathrm{)_{2}}$ ($x$ = 0.25, $y$ = 0.08) by means of angle-resolved photoemission spectroscopy. From the comparison with the results of $\mathrm{BaFe_{2}}(\mathrm{As}_{1-x}\mathrm{P}_{x}\mathrm{)_{2}}$, the effects of smaller structural anisotropy ($c/a$) on the Fermi surfaces (FSs) and the gap structures are discussed. The observed FSs have three dimensional shapes. One of the hole FSs is strongly warped between the $Γ$ and $Z$ points, and the innermost FS observed at the $Z$ point disappears at the $Γ$ point, which is similar to the FS features of $\mathrm{SrFe_{2}}(\mathrm{As}_{1-x}\mathrm{P}_{x}\mathrm{)_{2}}$ ($x$ = 0.35). In the superconducting state, the node like gap-minimum is present for the $d_{xy}$ electron FS near the $X$ point, while the gaps around the other high symmetry points are isotropic. Several theoretical models based on the spin and/or the orbital fluctuation are examined to explain all these experimental results.

cond-mat.supr-con↗

arXiv2019

Pressure-induced superconductivity in layered pnictogen diselenide NdO$_{0.8}$F$_{0.2}$Sb$_{1-x}$Bi$_x$Se$_2$ (x = 0.3 and 0.7)

Polycrystalline samples of layered pnictogen diselenide NdO0.8F0.2Sb1-xBixSe2 (x = 0 to 0.8) were successfully synthesized by solid-state reactions. Electrical resistivity in the synthesized samples was systematically decreased with an increase in Bi content x. Crystal structure analysis using synchrotron X-ray diffraction suggests that insulator to metal transition upon Bi doping correlates with anomalous change in c-axis length and/or corrugation in conducting layer. The emergence of superconductivity under high pressure is demonstrated using diamond anvil cell (DAC) with boron-doped diamond electrodes, for x = 0.3 and 0.7 as the representative samples. For Sb-rich one (x = 0.3), we observed a superconducting transition with Tconset = 5.3 K at 50 GPa, which is the first-ever report of the superconductivity in layered SbCh2-based (Ch: chalcogen) compounds. The Tconset of x = 0.3 increased with increasing pressure and reached 7.9 K at 70.8 GPa, followed by the gradual decrease in Tc up to 90 GPa. For Bi-rich one (x = 0.7), a superconducting transition with Tconset = 5.9 K was observed at 43.5 GPa, which is the almost comparable to that of x = 0.3; besides, upper critical field (Hc2) is evaluated to be ~10 T for x = 0.7, which is higher than that of x = 0.3 (Hc2 = 6.7 T at 50 GPa).

cond-mat.supr-con↗

arXiv2019

Model construction and a possibility of cuprate-like pairing in a new d9 nickelate superconductor (Nd,Sr)NiO2

Effective models are constructed for a newly discovered superconductor (Nd,Sr)NiO2, which has been considered as a possible nickelate analogue of the cuprates owing to the d9 electron configuration. Estimation of the effective interaction, which turns out to require a multiorbital model that takes account of all the orbitals involved on the Fermi surface, shows that the effective interactions are significantly larger than in the cuprates. A fluctuation exchange study for the model indicates that dx2-y2-wave superconductivity is likely to occur as in the cuprates, where the transition temperature in the nickelate can be lower from the cuprates due to the larger interaction and narrower bandwidth.

cond-mat.supr-con↗

arXiv2019

First-principles study of LaOPbBiS$_3$ and its analogous compounds as thermoelectric materials

LaOBiPbS$_3$ is a kind of pnictogen-dichalcogenide layered compounds, which have recently been experimentally investigated as thermoelectric materials owing to their low thermal conductivity and high controllability of constituent elements. However, thermoelectric performance of LaOBiPbS$_3$ is at present not very high and that of its analogous compounds remains to be unknown. In this study, we theoretically investigate thermoelectric properties of 24 possible variations of the constituent elements in LaOBiPbS$_3$ from the viewpoint of the electronic structure. We find that some compounds can have much better thermoelectric performance than LaOBiPbS$_3$; in particular, LaOSbPbSe$_3$ is predicted to have a power factor five times as large as that of LaOBiPbS$_3$. Here, the choice of the pnictogen atom (As, Sb, and Bi), of which the low-energy conduction bands mainly consist, correlates with the calculated power factor and the dimensionless figure of merit, $ZT$. Such correlation comes from the fact that the low-dimensionality of the electronic structure, which enhances the density of states near the band edge, strongly depends on the pnictogen atom through, e.g., the strength of the spin-orbit coupling. Moreover, hybridization of the wave functions in the pnictogen-dichalcogenide layer and those in the rock-salt layer plays a key role in gap opening, and thus is important for achieving high thermoelectric performance. In LaOSbPbSe$_3$, such hybridization also pushes up the conduction band bottom, which enhances the density of states near the band edge and thus the power factor.

cond-mat.mtrl-sci↗

arXiv2019

Hidden robust presence of a hole Fermi surface in a heavily electron doped iron based superconductor LaFe$_2$As$_2$

We investigate the electronic structure of a recently discovered, heavily electron-doped iron based superconductor LaFe$_2$As$_2$. Although first principles calculation shows apparent absence of hole Fermi surfaces around the $Γ$ point, we reveal, by hypothetically removing the La $d$ orbital contribution, that a hole Fermi surface around the $Γ$ point is essentially present. In the collapsed phase of LaFe$_2$As$_2$, which is non-superconducting, the hole Fermi surface is found to be absent, and the difference from the uncollapsed superconducting phase can be naturally understood within the spin-fluctuation mediated pairing scenario.

cond-mat.supr-con↗

arXiv2019

Hidden kagome-lattice picture and origin of high conductivity in delafossite PtCoO$_2$

We study the electronic structure of delafossite PtCoO$_2$ to elucidate its extremely small resistivity and high mobility. The band exhibits steep dispersion near the Fermi level despite the fact that it is formed mainly by Pt $d$ orbitals that are typically localized. We propose a picture based on two hidden kagome-lattice-like electronic structure: one originating from Pt $s+p_x/p_y$ orbitals, and the other from Pt $d_{3z^2-r^2}+d_{xy}/d_{x^2-y^2}$ orbitals, each placed on the bonds of the triangular lattice. In particular, we find that the underlying Pt $s+p_x/p_y$ bands actually determine the steepness of the original dispersion, so that the large Fermi velocity can be attributed to the large width of the Pt $s+p_x/p_y$ band. More importantly, the kagome-like electronic structure gives rise to "orbital-momentum locking" on the Fermi surface, which reduces the electron scattering by impurities. We conclude that the combination of the large Fermi velocity and the orbital-momentum locking is likely to be the origin of the extremely small resistivity in PtCoO$_2$.

cond-mat.mtrl-sci↗

arXiv2018

Spin Hall effect in 2D metallic delafossite PtCoO$_2$ and vicinity topology

The two-dimensional (2D) metal PtCoO$_2$ is renowned for the lowest room temperature resistivity among all oxides, close to that of the top two materials Ag and Cu. In addition, we theoretically predict a strong intrinsic spin Hall effect. This originates from six strongly-tilted Dirac cones that we find in the electronic structure near the Fermi surface, where a gap is opened by large spin-orbit coupling (SOC). This is underpinned by rich topological properties; in particular, the phenomenology of a mirror Chern metal is realized not exactly, but very accurately, on account of an approximate crystalline symmetry. We expect that such 'vicinity topology' to be a feature of relevance well beyond this material. Our Wilson loop analysis indicates further elaborate features such as fragile topology. These findings highlight PtCoO$_2$ as a promising material for spintronic applications as well as a platform to study the interplay of symmetry and topology.

cond-mat.mes-hall↗

arXiv2018

Thermoelectric performance of materials with Cu$Ch_4$ ($Ch=$ S, Se) tetrahedra: Similarities and differences among their low-dimensional electronic structure from first principles

In this study, we perform a comparative theoretical study on the thermoelectric performance of materials with Cu$Ch_4$ ($Ch=$ S, Se) tetrahedra, including famous thermoelectric materials BiCuSeO and tetrahedrite Cu$_{12}$Sb$_4$S$_{13}$, by means of first-principles calculations. By comparing these electronic band structures, we find that many of these materials possess a Cu-$t_{2g}$ band structure consisting of quasi-one-dimensional band dispersions and the isotropic (two-dimensional for layered compounds) band dispersion near the valence-band edge. Therefore, the key factors for the thermoelectric performance are the anisotropy of the former band dispersion and the degeneracy of these two kinds of band dispersions. We also find that a large extension of the chalcogen orbitals often improves their thermoelectric performance by improving these two factors or by going beyond such a basic band structure through a large alternation of its shape. Such a large extension of the chalcogen orbitals might partially originate from the anisotropic Cu-$Ch$ bond geometry of a tetrahedron. Our study reveals interesting similarities and differences of materials with Cu$Ch_4$, which provides important knowledge for a future search of high-performance thermoelectric materials.

cond-mat.mtrl-sci↗

arXiv2017

Prediction of the High Thermoelectric Performance of Pnictogen Dichalcogenide Layered Compounds with Quasi-One-Dimensional Gapped Dirac-like Band Dispersion

Thermoelectric power generation has been recognized as one of the most important technologies, and high-performance thermoelectric materials have long been pursued. However, because of the large number of candidate materials, this quest is extremely challenging, and it has become clear that a firm theoretical concept from the viewpoint of band-structure engineering is needed. In this study, we theoretically demonstrate that pnictogen-dichalcogenide layered compounds, which originally attracted attention as a family of superconductors and have recently been investigated as thermoelectric materials, can exhibit very high thermoelectric performance with elemental substitution. In particular, we clarify a promising guiding principle for materials design and find that LaOAsSe$_2$, a material that has yet to be synthesized, has a powerfactor that is six times as large as that of the known compound LaOBiS$_2$ and can exhibit a very large $ZT$ under some plausible assumptions. This large enhancement of the thermoelectric performance originates from the quasi-one-dimensional gapped Dirac-like band dispersion, which is realized by the square-lattice network. Our study offers one ideal limit of the band structure for thermoelectric materials. Because our target materials have high controllability of constituent elements and feasibility of carrier doping, experimental studies along this line are strongly awaited.

cond-mat.mtrl-sci↗