arXiv subjects

Ryosuke Akashi

Publications and source records attributed to Ryosuke Akashi.

At least 19 recordsLinked to original sources

arXiv2026

Yttrium Superhydrides Revisited: Advanced Experimental and Theoretical Studies of YH$_6$, YH$_9$ and YH$_{10}$

Yttrium polyhydrides are benchmark materials in high-pressure superconductivity, yet several key properties of the Y-H system remain insufficiently characterized. Here we combine contact transport, contactless radio-frequency measurements, pulsed-field experiments, and first-principles calculations to reinvestigate YH$_6$, YH$_9$, and YH$_{10}$ in the pressure range 140-213 GPa. Yttrium hydrides YH$_6$ ($\textit{$T_c$}$ = 218-221 K) and YH$_9$ ($\textit{$T_c$}$ = 235-237 K) demonstrate narrow superconducting transitions ($\textit{${\Delta}$T$_c$}$ = 2-5 K), approaching the limit imposed by thermal fluctuations. Pulsed-field measurements on YH$_6$ up to 60 T establish an extended superconducting phase diagram with a linear slope $\textit{dB$_{c2}$/dT}$ = -0.52 T/K, pronounced transition broadening above 30 T, and negligible normal-state magnetoresistance. We report the radio-frequency AC susceptibility study of YH$_6$, providing evidence for superconductivity via high-frequency field screening in a contactless geometry. Experiments involving Pd incorporation, Pd thin-film sputtering, and Al alloying show strong suppression of high-temperature superconductivity, with no transitions detected above 78-120 K. Finally, using density-functional theory with the stochastic self-consistent harmonic approximation, superconducting density-functional theory, and full-bandwidth Migdal-Eliashberg calculations, we show that anharmonic effects substantially reduce the predicted $\textit{$T_c$}$ of cubic YH$_{10}$ to approximately 260-270 K. These results strongly disfavor room-temperature superconductivity in binary yttrium superhydrides.

cond-mat.supr-con↗

arXiv2026

Quantum electrometry in a silicon carbide power device

For high-bias operation devices such as silicon carbide (SiC) power devices, early detection of failure mechanisms is essential to ensure reliability. This requires a method to map high electric fields with high spatial resolution, which has not been realized until now. Here we report that the silicon vacancy (Vsi) in SiC has outstanding characteristics for detecting electric fields applied in various directions within a high-biased SiC device. Vsi exhibits an equivalent response to electric field components parallel (Epara) and perpendicular (Eperp) to the c-axis, a feature unique among quantum sensors, and the responsiveness to Epara and Eperp enables detection of arbitrary electric fields encountered in cutting-edge SiC power devices. We confirmed high electric field detection of ~2.3 MV/cm, which is ~90% of the breakdown electric field of a 4H-SiC with typical carrier concentration. Selectively formed Vsi enables high-resolution mapping of electric field distribution. Vsi-based quantum sensors bring data-driven research and development methodologies as well as device degradation diagnosis.

quant-ph↗

arXiv2026

Electronic structure theory of H$_{3}$S: Plane-wave-like valence states, density-of-states peak and its guaranteed proximity to the Fermi level

Superconductivity in sulfur superhydride H$_{3}$S under extreme pressures has been explained theoretically, but it requires a peaked concentration of the electronic density of states (DOS), which has been found in first-principles calculations. The mechanism of this peak formation, though vital for its high transition temperature, has however remained obscure. We address this problem through detailed analysis of the first-principles electronic wave functions. The valence wave functions are shown to be significantly plane-wave-like. From the Fourier-mode analysis of the self-consistent potential and atomic pseudopotentials, we extract the nearly uniform models that accurately reproduce the first-principles band structure with very few parameters. The DOS peak is shown to be the consequence of the hybridization of specific plane waves. Adjacency of Jones' large zone to the plane-wave spherical Fermi surface is posited to be the root cause of the multiple plane-wave hybridization, the DOS peak formation and its proximity to the Fermi level. The present theory resolves the minimal modeling problem of electronic states in H$_{3}$S, as well as establishes a mechanism that may help to boost the transition temperatures in pressure induced superconductors.

cond-mat.supr-con↗

arXiv2025

Uniform electron benchmark for the first-principles $GW_{0}$-Eliashberg theory

We investigate the numerical behavior of the Eliashberg equations for phonon-mediated superconductivity, incorporating normal-state self-energy calculations within the consistent $GW_{0}$ approximation. We account for the full wavenumber and frequency dependences of both the screened Coulomb interaction and phonon-mediated attraction. We present results for the prototypical uniform electron gas system with model Einstein phonons at temperatures of a few kelvin. At extremely low temperatures, we efficiently execute the required convolutions of Green's functions and interactions in Matsubara frequency and wavenumber using intermediate representation and Fourier convolution techniques. In particular, we elucidate the interplay between electron-phonon $\omega$-mass and $k$-mass renormalizations of the electronic self-energy in determining the normal-state effective mass, spectral weight and the superconducting transition temperature. The electron density regimes where the plasmon effect enhances or suppresses the phonon-mediated superconductivity on top of the static Coulomb effect are revealed. We compare our comprehensive Eliashberg calculation results with those from density functional theory for superconductors, where the functionals have been constructed with reference to Eliashberg theory. Our model, methods, and results provide a valuable benchmark for first-principles superconducting calculations that treat screened Coulomb interaction effects non-empirically.

cond-mat.supr-con↗

arXiv2025

Can machines learn density functionals? Past, present, and future of ML in DFT

Density functional theory has become the world's favorite electronic structure method, and is routinely applied to both materials and molecules. Here, we review recent attempts to use modern machine-learning to improve density functional approximations. Many different researchers have tried many different approaches, but some common themes and lessons have emerged. We discuss these trends and where they might bring us in the future.

physics.comp-ph↗

arXiv2024

Assessing the possible superconductivity in doped perovskite hydride KMgH$_3$: Effects of lattice anharmonicity and spin fluctuations

The superconducting properties of uniformly hole-doped perovskite hydride KMgH$_3$ with varying doping concentration and lattice parameter corresponding to different pressures were investigated from first principles. The superconducting transition temperature ($T_{\mathrm{c}}$) was predicted from the density functional theory for superconductors (SCDFT), where the effects of lattice anharmonicity and spin-fluctuation were considered and examined. Although lattice anharmonicity tends to suppress superconductivity around the edge of dynamical stability, where the phase is stabilized due to anharmonic effects, $T_{\mathrm{c}}$ is enhanced. In the hole-doped \ce{KMgH3}, substantial spin-fluctuation (SF) effects were discovered, which counters the phonon-mediated pairing and decreases $T_{\mathrm{c}}$. Such anomalously strong SF is evaluated for similar hydrides, where the hydrogen 1-$s$ bands are isolated at the Fermi level, and its correlation with the electronics density of states was explored.

cond-mat.supr-con↗

arXiv2023

Illuminating the Bragg intersections as roots of Dirac nodal lines and high-order van Hove singularities

We theoretically reexamine nearly uniform electron models with weak crystalline potentials. In particular, we theorize the modulation of the plane-wave branches at linear regions where multiple Bragg planes intersect. Any such linear intersections involve three or more plane-wave branches diffracted by the periodic potential. Small inter-branch interactions can yield various crossing and anticrossing singularities with promised breakdown of the quadratic approximation, extending alongside the intersection lines. Most of the intersections run in low-symmetric paths in the Brillouin zone and therefore we cannot completely characterize their electronic states with standard band structure plotting methods. The present theory reveals a general mechanism in nearly uniform systems to induce the Dirac nodal lines and van-Hove singularities with broken quadratic band approximation in three dimensions, which may host a variety of anomalous low-energy electronic properties. We apply the theory to a recently discovered high temperature superconductor H$_{3}$S to interpret the enigmatic density-of-state (DOS) peaking therein. The results show how and {\it why there} the continuous saddle points--the source of the peaked DOS--emerge, as well as reveal the companion Dirac nodal lines hidden in the conduction bands.

cond-mat.mtrl-sci↗

arXiv2022

Semiconducting Electronic Structure of the Ferromagnetic Spinel $\mathbf{Hg}\mathbf{Cr}_2\mathbf{Se}_4$ Revealed by Soft-X-Ray Angle-Resolved Photoemission Spectroscopy

We study the electronic structure of the ferromagnetic spinel $\mathrm{Hg}\mathrm{Cr}_2\mathrm{Se}_4$ by soft-x-ray angle-resolved photoemission spectroscopy (SX-ARPES) and first-principles calculations. While a theoretical study has predicted that this material is a magnetic Weyl semimetal, SX-ARPES measurements give direct evidence for a semiconducting state in the ferromagnetic phase. Band calculations based on the density functional theory with hybrid functionals reproduce the experimentally determined band gap value, and the calculated band dispersion matches well with ARPES experiments. We conclude that the theoretical prediction of a Weyl semimetal state in $\mathrm{Hg}\mathrm{Cr}_2\mathrm{Se}_4$ underestimates the band gap, and this material is a ferromagnetic semiconductor.

cond-mat.mtrl-sci↗

arXiv2022

Lattice dielectric properties of rutile $\mathrm{TiO}_2$: First-principles anharmonic self-consistent phonon study

We calculate the lattice dielectric function of strongly anharmonic rutile $\mathrm{TiO}_2$ from ab initio anharmonic lattice dynamics methods. Since an accurate calculation of the $\Gamma$ point phonons is essential for determining optical properties, we employ the modified self-consistent approach, including third-order anharmonicity as well as fourth-order anharmonicity. The resulting optical phonon frequencies and linewidths at the $\Gamma$ point much better agree with experimental measurements than those from a perturbative approach. We show that the four-phonon scattering process contributes as much as the third-order anharmonic term to phonon linewidths. Furthermore, incorporating the frequency dependence of phonon linewidth reveals that experimentally known but unidentified peaks of the dielectric function are due to two-phonon process. This work emphasizes the importance of a self-consistent approach in predicting the optical properties of highly anharmonic materials.

cond-mat.mtrl-sci↗

arXiv2022

Density functional theory

Density functional theory (DFT) is an essential building block for modern theoretical physics, chemistry, and engineering, especially those concerning electronic properties. Through decades of development, various program packages for first-principles electronic structure calculation are now available. Their sophisticated interfaces allow users to apply DFT to actual systems, even without knowing the theory. It is hence becoming more and more important to recall the fundamentals of how DFT enables accurate calculations. This article attempts to provide such knowledge with a minimal overview of DFT -- its basic foundation, relations to observable electronic and nuclear dynamical properties, and some of its cutting-edge applications.

cond-mat.mtrl-sci↗

arXiv2022

A Noise-Robust Data Assimilation Method for Crystal Structure Prediction Using Powder Diffraction Intensity

Crystal structure prediction for a given chemical composition has long been a challenge in condensed-matter science. We have recently shown that experimental powder X-ray diffraction (XRD) data are helpful in a crystal structure search using simulated annealing, even when they are insufficient for structure determination by themselves (N. Tsujimoto et al., Phys. Rev. Materials 2, 053801 (2018)). In the method, the XRD data are assimilated into the simulation by adding a penalty function to the physical potential energy, where we used a crystallinity-type penalty function defined by the difference between experimental and simulated diffraction angles. To improve the success rate and noise robustness, we introduce a correlation-coefficient-type penalty function adaptable to XRD data with significant experimental noise. We apply the new penalty function to SiO$_2$ coesite and $\epsilon$-Zn(OH)$_2$ to determine its effectiveness in the data assimilation method.

cond-mat.mtrl-sci↗

arXiv2022

Development of exchange-correlation functionals assisted by machine learning

With the recent rapid progress in the machine-learning (ML), there have emerged a new approach using the ML methods to the exchange-correlation functional of density functional theory. In this chapter, we review how the ML tools are used for this and the performances achieved recently. It is revealed that the ML, not being opposed to the analytical methods, complements the human intuition and advance the development toward the first-principles calculation with desired accuracy.

cond-mat.mtrl-sci↗

arXiv2021

Machine-Learning-Based Exchange-Correlation Functional with Physical Asymptotic Constraints

Density functional theory is the standard theory for computing the electronic structure of materials, which is based on a functional that maps the electron density to the energy. However, a rigorous form of the functional is not known and has been heuristically constructed by interpolating asymptotic constraints known for extreme situations, such as isolated atoms and uniform electron gas. Recent studies have demonstrated that the functional can be effectively approximated using machine learning (ML) approaches. However, most ML models do not satisfy asymptotic constraints. In this study, by applying a novel ML model architecture, we demonstrate a neural network-based exchange-correlation functional satisfying physical asymptotic constraints. Calculations reveal that the trained functional is applicable to various materials with an accuracy higher than that of existing functionals, even for materials whose electronic properties are different from the properties of materials in the training dataset. Our proposed approach thus improves the accuracy and generalization performance of the ML-based functional by combining the advantages of ML and analytical modeling.

cond-mat.mtrl-sci↗

arXiv2021

The missing quantum number of the Floquet states

We reformulate the Floquet theory for periodically driven quantum systems following a perfect analogy with the proof of Bloch theorem. We observe that the current standard method for calculating the Floquet eigenstates by the quasi-energy alone is incomplete and unstable, and pinpoint an overlooked quantum number, the average energy. This new quantum number resolves many shortcomings of the Floquet method stemming from the quasi-energy degeneracy issues, particularly in the continuum limit. Using the average energy quantum number we get properties similar to those of the static energy, including a unique lower-bounded ordering of the Floquet states, from which we define a ground state, and a variational method for calculating the Floquet states. This is a first step towards reformulating Floquet first-principles methods, that have long been thought to be incompatible due to the limitations of the quasi-energy.

quant-ph↗

arXiv2021

Revisiting the homogeneous electron gas in pursuit of the properly normed ab initio Eliashberg theory

We address an issue of how to accurately include the self energy effect of the screened electron-electron Coulomb interaction in the phonon-mediated superconductors from first principles. In the Eliashberg theory for superconductors, self energy is usually decomposed using the $2\times 2$ Pauli matrices in the electron-hole space. We examine how the diagonal ($\sigma_{0}$ and $\sigma_{3}$) components resulting in the quasiparticle correction to the normal state, $Z$ and $\chi$ terms, behave in the homogeneous electron gas in order to establish a norm of treating those components in real metallic systems. Within the $G_{0}W_{0}$ approximation, we point out that these components are non-analytic near the Fermi surface but their directional derivatives and resulting corrections to the quasiparticle velocity are nevertheless well defined. Combined calculations using the $G_{0}W_{0}$ approximation and Eliashberg equations show us that the effective mass and pairing strength strikingly depend on both $Z$ and $\chi$, in a different manner. The calculations without the numerically demanding $\chi$ term is thus shown to be incapable of describing the homogeneous electron gas limit. This result poses a challenge to accurate first-principles Eliashberg theory.

cond-mat.supr-con↗

arXiv2021

Chemical physics of superconductivity in layered yttrium carbide halides from first principles

We perform a thorough first-principles study on superconductivity in yttrium carbide halide Y$_2$$X_2$C$_2$ ($X$=Cl, Br, I) whose maximum transition temperature ($T_{\rm c}$) amounts to $\sim$10 K. A detailed analysis on the optimized crystal structures reveals that the Y$_2$C$_2$ blocks are compressed uniaxially upon the halogen substitution from Cl, Br to I, contrary to the monotonic expansion of the lattice vectors. With a nonempirical method based on the density functional theory for superconductors within the conventional phonon mechanism, we successfully reproduce the halogen dependence of $T_{\rm c}$. Anomalously enhanced coupling of one C$_2$ libration mode is observed in Y$_2$I$_2$C$_2$, which imply possible departure from the conventional pairing picture. Utilizing the Wannier representation of the electron-phonon coupling, we show that the halogen electronic orbitals and ionic vibrations scarcely contribute to the superconducting pairing. The halogen dependence of this system is hence an indirect effect of the halogen ions through the uniaxial compressive force on the superconducting Y$_2$C$_2$ blocks. We thus establish a quantitatively reliable picture of the superconducting physics of this system, extracting a unique effect of the atomic substitution which is potentially applicable to other superconductors.

cond-mat.supr-con↗

arXiv2020

Superconductivity at 253 K in lanthanum-yttrium ternary hydrides

Polyhydrides offer intriguing perspectives as high-temperature superconductors. Here we report the high-pressure synthesis of a series of lanthanum-yttrium ternary hydrides: cubic hexahydride $(La,Y)H_{6}$ with a critical temperature $T_{C}$ = 237 +/- 5 K and decahydrides $(La,Y)H_{10}$ with a maximum $T_{C}$ ~${253 K}$ and an extrapolated upper critical magnetic field $B_{C2(0)}$ up to ${135 T}$ at 183 GPa. This is one of the first examples of ternary high-$T_{C}$ superconducting hydrides. Our experiments show that a part of the atoms in the structures of recently discovered ${Im3m}$-$YH_{6}$ and ${Fm3m}$-$LaH_{10}$ can be replaced with lanthanum (~70 %) and yttrium (~25 %), respectively, with a formation of unique ternary superhydrides containing incorporated $La@H_{24}$ and $Y@H_{32}$ which are specific for ${Im3m}$-$LaH_{6}$ and ${Fm3m}$-$YH_{10}$. Ternary La-Y hydrides were obtained at pressures of 170-196 GPa via the laser heating of $P6_{3}$${/mmc}$ lanthanum-yttrium alloys in the ammonia borane medium at temperatures above 2000 K. A novel tetragonal $(La,Y)H_{4}$ was discovered as an impurity phase in synthesized cubic $(La,Y)H_{6}$. The current-voltage measurements show that the critical current density $J_{C}$ in $(La,Y)H_{10}$ may exceed $2500 A/mm^{2}$ at 4.2 K, which is comparable with that for commercial superconducting wires such as ${NbTi}$, $Nb_{3}$${Sn}$. Hydrides that are unstable in a pure form may nevertheless be stabilized at relatively low pressures in solid solutions with superhydrides having the same structure.

cond-mat.supr-con↗

arXiv2020

Coexistence of spontaneous polarization and superconductivity in hole-doped oxyhydrides ATiO_2H (A=K, Rb, Cs): first-principles study

The polar metal is a material that hosts both polar distortion and metallicity. Such a material is expected to show exotic magneto-electric phenomena if superconducts. Here, we theoretically explore ferroelectric and superconducting properties in a series of perovskite-type oxyhydrides ATiO$_2$H (A=K, Rb, Cs) under hole-doping conditions using the first-principles calculations based on the density functional theory. Our simulation shows that these compounds host spontaneous polarization and superconductivity at optimal doping concentration. The unusual coexistence of superconductivity and large polarization (~100 ${\mu}$C/cm$^2$) originates from weak coupling of the polar distortion and superconducting states, the reason of which is separation of the displaced atoms and spacially confined metallic carriers. Besides, the superconductivity is enhanced by the unique electronic properties near the valence band maximum: quartic band dispersion with a sizable contribution of hydrogen 1s states. Our study thus feature the oxyhydrides as possible model polar superconducting systems, which may be utilizable for future magneto-electric devices.

cond-mat.supr-con↗