arXiv subjects

Hirokazu Kadobayashi

Publications and source records attributed to Hirokazu Kadobayashi.

18 recordsLinked to original sources

arXiv2026

The tetragonal-cubic transition of davemaoite: Implications for lower mantle seismic anomalies

Davemaoite (CaSiO3 perovskite) is the third most abundant mineral in Earth's lower mantle and a dominant phase in subducted oceanic crust. Its crystal structure is distorted (tetragonal or orthorhombic) at ambient conditions but is considered to transform to cubic at high temperatures. Previous experiments reported low, nearly pressure-independent transition temperatures (approximately 600 K), demonstrating a long-standing discrepancy with theoretical predictions that mostly exceed 1000 K. Here, we determine the phase stability and thermal equation of state of CaSiO3 davemaoite and its titanium-bearing solid solution [Ca(Si0.75,Ti0.25)O3] under simultaneous high-pressure and high-temperature conditions using a laser-heated diamond anvil cell combined with synchrotron X-ray diffraction. We find that the tetragonal-to-cubic transition occurs at substantially higher temperatures than previously reported, with the titanium substitution further stabilizing the tetragonal phase and shifting the transition boundary to even higher temperatures. These findings indicate that CaSiO3 davemaoite in subducted oceanic crust likely undergoes its ferroelastic transition in the mid-lower mantle, whereas Ti-rich davemaoite may remain tetragonal throughout most of the lower mantle, transforming to cubic near the core-mantle boundary. Our results demonstrate that the compositionally dependent phase behaviour of davemaoite can account for the seismic anomalies observed in both the mid-lower mantle and the lowermost mantle.

physics.geo-ph↗

arXiv2026

Low electrical conductivity of dry CaSiO3 perovskite under lower mantle conditions

Electrical conductivity (EC) provides important constraints on the composition and volatile distribution of Earth's deep mantle, yet the EC of davemaoite (CaSiO3 perovskite), a major lower-mantle phase, remains poorly constrained. We measured the EC of nominally dry CaSiO3 perovskite at pressures up to 89 GPa and temperatures up to 2200 K using impedance spectroscopy in a laser-heated diamond anvil cell. Conductivity increases with temperature but decreases systematically with pressure and it is substantially lower than previously reported, yet broadly consistent with recent theoretical predictions for oxygen-vacancy-mediated ionic transport. A distinct change in the temperature dependence coincides with the tetragonal-to-cubic phase boundary, revealing a modest enhancement of ionic transport across the structural transition. Along a normal lower-mantle geotherm, dry davemaoite is comparable in conductivity to bridgmanite near the top of the lower mantle but becomes progressively less conductive with depth. Under cold-slab conditions, dry davemaoite is substantially less conductive than dry subducted MORB and cannot account for the observed high-conductivity anomalies. Dry davemaoite therefore contributes little to bulk lower-mantle conductivity.

physics.geo-ph↗

arXiv2026

Single-crystal structural phase diagram of stoichiometric bilayer nickelate La3Ni2O7 under hydrostatic pressure

The bilayer nickelate La3Ni2O7 has attracted intense interest following the discovery of high-temperature superconductivity under pressure, representing the first nickelate superconductor realized in bulk form. However, the crystal structure of the superconducting phase remains under active discussion, complicating efforts to establish its microscopic origin. Here we resolve these structural controversies by establishing a definitive pressure-temperature phase diagram, including the superconducting region of stoichiometric La3Ni2O7 single crystals under hydrostatic conditions using helium as the pressure-transmitting medium. At ambient pressure, La3Ni2O7 adopts a polar orthorhombic Am2m structure characterized by charge order between inequivalent Ni sites and NiO6 octahedral tilting. Upon compression, the system undergoes a direct transition from the charge-ordered Am2m phase to the tetragonal I4/mmm phase near 10 GPa, coinciding with the onset of bulk superconductivity. These results establish the intrinsic structural evolution of La3Ni2O7 and provide a structural framework for microscopic theories of nickelate superconductivity.

cond-mat.supr-con↗

arXiv2026

Tellurium sublattice instability driven amorphization in the chalcogenide AgSbTe2 under pressure

Pressure provides a powerful thermodynamic route to access hidden structural states in functional materials, yet the microscopic origin of pressure-induced amorphization remains elusive in many complex chalcogenides. Here we report a detailed high-pressure structural study of AgSbTe2,combining synchrotron X-ray diffraction with density functional theory and molecular dynamics calculations up to 60 GPa. We uncover a pressure-driven transformation from the ambient R-3m phase to a fully disordered cubic Im3m phase, through an extended intermediate amorphous state. Enthalpy calculations reveal a near-degeneracy between the R3m and Im3m structures over a broad pressure range, dictating amorphization. Contrary to previously speculated cation vacancies, the amorphization is governed by a pronounced displacement instability of the Te sublattice. Remarkably, the time dependent decompression pathway controls the final structural state, resulting in either amorphous (slow decompression) or fully crystalline (fast decompression) states, indicative of a strong counterintuitive kinetic effect.

cond-mat.mtrl-sci↗

arXiv2026

Bulk superconductivity up to 96 K in pressurized nickelate single crystals

Recently, the Ruddlesden-Popper bilayer nickelate $La_3Ni_2O_7$ has emerged as a superconductor with a transition temperature ($T_c$) of approximately 80 K above 14 GPa (Refs. 1-3). Achieving higher $T_c$ in nickelate superconductors, along with the synthesis of reproducible high-quality single crystals without relying on high-oxygen-pressure growth conditions, remains a significant challenge$^{[4-7]}$. Here we report superconductivity up to 96 K under high pressure in bilayer nickelate single crystals synthesized at ambient pressure. Energy-dispersive spectroscopy, single-crystal X-ray diffraction, nuclear quadrupole resonance and scanning transmission electron microscopy evidenced high crystal quality of the flux-grown $La_2SmNi_2O_{7-δ}$ single crystals. $La_2SmNi_2O_7$ exhibits clear bulk superconductivity, including zero resistivity ($T_{c,max}^{onset}$ = 92 K and $T_{c,max}^{zero}$ = 73 K at 21.6 GPa) and the Meissner effect ($T_c$= 60 K at 20.6 GPa). A low-temperature high-pressure structural study indicates that both monoclinic and tetragonal structures can support superconductivity in this bilayer nickelate. Furthermore, we established a correlation between higher $T_c$ under high pressures and larger in-plane lattice distortion under ambient conditions, corroborated by observing even higher $T_c^{onset}$ of 96 K in $La_{1.57}Sm_{1.43}Ni_2O_{7-δ}$. This study overcomes key limitations in growing nickelate superconductor crystals, resolves the crystal structure in the superconducting state and demonstrates an effective pathway towards achieving higher $T_c$.

cond-mat.supr-con↗

arXiv2026

Superhydrides on the way to ambient pressure: weak localization and persistent X-ray photoconductivity in BaSiH$_{8}$

Reducing the stabilization pressure of superhydrides represents one of the most important challenges in hydrogen-saturated compound chemistry. Moving in this direction, we studied the Ba-Si-H system at 0-142 GPa using transport measurements, 1H nuclear magnetic resonance, single-crystal and powder X-ray diffraction in the temperature range of 4-317 K. We synthesized the previously predicted cubic BaSiH$_{8}$ at pressures of 18-31 GPa. Remarkably, we demonstrate that BaSiH$_8$ remains stable upon decompression to ambient conditions and can be recovered from the diamond anvil cell. Obtained Ba-Si polyhydrides exhibit metallic and superconducting properties ($\textit{T$_c$}$ = 9 K, $\textit{B$_{c2}$}$(0)=13-16 T) at 142 GPa. However, at pressures below 50 GPa, these hydrides behave as degenerate semiconductors (bandgap < 0.4 meV) or poor metals with weak electron localization, negative magnetoresistance, photovoltaic effect, and persistent photoconductivity in the X-ray and visible range. Our work demonstrates the high-pressure synthesis of Ba-Si polyhydrides that remain stable upon decompression to ambient conditions, overcoming a critical bottleneck in superhydride chemistry and establishing a foundation for practical applications in hydrogen storage.

cond-mat.supr-con↗

arXiv2026

Reply to "Threefold error in the reported zero-field cooled magnetic moment of single crystal $La_2SmNi_2O_7$ (arXiv: 2602.23240)"

We respond to the critique by Aleksandr V. Korolev and Evgeny F. Talantsev on the superconducting phase fraction ($f$) calculations in Li et al. Nature 649, 871-878 (2026). First, the weak upturn in the low-temperature tail of our data has been confirmed to originate from the background, and the paramagnetic Meissner effect is absent in our case; thus, field-cooled (FC) data can be used for superconducting phase fraction calculations. Second, demagnetization effect must be calculated based on the actual measured moment as a function of $f$, which has been well-established and routinely employed in the superconductivity community. In contrast, Korolev and Talantsev treated the demagnetization field as a constant; thus, their calculation underestimates $f$ by a factor of $(1-Nχ_{meas})(1-N)$. This factor is close to 1/3, given $N$ = 0.849, $χ_{meas}$ = -1.313 in our study, which explains the origin of their deviated result (nearly three times smaller than our results). Third, our sample is a homogeneous high-quality bulk single crystal, evidenced by various techniques, making the existence of multiple discrete superconducting regions highly unlikely. We conclude that the superconducting phase fraction calculations reported in Li et al. Nature 649, 871-878 (2026) are not invalidated by the analyses presented in Korolev et al. arXiv: 2602.23240 (2026).

cond-mat.supr-con↗

arXiv2026

Unveiling pressurized bulk superconductivity in a trilayer nickelate Pr4Ni3O10 single crystal

The recent discovery of superconductivity in pressurized Ruddlesden-Popper (RP) nickelates has provided new perspectives on the mechanism of high-temperature superconductivity. Up to now, most experiments concentrated on the lanthanum-related RP phase, so the discovery of new superconducting RP nickelates is highly desirable to reveal their generality. Here we report that high-quality Pr4Ni3O10 single crystal is grown with an optical floating zone furnace under high oxygen pressure. High-pressure transport measurements show that the superconducting state arises above 10 GPa, and the maximum Tc reaches 39 K without saturation, significantly exceeding the value of 25-30 K of La4Ni3O10. Ultrasensitive d.c. magnetic susceptibility measurements under high pressure indicate bulk superconductivity with appreciable superconducting volume fractions. By performing in situ high-pressure synchrotron X-ray diffraction measurements at 16 K, a structural transition is found from monoclinic to tetragonal. Unlike La4Ni3O10, the electronic structure of the high-pressure phase of Pr4Ni3O10 from density functional theory exhibits a dramatic metallization of the sigma-bonding band consisting of three dz2 orbitals and van Hove singularity of coupled bands of dx2-y2 orbitals near the Fermi level, similar to the bilayer nickelate La3Ni2O7. These findings reveal some generic features of both crystal and electronic structures for high-temperature superconductivity in nickelates and multi-layer cuprates.

cond-mat.supr-con↗

arXiv2026

High-pressure structural and lattice-dynamics study of Yttria-Stabilized Zirconia

The structural evolution of two selected compositions of Yttria-Stabilized Zirconia (YSZ), with 3mol% (3YSZ) and 8mol% (8YSZ) of Y2O3, have been investigated under pressure using in-situ synchrotron X-ray diffraction (XRD) and Raman spectroscopy in a diamond anvil cell up to 40 GPa (at room temperature).The close crystallographic relation between the observed structures and the relatively large difference in the atomic numbers of Y/Zr and O, imposes the simultaneous study using both techniques, aiming to fully elucidate the structural evolution under pressure. The results, by combining both techniques, reveal that for both 3YSZ and 8YSZ, pressure promotes higher-symmetry structures. Under initial compression, the minority at ambient conditions monoclinic phase (m-phase) gradually transforms towards t-phase, a transition that is concluded for both 3YSZ/8YSZ at ~10 GPa. At higher pressures, the solely remaining t-phase of 3YSZ transforms to the t'', that in turns transforms to the c-phase above 28 GPa. Likewise, for 8YSZ the coexistence of t- and t''-phases continue up to 31 GPa, where both transforms towards c-phase, that remains stable up to the highest pressure of this study. Upon pressure release, all observed transitions are fully reversible with negligible hysteresis, with the exception of the practical disappearance of the monoclinic phase at ambient conditions. Our study underscores the significance of simultaneously performing and analyzing the results of both XRD and Raman spectroscopy studies in relevant crystallographic systems. Moreover, it provides a route towards a ``structural purification'' of YSZ through the elimination of the m-phase aiming to improve material properties.

cond-mat.mtrl-sci↗

arXiv2025

Subtle Structural Anomaly under Compression in Line-Nodal CaSb$_2$

We report X-ray diffraction patterns and calculated electronic band structures of the Dirac line-nodal material CaSb$_2$ under pressure. Its superconducting transition temperature ($T_{\mathrm{c}}=1.7$ K) increases under pressure and reaches a maximum at 3.4 K at around 3 GPa. We observed subtle anomalies in lattice parameters accompanied by a jump in bulk modulus without any change in crystal symmetry at around 3 GPa. First-principles calculations revealed that the distorted lattice of Sb(1) site deforms in the pressure range of 0-3 GPa. Those results suggest the existence of a first-order structural transition and arouse expectations for unusual phononic properties affecting the superconducting state. The calculated pressure dependence of the electronic density of states (DOS) confirms that it is not the change in the DOS that governs the variations in $T_{\mathrm{c}}$.

cond-mat.mtrl-sci↗

arXiv2025

Comparative high-pressure structural and electrical transport properties study of thermoelectric (Bi1-xSbx)2Te3 compounds

Thermoelectric (Bi1-x Sbx)2Te3 (BST-x) compounds with x=0.2, 0.7 and 0.9 have been studied using synchrotron angle-dispersive powder x-ray diffraction in a diamond anvil cell up to 25 GPa (at room temperature). The results clearly indicate that all compounds of this study follow a similar structural evolution with the one of pure Bi2Te3 and Sb2Te3 under pressure. From the comparison between the critical pressures of the corresponding phase transitions, a clear trend of increasing critical pressure for the transition to the disordered solid-solution BCC phase was observed with the increase of Sb concentration. In the case of the BST-0.7, an extended stability of the solid-solution BCC phase up to, at least, 180 GPa was observed. Finally, electrical transport properties measurements under pressure for BST-0.7, document a reversible pressure-induced metallization above 12 GPa.

cond-mat.mtrl-sci↗

arXiv2025

Observation of a $Pbca$ phase and robust metallicity in $\rm{RuO_2}$ under pressure

$\rm{RuO_2}$ stands as a quintessential rutile-type compound under ambient conditions, with its structural exploration under pressure bearing significant implications for both phase transition investigations and Earth science. Nonetheless, the precise phase transition sequence remains a debate. In this study, we disclose the emergence of the $Pbca$ phase alongside the enduring metallic character of $\rm{RuO_2}$ under megabar pressure. Employing state-of-the-art synchrotron X-ray diffraction, our observations delineate a phase transition trajectory progressing through rutile, $\rm{CaCl_2}$, and ultimately $Pbca$ phases. Notably, the $Pbca$ phase manifests immediately just after the rutile-$\rm{CaCl_2}$ transition, confining a narrow pressure regime for the pure $\rm{CaCl_2}$-type phase. Within the pressure range of 15.5 to 35.0 GPa, a coexistence of the $\rm{CaCl_2}$-type and $Pbca$ phases is observed, transforming to a sole presence of the $Pbca$ phase beyond 35.0 GPa. Electrical transport measurements conducted on both single crystal and powder samples confirm the enduring metallic conductivity of $\rm{RuO_2}$, persisting up to at least $\sim$120 GPa, albeit exhibiting a diminished conductivity at ultrahigh pressures due to a reduction in electronic density of states at the Fermi level. This study furnishes compelling evidence for the presence of the $Pbca$ phase across a broad pressure range, diverging from the previously widely acknowledged $Pa\bar{3}$ phase, thereby offering crucial insights into phase transition phenomena in other metal dioxides and advancing our comprehension of electronic behaviors within 4d and 5d electron systems.

cond-mat.mtrl-sci↗

arXiv2025

High pressure structural and lattice dynamics study of α-In$_2$Se$_3$

Layered $α$-In$_2$Se$_3$has been studied using a concomitant in-situ synchrotron angle dispersive powder x-ray diffraction and Raman spectroscopy study in a diamond anvil cell up to 60+ GPa, at room temperature. Helium, that remains fairly hydrostatic up to the highest pressure in this study, was used as the pressure-transmitting medium. The results from both experimental methods reveal a pressure-induced structural phase transition from $α$-In$_2$Se$_3$ to a monoclinic $β$'-In2Se3 structure at $\approx$1 GPa, in agreement with previous studies. Based on our detailed measurements using both experimental techniques and F-f formalism, the $β$'-In$_2$Se$_3$ structure remains stable up to 45 GPa, without a clear indication of a phase transition towards the previously reported $β$-In2Se3 phase. Above this pressure, In$_2$Se$_3$ adopts a disordered solid-solution-like orthorhombic structure, phase IV. The results are discussed in comparison with the relevant previous studies of $α$-In$_2$Se$_3$ under pressure.

cond-mat.mtrl-sci↗

arXiv2024

Coexistence of superconductivity and sliding polar metal state in HgPSe3

The simultaneous presence of polarity and metallicity in a material signifies an exotic polar metal state, but such materials are extremely rare, especially in bulk form, due to mutually exclusive nature of the fundamental defining properties. Here, we report experimental findings that HgPSe3 is a robust bulk polar metal at room temperature with a chiral structure stabilized by pressure and, remarkably, this polar metal hosts superconductivity with critical temperature Tc up to 11 K. Theoretical analysis reveals a two-step interlayer sliding-then-compressing mechanism for coexistence of polarity and metallicity in HgPSe3. This work unveils a new paradigm for creating the bulk polar metal state and simultaneous presence of coexisting quantum orders, raising the prospect of discovering novel emergent physics using pressure as a tuning knob.

cond-mat.supr-con↗

arXiv2023

Structure responsible for the superconducting state in La3Ni2O7 at high pressure and low temperature conditions

Very recently, a new superconductor with Tc = 80 K was reported in nickelate (La3Ni2O7) at around 15 - 40 GPa conditions (Nature, 621, 493, 2023) [1], which is the second type of unconventional superconductor, beside the cuprates, with Tc above liquid nitrogen temperature. However, the phase diagram plotted in this report was mostly based on the transport measurement at low temperature and high pressure conditions, and the assumed corresponding X-ray diffraction (XRD) results was carried out at room temperature. This encouraged us to carry out in situ high pressure and low temperature synchrotron XRD experiments to determine which phase is responsible for the high Tc state. In addition to the phase transition from orthorhombic Amam structure to orthorhombic Fmmm structure, a tetragonal phase with space group of I4/mmm was discovered when the sample was compressed to 19 GPa at 40 K where the superconductivity takes palce in La3Ni2O7. The calculations based on this tetragonal structure reveal that the electronic states approached to the Fermi energy were mainly dominated by the eg orbitals (3dz2 and 3dx2-y2) of Ni atoms, which are located in the oxygen octahedral crystal field. The correlation between Tc and this structural evolution, especially Ni-O octahedra regularity and the in-plane Ni-O-Ni bonding angles, are analyzed. This work sheds new lights to identify what is the most likely phase responsible for superconductivity in the double layered nickelate.

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↗

arXiv2023

Absence of Tc-Pinning Phenomenon Under High Pressure in High-Entropy REO0.5F0.5BiS2 Layered Superconductor

Recently, robustness of superconductivity (transition temperature, Tc) under high pressures has been observed in high-entropy alloy (HEA), bcc-type Ti-Zr-Hf-Nb-Ta, and HEA-type compounds (Ag,In,Sn,Pb,Bi)Te with a NaCl-type structure. Since those materials have three-dimensional crystal structure, investigation on the pressure dependence of Tc of low-dimensional materials is needed to understand the phenomena. Here, we investigated the superconducting properties and the crystal structure of BiS2-based layered system REO0.5F0.5BiS2. Although the robustness of Tc was induced in MTe with increasing M-site configurational entropy, the increase in RE-site configurational entropy does not induce robustness of Tc under high pressures in REO0.5F0.5BiS2. The crystal structure of HEA-type REO0.5F0.5BiS2 was confirmed as monoclinic P21/m, which is the same space group as the zero-entropy counterpart LaO0.5F0.5BiS2. The results suggest that an increase in configurational entropy at blocking layers do not affect crystal structure and superconducting properties under high pressures in the BiS2-based layered system.

cond-mat.supr-con↗

arXiv2021

Nature of low-temperature dense ice up to 80 GPa observed by x-ray diffraction

We have measured the lattice volume of ice VIII in different pressure-temperature pathways and found isothermal compression at low-temperature conditions makes the volume larger. Ice VIII has become its high-pressure phase with the molar volume of 6.45 cm^3 at 10 K where the pressure can be estimated as 60.4 GPa based on the third-order Birch-Murnaghan equation with parameters determined in this study (K_0= 32.4 GPa, K'_0= 3.7, and V_0= 11.9 cm^3). The present results indicate that this high-pressure state is paraelectric with tetragonal symmetry.

cond-mat.mtrl-sci↗