arXiv subjects

Hiraku Ogino

Publications and source records attributed to Hiraku Ogino.

At least 19 recordsLinked to original sources

arXiv2026

Room-Temperature Calcium Intercalation into Graphite Catalyzed by Sodium

Calcium (Ca) insertion into graphite (C) has been considered to require elevated temperatures, and its occurrence at room temperature (RT) has been regarded as highly unlikely. Here, we demonstrate that sodium (Na) catalysis enables the formation of superconducting CaC$_6$ even at RT. In mixtures of Ca, Na, and graphite, the gradual development of superconducting diamagnetism and the emergence of X-ray diffraction peaks confirm the formation of CaC$_6$ during storage at RT. The superconducting transition temperature increases with storage time, and the amount of CaC$_6$ scales proportionally to the square root of storage time. These findings provide new insights into the mechanism of superconductivity and Na-catalyzed formation of CaC$_6$, and highlight the potential of this RT intercalation process for practical applications such as electrode materials in Ca-ion batteries.

cond-mat.supr-con↗

arXiv2026

Fluorine-substitution-dependent phase diagram and superconducting properties of Sm-based oxypnictides synthesized by a high-pressure growth technique

A series of SmFeAsO1-xFx (Sm1111) bulk samples (x = 0.05 to 0.40) are synthesized by an in-situ cubic-anvil high-pressure technique at 4 GPa and systematically characterized through structural, microstructural, Raman, transport, and magnetic measurements. Structural analysis confirms that the tetragonal Sm1111 phase remains dominant across the entire substitution range, with lattice parameters decreasing smoothly as fluorine content increases, demonstrating effective incorporation of F even in the overdoped regime (x = 0.4). Raman spectroscopy provides complementary, local-phase-sensitive evidence that supports the structural analysis and confirms fluorine substitution in the main Sm1111 phase. In the underdoped region, the superconducting transition temperature (Tc) is enhanced by 10-17 K and the critical current density (Jc) is increased by up to an order of magnitude compared with conventionally synthesized samples at the ambient pressure. The upper critical field, estimated using the WHH model, reaches values approaching 200 T, reflecting strong paramagnetic limitation and multiband effects. TAFF analysis reveals a power-law field dependence of the activation energy, consistent with collective vortex pinning in polycrystalline iron-based superconductors. The superconducting phase diagram constructed from Tc and Jc versus fluorine content reveals a dome-like trend, with a maximum Tc of 57 K and Jc of 10^4 A cm^-2 at the optimal doped region. Comparison with conventionally synthesized Sm1111 samples demonstrates that high-pressure growth significantly extends the effective fluorine substitution range and enhances the superconducting performance, particularly in the underdoped regime. These results establish high-pressure fluorine substitution as an effective materials-engineering approach for tuning the phase diagram and optimizing the superconducting properties of Sm1111.

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arXiv2025

Optimization of superconducting properties of F-doped SmFeAsO by cubic anvil high-pressure technique

We optimize the synthesis conditions for SmFeAsO0.80F0.20 (Sm1111) bulks using a cubic-anvil high-pressure (CA-HP) apparatus through both ex-situ and in-situ processes, applying pressures of up to 4 GPa and heating temperatures of up to 1600°C. A comprehensive characterization has been performed, including structural, microstructural, transport, and magnetic measurements. Our findings indicate that a modest growth pressure of approximately 0.5 GPa is sufficient for the formation of the Sm1111 phase in the ex-situ process. In contrast, the in-situ process requires higher synthesis pressure (4 GPa) and temperature (1400 °C for 1 hour) to achieve the Sm1111 phase with enhanced superconducting properties. Notably, the optimized in-situ process significantly reduces the reaction time needed for the formation of the Sm1111 phase compared to conventional synthesis process at ambient pressure (CSP), leading to an increase in the transition temperature by 3 K and improvements in critical current density (Jc). Conversely, the optimized ex-situ process results in an onset transition temperature (Tc) of approximately 53 K, similar to that of CSP, though it enhances the Jc by an order of magnitude. Despite these advancements, a small amount of impurity phases, as observed during CSP, persists in all Sm1111 samples prepared through either the in-situ or ex-situ CA-HP processes. These results suggest that the in-situ process under optimized conditions (1400 °C, 4 GPa for 1 hour) can effectively improve the superconducting properties of Sm1111. Additionally, a comprehensive analysis comparing these results with high gas pressure techniques, spark plasma sintering, and CSP methods suggests that a small amount of impurity phases in Sm1111 is persistent and cannot be completely eliminated by various pressure techniques, even at the applied pressure of up to 4 GPa.

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arXiv2025

Rapid and Scalable Synthesis of Alkali Metal-Intercalated C$_{60}$ Superconductors

Alkali metal-intercalated C$_{60}$, $A_3$$C_{60}$ ($A$ = K, Rb, Cs, and their combinations), holds significant potential for practical applications due to its high superconducting transition temperature (33 K), high upper critical field (900 kOe), and isotropic superconductivity. However, application-oriented research has been limited by the lack of an efficient $A_3$$C_{60}$ synthesis process. In this study, we demonstrate a rapid and scalable synthesis of $A_3$$C_{60}$ ($A$ = K, Rb, and Cs$_{1/3}$Rb$_{2/3}$) via direct mixing of $A$ and C$_{60}$, realizing the fabrication of high-quality sintered $A_3$$C_{60}$ pellets within just 1 hour of heating at 200-300°C. The pellets exhibited large superconducting shielding volume fractions with sharp transitions, and the relationship between the lattice constant and transition temperature was in good agreement with previous reports. This direct mixing method enables simple and rapid production of large quantities of $A_3$$C_{60}$, which is expected to accelerate research into applications such as superconducting wires and bulk magnets.

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arXiv2025

The uncollapsed LaFe2As2 phase: compensated, highly doped, electron-phonon coupled, iron-based superconductor

The recently discovered LaFe2As2 superconducting compound, member of the 122 family of iron pnictide superconductors, becomes superconducting below Tc=13K, yet its nominal doping apparently places it in the extreme overdoped limit, where superconductivity should be suppressed. In this work, we investigate the normal state of magneto- and thermo-electric transport and specific heat of this compound. The experimental data are consistent with the presence of highly compensated electron and hole bands, with around 0.42 electrons per unit cell just above Tc, and high effective masses around 3m0. The temperature dependence of transport properties strongly resembles that of conventional superconductors, pointing to a key role of electron-phonon coupling. From these evidences, LaFe2As2 can be regarded as the connecting compound between unconventional and conventional superconductors.

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arXiv2024

Doping Dependence of Upper Critical Field of High-Tc Cuprate Bi2+xSr2-xCaCu2O8+d Estimated from Irreversibility Field at Zero Temperature

We investigated the temperature (T) dependence of the irreversibility field Hirr(T) in high-critical-temperature cuprate Bi2+xSr2-xCa1-yYyCu2O8+d (Bi-2212) single crystals over a wide range of hole doping level (p). Hirr(T) was evaluated by measuring the magnetization hysteresis loop. The value of Hirr(T) extrapolated to T = 0 K [Hirr(0)], is either equal to or sets the lower boundary for the upper critical field at T = 0 K [Hc2(0)]. Tc shows a parabolic p-dependence (peak at p = 0.16), whereas Hirr(0) increases monotonically with p by approximately one order of magnitude, from 19 T for the most underdoped sample (p = 0.065, Tc = 24 K) to 209 T for the most overdoped sample (p = 0.200, Tc = 75 K). The present results qualitatively agree with Hc2(0) values evaluated from the specific heat measurements. The observed p-dependence of Hirr(0) in Bi-2212 is distinct from those in YBa2Cu3O7-d and HgBa2CuO6+d, in which a pronounced dip structure appears in the underdoped region. Considering that the dip structures observed in these two systems are likely associated with the formation of competing orders (most likely field-induced charge orders), the present results indicate that the influence of the competing order in Bi-2212 is less prominent than that in the other two systems.

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arXiv2024

Accelerated Lanthanide Intercalation into Graphite Catalyzed by Na

Lanthanides ($Ln$) are notoriously difficult to intercalate into graphite. We investigated the possibility of using Na to catalyze the formation of $Ln$-intercalated graphite and successfully synthesized $Ln$C$_6$ ($Ln$ = Sm, Eu, and Yb) significantly rapidly in high yields. The synthesis process involves the formation of the reaction intermediate NaC$_x$, through the mixing of Na and C, which subsequently reacts with $Ln$ upon heating to form $Ln$C$_6$. Well-sintered $Ln$C$_6$ pellets with low residual Na concentrations ($Ln$:Na = 98:2) were fabricated by the two-step method. The pellets enabled the evaluation of $Ln$C$_6$ by powder X-ray diffraction and electrical resistivity measurements. This study highlights the versatility of the Na-catalyzed method and lays the foundation for the rapid mass production of $Ln$C$_6$, with potential applications in superconducting and rechargeable battery materials.

cond-mat.mtrl-sci↗

arXiv2024

Synthesis of $c$-axis textured CaKFe$_4$As$_4$ superconducting bulk via spark plasma texturing technique

Grain alignment is a key factor that determines the performance of a superconducting bulk. In this study, the spark plasma texturing (SPT) technique was used to fabricate a CaKFe$_4$As$_4$ superconducting bulk. X-ray diffraction and electron backscatter diffraction revealed that the $c$-axes of the CaKFe$_4$As$_4$ grains in the SPT bulk are aligned, demonstrating that the SPT technique is effective in achieving $c$-axis texture. In addition, chemical composition analysis showed that oxide impurities, which affect the grain boundary characteristics that determine the inter-grain critical current density ($J_c$), are randomly distributed in the SPT bulk. Magnetization measurements showed high $J_c$ values of the SPT bulk, reaching 127 kA cm$^{-2}$ and 26 kA cm$^{-2}$ at 4.2 K under a self-field and magnetic field of 5 T, respectively. These results suggest that the SPT technique is a promising approach for obtaining a high-performance superconducting bulk material for high-field applications.

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arXiv2024

Synthesis of CaKFe$_4$As$_4$ bulk samples with high critical current density using a spark plasma sintering technique

A high density CaKFe$_4$As$_4$ bulk sample was successfully synthesized using a spark plasma sintering (SPS) technique. The density of the synthesized sample was 5.02 g cm$^{-3}$, corresponding to 96.2% of the theoretical density of CaKFe$_4$As$_4$. Moreover, a reasonably high Vickers hardness of 1 GPa was measured. The electrical resistivity of the SPS bulk sample was as low as approximately 600 $μΩ$ cm at 300 K, which is smaller than that of the ordinary sintered polycrystalline sample by nearly one order of magnitude, and exhibited a sharp superconducting transition, with the transition width $Δ\textit{T}_c$ less than 2 K, indicating an improved grain connectivity. The critical current density of the SPS bulk sample, as calculated from the magnetization hysteresis loops (magnetic $\textit{J}_c$), reached 18 kA cm$^{-2}$ at 4.2 K under 5 T, which is the highest among the iron-based superconductor polycrystalline samples reported thus far.

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arXiv2023

Na-catalyzed rapid synthesis and characterization of intercalated graphite CaC6

In this study, we conducted experiments on CaC6 for elucidating the Na-catalyzed formation mechanism and achieving rapid mass synthesis of graphite intercalation compounds (GICs). Rapidly synthesized CaC6 was characterized by analysis of its crystal structure and physical properties. We found that the formation of the reaction intermediate Na-GIC (NaCx, x = 64) requires a larger amount of Na than is intercalated between the graphite interlayers. The requirement for excess Na may provide insights into the mechanism of Na-catalyzed GIC formation. A Na-to-C molar mixing ratio of 1.5-2.0:6 was suitable for the efficient formation of CaC6 under heat treatment at 250°C for 2 h, and the catalytic Na remaining in the sample was demonstrably reduced to a Na:Ca ratio of approximately 3:97. The upper critical field Hc2 was enhanced approximately three times compared to those of previous reports. Based on X-ray diffraction and experimental parameter analysis, we concluded that the enhancement of Hc2 was attributed to the disordered stacking sequence in CaC6, possibly because of the rapid and low-temperature formation. Physical properties derived from specific heat measurements were comparable to those of high-quality CaC6, which is slowly synthesized using the molten Li-Ca alloy method. This study provides new avenues for future research and exploration in the rapid mass synthesis of GICs as practical materials, for applications such as battery electrodes and superconducting wires.

cond-mat.mtrl-sci↗

arXiv2023

Experimental investigation of electronic interactions in collapsed and uncollapsed LaFe2As2 phases

The iron-based pnictide LaFe2As2 is not superconducting as-synthesized, but it becomes such below Tc around 12 K upon annealing, as a consequence of a structural transition from a phase with collapsed tetragonal crystal structure to an uncollapsed phase. In this work, we carry out specific heat, Raman spectroscopy and normal state electric and thermoelectric transport measurements in the collapsed and uncollapsed LaFe2As2 phases to gain insight into the electron interactions and their possible role in the superconducting pairing mechanism. Despite clear features of strong electron-phonon coupling observed in both phases, neither the low energy phonon spectra nor the electron-phonon coupling show significant differences between the two phases. Conversely, the Sommerfield constants are significantly different in the two phases, pointing to much higher electron correlation in the superconducting uncollapsed phase and confirming theoretical studies.

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arXiv2023

Dramatically Accelerated Formation of Graphite Intercalation Compounds Catalyzed by Sodium

Graphite intercalation compounds (GICs) have a variety of functions due to their rich material variations, and thus,innovative methods for their synthesis are desired for practical applications. We have discovered that Na has a catalytic property that dramatically accelerates the formation of GICs. We demonstrate that LiC6n (n = 1, 2), KC8, KC12n (n = 2, 3, 4), and NaCx are synthesized simply by mixing alkali metals and graphite powder with Na at room temperature (~25 °C), and AEC6 (AE = Ca, Sr, Ba) are synthesized by heating Na-added reagents at 250 °C only for a few hours. The NaCx, formed by the mixing of C and Na, is understood to act as a reaction intermediate for a catalyst, thereby accelerating the formation of GICs by lowering the activation energy of intercalation. The Na-catalyzed method, which enables the rapid and mass synthesis of homogeneous GIC samples in a significantly simpler manner than conventional methods, is anticipated to stimulate research and development for GIC applications.

cond-mat.mtrl-sci↗

arXiv2021

Posttreatment Effects on the Crystal Structure and Superconductivity of Ca-Free Double-Layered Cuprate Sr$_2$SrCu$_2$O$_{4+y}$F$_{2-y}$

We report the effects of low-temperature postannealing on the structural and superconducting properties of the recently discovered Ca-free double-layered cuprate, Sr$_2$SrCu$_2$O$_{4+y}$F$_{2-y}$. Although the as-synthesized sample prepared under high pressure has a tetragonal structure with a rock-salt-type blocking layer (the so-called $T$-phase), we found that the symmetry of the structure lowered to that of an orthorhombic system when annealed with CuF$_2$. The structural refinements reveal that such a topochemical reaction leads not only to the removal of excess O$^{2-}$ from the apical site but also to the intercalation of extra F$^-$ into the interstitial site. The orthorhombic phase exhibits bulk superconductivity at a critical temperature of 107 K, which is significantly higher than that of the $T$-phase ($\sim$50 K). Meanwhile, the $T$-phase turns into another structure possessing a fluorite-type blocking layer without apical fluorine (known as the $T^\prime$-phase) by annealing without CuF$_2$. Density functional theory calculations show that the $T^\prime$-phase is more stable than the $T$-phase. This is the first report on the formation of a $T^\prime$-type double-layered cuprate. Furthermore, the structural stability of the three phases of Sr$_2$SrCu$_2$O$_{4+y}$F$_{2-y}$ is discussed in terms of lattice matching between the blocking and conducting layers.

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arXiv2021

Superconductivity-driven ferromagnetism and spin manipulation using vortices in the magnetic superconductor EuRbFe4As4

Magnetic superconductors are specific materials exhibiting two antagonistic phenomena, superconductivity and magnetism, whose mutual interaction induces various emergent phenomena, such as the reentrant superconducting transition associated with the suppression of superconductivity around the magnetic transition temperature (Tm), highlighting the impact of magnetism on superconductivity. In this study, we report the experimental observation of the ferromagnetic order induced by superconducting vortices in the high-critical-temperature (high-Tc) magnetic superconductor EuRbFe4As4. Although the ground state of the Eu2+ moments in EuRbFe4As4 is helimagnetism below Tm, neutron diffraction and magnetization experiments show a ferromagnetic hysteresis of the Eu2+ spin alignment. We demonstrate that the direction of the Eu2+ moments is dominated by the distribution of pinned vortices based on the critical state model. Moreover, we demonstrate the manipulation of spin texture by controlling the direction of superconducting vortices, which can help realize spin manipulation devices using magnetic superconductors.

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arXiv2020

Experimental and Computational Determination of Optimal Boron Content in Layered Superconductor Sc$_{20}$C$_{8-x}$B$_x$C$_{20}$

It is generally difficult to quantify the amounts of light elements in materials because of their low X-ray-scattering power, as this means that they cannot be easily estimated via X-ray analyses. Meanwhile, the recently reported layered superconductor, Sc$_{20}$C$_{8-x}$B$_x$C$_{20}$, requires a small amount of boron, which is a light element, for its structural stability. In this context, here, we quantitatively evaluate the optimal $x$ value using both the experimental and computational approaches. Using the high-pressure synthesis approach that can maintain the starting composition even after sintering, we obtain the Sc$_{20}$(C,B)$_{8}$C$_{20}$ phase by the reaction of the previously reported Sc$_{15}$C$_{19}$ and B (Sc$_{15}$B$_y$C$_{19}$). Our experiments demonstrate that an increase in $y$ values promotes the phase formation of the Sc$_{20}$(C,B)$_{8}$C$_{20}$ structure; however, there appears to be an upper limit to the nominal $y$ value to form this phase. The maximum $T_\mathrm{c}$ $(=7.6\text{ K})$ is found to correspond with the actual $x$ value of $x \sim 5$ under the assumption that the sample with the same $T_\mathrm{c}$ as the reported value $(=7.7\text{ K})$ possesses the optimal $x$ amount. Moreover, we construct the energy convex hull diagram by calculating the formation enthalpy based on first principles. Our computational results indicate that the composition of Sc$_{20}$C$_4$B$_4$C$_{20}$ $(x=4)$ is the most thermodynamically stable, which is reasonably consistent with the experimentally obtained value.

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arXiv2019

Superconductivity in a Scandium Borocarbide with a Layered Crystal Structure

The discovery of nearly room-temperature superconductivity in superhydrides has motivated further materials research for conventional superconductors. To realize the moderately high critical temperature $(T_\mathrm{c})$ in materials containing light elements, we explored new superconducting phases in a scandium borocarbide system. Here, we report the observation of superconductivity in a new ternary Sc-B-C compound. The crystal structure, which was determined through a Rietveld analysis, belongs to tetragonal space group $P4/ncc$. By complementarily using the density functional theory calculations, a chemical formula of the compound was found to be expressed as Sc$_{20}$C$_{8-x}$B$_x$C$_{20}$($x=1\:\mathrm{or}\:2$). Interestingly, a small amount of B is essential to stabilize the present structure. Our experiments revealed the typical type-II superconductivity at $T_\mathrm{c}=7.7\:\mathrm{K}$. Additionally, we calculated the density of states within a first-principles approach and found that the contribution of the Sc-3d orbital was mainly responsible for the superconductivity.

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arXiv2019

Unique defect structure and advantageous vortex pinning properties in superconducting CaKFe4As4

The lossless current-carrying capacity of a superconductor is limited by its critical current density (Jc). A key to enhance Jc towards real-life applications is engineering defect structures to optimize the pinning landscape. For iron-based superconductors (IBSs) considered as candidate materials for high-field applications, high Jc values have been achieved by various techniques to introduce artificial pinning centres. Here we report extraordinary vortex pinning properties in CaKFe4As4 (CaK1144) arising from the inherent defect structure. Scanning transmission electron microscopy revealed the existence of nanoscale intergrowths of the CaFe2As2 phase, which is unique to CaK1144 formed as a line compound. The Jc properties in CaK1144 are found to be distinct from other IBSs characterized by a significant anisotropy with respect to the magnetic field orientation as well as a remarkable pinning mechanism significantly enhanced with increasing temperature. We propose a comprehensive explanation of the Jc properties based on the unique intergrowths acting as pinning centres.

cond-mat.supr-con↗

arXiv2017

Doping-dependent critical current properties in K, Co, and P-doped BaFe2As2 single crystals

In order to establish the doping dependence of the critical current properties in the iron-based superconductors, the in-plane critical current density (Jc) of BaFe2As2-based superconductors, Ba1-xKxFe2As2 (K-Ba122), Ba(Fe1-xCox)2As2 (Co-Ba122), and BaFe2(As1-xPx)2 (P-Ba122) in a wide range of doping concentration (x) was investigated by means of magnetization hysteresis loop (MHL) measurements on single-crystal samples. Depending on the dopant elements and their concentration, Jc exhibits a variety of magnetic-field (H) and temperature (T) dependences. (1) In the case of K-Ba122, MHL of the underdoped samples (x < 0.33) exhibits the second magnetization peak (SMP), which sustains high Jc at high H and high T, exceeding 10^5 A/cm2 at T = 25 K and H = 6 T for x = 0.30. On the other hand, SMP is missing in the optimally (x ~ 0.36-0.40) and overdoped (x ~ 0.50) samples, and consequently Jc rapidly decreases by more than one order of magnitude, although the change in Tc is within a few K. (2) For Co-Ba122, SMP is always present over the entire superconducting (SC) dome from the under (x ~ 0.05) to the overdoped (x ~ 0.12) region. However, the magnitude of Jc significantly changes with x, exhibiting a sharp maximum at x ~ 0.057, which is a slightly underdoped composition for Co-Ba122. (3) For P-Ba122, the highest Jc is attained at x = 0.30 corresponding to the highest Tc composition. For the overdoped samples, MHL is characterized by SMP located close to the irreversibility field. Common to the three doping variations, Jc becomes highest at the under-doping side of SC dome near the phase boundary between SC phase and the antiferromagnetic/orthorhombic phase. Also, the peak appears in a narrow range of doping, distinct from the Tc dome with broad maximum. These similarities in the three cases indicate that the observed doping dependence of Jc is intrinsic to the BaFe2As2-based superconductors.

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