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Akira Iyo

Publications and source records attributed to Akira Iyo.

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↗
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{\deg}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.

cond-mat.supr-con↗
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.

cond-mat.supr-con↗
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.

cond-mat.supr-con↗
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.

cond-mat.supr-con↗
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 $\mu\Omega$ 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 $\Delta\textit{T}_c$ 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.

cond-mat.supr-con↗
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.

cond-mat.supr-con↗
arXiv2023

Smectic Pair Density Wave Order in EuRbFe4As4

The pair density wave (PDW) is a novel superconducting state in which Cooper pairs carry center-of-mass momentum in equilibrium, leading to the breaking of translational symmetry. Experimental evidence for such a state exists in high magnetic field and in some materials that feature density wave orders that explicitly break translational symmetry. However, evidence for a zero-field PDW state that exists independent of other spatially ordered states has so far been elusive. Here, we show that such a state exists in the iron pnictide superconductor EuRbFe4As4 (Eu-1144), a material that features coexisting superconductivity (Tc ~ 37K) and magnetism (Tm ~ 15 K). We show from the Spectroscopic Imaging Scanning Tunneling Microscopy (SI-STM) measurements that the superconducting gap at low temperature has long-range, unidirectional spatial modulations with an incommensurate period of ~8 unit cells. Upon raising the temperature above Tm, the modulated superconductor disappears, but a uniform superconducting gap survives to Tc. When an external magnetic field is applied, gap modulations disappear inside the vortex halo. The SI-STM and bulk measurements show the absence of other density wave orders, showing that the PDW state is a primary, zero-field superconducting state in this compound. Both four-fold rotational symmetry and translation symmetry are recovered above Tm, indicating that the PDW is a smectic order.

cond-mat.supr-con↗
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↗
arXiv2022

Charge Transport in Ba$_{1-x}$Rb$_{x}$Fe$_{2}$As$_{2}$ Single Crystals

Recent studies in heavily hole-doped iron-based superconductor RbFe$_2$As$_2$ have suggested the emergence of novel electronic nematicity directed along the Fe-As direction, 45$^\circ$ rotated from the usual nematicity ubiquitously found in BaFe$_2$As$_2$ and related materials. This motivates us to study the physical properties of Ba$_{1-x}$Rb$_{x}$Fe$_{2}$As$_{2}$, details of which remain largely unexplored. Here we report on the normal-state charge transport in Ba$_{1-x}$Rb$_{x}$Fe$_{2}$As$_{2}$ superconductors by using high-quality single crystals in the range of Rb concentration $0.14\le x \le 1.00$. From the systematic measurements of the temperature dependence of electrical resistivity $ρ(T)$, we find a signature of a deviation from the Fermi liquid behavior around the optimal composition, which does not seem related to the antiferromagnetic quantum criticality but has a potential link to hidden nematic quantum criticality. In addition, electron correlations derived from the coefficient of $T^2$ resistivity show a marked increase with Rb content near the heavily hole-doped end, consistent with the putative Mott physics near the $3d^5$ electron configuration in iron-based superconductors.

cond-mat.supr-con↗
arXiv2022

Hidden Structural and Superconducting Phase Induced in Antiperovskite Arsenide SrPd$_{3}$As

Enriching the material variation often contributes to the progress of materials science. We have discovered for the first time antiperovskite arsenide SrPd$_{3}$As and revealed a hidden structural and superconducting phase in Sr(Pd$_{1-x}$Pt$_{x}$)$_{3}$As. The Pd-rich samples (0 $\leq$ x $\leq$ 0.2) had the same non-centrosymmetric (NCS) tetragonal structure (a space group of $I41md$) as SrPd$_{3}$P. For the samples with 0.3 $\leq$ x $\leq$ 0.7, a centrosymmetric (CS) tetragonal structure ($P4/nmm$) identical to that of SrPt$_{3}$P was found to appear, accompanied by superconductivity at a transition temperature ($T_\mathrm{c}$) up to 3.7 K. In the samples synthesized with Pt-rich nominal compositions (0.8 $\leq$ x $\leq$ 1.0), Sr$_{2}$(Pd,Pt)$_{8-y}$As$_{1+y}$ with an intergrowth structure (CS-orthorhombic with Cmcm) was crystallized. The phase diagram obtained for Sr(Pd,Pt)$_{3}$As was analogous to that of (Ca,Sr)Pd$_{3}$P in that superconductivity ($T_\mathrm{c}$ $\geq$ 2 K) occurred in the CS phases induced by substitutions to the NCS phases. This study indicates the potential for further material variation expansion and the importance of elemental substitutions to reveal hidden phases in related antiperovskites.

cond-mat.supr-con↗
arXiv2022

High-pressure synthesis and superconductivity of the novel Laves phase BaIr2

Superconductors comprising 5d transition metals of Ir and Pt have been widely explored because they have the potential of unique superconductivity caused by the strong spin-orbit interaction (SOI). We successfully synthesized BaIr2, the last Laves phase remaining unsynthesized in the MgCu2-type AM2 (A = Ca, Sr, Ba; M = Rh, Pd, Ir, Pt). BaIr2 was crystallized at 925 C under a pressure of 3.3 GPa via a solid-state reaction between Ba and Ir powders; it was found to have the longest a-lattice constant of 8.038(1) A among AM2. BaIr2 exhibited bulk superconductivity at a transition temperature (Tc) of 2.7 K. BaIr2 was found to have a type-II superconductor with an upper critical field of 67.7 kOe, which was above the Pauli paramagnetic limit (50 kOe). The electron-phonon coupling constant and normalized specific heat jump were measured to be 0.63 and 1.2, respectively, indicating that BaIr2 is a weak-coupling superconductor. The electronic-structure calculations for BaIr2 revealed that the Ir-5d states are dominant at the Fermi energy (EF) and the density of states at the EF is strongly affected by SOI as in the case of CaIr2 and SrIr2.

cond-mat.supr-con↗
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.

cond-mat.supr-con↗
arXiv2021

Antiperovskite superconductor LaPd$_{3}$P with noncentrosymmetric cubic structure

Antiperovskites are a promising candidate structure for the exploration of new materials. We discovered an antiperovskite phosphide, LaPd$_{3}$P, following our recent synthesis of $A$Pd$_{3}$P ($A$ = Ca, Sr, Ba). While $A$Pd$_{3}$P and (Ca,Sr)Pd$_{3}$P were found to be tetragonal or orthorhombic systems, LaPd$_{3}$P is a new prototype cubic system ($a$ = 9.0317(1) A) with a noncentrosymmetric space group ($I-43m$). LaPd$_{3}$P exhibited superconductivity with a transition temperature ($T_\mathrm{c}$) of 0.28 K. The upper critical field, Debye temperature, and Sommerfeld constant ($γ$) were determined as 0.305(8) kOe, 267(1) K, 6.06(4) mJ mol-1 K-2 f.u.-1, respectively. We performed first-principles electronic band structure calculations for LaPd$_{3}$P and compared the theoretical and experimental results. The calculated Sommerfeld constant (2.24 mJ mol-1 K-2 f.u.-1) was much smaller than the experimental value of $γ$ because the Fermi energy ($E_\mathrm{F}$) was located slightly below the density of states (DOS) pseudogap. This difference was explained by the increase in the DOS at $E_\mathrm{F}$ due to the approximately 5 at.% La deficiency (hole doping) in the sample. The observed Tc value was much lower than that estimated using the Bardeen-Cooper-Schrieffer equation. To explain the discrepancy, we examined the possibility of an unconventional superconductivity in LaPd$_{3}$P arising from the lack of space inversion symmetry.

cond-mat.supr-con↗
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.

cond-mat.supr-con↗
arXiv2021

Superconductivity of centrosymmetric and non-centrosymmetric phases in antiperovskite (Ca,Sr)Pd$_3$P

In the recently discovered antiperovskite phosphide (Ca,Sr)Pd$_3$P, centrosymmetric (CS) and non-centrosymmetric (NCS) superconducting phases appear depending on the Sr concentration, and their transition temperatures ($T_\mathrm{c}$) differ by as much as one order of magnitude. In this study, we investigated the superconducting properties and electronic band structures of CS orthorhombic (CSo) (Ca$_{0.6}$Sr$_{0.4}$)Pd$_3$P ($T_\mathrm{c}$ = 3.5 K) and NCS tetragonal (NCSt) (Ca$_{0.25}$Sr$_{0.75}$)Pd$_3$P ($T_\mathrm{c}$ = 0.32 K) samples with a focus on explaining their large $T_\mathrm{c}$ difference. Specific heat measurements indicated that CSo (Ca$_{0.6}$Sr$_{0.4}$)Pd$_3$P was an s-wave superconductor in a moderate-coupling regime with a 2$Δ$$_0$/k$_B$$T_\mathrm{c}$ value of 4.0. Low-lying phonons leading to the strong coupling in the structurally analogous SrPt$_3$P were unlikely to be present in CSo (Ca$_{0.6}$Sr$_{0.4}$)Pd$_3$P. Given that CSo (Ca$_{0.6}$Sr$_{0.4}$)Pd$_3$P and NCSt (Ca$_{0.25}$Sr$_{0.75}$)Pd$_3$P exhibited similar Debye temperatures ($Θ$$_D$) of approximately 200 K, the large $T_\mathrm{c}$ difference could not be attributed to $Θ$$_D$.$T_\mathrm{c}$ of each phase was accurately reproduced based on the Bardeen-Cooper-Schrieffer (BCS) theory using experimental data and the density of states of the Fermi level $N$(0) calculated from their band structures. We concluded that the considerable suppression of $T_\mathrm{c}$ in NCSt (Ca$_{0.25}$Sr$_{0.75}$)Pd$_3$P can be primarily attributed to the decrease in $N$(0) associated with the structural phase transition without considering the lack of inversion symmetry.

cond-mat.supr-con↗