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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., Comment: 16 pages, 7 figures

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.

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., Comment: 13 pages, 6 figures, 1 table

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{\deg}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., Comment: 17 pages, 6 figures, 1 table

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., Comment: In press on Physical Review B

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 {\deg}C), and AEC6 (AE = Ca, Sr, Ba) are synthesized by heating Na-added reagents at 250 {\deg}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., Comment: 10 pages, 4 figures, 1 table

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., Comment: 18 pages, 9 figures, 3 tables (including 3 pages, 3 figures for the Supporting Information)

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., Comment: Main text: 16 pages, 6 figures, Supplementary Information: 9 pages, 5 figures, 1 table

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., Comment: 10 pages, 1 table, 7 figures

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., Comment: 13 pages, 3 tables, 8 figures

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., Comment: 15 pages, 5 figures, and Supplementary Information. One literature on the calculation of anisotropic Jc [S. Pyon, et al. Phys. Rev. B 99, 104506 (2019)] was added to the reference list

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., Comment: 29 pages, 14 figures, to be published in Phys. Rev. B

Pressure effects on a recently discovered BiS2-based superconductor Bi2(O,F)S2 (Tc = 5.1 K) were examined via two different methods; high pressure resistivity measurement and high pressure annealing. The effects of these two methods on the superconducting properties of Bi2(O,F)S2 were significantly different although in both methods hydrostatic pressure is applied to the sample by the cubic-anvil-type apparatus. In high pressure resistivity measurement, Tc linearly decreased at the rate of -1.2 K GPa-1. In contrast, the Tc of 5.1 K is maintained after high pressure annealing under 2 GPa and 470{\deg}C of optimally doped sample despite significant change of lattice parameters. In addition, superconductivity was observed in fluorine-free Bi2OS2 after high pressure annealing. These results suggest that high pressure annealing would cause a unique effect on physical properties of layered compounds., Comment: 8 pages, 6 figures

A new BiS2-based superconductor Bi2(O,F)S2 was discovered. This is a layered compound consisting of alternate stacking structure of rock-salt-type BiS2 superconducting layer and fluorite-type Bi(O,F) blocking layer. Bi2(O,F)S2 was obtained as the main phase by topotactic fluorination of undoped Bi2OS2 using XeF2, which is the first topotactic synthesis of an electron-doped superconductor via reductive fluorination. With increasing F-content, a- and c-axis length increased and decreased, respectively, and Tc increased up to 5.1 K., Comment: 9 pages, 4 figures

Dependence of superconducting properties of (Ca,RE)(Fe,TM)As2 [(Ca,RE)112, TM: Co, Ni)] on RE elements (RE = La-Gd) was systematically investigated. Improvement of superconducting properties by Co or Ni co-doping was observed for all (Ca,RE)112, which is similar to Co-co-doped (Ca,La)112 or (Ca,Pr)112. Tc of Co-co-doped samples decreased from 38 K for RE = La to 29 K for RE = Gd with decreasing ionic radii of RE3+. However, Co-co-doped (Ca,Eu)112 showed exceptionally low Tc = 21 K probably due to the co-existence of Eu3+ and Eu2+ suggested by longer interlayer distance dFe-Fe of (Ca,Eu)112 than other (Ca,RE)112.

Superconducting properties of Co-co-doped (Ca,RE)FeAs2 ((Ca,RE)112: RE = La, Pr) were investigated. Co-co-doping increased Tc of (Ca,Pr)112 while Mn-co-doping suppressed superconductivity of (Ca,RE)112. Co-co-doped (Ca,La)112 showed large diamagnetic screening and sharper superconducting transition than Co-free (Ca,La)112. Tczero observed in resistivity measurements increased from 14 K to 30 K by Co-co-doping, while Tconset was not increased. The critical current density (Jc) of Co-co-doped (Ca,La)112 were approximately 2.1 x 104 Acm-2 and 3.2 x 103 Acm-2 at 2 K and 25 K, respectively, near zero field. These relatively high Jcs and large diamagnetic screening observed in susceptibility measurement as for polycrystalline bulks suggest bulk superconductivity of Co-co-doped (Ca,RE)112 compounds.

In order to clarify the origin of anomalous superconductivity in (Ca,RE)Fe2As2 system, Pr doped and Pr,Co co-doped CaFe2As2 single crystals were grown by the FeAs flux method. These samples showed two-step superconducting transition with Tc1 = 25~42 K, and Tc2 < 16 K, suggesting that (Ca,RE)Fe2As2 system has two superconducting components. Post-annealing performed for these crystals in evacuated quartz ampoules at various temperatures revealed that post-annealing at ~400{\deg}C increased the c-axis length for all samples. This indicates that as-grown crystals have a certain level of strain, which is released by post-annealing at ~400{\deg}C. Superconducting properties also changed dramatically by post-annealing. After annealing at 400{\deg}C, some of the co-doped samples showed large superconducting volume fraction corresponding to the perfect diamagnetism below Tc2 and high Jc values of 104~105 Acm-2 at 2 K in low field, indicating the bulk superconductivity of (Ca,RE)Fe2As2 phase occurred below Tc2. On the contrary, the superconducting volume fraction above Tc2 was always very small, suggesting that 40 K-class superconductivity observed in this system is originating in the local superconductivity in the crystal.

Synthesis of a series of layered iron arsenides Ca1-xRExFeAs2 (112) was attempted by heating at 1000 C under a high-pressure of 2 GPa. The 112 phase successfully forms with RE = La, Ce, Nd, Sm, Eu and Gd, while Tb, Dy and Ho substituted and RE free samples does not contain the 112 phase. The Ce, Nd, Sm, Eu and Gd doped Ca1-xRExFeAs2 are new compounds. All of them exhibit superconducting transition except for the Ce doped sample. The behaviour of the critical temperature, with the RE ionic radii have been investigated.

A new iron-based superconductor (Ca,Pr)FeAs2 was discovered. Plate-like crystals of the new phase were obtained and crystal structure was investigated by single-crystal X-ray diffraction analysis. The structure was identified as the monoclinic system with space group P21/m, and is composed of two Ca(Pr) planes, anti-fluorite Fe2As2 layers, and As2 zigzag chain layers. Plate-like crystals composed of the new phase showed superconductivity with Tc ~20 K in both magnetization and resistivity measurements., Comment: 5 pages, 1 table, 6 figures

We have investigated the microstructure, normal-state electrical connectivity, and critical current density of ex-situ MgB2 polycrystalline bulks prepared by systematically varying the sintering conditions under low pressure. Samples heated at a high temperature of ~900{\deg}C for a long period showed an increased packing factor, a larger intergrain contact area, and a significantly enhanced electrical connectivity, all of which indicate solid-state self-sintering of MgB2. Sintered ex-situ MgB2 bulks from a laboratory-made ball-milled powder exhibited a greatly enhanced connectivity of 28%, which is the highest connectivity of pressureless ex-situ MgB2 bulks, wires, and tapes. Surprisingly, grain growth did not occur during long-duration (~100 h) sintering in the sintered ex-situ MgB2 bulks. This is in marked contrast to in-situ processed MgB2 samples for which significant grain growth occurred during heat treatment at ~900{\deg}C, producing grains that are several tens of times larger than the initial boron grains. Consequently, the critical current density as a function of the external magnetic field at 20 K progressively improved with sintering due to the relatively small grain size and good intergrain connectivity. We thus conclude that solid-state self-sintering is an effective approach for producing strongly connected, dense ex-situ MgB2 polycrystals without grain growth., Comment: 21 pages, 9 figures, to be published in Supercond. Sci. Technol

We report an 75As-NMR study on iron (Fe)-based superconductors with thick perovskitetype blocking layers Sr4(Mg0.5-xTi0.5+x)2O6Fe2As2 with x=0 and 0.2. We have found that antiferromagnetic (AFM) order takes place when x=0, and superconductivity (SC) emerges below Tc=36 K when x=0.2. These results reveal that the Fe-pnictides with thick perovskitetype blocks also undergo an evolution from the AFM order to the SC by doping electron carriers into FeAs planes through the chemical substitution of Ti+4 ions for Mg+2 ions, analogous to the F-substitution in LaFeAsO compound. The reason why the Tc=36 K when x=0.2 being higher than the optimally electron-doped LaFeAsO with Tc=27 K relates to the fact that the local tetrahedron structure of FeAs4 is optimized for the onset of SC., Comment: 4 pages, 3 figures, 1 table

We report the pressure dependences of the superconducting transition temperature (T_c) in several perovskite-type Fe-based superconductors through the resistivity measurements up to ~4 GPa. In Ca_4(Mg,Ti)_3Fe_2As_2O_y with the highest T_c of 47 K in the present study, the T_c keeps almost constant up to ~1 GPa, and starts to decrease above it. From the comparison among several systems, we obtained a tendency that low T_c with the longer a-axis length at ambient pressure increases under pressure, but high T_c with the shorter a-axis length at ambient pressure hardly increases. We also report the ^75As-NMR results on Sr_2VFeAsO_3. NMR spectrum suggests that the magnetic ordering occurs at low temperatures accompanied by some inhomogeneity. In the superconducting state, we confirmed the anomaly by the occurrence of superconductivity in the nuclear spin lattice relaxation rate 1/T_1, but the spin fluctuations unrelated with the superconductivity are dominant. It is conjectured that the localized V-3d moments are magnetically ordered and their electrons do not contribute largely to the Fermi surface and the superconductivity in Sr_2VFeAsO_3., Comment: 7 pages, 9 figures

We have discovered a new homologous series of iron pnictide oxides (Fe2As2)(Can+2(Al,Ti)nOy)[n = 2,3,4]. These compounds have perovskite-like blocking layers between Fe2As2 layers. The structure of new compounds are tetragonal with space groups of P4/nmm for n = 2 and 4 and P4mm for n = 3, which are similar to those of (Fe2As2)(Can+1(Sc,Ti)nOy)[n = 3,4,5] found in our previous study. Compounds with n = 3 and 4 have new crystal structures with 3 and 4 sheets of perovskite layers, respectively, including a rock salt layer in each blocking layer. The a-axis lengths of the three compounds are approximately 3.8 A, which are close to those of FeSe and LiFeAs. (Fe2As2)(Ca6(Al,Ti)4Oy) exhibited bulk superconductivity in magnetization measurement with Tc(onset)~36 K and resistivity drop was observed at ~39 K. (Fe2As2)(Ca5(Al,Ti)3Oy) also showed large diamagnetism at low temperatures. These new compounds indicate considerable rooms are still remaining for new superconductors in layered iron pnictides., Comment: 10 pages, 5 figures

A new layered iron arsenide oxide (Fe2As2)(Ca5(Mg,Ti)4Oy) and its structural derivative were found in the Fe-As-Ca-Mg-Ti-O system. The crystal structure of (Fe2As2)(Ca5(Mg,Ti)4Oy) is identical to that of (Fe2As2)(Ca5(Sc,Ti)4Oy), which was reported in our previous study. The lattice constants of this compound are a = 3.86(4) A and c = 41.05(2) A. In addition, another phase with a thicker blocking layer was found. The structure of the compound and its derivative was tentatively assigned through STEM observation as (Fe2As2)(Ca8(Mg,Ti)6Oy) with sextuple perovskite-type sheets divided by a rock salt layer. The interlayer Fe-Fe distance of this compound is ~30 A. The compound and its derivative exhibited bulk superconductivity, as found from magnetization and resistivity measurements., Comment: 9 pages, 7 figures

A new layered iron arsenide oxide (Fe2As2)(Ca4(Mg,Ti)3Oy) was discovered. Its crystal structure is tetragonal with a space group of I4/mmm consisted of the anti-fluorite type FeAs layer and blocking layer of triple perovskite cells and is identical with (Fe2As2)(Sr4(Sc,Ti)3O8) discovered in our previous study. The lattice constants of (Fe2As2)(Ca4(Mg,Ti)3Oy) are a = 3.877 A and c = 33.37 A. This compound exhibited bulk superconductivity up to 43 K in susceptibility measurement without intentional carrier doping. A resistivity drop was observed at ~47 K and zero resistance was achieved at 42 K. These values correspond to the second highest Tc among the layered iron-based superconductors after REFeAsO system.

We synthesized new layered iron arsenide oxides (Fe2As2)(Sr4(Sc,Ti)3O8),(Fe2As2)(Ba4Sc3O7.5), and (Fe2As2)(Ba3Sc2O5). The crystal structures of these compounds are tetragonal with a space group of I4/mmm. The structure of (Fe2As2)(Sr4(Sc,Ti)3O8) and (Fe2As2)(Ba4Sc3O7.5) consists of the alternate stacking of antifluorite Fe2As2 layers and triple perovskite-type oxide layers. The interlayer distance between the Fe planes of (Fe2As2)(Ba4Sc3O7.5) is ~18.7 A. Moreover, the a-axis of (Fe2As2)(Ba3Sc2O5) is the longest among the layered iron pnictides, indicating the structural flexibility of the layered iron pnictide containing perovskite-type layers. The bulk sample of (Fe2As2)(Sr4(Sc0.6Ti0.4)3O8) exhibited diamagnetism up to 28 K in susceptibility measurements.

We have discovered first homologous series of iron pnictide oxide superconductors (Fe2As2)(Can+1(Sc,Ti)nOy) [n = 3,4,5]. These compounds have extremely thick blocking layers up to quintuple perovskite oxide layers sandwiched by the Fe2As2 layers. These samples exhibited bulk superconductivity with relatively high Tc up to 42 K. The relationship between Tc and the iron-plane interlayer distance suggested that superconductivity due to the mono Fe2As2 layer is substantially 40 K-class., Comment: 11pages, 5figures

We have discovered a new iron pnictide oxide superconductor (Fe2As2)(Sr4(Mg,Ti)2O6). This material is isostructual with (Fe2As2)(Sr4M2O6) (M = Sc, Cr, V), which were found in previous studies. The structure of this compound is tetragonal with a space group of P4/nmm and consists of the anti-fluorite type FeAs layer and perovskite-type block layer. The lattice constants are a = 3.935 A and c = 15.952 A for (Fe2As2)(Sr4MgTiO6). Bulk superconductivity with Tc(onset) of ~26 K was observed for a partially Co substituted sample. Moreover, Co-free and Ti-rich samples exhibited higher Tc(onset)'s above 35 K, which were further enhanced by applying high pressures up to ~43 K., Comment: Resubmission of arXiv:0909.2945 with new data

We have discovered new nickel-based pnictide oxide superconductors, (Ni2Pn2)(Sr4Sc2O6) (Pn = P, As). These compounds have a tetragonal unit cell with a space group of P4/nmm and they consist of alternate stacking of anti-fluorite Ni2Pn2 layers and K2NiF4-type Sr4Sc2O6 blocking layers. Lattice parameters were a = 4.044 A and c = 15.23 A for (Ni2P2)(Sr4Sc2O6) and a = 4.078 A and c = 15.41 A for (Ni2As2)(Sr4Sc2O6), indicating their thicker blocking layers than that of LaNiPO (c ~ 8.1 A). Both (Ni2P2)(Sr4Sc2O6) and (Ni2As2)(Sr4Sc2O6) exhibited superconductivity with zero resistivity at 3.3 K and 2.7 K, respectively. The perfect diamagnetism observed in both compounds guaranteed their bulk superconductivity., Comment: 4 pages, 3 figures, 1 table

We have discovered new layered oxyarsenides (Fe2As2)(Sr4M2O6) (M = Sc, Cr: M-22426). These materials are isostructural with (Fe2P2)(Sr4Sc2O6), which was found in our previous study. The new compounds are tetragonal with a space group of P4/nmm and consist of the anti-fluorite type FeAs layer and perovskite-type blocking layer. The lattice constants are a = 4.050 A, c = 15.809 A for M = Sc and a = 3.918 A, c = 15.683 A for M = Cr. These compounds have long interlayer Fe-Fe distances corresponding to the c-axis length, the 15.8 A in Sc-22426 is the longest in the iron-based oxypnictide systems. Chemical flexibility of the perovskite block in this system was probed by chromium containing (Fe2As2)(Sr4Cr2O6). Different trends were found in bond angle and bond length of the new oxypnictides compared to the reported systems, such as REFePnO. Absence of superconductivity in these compounds is considered to be due to insufficient carrier concentration as in the case of undoped REFeAsO., Comment: 7 pages, 5 figures, 1 table