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Register a new userFirst Homologous Series of Iron Pnictide Oxide Superconductors (Fe2As2)(Can+1(Sc,Ti)nOy) [n = 3,4,5] with Extremely Thick Blocking Layers
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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.
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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.
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.
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.
Structural features of newly found perovskite-based iron pnictide oxide system have been systematically studied. Compared to REFePnO system, perovskite-based system tend to have lower Pn-Fe-Pn angle and higher pnictogen height owing to low electronegativity of alkaline earth metal and small repulsive force between pnictogen and oxygen atoms. As-Fe-As angles of (Fe2As2)(Sr4Cr2O6), (Fe2As2)(Sr4V2O6) and (Fe2Pn2)(Sr4MgTiO6) are close to ideal tetrahedron and those pnictogen heights of about 1.40 A are close to NdFeAsO with optimized carrier concentration. These structural features of this system may leads to realization of high Tc superconductivity.
$^{75}$As and $^{45}$Sc NMR measurements unravel the electronic state for Fe-based superconductors with perovskite-type blocking layers Ca$_4$(Mg,Ti)$_3$Fe$_2$As$_2$O$_{8-y}$ ($T_c^{onset}=47$ K) and Ca$_5$(Sc,Ti)$_4$Fe$_2$As$_2$O$_{11-y}$ ($T_c^{onset}=41$ K). In Ca$_5$(Sc,Ti)$_4$Fe$_2$As$_2$O$_{11-y}$, the nuclear spin relaxation rate $1/T_1$ shows pseudogap behavior below $sim80$ K, suggesting that the electronic state is similar to that of LaFeAs(O,F) system with moderate electron doping. The presence of the pseudogap behavior gives an interpretation that the hole-like band (so-called $gamma$ pocket) is located just below the Fermi level from the analogy to LaFeAs(O,F) system and the disappearance of the $gamma$ pocket yields the suppression of the low-energy spin fluctuations. On the other hand, in Ca$_4$(Mg,Ti)$_3$Fe$_2$As$_2$O$_{8-y}$ satisfying the structural optimal condition for higher $T_c$ among the perovskite systems, the extrinsic contribution, which presumably originates in the Ti moment, is observed in $1/T_1T$; however, the moderate temperature dependence of $1/T_1T$ appears by its suppression under high magnetic field. In both systems, the high $T_c$ of $sim40$ K is realized in the absence of the strong development of the low-energy spin fluctuations. The present results reveal that the structural optimization does not induce the strong development of the low-energy spin fluctuations. If we consider that superconductivity is mediated by spin fluctuations, the structural optimization is conjectured to provide a benefit to the development of the high-energy spin fluctuations irrespective to the low-energy part.
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