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The intrinsically hole-doped RbEuFe$_4$As$_4$ exhibits bulk superconductivity at $T_{mathrm{sc}}=36.5$ K and ferromagnetic ordering in the Eu sublattice at $T_mathrm{m}=15$ K. Here we present a hole-compensation study by introducing extra itinerant electrons via a Ni substitution in the ferromagnetic superconductor RbEuFe$_4$As$_4$ with $T_{mathrm{sc}}>T_{mathrm{m}}$. With the Ni doping, $T_{mathrm{sc}}$ decreases rapidly, and the Eu-spin ferromagnetism and its $T_{mathrm{m}}$ remain unchanged. Consequently, the system RbEu(Fe$_{1-x}$Ni$_x$)$_4$As$_4$ transforms into a superconducting ferromagnet with $T_{mathrm{m}}>T_{mathrm{sc}}$ for $0.07leq xleq0.08$. The occurrence of superconducting ferromagnets is attributed to the decoupling between Eu$^{2+}$ spins and superconducting Cooper pairs. The superconducting and magnetic phase diagram is established, which additionally includes a recovered yet suppressed spin-density-wave state.
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Superconductivity (SC) and ferromagnetism (FM) are in general antagonistic, which makes their coexistence very rare. Following our recent discovery of robust coexistence of SC and FM in RbEuFe$_4$As$_4$ [Y. Liu et al., arXiv: 1605.04396 (2016)], here we report another example of such a coexistence in its sister compound CsEuFe$_4$As$_4$, synthesized for the first time. The new material exhibits bulk SC at 35.2 K and Eu$^{2+}$-spin ferromagnetic ordering at 15.5 K, demonstrating that it is a new robust ferromagnetic superconductor.
Temperature dependent $^{57}$Fe Mossbauer spectroscopy and specific heat measurements for CaK(Fe$_{1-x}$Ni$_x$)$_4$As$_4$ with $x$ = 0, 0.017, 0.033, and 0.049 are presented. No magnetic hyperfine field (e.g. no static magnetic order) down to 5.5 K was detected for $x$ = 0 and 0.017 in agreement with the absence of any additional feature below superconducting transition temperature, $T_c$, in the specific heat data. The evolution of magnetic hyperfine field with temperature was studied for $x$ = 0.033 and 0.049. The long-range magnetic order in these two compounds coexists with superconductivity. The magnetic hyperfine field, $B_{hf}$, (ordered magnetic moment) below $T_c$ in CaK(Fe$_{0.967}$Ni$_{0.033}$)$_4$As$_4$ is continuously suppressed with the developing superconducting order parameter. The $B_{hf}(T)$ data for CaK(Fe$_{0.967}$Ni$_{0.033}$)$_4$As$_4$, and CaK(Fe$_{0.951}$Ni$_{0.049}$)$_4$As$_4$ can be described reasonably well by Machidas model for coexistence of itinerant spin density wave magnetism and superconductivity [K. Machida, J. Phys. Soc. Jpn. {bf 50}, 2195 (1981)]. We demonstrate directly that superconductivity suppresses the spin density wave order parameter if the conditions are right, in agreement with the theoretical analysis.
Recently, An electron-doped 12442-type iron-based superconductor BaTh$_2$Fe$_4$As$_4$(N$_{0.7}$O$_{0.3}$)$_2$ has been successfully synthesized with high-temperature solid-state reactions on basis of a structural design. The inter-block-layer charge transfer between the constituent units of BaFe$_2$As$_2$ and ThFeAsN$_{0.7}$O$_{0.3}$ was found to be essential to stabilize the target compound. Dominant electron-type conduction and bulk superconducting transition at ~22 K were demonstrated.
We report an inelastic neutron scattering study on the spin resonance in the bilayer iron-based superconductor CaKFe$_4$As$_4$. In contrast to its quasi-two-dimensional electron structure, three strongly $L$-dependent modes of spin resonance are found below $T_c=35$ K. The mode energies are below and linearly scale with the total superconducting gaps summed on the nesting hole and electron pockets, essentially in agreement with the results in cuprate and heavy fermion superconductors. This observation supports the sign-reversed Cooper pairing mechanism under multiple pairing channels and resolves the long-standing puzzles concerning the broadening and dispersive spin resonance peak in iron pnictides. More importantly, the triple resonant modes can be classified into odd and even symmetries with respect to the distance of Fe-Fe planes within the Fe-As bilayer unit. Thus, our results closely resemble those in the bilayer cuprates with nondegenerate spin excitations, suggesting that these two high-$T_c$ superconducting families share a common nature.
$^{57}$Fe Mossbauer spectra at different temperatures between $sim 5$ K and $sim 300$ K were measured on an oriented mosaic of single crystals of CaKFe$_4$As$_4$ . The data indicate that CaKFe$_4$As$_4$ is a well formed compound with narrow spectral lines, no traces of other, Fe - containing, secondary phases in the spectra and no static magnetic order. There is no discernible feature at the superconducting transition temperature in any of the hyperfine parameters. The temperature dependence of the quadrupole splitting approximately follows the empirical $T^{3/2}$ law. The hyperfine parameters of CaKFe$_4$As$_4$ are compared with those for KFe$_2$As$_2$ measured in this work, and the literature data for CaFe$_2$As$_2$, and were found to be in between those for these two, ordered, 122 compounds, in agreement with the gross view of CaKFe$_4$As$_4$ as a structural analog of KFe$_2$As$_2$ and CaFe$_2$As$_2$ that has alternating Ca - and K - layers in the structure.
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