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Crystal Structure and Superconductivity at about 30 K in $A$Ca$_2$Fe$_4$As$_4$F$_2$ ($A$ = Rb, Cs)

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 Added by Guang-Han Cao
 Publication date 2017
  fields Physics
and research's language is English




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We have synthesized two iron fluo-arsenides $A$Ca$_2$Fe$_4$As$_4$F$_2$ with $A$ = Rb and Cs, analogous to the newly discovered superconductor KCa$_2$Fe$_4$As$_4$F$_2$. The quinary inorganic compounds crystallize in a body-centered tetragonal lattice with space group I4/mmm, which contain double Fe$_2$As$_2$ layers that are separated by insulating Ca$_2$F$_2$ layers. Our electrical and magnetic measurements on the polycrystalline samples demonstrate that the new materials undergo superconducting transitions at Tc = 30.5 K and 28.2 K, respectively, without extrinsic doping. The correlations between Tc and structural parameters are discussed.



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We have synthesized 10 new iron oxyarsenides, K$Ln_2$Fe$_4$As$_4$O$_2$ ($Ln$ = Gd, Tb, Dy, and Ho) and Cs$Ln_2$Fe$_4$As$_4$O$_2$ ($Ln$ = Nd, Sm, Gd, Tb, Dy, and Ho), with the aid of lattice-match [between $A$Fe$_2$As$_2$ ($A$ = K and Cs) and $Ln$FeAsO] approach. The resultant compounds possess hole-doped conducting double FeAs layers, [$A$Fe$_4$As$_4$]$^{2-}$, that are separated by the insulating [$Ln_2$O$_2$]$^{2+}$ slabs. Measurements of electrical resistivity and dc magnetic susceptibility demonstrate bulk superconductivity at $T_mathrm{c}$ = 33 - 37 K. We find that $T_mathrm{c}$ correlates with the axis ratio $c/a$ for all 12442-type superconductors discovered. Also, $T_mathrm{c}$ tends to increase with the lattice mismatch, implying a role of lattice instability for the enhancement of superconductivity.
We find evidence that the newly discovered Fe-based superconductor KCa$_2$Fe$_4$As$_4$F$_2$ ($T_c~=~33.36(7)$~K) displays multigap superconductivity with line nodes. Transverse field muon spin rotation ($mu$SR) measurements show that the temperature dependence of the superfluid density does not have the expected behavior of a fully-gapped superconductor, due to the lack of saturation at low temperatures. Moreover, the data cannot be well fitted using either single band models or a multiband $s$-wave model, yet are well described by two-gap models with line nodes on either one or both of the gaps. Meanwhile the zero-field $mu$SR results indicate a lack of time reversal symmetry breaking in the superconducting state, but suggest the presence of magnetic fluctuations. These results demonstrate a different route for realizing nodal superconductivity in iron-based superconductors. Here the gap structure is drastically altered upon replacing one of the spacer layers, indicating the need to understand how the pairing state is tuned by changes of the asymmetry between the pnictogens located either side of the Fe planes.
We report synthesis, crystal structure and physical properties of a quinary iron-arsenide fluoride KCa$_2$Fe$_4$As$_4$F$_2$. The new compound crystallizes in a body-centered tetragonal lattice (with space group $I4/mmm$, $a$ = 3.8684(2) {AA}, c = 31.007(1) {AA}, and $Z$ = 2), which contains double Fe$_2$As$_2$ conducting layers separated by insulating Ca$_2$F$_2$ layers. Our measurements of electrical resistivity, dc magnetic susceptibility and heat capacity demonstrate bulk superconductivity at 33 K in KCa$_2$Fe$_4$As$_4$F$_2$.
We have synthesized four iron-based oxyarsenide superconductors Rb$Ln_2$Fe$_4$As$_4$O$_2$ ($Ln$ = Sm, Tb, Dy and Ho) resulting from the intergrowth of RbFe$_2$As$_2$ and $Ln$FeAsO. It is found that the lattice match between RbFe$_2$As$_2$ and $Ln$FeAsO is crucial for the phase formation. The structural intergrowth leads to double asymmetric Fe$_2$As$_2$ layers that are separated by insulating $Ln_2$O$_2$ slabs. Consequently, the materials are intrinsically doped at a level of 0.25 holes/Fe-atom and, bulk superconductivity emerges at $T_mathrm{c}$ = 35.8, 34.7, 34.3 and 33.8 K, respectively, for $Ln$ = Sm, Tb, Dy and Ho. Investigation on the correlation between crystal structure and $T_mathrm{c}$ suggests that interlayer couplings may play an additional role for optimization of superconductivity.
We present a systematic study of electrical resistivity, Hall coefficient, magneto-optical imaging, magnetization, and STEM analyses of KCa${_2}$Fe${_4}$As${_4}$F${_2}$ single crystals. Sharp diamagnetic transition and magneto-optical imaging reveal homogeneity of single crystal and prominent Bean-like penetrations of vortices. Large anisotropy of electrical resistivity, with ${rho _c / rho _{ab}}$ > 100, and semiconductor-like ${rho _c}$ suggest that the electronic state is quasi two-dimensional. Hall effect measurements indicate that KCa${_2}$Fe${_4}$As${_4}$F${_2}$ is a multiband system with holes as main carriers. Magnetization measurements reveal significantly larger J$_c$ compared with that in other iron-based superconductors with different values of J$_c$ depending on the direction of magnetic field. Origin of these J$_c$ characteristics is discussed based on microstructural observations using STEM. In addition, further enhancement of J$_c$ in KCa${_2}$Fe${_4}$As${_4}$F${_2}$ for future application is demonstrated in terms of heavy-ion irradiation.
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