Magnetic suppression for a possible Fe-poor organic-inorganic hybrid superconductor Fe14Se16(tepa)0.8 (tepa = tetraethylenepentamine) with a superconducting transition at ∼42 K

doi:10.1016/j.jmst.2024.02.033

Abstract

Abstract: Composition/structure-dependent superconductivity for FeSe-based superconductors attracted great attention not only due to their high superconducting transition temperatures (T_C), but also for understanding the origin of iron-based superconductivity. Here, we report a new Fe-poor organic-inorganic hybrid material Fe₁₄Se₁₆(tepa)_0.8 with a paramagnetic-diamagnetic transition at ∼42 K grown by a high-temperature organic-solution-phase method with soluble iron/selenium sources in a tepa solution, alternative to previous intercalation strategies. The Fe₁₄Se₁₆(tepa)_0.8 phase is in a tetragonal layered hybrid structure with a nanoplate shape. Composition analyses reveal a Fe-poor characteristic of the hybrid in contrast to previous FeSe-intercalated superconductor, and selected area electron diffraction pattern is featured by Fe₃Se₄ superstructures with a √2 × √2 of Fe vacancy order. Ab initio density functional calculations show that minus Fe₃Se₄ ions are stable in the hybrid and ∼0.25e^-/Fe_0.75Se is obviously larger than the reported values of approximately 0.2e^-/FeSe in other FeSe-intercalated superconductors. Typical hysteresis loops and temperature dependence of dc/ac susceptibilities of the Fe₁₄Se₁₆(tepa)_0.8 measured below ∼42 K suggest a presence of the Meissner effect in this material. Effects of synthesis conditions on structures and magnetic properties of the hybrids show a magnetic evolution from a long-range ferrimagnetic (FIM) order of Fe₁₄Se₁₆(tepa) to a coexistence of FIM and superconducting (SC) orders of Fe₁₄Se₁₆(tepa)_0.9 and an SC order of Fe₁₄Se₁₆(tepa)_0.8. X-ray absorption spectrum (XAS) confirms the presence of ferric/ferrous irons. Mössbauer studies reveal that the high-T_C superconductivity originates from a suppression of the FIM order through tuning the spin states of irons from high-spin Fe³⁺ (S = 5/2) and Fe²⁺ (S = 2) in the Fe₁₄Se₁₆(tepa) to low-spin Fe³⁺ (S = 1/2) and Fe²⁺ (S = 0) in the Fe₁₄Se₁₆(tepa)_0.8. Although no zero resistance is detected even at a temperature of 2 K, the resistivity at 2 K decreases by more than 1600 times compared to that in a normal state calculated by a variable range hopping (VRH) model, suggesting that the high-T_C superconductivity of Fe₁₄Se₁₆(tepa)_0.8 is possible.

Key words: Iron-based hybrid superconductor, Superconductivity, Superconducting transition, Magnetic properties, Solution synthesis

Da Li, Qifeng Kuang, Xiaoling Men, Bo Zhang, Jianqi Huang, Xiaolei Shang, Bing Yang, Teng Yang, Zhiwei Li, Zhidong Zhang. Magnetic suppression for a possible Fe-poor organic-inorganic hybrid superconductor Fe₁₄Se₁₆(tepa)_0.8 (tepa = tetraethylenepentamine) with a superconducting transition at ∼42 K[J]. J. Mater. Sci. Technol., 2024, 198: 98-110.

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Magnetic suppression for a possible Fe-poor organic-inorganic hybrid superconductor Fe₁₄Se₁₆(tepa)_0.8 (tepa = tetraethylenepentamine) with a superconducting transition at ∼42 K

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