Superconductivity and phase instability of NH3-free Na-intercalated FeSe1-zSz

Abstract

The discovery of ThCr2Si2-type AxFe2-ySe2 (A = K, Rb, Cs and Tl) with Tc ~ 30K make much progress in iron-based superconducting field, but their multiple-phase separations are disadvantageous for understanding the origin. On the other hand, for small alkali metals, studies on (Li,Na)FeCu(S,Se)2 and NaFe2-δS2 shows that these compounds possess CaAl2Si2-type structure, implying that ThCr2Si2-type structure is unstable for small alkali-metal intercalated FeSe under high-temperature. Here we report a new intercalate Na0.65(1)Fe1.93(1)Se2 with Tc ~ 37 K, synthesized by low-temperature ammonothermal method. The notable finding is that the Na0.65(1)Fe1.93(1)Se2 shows a ThCr2Si2-type structure, which is the first instance of small-sized alkali metal intercalates without NH3 co-intercalation. Besides, the NH3-poor Na0.80(4)(NH3)0.60Fe1.86(1)Se2 and NH3-rich phase with Tcs at 45 K and 42 K are identified by tuning the concentration of Na-NH3 solutions. The modulation of interlayer spacing reveals the versatile evolution of structural stability and superconductivity in these intercalates.

22 pages, 4 figures, 1 tabel

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• Substitution Effects on FeSe Superconductor
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• Superconducting Phases in Potassium-Intercalated Iron Selenides
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• Protonation-induced discrete superconducting phases in bulk FeSe single crystals
• New Alkali-Metal- and 2-Phenethylamine-Intercalated Superconductors $A_x$(C${}_8$H${}_{11}$N)${}_y$Fe${}_{1-z}$Se ($A$ = Li, Na) with the Largest Interlayer Spacings and $T_{\mathrm{c}}$ $\sim$ 40 K
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