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Register a new userNegative ionic states of tin in the oxide superconductor Sr$_{3-x}$SnO revealed by M{o}ssbauer spectroscopy
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Atsutoshi Ikeda
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We report the temperature variation of the $^{119}$Sn-M{o}ssbauer spectra of the antiperovskite (inverse perovskite) oxide superconductor Sr$_{3-x}$SnO. Both superconductive (Sr-deficient) and non-superconductive (nearly stoichiometric) samples exhibit major $gamma$-ray absorption with isomer shift similar to that of Mg$_2$Sn. This fact shows that Sr$_{3-x}$SnO contains the metallic anion Sn$^{4-}$, which is rare especially among oxides. In both samples, we observed another $gamma$-ray absorption with a larger isomer shift, indicating that there is another ionic state of Sn with a higher oxidation number. The temperature dependence of the absorption intensities reveals that the Sn ions exhibiting larger isomer shifts have a lower energy of the local vibration. The larger isomer shift and lower vibration energy are consistent with the values estimated from the first-principles calculations for hypothetical structures with various Sr-deficiency arrangements. Therefore, we conclude that the additional $gamma$-ray absorptions originate from the Sn atoms neighboring the Sr deficiency.
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We report a $mu$SR study on the antiperovskite oxide superconductor Sr$_{3-x}$SnO. With transverse-field $mu$SR, we observed the increase of the muon relaxation rate upon cooling below the superconducting transition temperature $T_{mathrm{c}}=5.4$ K, evidencing bulk superconductivity. The exponential temperature dependence of the relaxation rate $sigma$ at low temperatures suggests a fully gapped superconducting state. We evaluated the zero-temperature penetration depth $lambda(0)propto1/sqrt{sigma(0)}$ to be around 320-1020 nm. Such a large value is consistent with the picture of a doped Dirac semimetal. Moreover, we revealed that the ratio $T_{mathrm{c}}/lambda(0)^{-2}$ is larger than those of ordinary superconductors and is comparable to those of unconventional superconductors. The relatively high $T_{mathrm{c}}$ for small carrier density may hint at an unconventional pairing mechanism beyond the ordinary phonon-mediated pairing. In addition, zero-field $mu$SR did not provide evidence of broken time-reversal symmetry in the superconducting state. These features are consistent with the theoretically proposed topological superconducting state in Sr$_{3-x}$SnO, as well as with $s$-wave superconductivity.
A large variety of perovskite oxide superconductors are known, including some of the most prominent high-temperature and unconventional superconductors. However, superconductivity among the oxidation state inverted material class, the antiperovskite oxides, was reported just recently for the first time. In this superconductor, Sr$_{3-x}$SnO, the unconventional ionic state Sn$^{4-}$ is realized and possible unconventional superconductivity due to a band inversion has been discussed. Here, we discuss an improved facile synthesis method, making it possible to control the strontium deficiency in Sr$_{3-x}$SnO. Additionally, a synthesis method above the melting point of Sr$_{3}$SnO is presented. We show temperature dependence of magnetization and electrical resistivity for superconducting strontium deficient Sr$_{3-x}$SnO ($T_{mathrm{c}}$ ~ 5 K) and for Sr$_{3}$SnO without a superconducting transition down to 0.15 K. Further, we reveal a significant effect of strontium raw material purity on the superconductivity and achieve 40% increased superconducting volume fraction (~100%) compared to the highest value reported so far. More detailed characterisation utilising powder X-ray diffraction and energy-dispersive X-ray spectroscopy show that a minor cubic phase, previously suggested to be a Sr$_{3-x}$SnO, is SrO. The improved characterization and controlled synthesis reported herein enable detailed investigations on the superconducting nature and its dependency on the strontium deficiency in Sr$_{3-x}$SnO.
We have performed $^{119}$Sn-NMR measurements on the antiperovskite oxide superconductor Sr$_{3-x}$SnO to investigate how its normal state changes with the Sr deficiency. A two-peak structure was observed in the NMR spectra of all the measured samples. This suggests that the phase separation tends to occur between the nearly stoichiometric and heavily Sr-deficient Sr$_{3-x}$SnO phases. The measurement of the nuclear spin-lattice relaxation rate $1/T_1$ indicates that the Sr-deficient phase shows a conventional metallic behavior due to the heavy hole doping. In contrast, the nearly stoichiometric phase exhibits unusual temperature dependence of $1/T_1$, attributable to the presence of a Dirac-electron band.
The class of antiperovskite compounds $A_3B$O ($A$ = Ca, Sr, Ba; $B$ = Sn, Pb) has attracted interest as a candidate 3D Dirac system with topological surface states protected by crystal symmetry. A key factor underlying the rich electronic structure of $A_3B$O is the unusual valence state of $B$, i.e., a formal oxidation state of $-4$. Practically, it is not obvious whether anionic $B$ can be stabilized in thin films, due to its unusual chemistry, as well as the polar surface of $A_3B$O, which may render the growth-front surface unstable. We report X-ray photoelectron spectroscopy (XPS) measurements of single-crystalline films of Sr$_3$SnO and Sr$_3$PbO grown by molecular beam epitaxy (MBE). We observe shifts in the core-level binding energies that originate from anionic Sn and Pb, consistent with density functional theory (DFT) calculations. Near the surface, we observe additional signatures of neutral or cationic Sn and Pb, which may point to an electronic or atomic reconstruction with possible impact on putative topological surface states.
We have performed x-ray magnetic circular dichroism (XMCD) measurements on the iron-based superconductor Sr$_2$VFeAsO$_{3-delta}$ to study the origin of weak ferromagnetism (WFM) reported for this compound. While Fe 3$d$ electrons show a magnetic response similar to the other iron pnictides, signals from V 3$d$ electrons remain finite at zero magnetic field and may be responsible for the WFM.
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