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Register a new userSuperconductivity and magnetism in Iron Sulfides Intercalated by Metal Hydroxides
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Inspired by naturally occurring sulfide minerals, we present a new family of iron-based superconductors. A metastable form of FeS known as the mineral mackinawite forms two-dimensional sheets that can be readily intercalated by various cationic guest species. Under hydrothermal conditions using alkali metal hydroxides, we prepare three different cation and metal hydroxide-intercalated FeS phases including (Li$_{1-x}$Fe$_x$OH)FeS, [(Na$_{1-x}$Fe$_x$)(OH)$_2$]FeS, and K$_x$Fe$_{2-y}$S$_2$. Upon successful intercalation of the FeS layer, the superconducting critical temperature $T_c$ of mackinawite is enhanced from 5 K to 8 K for the (Li$_{1-x}$Fe$_x$OH)$^{delta+}$ intercalate. Layered heterostructures of [(Na$_{1-x}$Fe$_x$)(OH)$_2$]FeS resemble the natural mineral tochilinite, which contains an iron square lattice interleaved with a hexagonal hydroxide lattice. Whilst heterostructured [(Na$_{1-x}$Fe$_x$)(OH)$_2$]FeS displays long-range magnetic ordering near 15 K, K$_x$Fe$_{2-y}$S$_2$ displays short range antiferromagnetism.
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Angle resolved photoemission spectroscopy (ARPES) reveals the features of the electronic structure of quasi-two-dimensional crystals, which are crucial for the formation of spin and charge ordering and determine the mechanisms of electron-electron interaction, including the superconducting pairing. The newly discovered iron based superconductors (FeSC) promise interesting physics that stems, on one hand, from a coexistence of superconductivity and magnetism and, on the other hand, from complex multi-band electronic structure. In this review I want to give a simple introduction to the FeSC physics, and to advocate an opinion that all the complexity of FeSC properties is encapsulated in their electronic structure. For many compounds, this structure was determined in numerous ARPES experiments and agrees reasonably well with the results of band structure calculations. Nevertheless, the existing small differences may help to understand the mechanisms of the magnetic ordering and superconducting pairing in FeSC.
Hydrothermal synthesis is described of layered lithium iron selenide hydroxides Li1-xFex(OH)Fe1-ySe (x ~ 0.2; 0.02 < y < 0.15) with a wide range of iron site vacancy concentrations in the iron selenide layers. This iron vacancy concentration is revealed as the only significant compositional variable and as the key parameter controlling the crystal structure and the electronic properties. Single crystal X-ray diffraction, neutron powder diffraction and X-ray absorption spectroscopy measurements are used to demonstrate that superconductivity at temperatures as high as 40 K is observed in the hydrothermally synthesised samples when the iron vacancy concentration is low (y < 0.05) and when the iron oxidation state is reduced slightly below +2, while samples with a higher vacancy concentration and a correspondingly higher iron oxidation state are not superconducting. The importance of combining a low iron oxidation state with a low vacancy concentration in the iron selenide layers is emphasised by the demonstration that reductive post-synthetic lithiation of the samples turns on superconductivity with critical temperatures exceeding 40 K by displacing iron atoms from the Li1-xFex(OH) reservoir layer to fill vacancies in the selenide layer
The parent compound of an unconventional superconductor must contain unusual correlated electronic and magnetic properties of its own. In the high-Tc potassium intercalated FeSe, there has been significant debate regarding what the exact parent compound is. Our studies unambiguously show that the Fe-vacancy ordered K2Fe4Se5 is the magnetic, Mott insulating parent compound of the superconducting state. Non-superconducting K2Fe4Se5 becomes a superconductor after high temperature annealing, and the overall picture indicates that superconductivity in K2-xFe4+ySe5 originates from the Fe-vacancy order to disorder transition. Thus, the long pending question whether magnetic and superconducting state are competing or cooperating for cuprate superconductors may also apply to the Fe-chalcogenide superconductors. It is believed that the iron selenides and related compounds will provide essential information to understand the origin of superconductivity in the iron-based superconductors, and possibly to the superconducting cuprates.
The complex interdigitated phases have greatly frustrated attempts to document the basic features of the superconductivity in the alkali metal intercalated iron chalcogenides. Here, using elastic neutron scattering, energy-dispersive x-ray spectroscopy, and resistivity measurements, we elucidate the relations of these phases in Rb$_{1-delta}$Fe$_y$Se$_{2-z}$S$_z$. We find: i) the iron content is crucial in stabilizing the stripe antiferromagnetic (AF) phase with rhombic iron vacancy order ($yapprox1.5$), the block AF phase with $sqrt{5}times sqrt{5}$ iron vacancy order ($yapprox1.6$), and the iron vacancy-free phase ($yapprox2$); ii) the superconducting phase ($z=0$) evolves into a metallic phase ($z>1.5$) with sulfur substitution due to the progressive decrease of the electronic correlation strength. Both the stripe AF phase and the block AF phase are Mott insulators. Our data suggest that there are miscibility gaps between these three phases. The existence of the miscibility gaps in the iron content is the key to understanding the relationship between these complicated phases.
The layered iron superconductors are discussed using electronic structure calculations. The four families of compounds discovered so far, including Fe(Se,Te) have closely related electronic structures. The Fermi surface consists of disconnected hole and electron cylinders and additional hole sections that depend on the specific material. This places the materials in proximity to itinerant magnetism, both due to the high density of states and due to nesting. Comparison of density functional results and experiment provides strong evidence for itinerant spin fluctuations, which are discussed in relation to superconductivity. It is proposed that the intermediate phase between the structural transition and the SDW transition in the oxy-pnictides is a nematic phase.
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