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Register a new userCorrelated disorder to order crossover in the local structure of K$_x$Fe$_{2-y}$Se$_{2-z}$S$_z$
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A detailed account of the local atomic structure and disorder at 5~K across the phase diagram of the high temperature superconductor K$_x$Fe$_{2-y}$Se$_{2-z}$S$_z$ $(0 leq z leq 2)$ is obtained from neutron total scattering and associated atomic pair distribution function (PDF) approaches. Various model independent and model dependent aspects of the analysis reveal a high level of structural complexity on the nanometer length-scale. Evidence is found for considerable disorder in the $c$-axis stacking of the FeSe$_{1-x}$S$_{x}$ slabs without observable signs of turbostratic character of the disorder. In contrast to the related FeCh (Ch = S, Se) type superconductors, substantial Fe-vacancies are present in K$_x$Fe$_{2-y}$Se$_{2-z}$S$_z$, deemed detrimental for superconductivity when ordered. Our study suggests that the distribution of vacancies significantly modifies the iron-chalcogen bond-length distribution, in agreement with observed evolution of the PDF signal. A crossover like transition is observed at a composition of $zapprox1$, from a predominantly vacancy-disordered state at the selenium end to a more vacancy-ordered (VO) phase closer to the sulfur end of the phase diagram. The S-content dependent measures of the local structure are found to exhibit distinct behavior on either side of this crossover, correlating well with the evolution of the superconducting state to that of a magnetic semiconductor towards the $zapprox2$ end. The behavior reinforces the idea of the intimate relationship of correlated Fe-vacancies order in the local structure and the emergent electronic properties.
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Structural phase separation in A$_x$Fe$_{2-y}$Se$_2$ system has been studied by different experimental techniques, however, it should be important to know how the electronic uniformity is influenced, on which length scale the electronic phases coexist, and what is their spatial distribution. Here, we have used novel scanning photoelectron microscopy (SPEM) to study the electronic phase separation in K$_x$Fe$_{2-y}$Se$_2$, providing a direct measurement of the topological spatial distribution of the different electronic phases. The SPEM results reveal a peculiar interconnected conducting filamentary phase that is embedded in the insulating texture. The filamentary structure with a particular topological geometry could be important for the high T$_c$ superconductivity in the presence of a phase with a large magnetic moment in A$_x$Fe$_{2-y}$Se$_2$ materials.
Recent discovery of superconducting (SC) ternary iron selenides has block antiferromagentic (AFM) long range order. Many experiments show possible mesoscopic phase separation of the superconductivity and antiferromagnetism, while the neutron experiment reveals a sizable suppression of magnetic moment due to the superconductivity indicating a possible phase coexistence. Here we propose that the observed suppression of the magnetic moment may be explained due to the proximity effect within a phase separation scenario. We use a two-orbital model to study the proximity effect on a layer of block AFM state induced by neighboring SC layers via an interlayer tunneling mechanism. We argue that the proximity effect in ternary Fe-selenides should be large because of the large interlayer coupling and weak electron correlation. The result of our mean field theory is compared with the neutron experiments semi-quantitatively. The suppression of the magnetic moment due to the SC proximity effect is found to be more pronounced in the d-wave superconductivity and may be enhanced by the frustrated structure of the block AFM state.
K$_x$Fe$_{2-y}$Se$_2$ exhibits an iron-vacancy ordering at $T_{rm s} {sim}270{deg}$C and separates into two phases: a minor superconducting (iron-vacancy-disordered) phase and a major non-superconducting (iron-vacancy-ordered) phase. The microstructural and superconducting properties of this intermixture can be tuned by an appropriate control of the quenching process through $T_{rm s}$. A faster quenching rate leads to a finer microstructure and a suppression of formation of the non-superconducting phase by up to 50%. Nevertheless, such a faster cooling rate does induce a monotonic reduction in the superconducting transition temperature (from 30.7 K down to 26.0 K) and, simultaneously, a decrease in the iron content within the superconducting phase such that the compositional ratio changed from K$_{0.35}$Fe$_{1.83}$Se$_2$ to K$_{0.58}$Fe$_{1.71}$Se$_2$.
We have combined elastic and inelastic neutron scattering techniques, magnetic susceptibility and resistivity measurements to study single-crystal samples of K$_x$Fe$_{2-y}$Se$_2$, which contain the superconducting phase that has a transition temperature of $sim$31 K. In the inelastic neutron scattering measurements, we observe both the spin-wave excitations resulting from the block antiferromagnetic ordered phase and the resonance that is associated with the superconductivity in the superconducting phase, demonstrating the coexistence of these two orders. From the temperature dependence of the intensity of the magnetic Bragg peaks, we find that well before entering the superconducting state, the development of the magnetic order is interrupted, at $sim$42 K. We consider this result to be evidence for the physical separation of the antiferromagnetic and superconducting phases; the suppression is possibly due to the proximity effect of the superconducting fluctuations on the antiferromagnetic order.
After our first discovery of superconductivity (SC) with $T_C$=3.7 K in TlNi$_2$Se$_2$, we grew successfully a series of TlNi$_2$Se$_{2-x}$S$_x$ (0.0 $leq$ x $leq$2.0) single crystals. The measurements of resistivity, susceptibility and specific heat were carried out. We found that SC with $T_C$=2.3 K also emerges in TlNi$_2$S$_2$ crystal, which appears to involve heavy electrons with an effective mass $m^*$=13$sim$25 $m_b$, as inferred from the normal state electronic specific heat and the upper critical field, $H_{C2}(T)$. It was found that the $T_C$ and superconducting volume fraction in TlNi$_2$Se$_{2-x}$S$_x$ crystals changes with the disorder degree induced by the partial substitution of S for Se, which is characterized by the residual resistivity ratio (textit{RRR}). The effect of the disorder on SC may provide some information for understanding the mechanism of SC in this new Ni-chalcogenide system.
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