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Register a new userNanoscale phase separation of antiferromagnetic order and superconductivity in K$_{0.75}$Fe$_{1.75}$Se$_2$
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We report an in-plane optical spectroscopy study on the iron-selenide superconductor K$_{0.75}$Fe$_{1.75}$Se$_2$. The measurement revealed the development of a sharp reflectance edge below T$_c$ at frequency much smaller than the superconducting energy gap on a relatively incoherent electronic background, a phenomenon which was not seen in any other Fe-based superconductors so far investigated. Furthermore, the feature could be noticeably suppressed and shifted to lower frequency by a moderate magnetic field. Our analysis indicates that this edge structure arises from the development of a Josephson-coupling plasmon in the superconducting condensate. Together with the transmission electron microscopy analysis, our study yields compelling evidence for the presence of nanoscale phase separation between superconductivity and magnetism. The results also enable us to understand various seemingly controversial experimental data probed from different techniques.
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Vibrational properties of iron-chalcogenide superconductor K$_{0.75}$Fe$_{1.75}$Se$_{2}$ with $T_{c}sim$ 30 K have been measured by Raman and optical spectroscopies over temperature range of 3-300 K. Sample undergoes textit{I4/m} $to $ textit{I4} structural phase transition accompanied by loss of inversion symmetry at $T_{1}$, below 250 K, observed as appearance of new fully-symmetric Raman mode at $sim$ 165 cm$^{-1}$. Small vibration mode anomalies are also observed at $T_{2}sim$ 160 K. From first-principles vibrational analysis of antiferromagnetic K$_{0.8}$Fe$_{1.6}$Se$_{2}$ utilizing pseudopotentials all observed Raman and infrared modes have been assigned and the displacement patterns of the new Raman mode identified as involving predominantly the Se atoms.
We have used scanning micro x-ray diffraction to characterize different phases in superconducting K$_{x}$Fe$_{2-y}$Se$_2$ as a function of temperature, unveiling the thermal evolution across the superconducting transition temperature (T$_csim$32 K), phase separation temperature (T$_{ps}sim$520 K) and iron-vacancy order temperature (T$_{vo}sim$580 K). In addition to the iron-vacancy ordered tetragonal magnetic phase and orthorhombic metallic minority filamentary phase, we have found a clear evidence of the interface phase with tetragonal symmetry. The metallic phase is surrounded by this interface phase below $sim$300 K, and is embedded in the insulating texture. The spatial distribution of coexisting phases as a function of temperature provides a clear evidence of the formation of protected metallic percolative paths in the majority texture with large magnetic moment, required for the electronic coherence for the superconductivity. Furthermore, a clear reorganization of iron-vacancy order around the T$_{ps}$ and T$_c$ is found with the interface phase being mostly associated with a different iron-vacancy configuration, that may be important for protecting the percolative superconductivity in K$_{x}$Fe$_{2-y}$Se$_2$.
The electronic structure of the vacancy-ordered K$_{0.5}$Fe$_{1.75}$Se$_2$ iron-selenide compound (278 phase) is studied using the first-principles density functional method. The ground state of the 278 phase is stripe-like antiferromagnetic, and its bare electron susceptibility shows a large peak around $(pi, pi)$ in the folded Brillouin zone. Near Fermi level, the density of states are dominated by the Fe-3d orbitals, and both electron-like and hole-like Fermi surfaces appear in the Brillouin zone. Unfolded band structure shows limited similarities to a hole doped 122 phase. With 0.1e electron doping, the susceptibility peak is quickly suppressed and broadened; while the two-dimensionality of the electron-like Fermi surfaces are greatly enhanced, resulting in a better nesting behavior. Our study should be relevant to the recently reported superconducting phase K$_{0.5+x}$Fe$_{1.75+y}$Se$_2$ with both $x$ and $y$ very tiny.
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.
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$_2$.
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