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A substance that reaches superconductivity, a state in which magnetic fields cannot penetrate, and there is no electrical resistance, is referred to as a superconductor. In 1911, Heike Kamerlingh Onnes of Leiden University, a Dutch physicist, observed a relation between the temperature and the resistance of the element mercury. The mercury sample was then cooled in liquid helium to study the linear dependence of resistance on temperature. It was observed that, as the temperature decreased, the...
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An ionic compound is stable because of the electrostatic attraction between its positive and negative ions. The lattice energy of a compound is a measure of the strength of this attraction. The lattice energy (ΔHlattice) of an ionic compound is defined as the energy required to separate one mole of the solid into its component gaseous ions. For the ionic solid sodium chloride, the lattice energy is the enthalpy change of the process:
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Li(C5H5N)Fe2-Se2: A Defect-Resilient Expanded-Lattice High-Temperature Superconductor.

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Molecule-intercalated iron selenides show enhanced superconductivity up to 44 K. This is linked to electronic and structural changes in the iron selenide layers, driven by interlayer spacing and iron-site vacancies.

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Area of Science:

  • Condensed Matter Physics
  • Materials Science
  • Superconductivity

Background:

  • Two-dimensional iron chalcogenides exhibit a correlation between interlayer spacing and superconducting critical temperature (Tc).
  • Understanding the relationship between doping, structure, and superconductivity in these materials is crucial for developing new superconductors.

Purpose of the Study:

  • To investigate the electronic and local structural changes in molecule-intercalated Li(C5H5N)Fe2-xSe2 that lead to enhanced superconductivity (Tc ~ 44 K).
  • To elucidate the role of interlayer spacing and iron-site vacancies in tuning the superconducting properties.

Main Methods:

  • Synchrotron X-ray absorption (XAS) and X-ray emission (XES) spectroscopies at Fe and Se K-edges.
  • Extended X-ray absorption fine structure (EXAFS) analysis.
  • Density functional theory (DFT) calculations.

Main Results:

  • XES revealed low-spin iron moieties with slightly reduced magnetic moments in the FeSe4 tetrahedra.
  • Pre-edge XAS indicated reduced mixing of Fe 3d-4p states upon lithiation.
  • EXAFS and DFT showed that Fe-site vacancies lead to a softer Fe network and stretched Fe sheets, alleviating electron-lattice correlations.

Conclusions:

  • The robust high-Tc in Li(C5H5N)Fe2-xSe2 arises from the interplay of electron-donating spacers and the iron selenide layer's tolerance to defect chemistry.
  • Fe-site vacancies favorably tune the Fermi surface properties, contributing to enhanced superconductivity.