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Area of Science:

  • Solid-state chemistry
  • Materials science
  • Ionic conductors

Background:

  • Disorder in crystalline solid electrolytes, particularly fluorites like (M,Sn)F2, is key to enhancing ionic conductivity.
  • Two types of disorder are known: cation occupational disorder and Sn(II) lone pair orientational disorder.

Purpose of the Study:

  • To characterize the structure and fluoride ion dynamics in cubic barium tin fluoride (BaSnF4).
  • To investigate the interplay between cation disorder, Sn lone pairs, and fluoride ion mobility.

Main Methods:

  • Rietveld refinement of X-ray diffraction (XRD) data.
  • 119Sn Mössbauer spectroscopy.
  • X-ray total-scattering PDF analysis.
  • Ab initio molecular dynamics (AIMD) simulations.
  • Variable-temperature 19F NMR spectroscopy.

Main Results:

  • Cubic BaSnF4 exhibits average fluorite structure with {Ba,Sn} cation disorder and stereoactive Sn(II) lone pairs.
  • Significant intrinsic fluoride ion disorder exists, with 1/3 of ions in octahedral sites due to Sn lone pair repulsion.
  • Fluoride ion dynamics are highly inhomogeneous, with higher mobility near Sn-rich environments.
  • Dynamical reorientation of Sn lone pairs is coupled to local cation configuration and ion dynamics.

Conclusions:

  • Intrinsic fluoride ion disorder and inhomogeneous dynamics are critical features of cubic BaSnF4.
  • The interplay between cation disorder, Sn lone pairs, and fluoride ion mobility governs ionic conductivity.
  • Understanding these local structural and dynamic effects is essential for designing advanced solid electrolytes.