Publication date: 10th April 2024
A subset of polyanionic salts of Li+ and Na+ exhibit crystalline phases with distinct rotational disorder of the polyanion that is typically commensurate with increased ionic conductivity of the cation. These mesophases are sometimes referred to as “plastic crystals” or “rotor phases” and combine properties of classical solids and classical liquids. Macroscopically they retain their shape and exhibit sharp Bragg diffraction ("solid-like") while locally they are dynamically disordered and exhibit high atomic mobility ("liquid-like").
The behavior of three such systems will be presented and contrasted, namely the “classical” Li2SO4 and Na3PO4, along with the recently discovered Na3PS4. [1,2] Classical crystallographic approaches (i.e. Rietveld refinement to diffraction data) either break down or provide limited information on the average structure without capturing the dynamics of such structures. Thus, attempts to complement the study of said systems via advanced crystallography (e.g. total scattering), spectroscopy (e.g. Raman, NMR, INS) and computations (e.g. molecular dynamics) will be presented.
The current understanding of how the polyanionic rotational diffusion might be correlated with the cationic translational diffusion (“paddle-wheel” effect etc.) will be discussed.
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