Publication date: 10th April 2024
Nuclear magnetic resonance offers plenty of advanced techniques, such as 1D and 2D EXSY [1,2], to study dynamic features of solid-state lithium ion conductors. Provided ultrafast ion dynamics is present at temperatures around ambient, i.e., dealing with jump rates in the order of some GHz, extremely low, if not cryogenic, temperatures are needed to completely freeze any Li+ ion dynamics on the NMR time scale. Taking advantage of two substances, viz. Ge-bearing Li6PS5I [3] and LiTi2(PS4)3 [4], we measured 7Li NMR line shapes and spin-lattice relaxation rates over a wide temperature range down to 9 K. The NMR experiments resolve the various Li+ exchange processes that ultimately give rise to overall, fast ionic transport at ambient conditions. As an example, for Ge-containing Li6PS5I we identified the spin-lock NMR rate peak appearing at 163 K as the one reflecting the rate-limiting intercage Li+ diffusion process that enables the ions to be transported over long distances. The corresponding Einstein-Smoluchowski diffusion coefficient excellently agrees with that indirectly probed by macroscopic conductivity spectroscopy.
We thank the DFG for financial support (former DFG research unit 1277, molife).
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