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Report No.

Revealing the ion dynamics in Li$$_{10}$$GeP$$_{2}$$S$$_{12}$$ by quasi-elastic neutron scattering measurements

Hori, Satoshi*; Kanno, Ryoji*; Kwon, O.*; Kato, Yuki*; Yamada, Takeshi*; Matsuura, Masato*; Yonemura, Masao*; Kamiyama, Takashi*; Shibata, Kaoru  ; Kawakita, Yukinobu  

Understanding Li-ion conduction in superionic conductors accelerates the development of new solid electrolytes to enhance the charge-discharge performances of all-solid-state batteries. We performed a quasi-elastic neutron scattering study on a model superionic conductor (Li$$_{10+x}$$Ge$$_{1+x}$$P$$_{2-x}$$S$$_{12}$$, LGPS), to reveal its ion dynamics on an angstrom-scale spatial range and a pico-to-nanosecond temporal range. The observation of spectra at 298 K confirmed the high lithium diffusivity. The obtained diffusion coefficient was in the order of 10$$^{-6}$$ cm$$^{2}$$s$$^{-1}$$ at temperatures ${textgreater}$ 338 K and was higher than the reported diffusion coefficient over a longer time scale, as determined by the pulse-field gradient nuclear magnetic resonance method. This difference indicates that there are impediments to ionic motion over a longer time scale. The dynamic behavior of the Li ions was compared with that observed for the Li$$_{9}$$P$$_{3}$$S$$_{9}$$O$$_{3}$$ phase, which possesses the same crystal structure type, but a lower ionic conductivity. The LGPS phase possessed a high lithium mobility over a distance of $${sim}$$ 10 ${AA}$, as well as a larger fraction of mobile Li ions, thereby indicating that these features enhance lithium conduction over a longer spatial scale, which is important in all-solidstate batteries.



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Category:Chemistry, Physical



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