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Microscopic dynamics of lithium diffusion in single crystal of the solid-state electrolyte La$$_{2/3-x}$$Li$$_{3x}$$TiO$$_{3}$$ (x = 0.13) studied by quasielastic neutron scattering

Matsuura, Masato*; Fujiwara, Yasuyuki*; Moriwake, Hiroki*; Ohara, Koji*; Kawakita, Yukinobu 

Quasielastic neutron scattering (QENS) measurements combined with first principles based molecular dynamics calculations were conducted to study the dynamics of Li$$^{+}$$ ions in a solid-state electrolyte La$$_{2/3-x}$$Li$$_{3x}$$TiO$$_{3}$$ (LLTO) with $$x = 0.13$$. By using a large $$^{7}$$Li-enriched single crystal sample, a QENS signal was clearly observed along the three principal axes [110], [111], and [001] at a temperature ($$T$$) of 600 K. Wave vector dependence of the linewidth of the QENS signal along each direction was explained well using the Chudley-Elliot model for jumps between the A sites of the perovskite lattice through the bottleneck square, which was also supported by molecular dynamics calculations. The estimated self-diffusion coefficient of Li$$^{+}$$ ($$D_{rm Li}$$) in the ab plane was slightly larger than that along the c axis, suggesting quasi-isotropic diffusion, that is, the three-dimensional diffusion of Li$$^{+}$$ ions. The decrease in $$D_{rm Li}$$ with decreasing $$T$$ was reasonably explained by a thermal activation process with the activation energy determined from ionic-conductivity measurements. Furthermore, the estimated values of the self-diffusion coefficient are comparable to those in the sulfide-based Li$$^{+}$$ ion conductor, Li$$_{7}$$P$$_{3}$$S$$_{11}$$, with 10 times larger ionic conductivity, which clarifies how to understand the Li conduction mechanism in LLTO and Li$$_{7}$$P$$_{3}$$S$$_{11}$$ in a unified manner.

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