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Molecular dynamics simulations are performed to study the lithium jumps inLiPO3 glass. In particular, we calculate higher-order correlation functionsthat probe the positions of single lithium ions at several times. Three-timecorrelation functions show that the non-exponential relaxation of the lithiumions results from both correlated back-and-forth jumps and the existence ofdynamical heterogeneities, i.e., the presence of a broad distribution of jumprates. A quantitative analysis yields that the contribution of the dynamicalheterogeneities to the non-exponential depopulation of the lithium sitesincreases upon cooling. Further, correlated back-and-forth jumps betweenneighboring sites are observed for the fast ions of the distribution, but notfor the slow ions and, hence, the back-jump probability depends on thedynamical state. Four-time correlation functions indicate that an exchangebetween fast and slow ions takes place on the timescale of the jumpsthemselves, i.e., the dynamical heterogeneities are short-lived. Hence, sitesfeaturing fast and slow lithium dynamics, respectively, are intimately mixed.In addition, a backward correlation beyond the first neighbor shell for highlymobile ions and the presence of long-range dynamical heterogeneities suggestthat fast ion migration occurs along preferential pathways in the glassymatrix. In the melt, we find no evidence for correlated back-and-forth motionsand dynamical heterogeneities on the length scale of the next-neighbordistance.Comment: 12 pages, 13 figure

physical review. b, condensed matter

Complex lithium ion dynamics in simulated<mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mi mathvariant="normal">LiPO</mml:mi></mml:mrow><mml:mrow><mml:mn>3</mml:mn></mml:mrow></mml:msub></mml:mrow></mml:math>glass studied by means of multitime correlation functions

Complex lithium ion dynamics in simulatedLiPO3glass studied by means of multitime correlation functions