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The intriguing relationship between entropy and diffusion is a subject ofmuch current interest. However, the experimentally observed unusualnon-monotonic dependence of limiting ionic conductivity on inverse ion size isneither described by the Adam-Gibbs entropy crisis theory nor by the Rosenfeldentropy scaling. This failure is obvious because throughout the size variationthe bulk entropy of the solvent remains the same, or undergoes infinitesimalchange. We show that it is the entropy experienced by the tagged ion that needsto be calculated. This entropy can be quantified, at least partly, by thechange in the tetrahedral ordering of water molecules in the hydration layer ofthe ions which exhibits a nonmonotonic size dependence.

Tetrahedral entropy captures non-monotonicity of electrical conductivity in aqueous monatomic ions