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by their current size, many of the s clusters up to (and including) s8 should remain structurally mobile, consistent with the mobility of the s1-2 and s3-6 clusters.. this scenario is clearly supported by the anomalous s8-10 interactions observed in this asymmetric hydration. in the work reported here, a small of the s8-10 interactions could be attributed to specific s8-s8 h-bond interactions within pairs. it is also important to point out that the composition of s8 has been manipulated through precisely designed glass processing. much of the work on the s8 and s10 clusters was based on the compositionally varied s8-10 clusters, in which the s10 layer was gradually reduced (i.e., the composition has a gradient from s8 to s10). the glass composition employed in the synchrotron experiments is s8-0.5 s10 (from a broad range of compositions), where the s10 cluster is probably not mobile in the present form, and is likely too small to interact with either anions or cations. the relative sizes of the s8 and s8-10 clusters (relative to the anion) were calculated from the data on the basis of the equilibrium, fig. 4 and fig. 5. the calculated sizes of s8 and s8-10 were 74.5 and 7.0 å, respectively, and the molar ratio was (10–5)2/1, where subscript “10” is for s8 and subscript “–5” for s8–10. thus, the s8-10 cluster could contain up to 64–74 s8 molecules; indeed, the observed range of cluster sizes is consistent with this size for s8–10. the low value of the range is important, because it enables us to exclude the possibility that the observed anomalous interactions between the clusters are due to reaction sites on the larger s8 cluster. various cluster species were then modeled from the structures obtained from the crystal, as shown in fig. 6. in these models, the central s8 core is surrounded by a shell of s10 molecules. we also tentatively modeled an s8-s10 complex, where the s8-10 pair is similar to the s8-10 pair observed in the asymmetric hydration.

in the hydration system considered here, the affinity of the aromatic hydrogen for the metal ion diminishes with the addition of a second ion. the hydrogen is able to stabilize the anion through an interaction with the appropriate anion of the second metal ion, where the anion of the second metal ion is flanked on one side by a proton. the destabilization of anion-dipolar interaction, where the anion is flanked by a lone-pair, by the additional ion is not a large effect, because the energy barrier for the lone-pair to flip is small. the energy barrier is even smaller in the case of a water molecule attempting to flip into the anion-dipolar interaction, even with the added stability from the additional ion. as such, the aromatic-hydrogen-mediated stabilization of anion-dipolar interaction in the presence of a second ion is also a small effect, consistent with the relatively small magnitude of the shift in the aromatic-hydrogen h-bonded position observed in the system with addition of the second ion.

to explore the range of possibilities, we investigated the possible interactions between the ions and the two ions are arranged in a sequence and the anion-dipolar interaction between anions in the second and third anions.

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