31. M. L. Hair (private communication) states that, at pressures of 16 torr and above, the very rapid increase in the amount of absorbed water makes it difficult to make precise measurements, and a fairly broad range of values for the number of molecules absorbed per hydrogen-bonded hydroxyl pair may be indicated. Hair's failure to produce anomalous water may have been due to the special nature of the surface treatment, which may prevent a clustering of hydroxyl pairs sufficient to form successive layers. Fortunately all that is needed for understanding the formation process is identification of hydrogen-bonded surface hydroxyl pairs with an increased absorption under the pressure condiitons favorable to the formation of anomalous water.Hair also proposed the anomalous water geometry given in Fig. 4h, but this has a higher energy than either squares or planar hexagons. 32. Even though the asymmetric cyclic hexamer has a per-bond binding energy comparable to, or slightly greater than, tetrahedral coordination, its geometry is not favorable for formation of the normal liquid because of its very low entropy relative to the tetrahedral arrangements. 33. There is a further decrease in the free energy, due to the lower vibration frequency, hence the higher entropy, of the symmetric hexamer over the asymmetric hexamer. 34. L. Pedersen and K. Morokuma, J. Chem. Phys. 46, 3941 (1967). 35. When an anomalous-water bond is broken, the energy of the conformation immediately after breakage is close to that of a symmetric bonded chain. A concerted motion of each. symmetric hydrogen to a corresponding asymmetric position is highly unlikely because of the between-layer interconnections.
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