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Molecular-undercoordination-induced, a slight, Goldschmidt-Pauling-Sun contraction of the stronger “O2--H+/p” real-bond and the inter-electron-pair Coulomb-repulsion-driven, a significant, elongation of the weaker “H+/p:O2-” non-bond of the segmented “O2-:H+/p-O2-” bond, and the associated stiffness relaxation, are recognized as the key to the excessive anomalies of (H2O)N clusters. Consistency between calculations, measurements, and expectations, confirmed that the shortened-and-stiffened real-bond stiffens the high-frequency phonons (>3000 cm-1), densifies and entraps bonding electrons and binding energy, and elevates the melting point (and hence the viscosity, surface tension, and elasticity), consequently; and that the lengthened-and-softened non-bond softens the low-frequency phonons (<300 cm-1), expands the volume, and polarizes the electron pairs of the undercoordinated molecules in freestanding and encapsuled clusters, water surface and ultrathin films that exhibit ice- or glue-like and hydrophobic nature at room temperature.
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