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The interplay between intra-molecular H-O covalent bond contraction, due tomolecular under-coordination, and inter-molecular O:H expansion, due tointer-electron pair Coulomb repulsion, has been shown to be the source of theanomalous behavior of under-coordinated water molecules in nanoclusters and inthe surfaces of water. The shortening of the H-O bond raises the local densityof bonding electrons, which in turn polarizes the lone pairs of electrons onoxygen. The stiffening of the H-O bond increases the magnitude of O1s bindingenergy shift, causes the blueshift of the H-O phonon frequencies, andfurthermore, elevates the melting point of molecular clusters and ultrathinfilms of water, which gives rise to their ice-like behavior at roomtemperature. At the same time, the elongation of the entire O:H-O bondpolarizes and enlarges the under-coordinated H$_2$O molecules.

Mass-density and Phonon-frequency Relaxation Dynamics of Under-coordinated Water Molecules