Abstract
Water skin is the toughest of ever known with a mechanism that remains unclear. We show phonon spectrometrically that molecular undercoordination induced hydrogen bond (O:HO) relaxation and nonbonding electron polarization furnished the skin with the supersolid nature – less dense, elastic, thermally more stable than the bulk. Heating from 5 to 95°C stiffens the skin HO phonon (or bond stiffness) from 3443cm−1 by 0.38%, and the bulk phonon from 3239cm−1 by 1.48%, but softens the HO dangling bonds from 3604cm−1 by −0.40%. Heating also changes the respective molecular structural order and phonon abundance by −8.4/−19.7%, 4.9/−2.6%, and 13.0/137.0%. Observations also evidenced that both heating and molecular undercoordination have the same effect on O:HO bond relaxation but opposite on polarization, which improves our understanding of the anomalous skin of liquid water.
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