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A combination of the differential Raman spectrometrics and contact-angle measurements has enabled resolution of the hydrogen bond(HB,O:H-O)relaxation and molecular dynamics in the NaX hydration shells.Observations suggest that the aqueous ions create each an electric field to form the hydration shells through O:H-O bond elongation and polarization.The ionic polarization shares the same,and even stronger,effect of molecular undercoordination that shortens the H-O bond and stiffen its phonon,and meanwhile,the O-O Coulomb repulsion lengthen and soften the O:H nonbond with an association of polarization.O:H-O bond electrification raises not only the structure order of molecules and the viscosity in the hydration shells but also the skin stress and thermal stability of the solution.Exercises not only deepen our insight into the salt solute-solvent interaction involved in the Hofmeister series in terms of O:H-O bond electrification but also provide a powerful means quantifying the dynamic,local,molecular-site-resolved information regarding the O:H-O bond cooperativity in aqueous solutions.