4.7 Article

Perturbative vibration of the coupled hydrogen-bond (O:H-O) in water

Journal

ADVANCES IN COLLOID AND INTERFACE SCIENCE
Volume 310, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.cis.2022.102809

Keywords

Hydrogen bond; Relaxation; Polarization; Hydration; Perturbation

Funding

  1. National Natural Science Foundation of China [11872052, 21875024, 11832019, 12150001]
  2. Advanced Research Projects of Chongqing Municipal Science and Technology Commission [cstc2019jcyj-msxmX0674]

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Perturbation Raman spectroscopy provides insights into the behavior of water molecules under disturbance, by studying the cooperativity and polarizability of hydrogen bonds. This research is important for understanding the anomalies of water.
Perturbation Raman spectroscopy has underscored the hydrogen bond (O:H-O or HB) cooperativity and polarizability (HBCP) for water, which offers a proper parameter space for the performance of the HB and electrons in the energy-space-time domains. The O-O repulsive coupling drives the O:H-O segmental length and energy to relax cooperatively upon perturbation. Mechanical compression shortens and stiffens the O:H nonbond while lengthens and softens the H-O bond associated with polarization. However, electrification by an electric field or charge injection, or molecular undercoordination at a surface, relaxes the O:H-O in a contrasting way to the compression with derivation of the supersolid phase that is viscoelastic, less dense, thermally diffusive, and mechanically and thermally more stable. The H-O bond exhibits negative thermal expansivity in the liquid and the ice-I phase while its length responds in proportional to temperature in the quasisolid phase. The O:H-O relaxation modifies the mass densities, phase boundaries, critical temperatures and the polarization endows the slipperiness of ice and superfluidity of water at the nanometer scale. Protons injection by acid solvation creates the H <-> H anti-HB and introduction of electron lone pairs derives the O:double left right arrow:O super-HB into the solutions of base or H2O2 hydrogen-peroxide. The repulsive H <-> H and O:double left right arrow:O interactions lengthen the solvent H-O bond while the solute H-O bond contracts because its bond order loss. Differential phonon spectroscopy quantifies the abundance, structure order, and stiffness of the bonds transiting from the mode of pristine water to the perturbed states. The HBCP and the perturbative spectroscopy have enabled the dynamic potentials for the relaxing O:H-O bond. Findings not only amplified the power of the Raman spectroscopy but also substantiated the understanding of anomalies of water subjecting to perturbation.

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