A calculating proof on hydrogen bonding in ordinary ice by the first-principles density functional theory

Abstract

We computationally constructed a special geometrical structure of pairwise H2O configuration in the ice crystal lattice and performed ab initio calculations to demonstrate that the model introduced by Li and Ross to explain the two hydrogen bonds (HBs) [J. C. Li and K. D. Ross, Nature, 1993, 365, 327–329] is incorrect. According to the phonon density of states (PDOS) with deferent bond lengths, we observed that the intramolecular O–H stretching vibration modes produce energy level splitting that strongly correlates with the double peaks of HBs. Our simulations provide evidence that intermolecular HB splitting may be attributed to the coupling with the internal covalent vibrations.