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Hydrogen-bond Structure Dynamics in Bulk Water: Insights from ab initio Simulations with Coupled Cluster Theory

Abstract

Accurate and efficient ab initio molecular dynamics (AIMD) simulation of liquid water was made possible using the fragment-based approach (Phys. Chem. Chem. Phys., 19, 11931, (2017)). In this study, we advance the AIMD simulations by using the fragment-based coupled cluster (CC) theory, more accurately revealing the structural and dynamical properties of liquid water at ambient conditions. The results show that the double-donor hydrogen-bond configurations in the liquid water is nearly in balance with the single-donor configurations, with a slight bias towards the former. Our observation is in contrast to the traditional tetrahedral water structure. The hydrogen-bond switching dynamics in the liquid water was very fast, with the hydrogen-bond life time of around 0.78 picoseconds from AIMD simulation at the CCD/aug-cc-pVDZ level. This time scale is remarkably shorter than ~3.0 picoseconds that is commonly obtained from traditional nonpolarized force fields and density functional theory (DFT) based first-principles simulations. Additionally, the obtained radial distribution functions, triplet oxygen angular distribution, diffusion coefficient, and the dipole moment of the water molecule are uniformly in good agreement with the experimental observations. The current high-level AIMD simulation sheds light on the understanding of the structural and dynamical properties of liquid water.

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Publication details

The article was received on 26 Sep 2017, accepted on 04 Dec 2017 and first published on 04 Dec 2017


Article type: Edge Article
DOI: 10.1039/C7SC04205A
Citation: Chem. Sci., 2017, Accepted Manuscript
  • Open access: Creative Commons BY-NC license
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    Hydrogen-bond Structure Dynamics in Bulk Water: Insights from ab initio Simulations with Coupled Cluster Theory

    J. Liu, X. He, J. Z. H. Zhang and L. Qi, Chem. Sci., 2017, Accepted Manuscript , DOI: 10.1039/C7SC04205A

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