期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 42, 页码 18578-18585出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202009640
关键词
ab initio calculations; hydrogen bonds; molecular dynamics; supercritical fluids; water
资金
- DFG [MA 1547/11]
- Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) [EXC 2033-390677874-RESOLV]
- Projekt DEAL
Thinking about water is inextricably linked to hydrogen bonds, which are highly directional in character and determine the unique structure of water, in particular its tetrahedral H-bond network. Here, we assess if this common connotation also holds for supercritical water. We employ extensive ab initio molecular dynamics simulations to systematically monitor the evolution of the H-bond network mode of water from room temperature, where it is the hallmark of its fluctuating three-dimensional network structure, to supercritical conditions. Our simulations reveal that the oscillation period required for H-bond vibrations to occur exceeds the lifetime of H-bonds in supercritical water by far. Instead, the corresponding low-frequency intermolecular vibrations of water pairs as seen in supercritical water are found to be well represented by isotropic van-der-Waals interactions only. Based on these findings, we conclude that water in its supercritical phase is not a H-bonded fluid.
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