期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 14, 期 32, 页码 11371-11385出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c2cp41497j
关键词
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资金
- Czech Science Foundation [P208/10/1724]
- Ministry of Education of the Czech Republic [ME09064, P208/12/G016]
- Institute of Organic Chemistry and Biochemistry AS CR [RVO 61388963]
- AirUCI Institute
- U.S. National Science Foundation [0909227]
We present a molecular dynamics simulation study in which we determined the melting point of ice I-h for the polarizable SWM4-NDP water model (Lamoureux et al., Chem. Phys. Lett., 2006, 418, 245-249) and compared the performance of several popular water force fields, both polarizable and nonpolarizable, in terms of melting temperature, stability and orientational structuring of ice. The simulations yield the melting temperature of SWM4-NDP ice as low as T-m = 185 +/- 10 K, despite the quadrupole moment of a SWM4-NDP water molecule being close to the experimental gas phase value. The results thus show that the dependence of T-m on the molecular quadrupole, observed for the three-and four-site water models, is generally lost if polarization is explicitly included. The study also shows that adding polarizability to a planar three-charge water model increases orientational disorder in hexagonal ice. In addition, analysis of the tetrahedral order in bulk ice reveals a correlation between the pre-existing degree of orientational disorder in ice simulated using different polarizable and nonpolarizable models and the melting temperature of the models. Our findings thus suggest some new considerations regarding the role of polarization forces in a crystalline solid that may guide future development of reliable polarizable water models for ice.
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