Journal
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
Volume 13, Issue 5, Pages 2021-2034Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jctc.7b00149
Keywords
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Funding
- National Natural Science Foundation of China [21303057, 21673074, 21433004]
- Ministry of Science and Technology of China [2016YFA0501700]
- Specialized Research Fund for the Doctoral Program of Higher Education [20130076120019]
- Youth Top-Notch Talent Support Program of Shanghai, Shanghai Putuo District [2014-A-02]
- NYU-ECNU Center for Computational Chemistry at NYU Shanghai
- NYU Global Seed Grant for Collaborative Research
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Fragmentation methods have been widely studied for computing quantum mechanical (QM) energy of medium-sized water clusters, but less attention has been paid to large-sized ion water clusters, in which many-body QM interaction is more significant, because of the charge-transfer effect between ions and water molecules. In this study, we utilized electrostatically embedded generalized molecular fractionation (EE-GMF) method for full QM calculation of the large-sized ion water clusters (up to 15 Na+ and 15 Cl- ions solvated with 119 water molecules). Through systematic validation using different fragment sizes, we show that, by using distance thresholds of 6 A for both the two-body and three-body QM interactions, the EE-GMF method is capable of providing accurate ground-state energies of large-sized ion water clusters at different ab initio levels (including HF, B3LYP,M06-2X, and MP2) with significantly reduced computational cost. The deviations of EE-GMF from full system calculations are within a few kcal/mol. The result clearly shows that the calculated energies of the ion water clusters using EEGMF are close to converge after the distance thresholds are larger than 6 angstrom for both the two-body and three-body QM interactions. This study underscores the importance of the three-body interactions in ion water clusters. The EE-GMF method can also accurately reproduce the relative energy profiles of the ion-water clusters.
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