期刊
JOURNAL OF CHEMICAL PHYSICS
卷 136, 期 4, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.3677184
关键词
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资金
- Japan Society for the Promotion of Science [21300111, 23651202]
- Ministry of Education, Culture, Sports, Science, and Technology [20118002, 23118701]
- Nanoscience Program
- Computational Materials Science Initiative of the Next-Generation Supercomputing Project
- Grants-in-Aid for Scientific Research [20118002, 23651202, 20118001, 21300111] Funding Source: KAKEN
The relationship is investigated for QM/MM (quantum-mechanical/molecular-mechanical) systems between the fluctuations of the electronic state of the QM subsystem and of the solvation effect due to the QM-MM interaction. The free-energy change due to the electron-density fluctuation around its average is highlighted, and is evaluated through an approximate functional formulated in terms of distribution functions of the many-body coupling (pairwise non-additive) part of the QM-MM interaction energy. A set of QM/MM simulations are conducted in MM water solvent for QM water solute in ambient and supercritical conditions and for QM glycine solute in the neutral and zwitterionic forms. The variation of the electronic distortion energy of the QM solute in the course of QM/MM simulation is then shown to be compensated by the corresponding variation of the free energy of solvation. The solvation free energy conditioned by the electronic distortion energy is further analyzed with its components. It is found that the many-body contribution is essentially equal between the free energy and the average sum of solute-solvent interaction energy. (C) 2012 American Institute of Physics. [doi:10.1063/1.3677184]
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