First-principles simulations of water on the basis of quantum Monte Carlo and fragment molecular orbital methods

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Ab initio, first-principles simulation methods for describing the correlational and thermodynamic properties of water systems have been developed. The quantum Monte Carlo (QMC) method, the fragment molecular orbital (FMO) method, and the reference interaction site model (RISM) combined with the density functional theory were employed for the simulations. The QMC method is useful for the accurate descriptions of the electronic state and the nuclear quantum effect of molecular systems. The FMO method enables us to perform ab initio calculations of the electronic state of large molecular systems with high accuracy. The RISM method was used to carry out the statistical-mechanical description of intermolecular correlations of liquid water. Through the novel developments of these simulation methods and their combinations, we have been led to a status where it is possible to perform highly parallelized, first-principles simulations for water systems on high-performance supercomputers.