Water: Many-Body Potential from First Principles (From the Gas to the Liquid Phase)
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Computer simulations have become an integral part of the toolbox of any researcher interested in molecular sciences, often providing new insights that are difficult (if not impossible) to obtain by other means. However, the predictive power of a computer simulation directly depends on the level of realism that can be used to represent the molecular system of interest. Since the early times of computer simulations, the search for a molecular model of water capable of describing its unique properties across different phases has been the focus of intense research. The continued increase in computer power accompanied by advances in the design of efficient algorithms for correlated electronic structure calculations and tremendous progress in the representation of global potential energy surfaces have recently opened the doors to the development of molecular models rigorously derived from many-body expansions of interaction energies. By quantitatively reproducing individual interaction terms between molecules, it has been shown that these many-body potential energy functions can achieve unprecedented accuracy in computer simulations. This chapter provides an overview of the theoretical formalism underlying such many-body representations, with a particular focus on the performance of the MB-pol potential energy function in predicting the energetics as well as structural, thermodynamic, dynamical, and spectroscopic properties of water from the gas to the condensed phase.
This work was supported by the National Science Foundation through Grants CHE-1453204, ACI-1642336, and ACI-1053575.
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