Why different water models predict different structures under 2D confinement

Dix, James and Lue, Leo and Carbone, Paola (2018) Why different water models predict different structures under 2D confinement. Journal of Computational Chemistry, 39 (25). pp. 2051-2059. ISSN 0192-8651 (https://doi.org/10.1002/jcc.25369)

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Experiments of nanoconfined water between graphene sheets at high pressure suggest that it forms a square ice structure (G. Algara-Siller, et al. Nature, 519 (2015) 443). Molecular dynamics (MD) simulations have been used to attempt to recreate this structure, but there have been discrepancies in the structure formed by the confined water depending on the simulation set-up that was employed and particularly on the choice of water model. Here, using classical molecular dynamics simulations, we have systematically investigated the effect that three different water models (SPC/E, TIP4P/2005 and TIP5P) have on the structure of water confined between two rigid graphene sheets with a 0.9 nm separation. We show that the TIP4P/2005 and the TIP5P water models form a hexagonal AA-stacked structure, whereas the SPC/E model forms a rhombic AB-stacked structure. Our work demonstrates that the formation of these structures is driven by differences in the strength of hydrogen bonds predicted by the three water models, and that the nature of the graphene/water interaction only mildly affects the phase diagram. Considering the available experimental data and first-principle simulations we conclude that, among the models tested, the TIP4P/2005 and TIP5P force fields are for now the most reliable when simulating water under confinement.