Quasistatic computer simulation study of the shear behavior of Bi- and trilayer water films confined between model hydrophilic surfaces.

In this paper, our previous simulations of the shear behavior of confined water monolayers (Pertsin, A.; Grunze, M. Langmuir 2008, 24, 135) are extended to water films two and three monolayers thick. The shear response of the films is studied in the quasistatic regime corresponding to the infinitely low shear rate. In certain ranges of wall-to-wall separations, bilayer films are found to be capable of sustaining shear stress, as is characteristic of solids, while remaining fluidlike in respect of the lateral order and molecular mobility. The relation between the solidlike and fluidlike properties of the films is dependent on the relative alignment of the walls and on the period of the wall lattice. The films become more fluid when the walls are moved out of alignment and when the wall lattice is uniformly compressed or stretched with respect to the "optimum" lattice that favors crystal-like packing. Trilayer films do not sustain shear stress in the whole range of wall-to-wall separations where these films are formed.