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Two-dimensional square ice in graphene nanocapillaries at room temperature isa fascinating phenomenon and has been confirmed experimentally. Instead oftemperature for bulk ice, the high van der Waals pressure becomes anall-important factor to induce the formation of square ice and needs to bestudied further. By all-atom molecular dynamics simulations of water confinedbetween two parallel graphene sheets, which are changed in size (the length andthe width of the graphene sheets) over a wide range, we find that the criticalcrystallization pressure for the formation of square ice in nanocapillarystrongly depends on the size of the graphene sheet. The criticalcrystallization pressure slowly decreases as the graphene size increases,converging to approximately macroscopic crystallization pressure. Theunfreezable threshold for graphene size is obtained by estimating the actualpressure and it is difficult to form the square ice spontaneously in practicewhen the graphene sheet is smaller than the threshold. Moreover, the criticalcrystallization pressure fluctuates when the graphene size is minuscule, andthe range of oscillation narrows as the sheet size increases, converging to themacroscopic behavior of a single critical icing pressure for large sheets. Thegraphene size also affects the stability and crystallization time of squareice.

Variation of Critical Crystallization Pressure for the Formation of Square Ice in Graphene Nanocapillaries