Robustness of Bilayer Hexagonal Ice against Surface Symmetry and Corrugation

Two-dimensional (2D) bilayer hexagonal ice (BHI) is regarded as the first intrinsic 2D ice crystal. However, the robustness of such a structure or its derivatives against surface symmetry and corrugation is still unclear. Here, we report the formation of 2D BHI on gold surfaces with 1D corrugation, using noncontact atomic force microscopy. The hexagonal arrangement of the first wetting layer was visualized on the Au(110)-1×2 surface. Upon depositing more water molecules, the first layer would rearrange and shrink, resulting in the formation of buckled BHI. Such a buckled BHI is hydrophobic despite the appearance of dangling OH, due to the strong interlayer bonding. Furthermore, the BHI is also stable on the Au(100)-5×28 surface. This work reveals the unexpected generality of the BHI on corrugated surfaces with nonhexagonal symmetry, thus shedding new light on the microscopic understandings of the low-dimensional ice formation on solid surfaces or under confinement.