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Ionic layer epitaxy (ILE) has recently been developed as an effectivestrategy to synthesize nanometer-thick 2D materials with a non-layered crystalstructure, such as ZnO. The packing density of the amphiphilic monolayer isbelieved to be a key parameter that controls the nanosheet nucleation andgrowth. In this work, we systematically investigated the growth behavior ofsingle-crystalline ZnO nanosheets templated at the water-air interface by ananionic oleylsulfate monolayer with different packing densities. Thethicknesses of ZnO nanosheets were tuned from one unit cell to four unit cells,and exhibited good correlation with the width of Zn2+ ion concentration zone(the Stern layer) underneath the ionized surfactant monolayer. Further analysisof the nanosheet sizes and density revealed that the nanosheet growth wasdominated by the steric hindrance from the surfactant monolayer at lowersurface pressure; while the nucleation density became the dominating factor athigher surface pressure. The ZnO nanosheets exhibited a decreasing workfunction as the thickness reduced to a few unit cells. This research validateda critical hypothesis that the nanosheet growth is self-limited by theformation of a double layer of ionic precursors. This work will open up a newway towards controlled synthesis of novel 2D nanosheets from non-layeredmaterials with a thickness down to one unit cell.

Unit Cell-Level Thickness Control of Single-Crystalline Zinc Oxide Nanosheets Enabled by Electrical Double Layer Confinement