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We demonstrate the formation of ionic metal chloride (CuCl) two-dimensional (2D) nanocrystals epitaxially templated on the surface of monolayer molybdenum disulfide (MoS 2 ). These 2D CuCl nanocrystals are single atomic planes from a nonlayered bulk CuCl structure. They are stabilized as a 2D monolayer on the surface of the MoS 2 hrough interactions with the uniform periodic surface of the MoS 2 . The heterostructure 2D system is studied at the atomic level using aberration-corrected transmission electron microscopy at 80 kV. Dynamics of discrete rotations of the CuCl nanocrystals are observed, maintaining two types of preferential alignments to the MoS 2 lattice, confirming that the strong interlayer interactions drive the stable CuCl structure. Strain maps are produced from displacement maps and used to track real-time variations of local atomic bonding and defect production. Density functional theory calculations interpret the formation of two types of energetically advantageous commensurate superlattices via strong chemical bonds at interfaces and predict their corresponding electronic structures. These results show how vertical heterostructured 2D nanoscale systems can be formed beyond the simple assembly of preformed layered materials and provide indications about how different 2D components and their interfacial coupling mode could influence the overall property of the heterostructures.

Epitaxial Templating of Two-Dimensional Metal Chloride Nanocrystals on Monolayer Molybdenum Disulfide