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Functionalized two-dimensional (2D) materials play an important role in both fundamental sciences and practical applications. The construction and precise control of patterns at the atomic-scale are necessary for selective and multiple functionalization. Here we report the fabrication of monolayer pentasilver diselenide (Ag5Se2), a new type of intrinsically patterned 2D material, by direct selenization of a Ag(111) surface. The atomic arrangement is determined by a combination of scanning tunneling microscopy (STM), low-energy electron diffraction (LEED), and density-functional-theory (DFT) calculations. Large-scale STM images exhibit a quasi-periodic pattern of stoichiometric triangular domains with a side length of ~ 15 nm and apical offsets. The boundaries between triangular domains are sub-stoichiometric. Deposition of different molecules on the patterned Ag5Se2 exhibits selective adsorption behavior. Pentacene molecules preferentially adsorb on the boundaries, while tetracyanoquinodimethane (TCNQ) molecules adsorb both on the boundaries and the triangular domains. By co-depositing pentacene and TCNQ molecules, we successfully construct molecular corrals with pentacene on the boundaries encircling TCNQ molecules on the triangular domains. The realization of epitaxial large-scale and high-quality, monolayer Ag5Se2 extends the family of intrinsically patterned 2D materials and provides a paradigm for dual functionalization of 2D materials.
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