Intrinsically patterned corrals in monolayer Ag5Se2 and selective molecular co-adsorption
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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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Intrinsically patterned corrals in monolayer Ag5Se2 and selective molecular co-adsorption
Abstract
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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Acknowledgements
This work was supported by the financial support from the National Key R&D Program of China (Nos. 2018YFA0305800 and 2019YFA0308500), National Natural Science Foundation of China (Nos. 61901200, 61925111, 61888102, and 21661132006), the Strategic Priority Research Program of Chinese Academy of Sciences (Nos. XDB30000000 and XDB28000000), the International Partnership Program of Chinese Academy of Sciences (No. 112111KYSB20160061), the KC Wong Education Foundation, the Yunnan Fundamental Research Projects (Nos. 2019FD041, 202201AT070078, and 202101AW070010), and the China Postdoctoral Science Foundation. Part of the research was performed in the Key Laboratory of Vacuum Physics, Chinese Academy of Sciences. Computational resources were provided by the National Supercomputing Center in Tianjin Municipality, China. Work at Vanderbilt University was supported by the U. S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division grant No. DE-FG-02-09ER46554 and by the McMinn endowment.
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