Spontaneous chemical functionalization via coordination of Au single atoms on monolayer MoS2

He Liu; Daniel Grasseschi; Akhil Dodda; Kazunori Fujisawa; David Olson; Ethan Kahn; Fu Zhang; Tianyi Zhang; Yu Lei; Ricardo Braga Nogueira Branco; Ana Laura Elías; Rodolfo Cruz Silva; Yin-Ting Yeh; Camila M Maroneze; Leandro Seixas; Patrick Hopkins; Saptarshi Das; Christiano J S de Matos; Mauricio Terrones

doi:10.1126/sciadv.abc9308

Spontaneous chemical functionalization via coordination of Au single atoms on monolayer MoS₂

Sci Adv. 2020 Dec 2;6(49):eabc9308. doi: 10.1126/sciadv.abc9308. Print 2020 Dec.

Authors

He Liu¹, Daniel Grasseschi^{2

3}, Akhil Dodda⁴, Kazunori Fujisawa^{5

6

7}, David Olson⁸, Ethan Kahn⁹, Fu Zhang⁹, Tianyi Zhang⁹, Yu Lei⁹, Ricardo Braga Nogueira Branco¹⁰, Ana Laura Elías^{6

7

11}, Rodolfo Cruz Silva^{5

12}, Yin-Ting Yeh^{6

7}, Camila M Maroneze¹³, Leandro Seixas¹³, Patrick Hopkins^{8

14

15}, Saptarshi Das^{4

9}, Christiano J S de Matos¹³, Mauricio Terrones^{16

6

7

9}

Affiliations

¹ Department of Chemistry, The Pennsylvania State University, University Park, PA 16802, USA.
² MackGraphe-Graphene and Nanomaterials Research Center, Mackenzie Presbyterian University, 01302-907 São Paulo, Brazil. mut11@psu.edu dgrasseschi@iq.ufrj.br.
³ Surface Chemistry and Nanomaterials Laboratory, Inorganic Chemistry Department, Chemistry Institute, Federal University of Rio de Janeiro (UFRJ), 21941-909 Rio de Janeiro, Brazil.
⁴ Engineering Science and Mechanics, The Pennsylvania State University, University Park, PA 16802, USA.
⁵ Research Initiative for Supra-Materials (RISM), Shinshu University, 4-17-1 Wakasato, Nagano 380-8553, Japan.
⁶ Department of Physics, The Pennsylvania State University, University Park, PA 16802, USA.
⁷ Center for 2-Dimensional and Layered Materials, The Pennsylvania State University, University Park, PA 16802, USA.
⁸ Department of Mechanical and Aerospace Engineering, University of Virginia, Charlottesville, VA 22904, USA.
⁹ Department of Materials Science and Engineering, The Pennsylvania State University, University Park, PA 16802, USA.
¹⁰ Department of Aerospace Engineering, The Pennsylvania State University, University Park, PA 16802, USA.
¹¹ Department of Physics, Binghamton University, Binghamton, NY 13902, USA.
¹² Global Aqua Innovation Center, Faculty of Engineering, Shinshu University, 4-17-1 Wakasato, Nagano 8553, Japan.
¹³ MackGraphe-Graphene and Nanomaterials Research Center, Mackenzie Presbyterian University, 01302-907 São Paulo, Brazil.
¹⁴ Department of Materials Science and Engineering, University of Virginia, Charlottesville, VA 22904, USA.
¹⁵ Department of Physics, University of Virginia, Charlottesville, VA 22904, USA.
¹⁶ Department of Chemistry, The Pennsylvania State University, University Park, PA 16802, USA. mut11@psu.edu dgrasseschi@iq.ufrj.br.

Abstract

Surface functionalization of metallic and semiconducting 2D transition metal dichalcogenides (TMDs) have mostly relied on physi- and chemi-sorption at defect sites, which can diminish the potential applications of the decorated 2D materials, as structural defects can have substantial drawbacks on the electronic and optoelectronic characteristics. Here, we demonstrate a spontaneous defect-free functionalization method consisting of attaching Au single atoms to monolayers of semiconducting MoS₂(1H) via S-Au-Cl coordination complexes. This strategy offers an effective and controllable approach for tuning the Fermi level and excitation spectra of MoS₂ via p-type doping and enhancing the thermal boundary conductance of monolayer MoS₂, thus promoting heat dissipation. The coordination-based method offers an effective and damage-free route of functionalizing TMDs and can be applied to other metals and used in single-atom catalysis, quantum information devices, optoelectronics, and enhanced sensing.

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