4.8 Article

Promoting a Weak Coupling of Monolayer MoSe2 Grown on (100)-Faceted Au Foil

Journal

ACS NANO
Volume 15, Issue 3, Pages 4481-4489

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c08513

Keywords

transition-metal dichalcogenides; MoSe2; chemical vapor deposition; scanning tunneling microscopy; scanning tunneling spectroscopy; Raman spectroscopy

Funding

  1. National Natural Science Foundation of China [51772087, 51972106, 11904094, 11804089]
  2. Strategic Priority Research Program of Chinese Academy of Sciences [XDB30000000]
  3. Natural Science Foundation of Hunan Province, China [2019JJ50034, 2018JJ3025, 2019JJ50073]
  4. Fundamental Research Funds for the Central Universities of China
  5. MOE Tier 2 [MOE2017-T2-2-139]

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This study demonstrates a practical approach to producing highly crystalline monolayer MoSe2 using high-temperature-annealed Au foil as a weakly interacting substrate for atmospheric pressure chemical vapor deposition. The low-temperature scanning tunneling microscopy/spectroscopy measurements reveal a honeycomb structure of MoSe2 with a quasi-particle bandgap of 1.96 eV. The weak coupling between the Au(100) surface and MoSe2 is critical for easy transfer of monolayers to another host substrate.
As a two-dimensional semiconductor with many physical properties, including, notably, layer-controlled electronic bandgap and coupled spin-valley degree of freedom, monolayer MoSe2 is a strong candidate material for next-generation opto- and valley-electronic devices. However, due to substrate effects such as lattice mismatch and dielectric screening, preserving the monolayer's intrinsic properties remains challenging. This issue is generally significant for metallic substrates whose active surfaces are commonly utilized to achieve direct chemical or physical vapor growth of the monolayer films. Here, we demonstrate high-temperature-annealed Au foil with well-defined (100) facets as a weakly interacting substrate for atmospheric pressure chemical vapor deposition of highly crystalline monolayer MoSe2. Low-temperature scanning tunneling microscopy/spectroscopy measurements reveal a honeycomb structure of MoSe2 with a quasi-particle bandgap of 1.96 eV, a value comparable with other weakly interacting systems such as MoSe2/graphite. Density functional theory calculations indicate that the Au(100) surface exhibits the preferred energetics to electronically decouple from MoSe2, compared with the (110) and (111) crystal planes. This weak coupling is critical for the easy transfer of monolayers to another host substrate. Our study demonstrates a practical means to produce high-quality monolayers of transition-metal dichalcogenides, viable for both fundamental and application studies.

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