4.8 Article

Compact Super Electron-Donor to Monolayer MoS2

Journal

NANO LETTERS
Volume 22, Issue 11, Pages 4501-4508

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.2c01167

Keywords

Two-dimensional materials; molybdenum disulfide; surface functionalization; molecular doping; atomic force microscopy (AFM); electric transport properties

Funding

  1. CAREER award from the NSF [1749742]
  2. Army Research Office [W911NF-18-1-0367]
  3. Ford Foundation for a graduate student fellowship
  4. NSF
  5. Ministry of Education, Singapore [MOE2016-T2-2-132]
  6. Singapore National Research Foundation, Prime Minister's Office, under its medium-sized centre program

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The surface functionalization of two-dimensional (2D) material MoS2 with organic electron donors (OEDs) has been successfully achieved using the novel molecular dopant Me-OED, which demonstrates record-breaking molecular doping with significantly higher carrier density compared to other OEDs. The impressive doping power of Me-OED is attributed to its compact size, enabling high surface coverage and molecular interactions with MoS2.
The surface functionalization of two-dimensional (2D) materials with organic electron donors (OEDs) is a powerful tool to modulate the electronic properties of the material. Here we report a novel molecular dopant, Me-OED, that demonstrates record-breaking molecular doping to MoS2, achieving a carrier density of 1.10 +/- 0.37 X 10(14) cm(-2) at optimal functionalization conditions; the achieved carrier density is much higher than those by other OEDs such as benzyl viologen and an OED based on 4,4'-bipyridine. This impressive doping power is attributed to the compact size of Me-OED, which leads to high surface coverage on MoS2. To confirm, we study Bu-t-OED, which has an identical reduction potential to Me-OED but is significantly larger. Using field-effect transistor measurements and spectroscopic characterization, we estimate the doping powers of Me- and Bu-t-OED are 0.22-0.44 and 0.11 electrons per molecule, respectively, in good agreement with calculations. Our results demonstrate that the small size of Me-OED is critical to maximizing the surface coverage and molecular interactions with MoS2, enabling us to achieve unprecedented doping of MoS2.

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