4.8 Article

Stabilization of Three-Particle Excitations in Monolayer MoS2 by Fluorinated Methacrylate Polymers

Journal

JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 13, Issue 21, Pages 4794-4799

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.2c01150

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Funding

  1. National Science Foundation [NSF-BSF 1808011]
  2. US-Israel Binational Science Foundation [2017655]
  3. UMass Amherst

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This study demonstrates the important interplay between electron exchange and electrostatic interactions at the interface between polymers and transition metal dichalcogenides (TMDCs), which is crucial for controlling fundamental electronic properties relevant to next-generation devices.
While extrinsic factors, such as substrates and chemical doping, are known to strongly influence visible photoemission from monolayer MoS2, key fundamental knowledge for p-type polymeric dopants is lacking. We investigated perturbations to the electronic environment of 2D MoS2 using fluorinated polymer coatings and specifically studied stabilization of three-particle states by monitoring changes in intensities and emission maxima of three-particle and two-particle emissions. We calculated changes in carrier density and trion binding energy, the latter having an additional contribution from MoS2 polarization by the polymer. Polarization is further suggested by Kelvin probe force microscopy (KPFM) measurements of large Fermi level shifts. Changes similar in magnitude, but opposite in sign, were observed in 2D MoS2 coated with an analogous nonfluorinated polymer. These findings highlight the important interplay between electron exchange and electrostatic interactions at the interface between polymers and transition metal dichalcogenides (TMDCs), which govern fundamental electronic properties relevant to next-generation devices.

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