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

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.