Metallic Transport in Monolayer and Multilayer Molybdenum Disulfides by Molecular Surface Charge Transfer Doping

Carrier modulation in transition-metal dichalcogenides (TMDCs) is of importance for applying electronic devices to tune their transport properties and controlling phases, including metallic to superconductivity. Although the surface charge transfer doping method has shown a strong modulation ability of the electronic structures in TMDCs and a degenerately doped state has been proposed, the details of the electronic states have not been elucidated, and this transport behavior should show a considerable thickness dependence in TMDCs. In this study, we characterize the metallic transport behavior in the monolayer and multilayer MoS₂ under surface charge transfer doping with a strong electron dopant, benzyl viologen (BV) molecules. The metallic behavior transforms to an insulative state under a negative gate voltage. Consequently, metal-insulator transition (MIT) was observed in both monolayer and multilayer MoS₂ correlating with the critical conductivity of order e²/h. In the multilayer case, the BV molecules strongly modulated the topmost surface layer in the bulk MoS₂; the transfer characteristics suggested a crossover from a heterogeneously doped state with a doped topmost layer to doping in the deep layers caused by the variation in the gate voltage. The findings of this work will be useful for understanding the device characteristics of thin-layered materials and for applying them to the controlling phases via carrier modulation.