The electrical properties of transition-metal dichalcogenides
(TMDs),
such as MoS2, are highly dependent on carrier doping and
layer thickness. The ability to selectively control these two critical
characteristics is of great importance in order to develop TMD-based
multifunctional nanoelectronic device applications, which remains
challenging. Here, we report a strategy for controllable surface modification
and layer thinning of MoS2 via ultraviolet (UV)-light irradiation
in a silver ionic (Ag+) solution environment. The results
show that, by adjustment of the UV irradiation time, nanostructured
Ag ultrathin films (∼2.9 nm) are uniformly deposited on monolayer
MoS2 and can lead to a controllable p-type doping effect,
while the thickness of MoS2 from few-layer to thick-layer
could be thinned to the atomic monolayer limit. Both Ag nanostructure
deposition and layer thinning have been evidenced to initiate from
the edges of MoS2, independent of the edge type, thus revealing
a unique UV-light-assisted defect-induced surface modification and
layer-thinning mechanism. Overall, this study provides a simple methodology
for the selective control of doping and layer thickness in TMDs, paving
the way for developing multifunctional nanoelectronics and integrated
optoelectronics.