The
etching process can serve as an effective top-down approach
that facilitates direct construction of tuned patterns, reversely
studying growth mechanisms and further inducing unexpected physical
properties. Currently, etching behaviors of monolayer transition-metal
dichalcogenides (TMDs) have been rarely explored and the intrinsic
etching mechanism still needs to be fully elucidated. Here, we demonstrate
a facile and controllable oxygen-assisted anisotropic chemical etching
of two-dimensional (2D) materials. Taking MoSe2 as an example,
a series of well-defined etched patterns can be fabricated by precisely
modulating the pretreatment time of oxygen plasma and the etching
time. Atomic characterization exhibits that the edges of etched patterns
are mainly zigzag-terminated. Density functional theory calculations
highly agree with the experimental results, indicating an energy preference
for zigzag edges. The as-produced MoSe2 flakes can be used
as part of heterojunctions to display intriguing optoelectronic properties.
The field-effect transistor based on as-etched MoSe2 flakes
and the 2D poly(3-hexylthiophene-2,5-diyl) crystal shows a distinct
enhanced ambipolar photoresponse. Our strategy offers a new direction
for preparing patterned 2D TMDs with desirable characteristics, opening
the door for facilitating the development of optoelectronics.