The manipulation of diverse one-dimensional edges in two-dimensional (2D) materials has provoked numerous interest in recent years owing to their intriguing physical and chemical features beyond 2D basal plane. However, the controllable preparation of edge arrangements, particularly the customization of zigzag edges on demand, i.e., transition metal zigzag edge and chalcogens zigzag edge, remains elusive. Here, a selective etching strategy to directly regulate Mo-zigzag and S-zigzag edges of the bilayer MoS2 kirigami structure is proposed. The selective etching is fully established by a space-confined method to adjust the precursor concentration during chemical vapor deposition growth. Morphological and spectroscopic characterization demonstrate the high quality of as-etched MoS2 structures. Atomic-resolution scanning transmission electron microscopy imaging verifies the different etching behaviors of Mo-zigzag edge and S-zigzag edge, further confirmed by theory calculations. S-zigzag edges are prone to be etched in a Mo-sufficient atmosphere, while both Mo-zigzag and S-zigzag edges exhibit an etching tendency at the stoichiometric ratio, attributed to the disparity in free energy. Moreover, the stacking phase and highly anisotropic features are revealed via second harmonic generation responses. This work opens up a new avenue for edge engineering of 2D materials and provides a promising candidate for next-generation optoelectronics.
