Transition metal
dichalcogenide (TMD) materials attract significant
research attention thanks to their exceptional excitonic and optical
properties. In this work, we analyze the formation of strained ultrasharp
zigzag edges in MoS2 multilayers produced by anisotropic
wet etching. The topography of the edges is determined by the relative
stability of the different crystallographic directions of the multilayer
as well as the interlayer interactions. Furthermore, we study the
linear (Raman) and nonlinear (second-harmonic generation) spectroscopic
characteristics of such edges and observe enhanced second-order nonlinearity
originating from the strained zigzag edges. We also confirm that ultrasharp
hexagonal nanoholes in MoS2 grow along the most stable
crystallographic directions despite potential stacking faults or instabilities
in the crystal quality. Our results open the way to exploit a broad
range of phenomena occurring at the edges of MoS2 material,
including the unique determination of crystal orientation for moiré
engineering and strongly correlated phenomena in 2D material-based
systems, as well as potential applications in TMD-based electrocatalysis
and gas sensing.