Engineering the Crack Structure and Fracture Behavior in Monolayer MoS(2) By Selective Creation of Point Defects

Monolayer transition‐metal dichalcogenides, e.g., MoS(2), typically have high intrinsic strength and Young's modulus, but low fracture toughness. Under high stress, brittle fracture occurs followed by cleavage along a preferential lattice direction, leading to catastrophic failure. Defects have been reported to modulate the fracture behavior, but pertinent atomic mechanism still remains elusive. Here, sulfur (S) and MoS (n) point defects are selectively created in monolayer MoS(2) using helium‐ and gallium‐ion‐beam lithography, both of which reduce the stiffness of the monolayer, but enhance its fracture toughness. By monitoring the atomic structure of the cracks before and after the loading fracture, distinct atomic structures of the cracks and fracture behaviors are found in the two types of defect‐containing monolayer MoS(2). Combined with molecular dynamics simulations, the key role of individual S and MoS (n) point defects is identified in the fracture process and the origin of the enhanced fracture toughness is elucidated. It is a synergistic effect of defect‐induced deflection and bifurcation of cracks that enhance the energy release rate, and the formation of widen crack tip when fusing with point defects that prevents the crack propagation. The findings of this study provide insights into defect engineering and flexible device applications of monolayer MoS(2).