Upon crumpling, graphene sheets yield intriguing hierarchical structures with high resistance to compression and aggregation, garnering a great deal of attention in recent years for their remarkable potential in a variety of applications. Here, we aim to understand the effect of Stone-Wales (SW) defects, i.e., a typical topological defect of graphene, on the crumpling behavior of graphene sheets at a fundamental level. By employing atomistically informed coarse-grained molecular dynamics (CG-MD) simulations, we find that SW defects strongly influence the sheet conformation as manifested by the change in size scaling laws and weaken the self-adhesion of the sheet during the crumpling process. Remarkably, the analyses of the internal structures (i.e., local curvatures, stresses, and cross-section patterns) of crumpled graphene emphasize the enhanced mechanical heterogeneity and "glass-like" amorphous state elicited by SW defects. Our findings pave the way for understanding and exploring the tailored design of crumpled structure via defect engineering.
Keywords: Stone−Wales defect; coarse-grained modeling; crumpled graphene; mechanical state; molecular dynamics simulations; structural behavior.