▎ 摘　　要

In view of the inevitability of forming defect in the process of nanomaterial synthesis, we investigated the structures and nonlinear optical( NLO) properties of the donor/acceptor-decorated zigzag graphene nanoribbons with the 5-9 defect(zGNR-D5-9) by means of the density functional theory computations. It is revealed that these donor/acceptor-decorated zGNR-D5-9 exhibit considerable NLO response, and the modified site of functional group can significantly impact the beta(0) value. Particularly, simultaneously employing donor/acceptor pair to decorate both sides of zGNR-D5-9 can achieve much larger beta(0) value, where the synergistic effect of donor-pi-acceptor framework and the 5-9 defect should be responsible for the large first hyperpolarizability of systems. These interesting results can provide the valuable insights and more reliable information for the design of new NLO material based on the graphene nanoribbons.