Bi-directional configuration evolution of homo/heterogeneous graphyne nanoribbons encircling a rotating CNT

Abstract Graphyne (GY) nanomaterials, with their highly tunable properties, show great potential as building blocks for composite nanodevices. Using molecular dynamics simulations, this study investigates the bi-directional folding and unfolding evolution of homogeneous and heterogeneous GY nanoribbons (GYNRs) around a rotating carbon nanotube (CNT). The results reveal distinct configuration rules: homogeneous GYNRs consistently undergo synchronous folding to form interlaced GY nanoscrolls (GYNSs), whereas heterogeneous GYNRs may fold synchronously or in a layered manner, producing either interlaced or covered GYNSs depending on atomic density differences and temperature. Moreover, GYNSs can be reversibly unfolded into GYNRs under CNT rotation. Unified unfolding, initiated from the innermost layer, typically occurs in interlaced GYNSs, while segmented unfolding-unique to covered GYNSs with large atomic density differencesproceeds sequentially from the outermost edge of the outer GYNS to the innermost layer of the inner GYNS. These findings establish key principles for the flexible design and engineering of novel homoand heterogeneous GY-based nanostructures.