Abstract

Two-dimensional (2D) carbon materials, such as graphene, have attracted particular attention owing to the exceptional carrier transport characteristics that arise from the unique π-electron system in their conjugated carbon network structure1-4. To complement zero-bandgap graphene, material scientists have devoted considerable effort to identifying 2D carbon materials5-8. However, it is a challenge to prepare large-sized single-crystal 2D carbon materials with moderate bandgaps5,9. Here we prepare a single-crystal 2D carbon material, namely monolayer quasi-hexagonal-phase fullerene (C60), with a large size via an interlayer bonding cleavage strategy. In this monolayer polymeric C60, cluster cages of C60 are covalently bonded with each other in a plane, forming a regular topology that is distinct from that in conventional 2D materials. Monolayer polymeric C60 exhibits high crystallinity and good thermodynamic stability, and the electronic band structure measurement reveals a transport bandgap of about 1.6 electronvolts. Furthermore, an asymmetric lattice structure endows monolayer polymeric C60 with notable in-plane anisotropic properties, including anisotropic phonon modes and conductivity. This 2D carbon material with a moderate bandgap and unique topological structure offers an interesting platform for potential application in 2D electronic devices.

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