Formation of Graphene Nanoscrolls and Their Electronic Structures Based on Ab Initio Calculations

Rolling up two-dimensional (2D) materials can form quasi-one-dimensional nanoscrolls, which are expected to have novel properties due to their larger space of structural parameters. In this Letter, the structural dependence of formation energy was investigated based on more than 90 different graphene nanoscrolls (GNSs) through ab initio calculations. A quantified relationship between formation energy and structural parameters is discovered, which could provide universal description of rolling up 2D materials beyond graphene. Further calculations on electronic structures show the opening of bandgap in GNSs with ultrahigh carrier mobilities up to 10⁷ cm² V^-1 s^-1. The structural stability under room temperature was also testified by using molecular dynamic simulations. This work provides general insights into the rolling-up strategy and demonstrates the tunable properties of GNSs, thus extending the scope of the research field for 2D materials.