Two-dimensional fullerene-based monolayer materials assembled by C80 and Sc3N@C80

Construction of two-dimensional (2D) materials using fullerenes as building blocks has attracted particular attention, primarily due to their ability to integrate desired functionalities into devices. However, realization of stable 2D phases of polymerized fullerenes remains a big challenge. Here, we propose two stable 2D monolayer phases with covalently bridged C-80 cages, namely alpha-C-80-2D and beta-C-80-2D, which are semiconductors with strong absorption in the long wave range and appreciable carrier mobility, respectively. The high stability originates from the bond energy released by the [2+2] cycloaddition polymerization of C-80 is greater than the deformation energy of a cage. Starting from alpha-C-80-2D, endohedral incorporation of the Sc3N molecule into each C-80 cage leads to 2D semiconductors of alpha-Sc3N@C-80-2D and alpha '-Sc3N@C-80-2D, which possess exceptional stability and diverse physical properties, including unique electronic band structures, strong optical absorption in the visible (VIS) to near-infrared (NIR) regime, and anisotropic optical characteristics. Remarkably, a temperature-induced order-disorder transition in the alpha-Sc3N@C-80-2D phase has been observed at elevated temperatures above 600 K. These findings expand the family of 2D carbon materials and provide useful clue for the potential applications of fullerene-assembled monolayer networks.