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Two-dimensional (2D) carbon nitride materials play an important role inenergy-harvesting, energy-storage and environmental applications. Recently, anew carbon nitride, 2D polyaniline (C3N) was proposed [PNAS 113 (2016)7414-7419]. Based on the structure model of this C3N monolayer, we propose twonew carbon nitride monolayers, named dumbbell (DB) C4N-I and C4N-II. Usingfirst-principles calculations, we systematically study the structure,stability, and band structure of these two materials. In contrast to othercarbon nitride monolayers, the orbital hybridization of the C/N atoms in the DBC4N monolayers is sp3. Remarkably, the band structures of the two DB C4Nmonolayers have a Dirac cone at the K point and their Fermi velocities arecomparable to that of graphene. This makes them promising materials forapplications in high-speed electronic devices. Using a tight-binding model, weexplain the origin of the Dirac cone.

Carbon-Rich Carbon Nitride Monolayers with Dirac Cones: Dumbbell C4N