Exploiting the Novel Electronic and Magnetic Structure of C3N via Functionalization and Conformation

2D polyaniline, C3N, is of recent high interest due to its unusual properties and potential use in various technological applications. In this work, through systematic first‐principles calculations, the atomic, electronic, and magnetic structure of C3N and the changes induced due to functionalization by the adsorption of hydrogen, oxygen, and fluorine, for different coverages and sites, as well as on formation of nanoribbons including the effect of adsorbed hydrogen and oxygen, and the effect of strain, are investigated. Among other interesting phenomena, for hydrogen adsorption, a semiconductor‐to‐topological insulator transition, where two Dirac‐points appear around the Fermi level, as well as ferromagnetic ordering for both hydrogen and oxygen functionalization, is identified. Considering C3N nanoribbons, adsorption of H leads to significant changes in the electronic properties, such as transforming the structures from semiconductor to metallic. Furthermore, investigating the effect of strain on the physical properties, it is found that the band gap can be significantly altered and controlled. The present findings predict that a wide variation in the magnetic and electronic structure of C3N can be achieved by adatom functionalization and conformation indicating its high potential for use in various technological applications, ranging from catalysis, energy storage, and nanoelectronic devices. First principles calculations for two dimensional polyaniline, C3N, show that a wide variation in the magnetic and electronic structure can be achieved by adatom functionalization and geometric conformation, which range from semiconductor‐to‐metallic transitions, semiconductor‐to‐topological insulator transitions, as well as magnetism, and indicate its high potential for use in various technological applications, such as catalysis, energy storage, and nanoelectronic devices.