First-principles calculations on the curvature evolution and cross-linkage in carbon nitride

First-principles calculations were utilized to study the formation mechanisms and structural features of fullerene-like carbon nitride (FL CNx). Cohesive energy comparisons reveal the energy cost for different defects arising from substitution of C for N as a function of the nitrogen concentration. In FL CNx, combinations of pentagons and heptagons compete in causing graphene sheet curvature during the addition of CN-precursors and single species. Also, cross-linkage between graphene layers in FL CNx can be explained by the bond rotation due to incorporated N atoms. The computational results agree with recent experimental observations from the growth of FL CNx thin films.