▎ 摘　　要

Motivated from a recent experimental study on filling of a graphene nanocavity by iron membrane at room temperature (Science 2014, 343, 1228), we perform a comprehensive study of morphology changes of two-dimensional Fe membranes and iron carbides embedded in graphene nanocavities with specific sizes and shapes using the first-principles calculations and ab initio molecular dynamics simulations. Our simulations show that Fe atoms tend to gradually seal the graphene nanocavity via growing a metastable Fe membrane until the nanocavity is completely covered. Notably, a densely packed Fe membrane in the graphene nanocavity shows higher structural stability than a loosely packed one as long as more triangular lattices can form to release high tensile strain. The Fe membrane under high tensile strain tends to collapse and turns into a three-dimensional Fe cluster upon detaching from the edge. The structural transformation of Fe nanostructures follows the melting recrystallization mechanism at ambient temperatures in high vacuum. Moreover, the iron carbide can also exist in the graphene nanocavity and once formed can be highly stable even at 1200 K.