Graphene–transition
metal phthalocyanine (G–MPc)
hybrid systems constitute promising platforms for densely packed single-molecule
magnets (SMMs). Here, we selected iron(II) phthalocyanine (FePc) and
investigated its interaction with pristine and defective graphene
layers employing density functional theory. Our calculations indicate
that through proper dehydrogenation of the benzol rings in the FePc
molecule, its adsorption to graphene is thermodynamically favorable.
In general, the presence of anchoring sites on the graphene layer,
i.e., point defects, additionally facilitates the adsorption of FePc,
allowing one to achieve high density of SMMs per unit area. Using
the combination of group theory, ligand field splitting, and the calculated
PBE0 Kohn-Sham eigenvalue spectrum, we resolved the electronic structure
and predicted the spin states of both isolated FePc and G–FePc
hybrid systems. Regardless of the adsorption site and the number of
removed hydrogen atoms from the benzol rings of FePc, the magnetic
moment of the SMM remains unchanged with respect to the free FePc.
These results should mediate a successful synthesis of densely packed
G–MPc systems and may open up a new avenue in designing scalable
graphene–SMM systems for spintronics applications.