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Decorating two-dimensional materials with transition-metal adatoms is aneffective way to bring about new physical properties that are intriguing forapplications in electronics and spintronics devices. Here, we systematicallystudied the coverage-dependent magnetic and electronic properties of graphenedecorated by Co adatoms, based on first-principles calculations. We found thatthe if the Co coverage is larger than 1/3 ML, the Co atoms will aggregate toform a Co monolayer and then a van der Waals bilayer system between the Comonolayer and graphene forms. When the Co coverage is <= 1/3 ML, the Co adatomis spin polarized with spin moment varying from 1.1 ~ 1.4 {\mu}B. The d(xz/yz)and d(xy/x2-y2 ) orbitals of Co hybridize significantly with the {\pi} bands ofgraphene, which generates a series of new bands in the energy range from -2 eVto 1 eV with respect to Dirac point of graphene. In most cases, the new bandsnear the Fermi level lead to topological states characterized by the quantumanomalous Hall effect.

Coverage-dependent magnetic and electronic properties of graphene with Co adatoms