Heterostructural bilayers of graphene and molybdenum disulfide: Configuration types, band opening and enhanced light response

•Advanced method for configuration classification of layers-composite is presented.•Graphene corrugation modulates the stacking arrangement of graphene and MoS2.•The bandgaps of all types graphene and MoS2 nanocomposite are opened.•All types graphene and MoS2 nanocomposites display an enhanced light absorption. The properties of graphene absorption on graphene-like material can be modulated by the stacking arrangement. Here, we propose a “least squares” classification method for analyzing configuration types of graphene/molybdenum disulfide heterobilayers (G/MoS2 HBLs) while binding energy, electronic structure and optical absorption of G/MoS2 HBLs are investigated via first principles calculations. Owing to the lattice mismatch, no traditional AA and AB stacking exist but AA- and AB-stacking-like configurations have been found. Paradoxically, AB-stacking-like configuration, generally as the most stable stacking sequence, does not correspond to the relaxed structure. We interpret this paradox in terms of graphene corrugation. A detailed analysis of the electronic structure indicates that bandgaps of all configurations types (types of G/MoS2 HBLs) are opened and tunable under the different interlayer distance. Furthermore, compared with monolayer MoS2, G/MoS2 HBLs display an enhanced light response, a promising feature for photocatalytic applications.