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Multilayer van der Waals (vdWs) heterostructures assembled by diverseatomically thin layers have demonstrated a wide range of fascinating phenomenaand novel applications. Understanding the interlayer coupling and itscorrelation effect is paramount for designing novel vdWs heterostructures withdesirable physical properties. Using a detailed theoretical study of 2DMoS2-graphene (GR)-based heterostructures based on state-of-the-art hybriddensity functional theory, we reveal that for 2D few-layer heterostructures,vdWs forces between neighboring layers depend on the number of layers. Comparedto that in bilayer, the interlayer coupling in trilayer vdW heterostructurescan significantly be enhanced by stacking the third layer, directly supportedby short interlayer separations and more interfacial charge transfer. Thetrilayer shows strong light absorption over a wide range (<700 nm), making itvery potential for solar energy harvesting and conversion. Moreover, the Diracpoint of GR and band gaps of each layer and trilayer can be readily tuned byexternal electric field, verifying multilayer vdWs heterostructures with unqiueoptoelectronic properties found by experiments. These results suggest thattuning the vdWs interaction, as a new design parameter, would be an effectivestrategy for devising particular 2D multilayer vdWs heterostructures to meetthe demands in various applications.

chemistry of materials

2D MoS2-Graphene-based multilayer van der Waals heterostructures:  Enhanced charge transfer and optical absorption, and electric-field tunable  Dirac point and band gap