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

TL;DR

This study uses advanced theoretical methods to analyze 2D MoS2-graphene heterostructures, revealing layer-dependent interlayer coupling, enhanced optical absorption, and electric-field tunable electronic properties, with implications for energy and optoelectronic applications.

Contribution

It provides a detailed theoretical analysis of multilayer vdWs heterostructures, highlighting how stacking layers influences interlayer coupling and optoelectronic properties, which was less understood before.

Findings

Interlayer coupling increases with more layers.

Trilayer heterostructures exhibit broad light absorption (<700 nm).

Electric fields can tune Dirac points and band gaps.

Abstract

Multilayer van der Waals (vdWs) heterostructures assembled by diverse atomically thin layers have demonstrated a wide range of fascinating phenomena and novel applications. Understanding the interlayer coupling and its correlation effect is paramount for designing novel vdWs heterostructures with desirable physical properties. Using a detailed theoretical study of 2D MoS2-graphene (GR)-based heterostructures based on state-of-the-art hybrid density functional theory, we reveal that for 2D few-layer heterostructures, vdWs forces between neighboring layers depend on the number of layers. Compared to that in bilayer, the interlayer coupling in trilayer vdW heterostructures can significantly be enhanced by stacking the third layer, directly supported by short interlayer separations and more interfacial charge transfer. The trilayer shows strong light absorption over a wide range (<700 nm), making it very potential for solar energy harvesting and conversion. Moreover, the Dirac point of GR and band gaps of each layer and trilayer can be readily tuned by external electric field, verifying multilayer vdWs heterostructures with unqiue optoelectronic properties found by experiments. These results suggest that tuning the vdWs interaction, as a new design parameter, would be an effective strategy for devising particular 2D multilayer vdWs heterostructures to meet the demands in various applications.