Van der Waals (vdW) heterostructures, achieved by binding various two-dimensional (2D) materials together via vdW interaction, expand the family of 2D materials and show fascinating possibilities. In this work, we have systematically investigated the geometrical structures, electronic structures, and optical properties of III–VI (MX, M = Ga, In and X = S, Se, Te) vdW heterostructures and their corresponding applications in sustainable energy related areas based on first principles calculations. It is highlighted that different heterostructure types can be achieved in spite of the similar electronic structures of MX monolayers. Meanwhile, the potential applications of the heterostructures for sustainable energy related areas have been further unraveled. For instance, type-II InS/GaSe and GaS/GaSe vdW heterostructures can separately produce hydrogen and oxygen at the opposite parts. On the other hand, a type-II GaSe/GaTe heterostructure with a direct band gap compatible with silicon has been proposed to be a potential solar cell material with a power conversion efficiency over 18%. Furthermore, a gapless type-IV semi-metallic InTe/GaS heterostructure has been predicted to be a Li-ion battery anode material based on three-step lithiated analysis. The present results will shed light on the sustainable energy applications of such remarkable artificial MX vdW heterostructures in the future.

Monolayers of III–VI group two-dimensional (2D) materials MX (M = Ga and In and X = S, Se, and Te) have attracted global interest for potential applications in electronic and photoelectric devices due to their attractive physical and chemical characteristics. However, a comprehensive understanding of the distinguished carrier mobility in MX monolayers is of great importance and not yet clear. Herein, using a Boltzmann transport equation (BTE) solver and first principles calculations, we have precisely revealed that the intrinsic mobility in MX monolayers is significantly limited by phonon scattering. Note that the longitudinal acoustic phonon mode and optic phonon modes and were found predominantly coupled with electrons, which strongly restrained the intrinsic mobility in the MX monolayers. Interestingly, apart from a moderate band gap, the GaSe and GaTe monolayers exhibit high electron mobility exceeding 10³ cm² V⁻¹ s⁻¹ and may serve as outstanding electron transport channels. We believe that our findings will shed light on the design and applications of MX monolayers and 2D materials in nanoscale electronic and photoelectric devices.

The flourish of two-dimensional (2D) materials provides a versatile platform for building high-performance electronic devices in the atomic thickness regime. However, the presence of the high Schottky barrier at the interface between the metal electrode and the 2D semiconductors, which dominates the injection and transport efficiency of carriers, always limits their practical applications. Herein, we show that the Schottky barrier can be controllably lifted in the heterostructure consisting of Janus MoSSe and 2D vdW metals by different means. Based on density functional theory calculations and machine learning modelings, we studied the electrical contact between semiconducting monolayer MoSSe and various metallic 2D materials, where a crossover from Schottky to Ohmic/quasi-Ohmic contact is realized. We demonstrated that the band alignment at the interface of the investigated metal-semiconductor junctions (MSJs) deviates from the ideal Schottky–Mott limit because of the Fermi-level pinning effects induced by the interface dipoles. Besides, the effect of the thickness and applied biaxial strain of MoSSe on the electronic structure of the junctions are explored and found to be powerful tuning knobs for electrical contact engineering. It is highlighted that using the sure-independence-screening-and-sparsifying-operator machine learning method, a general descriptor W_M ³/exp(D_int) was developed, which enables the prediction of the Schottky barrier height for different MoSSe-based MSJ. These results provide valuable theoretical guidance for realizing ideal Ohmic contacts in electronic devices based on the Janus MoSSe semiconductors.