Metal contacts to two-dimensional (2D) semiconductors are often plagued by the strong Fermi level pinning (FLP) effect which reduces the tunability of the Schottky barrier height (SBH) and degrades the performance of 2D semiconductor devices. Here, we show that MoSi2N4 and WSi2N4 monolayers—an emerging 2D semiconductor family with exceptional physical properties—exhibit strongly suppressed FLP and wide-range tunable SBH. An exceptionally large SBH slope parameter of S ≈ 0.7 is obtained which outperforms the vast majority of other 2D semiconductors. Such intriguing behavior arises from the septuple-layered morphology of MoSi2N4 and WSi2N4 monolayers in which the semiconducting electronic states are protected by the outlying Si–N sublayer. We identify Ti, Sc, and Ni as highly efficient Ohmic contacts to MoSi2N4 and WSi2N4 with zero interface tunneling barrier. Our findings reveal the potential of MoSi2N4 and WSi2N4 as a practical platform for designing high-performance and energy-efficient 2D semiconductor electronic devices.

A two-dimensional (2D) MoSi2N4 monolayer is an emerging class of air-stable 2D semiconductors possessing exceptional electrical and mechanical properties. Despite intensive recent research effort devoted to uncover the material properties of MoSi2N4, the physics of electrical contacts to MoSi2N4 remains largely unexplored thus far. In this work, we study van der Waals heterostructures composed of MoSi2N4 contacted by graphene and NbS2 monolayers using first-principles density functional theory calculations. We show that the MoSi2N4/NbS2 contact exhibits an ultralow Schottky barrier height (SBH), which is beneficial for nanoelectronics applications. For the MoSi2N4/graphene contact, the SBH can be modulated via the interlayer distance or via external electric fields, thus opening up an opportunity for reconfigurable and tunable nanoelectronic devices. Our findings provide insights into the physics of 2D electrical contacts to MoSi2N4 and shall offer a critical first step toward the design of high-performance electrical contacts to MoSi2N4-based 2D nanodevices.

With exceptional electrical and mechanical properties and at the same time air-stability, layered MoSi2N4 has recently drawn great attention. However, band structure engineering via strain and electric field, which is vital for practical applications, has not yet been explored. In this work, we show that the biaxial strain and external electric field are effective ways for the bandgap engineering of bilayer MoSi2N4 and WSi2N4. It is found that strain can lead to indirect bandgap to direct bandgap transition. On the other hand, electric field can result in semiconductor to metal transition. Our study provides insights into the band structure engineering of bilayer MoSi2N4 and WSi2N4 and would pave the way for its future nanoelectronics and optoelectronics applications.

Janus transition metal dichalcogenides with a built-in structural cross-plane asymmetry have recently emerged as a new class of two-dimensional materials with a large cross-plane dipole. By using the density functional theory calculation, we report the formation of different Schottky barriers for Janus PtSSe and graphene based van der Waals heterostructures, where the Schottky barrier height (SBH) and type of contact can be controlled by adjusting the interlayer distance, by applying an external electric field, and by having multiple layers of Janus PtSSe. It is found that the effects of tuning are more prominent for SPtSe/graphene as compared to SePtS/graphene. Besides, a transition from n-type Schottky contact to p-type Schottky contact and to Ohmic contact is also observed in the SPtSe/Gr heterostructure for different SPtSe stackings from 1 layer, to 2- and 3-layers, respectively. Our findings indicate that the SPtSe/graphene heterostructure is a suitable candidate for applications that require a tunable SBH.