Heterostacks consisting of low-dimensional materials are attractive candidates for future electronic nanodevices in the post-silicon era. In this paper, using first-principles calculations based on density functional theory (DFT), we explore the structural and electronic properties of MoTe2/ZrS2 heterostructures with various stacking patterns and thicknesses. Our simulations show that the valence band (VB) edge of MoTe2 is almost aligned with the conduction band (CB) edge of ZrS2, and (MoTe2)m/(ZrS2)m (m = 1, 2) heterostructures exhibit the long-sought broken gap band alignment, which is pivotal for realizing tunneling transistors. Electrons are found to spontaneously flow from MoTe2 to ZrS2, and the system resembles an ultrascaled parallel plate capacitor with an intrinsic electric field pointed from MoTe2 to ZrS2. The effects of strain and external electric fields on the electronic properties are also investigated. For vertical compressive strains, the charge transfer increases due to the decreased coupling between the layers, whereas tensile strains lead to the opposite behavior. For negative electric fields a transition from the type-III to the type-II band alignment is induced. In contrast, by increasing the positive electric fields, a larger overlap between the valence and conduction bands is observed, leading to a larger band-to-band tunneling (BTBT) current. Low-strained heterostructures with various rotation angles between the constituent layers are also considered. We find only small variations in the energies of the VB and CB edges with respect to the Fermi level, for different rotation angles up to 30°. Overall, our simulations offer insights into the fundamental properties of low-dimensional heterostructures and pave the way for their future application in energy-efficient electronic nanodevices.
Keywords: 2D heterostructures; band alignment; electronic properties; external electric field; strain.