LAUSR

Abstract The emerging mixed-dimensional heterostructures of transition metal dichalcogenides with wide bandgap semiconductors of piezoelectric characteristics have shown excellent performance with novel pressure-modulation in flexible devices. Meanwhile, the recent introduction of “twist” at the interface of van der Waals (vdW) systems brought much flexibility in the manipulation of electrical and optical properties, giving rise to new physics. In this work, twisted angles ranging from 0° to 150° were introduced to the interface of the newly MoS2/AlN(0001) vdW mixed-dimensional heterostructures. Although all systems form type-I band alignment, the interfacial coupling can be evidently modulated by the twisted angles, leading to twisted angle-dependent structural characteristics, electronic structure, and carrier transport with a period of 60°. The most intriguing is that a large manipulating scale of band offset and carrier transmission window (intensity) can be achieved by specifying the rotation, suggesting an effective route to design the electronic structure. It was further revealed that twisted angle modulated interfacial coupling gives rise to a diversity of resonant states’ distribution in the momentum space. Our study not only systemically investigated the newly MoS2/AlN(0001) vdW mixed-dimensional heterostructure, but also proposed a novel route to effectively manipulate the properties of mixed-dimensional heterostructure layer by layer.