Twist-assisted optoelectronic phase control in two-dimensional (2D) Janus heterostructures

Abstract Atomically thin two-dimensional (2D) Janus materials and their Van der Waals heterostructures (vdWHs) have emerged as a new class of intriguing semiconductor materials due to their versatile application in electronic and optoelectronic devices. Herein, We have invstigated most probable arrangements of different inhomogeneous heterostructures employing one layer of transition metal dichalcogenide, TMD (MoS 2 , WS 2 , MoSe 2 , and WSe 2 ) piled on the top of Janus TMD (MoSeTe or WSeTe) and investigated their structural, electronic as well as optical properties through first-principles based calculations. After that, we applied twist engineering between the monolayers from 0 $$^{\circ } \rightarrow$$ ∘ → 60 $$^{\circ }$$ ∘ twist angle, which delivers lattice reconstruction and improves the performance of the vdWHs due to interlayer coupling. The result reveals that all the proposed vdWHs are dynamically and thermodynamically stable. Some vdWHs such as MoS 2 /MoSeTe, WS 2 /WSeTe, MoS 2 /WSeTe, MoSe 2 /MoSeTe, and WS 2 /MoSeTe exhibit direct bandgap with type-II band alignment at some specific twist angle, which shows potential for future photovoltaic devices. Moreover, the electronic property and carrier mobility can be effectively tuned in the vdWHs compared to the respective monolayers. Furthermore, the visible optical absorption of all the Janus vdWHs at $$\theta$$ θ = 0 $$^{\circ }$$ ∘ can be significantly enhanced due to the weak inter-layer coupling and redistribution of the charges. Therefore, the interlayer twisting not only provides an opportunity to observe new exciting properties but also gives a novel route to modulate the electronic and optoelectronic properties of the heterostructure for practical applications.