Mobility calculation in disordered WS2-Al2O3 stacks from first principles

Transition metal dichalcogenides (TMDCs) are promising candidates for future nano-transistor channels due to their outstanding intrinsic transport properties. However, their electron mobility is highly sensitive to the surrounding dielectric, often falling well below theoretical expectations. In this work, we explore how a stacked Al₂O₃ dielectric affects electron mobility in monolayer WS₂ using first-principles quantum transport simulations. We identify that fluctuations in the electrostatic potential, arising from the disordered structure of Al₂O₃, significantly degrade mobility, especially when WS₂ interfaces with under-coordinated aluminum atoms. Our calculated mobilities (≃1–30 cm²/(V ⋅ s)) align with experimental observations and remain far from the ideal limit (≃300 cm²/(V ⋅ s)). We further demonstrate that encapsulating WS₂ with hexagonal boron nitride (hBN) or employing a crystalline oxide can recover high mobility values. However, these strategies introduce trade-offs in electrostatic control and fabrication complexity, underlining the need for careful dielectric engineering in TMDC-based devices.