Boosting and Balancing Electron and Hole Mobility in Single- and Bilayer WSe₂ Devices via Tailored Molecular...

WSe₂ is a layered ambipolar semiconductor enabling hole and electron transport, which renders it a suitable active component for logic circuitry. However, solid-state devices based on single- and bilayer WSe₂ typically exhibit unipolar transport and poor electrical performance when conventional SiO₂ dielectric and Au electrodes are used. Here, we show that silane-containing functional molecules form ordered monolayers on the top of the WSe₂ surface, thereby boosting its electrical performance in single- and bilayer field-effect transistors. In particular, by employing SiO₂ dielectric substrates and top Au electrodes, we measure unipolar mobility as high as μ_h = 150 cm² V^-1 s^-1 and μ_e = 17.9 cm² V^-1 s^-1 in WSe₂ single-layer devices when ad hoc molecular monolayers are chosen. Additionally, by asymmetric double-side functionalization with two different molecules, we provide opposite polarity to the top and bottom layer of bilayer WSe₂, demonstrating nearly balanced ambipolarity at the bilayer limit. Our results indicate that the controlled functionalization of the two sides of the WSe₂ mono- and bilayer flakes with highly ordered molecular monolayers offers the possibility to simultaneously achieve energy level engineering and defect functionalization, representing a path toward deterministic control over charge transport in 2D materials.