Selective Synthesis of Bi₂Te₃/WS₂Heterostructures with Strong Interlayer Coupling

The vertical integration of atomically thin-layered materials to create van der Waals heterostructures (vdWHs) has been proposed as a method to design nanostructures with emergent properties. In this work, epitaxial Bi2Te3/WS2 vdWHs are synthesized via a two-step vapor deposition process. It is calculated that the vdWH has an indirect band gap with a valence band edge that bridges the vdW gap, resulting in a quenched photoluminescence (PL) from the WS2 monolayer, reduced intensity of its resonance Raman vibrational peaks, improved vertical charge transport, and a decrease in the intensity of second harmonic generation (SHG). Furthermore, it is observed that induced defects strongly influence the nucleation and growth of vdWHs. By creating point defects in WS2 monolayers, it is shown that the growth of Bi2Te3 platelets can be patterned. This work offers important insights into the synthesis, defect engineering, and moiré engineering of an emerging class of two-dimensional (2D) heterostructures.