Probing the Twist-Controlled Interlayer Coupling in Artificially Stacked Transition Metal Dichalcogenide Bilayers by...

Interlayer coupling plays a critical role in the electronic band structures and optoelectronic properties of van der Waals (vdW) materials and heterostructures. Here, we utilize optical second-harmonic generation (SHG) measurements to probe the twist-controlled interlayer coupling in artificially stacked WSe₂/WSe₂ homobilayers and WSe₂/WS₂ and WSe₂/MoS₂ heterobilayers with a postannealing procedure. In the large angle twisted WSe₂/WSe₂ and WSe₂/WS₂, the angular dependence of the SHG intensity follows the interference relations up to angles above 10°. For lower angles, the SHG is significantly suppressed. Furthermore, for the twisted WSe₂/MoS₂ the SHG intensity largely deviates from the coherent superposition model and shows consistent quenching for all the stacking angles. The suppressed SHG in twisted transition metal dichalcogenide (TMDC) bilayers is predominantly attributed to the interlayer coupling between the two adjacent monolayers. The evolution of the interlayer Raman mode in WSe₂ demonstrates that the interlayer coupling in the twisted WSe₂/WSe₂ and WSe₂/WS₂ is highly angle-dependent. Alternatively, the interlayer coupling generally exists in the twisted WSe₂/MoS₂, regardless of the different angles. The interlayer coupling is further confirmed by the quenching and red-shift of the photoluminescence of WSe₂ in the twisted TMDC bilayers. Combined with density functional theory calculations, we reveal that the stacking-angle-modulated interlayer coupling originates from the variation of the interlayer spacing and the binding energy in the twisted TMDC bilayers.