Modification of interlayer interaction in bilayer MoS₂ due to monolayer WSe₂ in heterostructures

Abstract

The low-frequency interlayer vibration modes in bilayer-MoS2/monolayer-WSe2 heterostructures were investigated to study the modification of interlayer interactions due to the moiré periodicity. The interplay of the interlayer interaction within bilayer MoS2 and the interfacial interaction between the two materials results in rich features in the phonon spectra. Several shear and breathing modes are observed for samples with small twist angles (<10°), whereas only one shear and two breathing modes are observed for larger twist angles. For larger twist angles, the interfacial interaction between the two materials amounts to ~75% of the intrinsic interlayer interaction between the MoS2 layers. The phonon spectrum evolves non-monotonically as the twist angle increases, which is explained with the help of atomistic calculations.