Role of interlayer coupling in ultra thin MoS2

The effects of interlayer coupling on the vibrational and electronic properties of ultra thin MoS2 were studied by ab initio calculations. For smaller slab thickness, the interlayer distance is significantly elongated because of reduced interlayer coupling. This explains the anomalous thickness dependence of the lattice vibrations observed by Lee et al. (ACS Nano, 2010, 4, 2695). The absence of interlayer coupling in mono-layer MoS2 induces a transition from direct to indirect band gap behaviour. Our results demonstrate a strong interplay between the intralayer chemical bonding and the interlayer van-der-Waals interaction.