Raman Fingerprint of Interlayer Coupling in 2D TMDCs

Vertical stacking of two-dimensional (2D) homo- and heterostructures are intriguing research objects, as they are essential for fundamental studies and a key towards 2D device applications. It is paramount to understand the interlayer coupling in 2D materials and to find a fast yet precise characteristic signature. In this work, we report on a Raman fingerprint of interlayer coupling in 2D transition metal dichalcogenides (TMDCs). We observed that the out-of-plane [Formula: see text] vibrational mode is absent when two monolayers form a vertical stack yet remain uncoupled but emerges after strong coupling. Using systematic Raman, photoluminescence (PL), and atomic force microscopy (AFM) studies of WSe [Formula: see text] /WSe [Formula: see text] homo-bilayers and MoSe [Formula: see text] /WSe [Formula: see text] hetero-bilayers, we conclude that the [Formula: see text] vibrational mode is a distinct Raman fingerprint of interlayer coupling in 2D TMDCs. Our results propose an easy, fast, precise, and reliable measure to evaluate the interlayer coupling in 2D TMDCs.