  2D layered materials have recently attracted tremendous interest due to their
fascinating properties and potential applications. The interlayer interactions
are much weaker than the intralayer bonds, allowing the as-synthesized
materials to exhibit different stacking sequences (e.g. ABAB, ABCABC), leading
to different physical properties. Here, we show that regardless of the space
group of the 2D material, the Raman frequencies of the interlayer shear modes
observed under the typical configuration blue shift for AB stacked materials,
and red shift for ABC stacked materials, as the number of layers increases. Our
predictions are made using an intuitive bond polarizability model which shows
that stacking sequence plays a key role in determining which interlayer shear
modes lead to the largest change in polarizability (Raman intensity); the modes
with the largest Raman intensity determining the frequency trends. We present
direct evidence for these conclusions by studying the Raman modes in few layer
graphene, MoS2, MoSe2, WSe2 and Bi2Se3, using both first principles
calculations and Raman spectroscopy. This study sheds light on the influence of
stacking sequence on the Raman intensities of intrinsic interlayer modes in 2D
layered materials in general, and leads to a practical way of identifying the
stacking sequence in these materials.
