Resonant Low Frequency Interlayer Shear Modes in Folded Graphene Layers

Naturally or artificially stacking extra layers on single layer graphene (SLG) forms few-layer graphene (FLG), which has attracted tremendous attention owing to its exceptional properties inherited from SLG and new features generated by introducing extra freedom. In FLG, shear modes play a critical role in understanding its distinctive properties. Unfortunately, energies of shear modes are so close to excitation lasers to be fully blocked by a Rayleigh rejecter. This greatly hinders investigations of shear modes in FLG. Here, we demonstrate dramatically enhanced shear modes in properly folded FLG. Benefiting from the extremely strong signals, for the first time, enhancement mechanism, vibrational symmetry, anharmonicity and electron-phonon coupling (EPC) of shear modes are uncovered through studies of two-dimensional (2D) Raman mapping, polarization- and temperature-dependent Raman spectroscopy. This work complements Raman studies of graphene layers, and paves an efficient way to exploit low frequency shear modes of FLG and other 2D layered materials.