Enhanced ultra-low-frequency interlayer shear modes in folded graphene layers

Few-layer graphene has attracted tremendous attention owing to its exceptional electronic properties inherited from single-layer graphene and new features led by introducing extra freedoms such as interlayer stacking sequences or rotations. Effectively probing interlayer shear modes are critical for unravelling mechanical and electrical properties of few-layer graphene and further developing its practical potential. Unfortunately, shear modes are extremely weak and almost fully blocked by a Rayleigh rejecter in Raman measurements. This greatly hinders investigations of shear modes in few-layer graphene. Here, we demonstrate enhancing of shear modes by properly folding few-layer graphene. As a direct benefit of the strong signal, enhancement mechanism, vibrational symmetry, anharmonicity and electron–phonon coupling of the shear modes are uncovered through studies of 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 few-layer graphene and other two-dimensional layered materials.