Interlayer Engineering of Lattice Dynamics and Elastic Constants of 2D Layered Nanomaterials under Pressure

Interlayer coupling in two-dimensional (2D) layered nanomaterials can provide us novel strategies to evoke their superior properties, such as the exotic flat bands and unconventional superconductivity of twisted layers, the formation of moir\'e excitons and related nontrivial topology. However, to accurately quantify interlayer potential and further measure elastic properties of 2D materials remains vague, despite significant efforts. Herein, the layer-dependent lattice dynamics and elastic constants of 2D nanomaterials have been systematically investigated via pressure-engineering strategy based on ultralow frequency Raman spectroscopy. The shearing mode and layer-breathing Raman shifts of MoS2 with various thicknesses were analyzed by the linear chain model. Intriguingly, it was found that the layer-dependent d{\omega}/dP of shearing and breathing Raman modes display the opposite trends, quantitatively consistent with our molecular dynamics simulations and density functional theory calculations. These results can be generalized to other van der Waals systems, and may shed light on the potential applications of 2D materials in nanomechanics and nanoelectronics.