Influence of anharmonicity and interlayer interaction on Raman spectra in mono- and few-layer MoS2: A computational study

Two-dimensional (2D) MoS2 possesses unique optical and electrical properties and has many practical applications in nano-optoelectronics. Raman spectroscopy allows readily identify monolayer of MoS2, but the unambiguous determination of the number of layers in a few-layer structure remains a challenging task. In this work, the modification of frequencies of the most intense bands arising from in-plane and out-of-plane vibrations in the spectra of mono- and few-layer MoS2 crystals is studied experimentally, using the Raman scattering technique, and systematically analyzed theoretically, considering the influence of the interlayer interaction as well as the anharmonic interactions within the layer. A good agreement between experimental spectra and theoretical simulations is demonstrated, which allows to estimate the thickness of few-layer MoS2 and also determine parameters of the interlayer and anharmonic interactions. Possible effects of Fermi resonance in 2D MoS2 and the corresponding frequency shift of fundamental modes are considered. The proposed theoretical approach can be used to analyze Raman spectra, estimate the interlayer interaction, anharmonism, and the number of layers for other 2D layered materials.