Anharmonic phonons in few layer MoS$_2$: Raman spectroscopy of ultra low energy compression and shear modes

TL;DR

This study combines ultra-low energy Raman spectroscopy and first-principles calculations to analyze anharmonic phonons in few-layer MoS$_2$, revealing enhanced phonon-phonon scattering in thinner samples, which impacts thermal transport in 2D materials.

Contribution

It provides the first comprehensive experimental and theoretical analysis of compression and shear modes in few-layer MoS$_2$, highlighting anharmonic effects and layer-dependent phonon scattering.

Findings

Compression modes are strongly anharmonic in few-layer MoS$_2$.

Phonon-phonon scattering increases as the number of layers decreases.

Anharmonicity is likely a general feature of nanolayered materials with weak interlayer coupling.

Abstract

Molybdenum disulfide (MoS$_2$) is a promising material for making two-dimensional crystals and flexible electronic and optoelectronic devices at the nanoscale. MoS$_2$ flakes can show high mobilities and have even been integrated in nanocircuits . A fundamental requirement for such use is efficient thermal transport. Electronic transport generates heat which needs to be evacuated, more crucially so in nanostructures. Anharmonic phonon-phonon scattering is the dominant intrinsic limitation to thermal transport in insulators. Here, using appropriate samples, ultra-low energy Raman spectroscopy and first principles calculations, we provide a full experimental and theoretical description of compression and shear modes of few-layer (FL) MoS$_2$. We demonstrate that the compression modes are strongly anharmonic with a marked enhancement of phonon-phonon scattering as the number of layers is reduced, most likely a general feature of nanolayered materials with weak interlayer coupling.