Direct View of Phonon Dynamics in Atomically Thin MoS2.

ABSTRACT

Transition-metal dichalcogenide monolayers and heterostructures are highly tunable material systems that provide excellent models for physical phenomena at the two-dimensional (2D) limit. While most studies to date have focused on electrons and electron-hole pairs, phonons also play essential roles. Here, we apply ultrafast electron diffraction and diffuse scattering to directly quantify, with time and momentum resolution, electron-phonon coupling (EPC) in monolayer molybdenum disulfide and phonon transport from the monolayer to a silicon nitride substrate. Optically generated hot carriers result in a profoundly anisotropic distribution of phonons in the monolayer within ∼5 ps. A quantitative comparison with ab initio ultrafast dynamics simulations reveals the essential role of dielectric screening in weakening EPC. Thermal transport from the monolayer to the substrate occurs with the phonon system far from equilibrium. While screening in 2D is known to strongly affect equilibrium properties, our findings extend this understanding to the dynamic regime.