Direct view of phonon dynamics in atomically thin MoS${}_2$

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 (MoS${}_2$) and phonon transport from the monolayer to a silicon nitride (Si${}_3$N${}_4$) substrate. Optically generated hot carriers result in a profoundly anisotropic distribution of phonons in the monolayer on the $\sim$ 5 ps time scale. 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.

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Cited by in corpus (13)

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• Strain-induced activation of chiral-phonon emission in monolayer WS${}_2$
• Momentum-Resolved Signatures of Carrier Screening Effects on Electron-Phonon Coupling in MoS${}_2$
• Excimer Formation in Zinc-phthalocyanine Revealed using Ultrafast Electron Diffraction
• Time-domain study of coupled collective excitations in quantum materials
• Ultrafast Phonon-Diffuse Scattering as a Tool for Observing Chiral Phonons in Monolayer Hexagonal Lattices
• Ultrafast Electron Diffuse Scattering as a Tool for Studying Phonon Transport: Phonon Hydrodynamics and Second Sound Oscillations
• Advancing Simulations of Coupled Electron and Phonon Nonequilibrium Dynamics Using Adaptive and Multirate Time Integration
• Element-specific ultrafast lattice dynamics in monolayer WSe2
• Prospects for Direct Electron Detectors in Ultrafast Electron Diffraction and Scattering Experiments