Exciton-Scattering-Induced Dephasing in Two-Dimensional Semiconductors

Abstract

Enhanced Coulomb interactions in monolayer transition metal dichalcogenides cause tightly bound electron-hole pairs (excitons) which dominate their linear and nonlinear optical response. The latter includes bleaching, energy renormalizations, and higher-order Coulomb correlation effects like biexcitons and excitation-induced dephasing (EID). While the first three are extensively studied, no theoretical footing for EID in exciton dominated semiconductors is available so far. In this study, we present microscopic calculations based on excitonic Heisenberg equations of motion and identify the coupling of optically pumped excitons to exciton-exciton scattering continua as the leading mechanism responsible for an optical power dependent linewidth broadening (EID) and sideband formation. Performing time-, momentum-, and energy-resolved simulations, we quantitatively evaluate the EID for the most common monolayer transition metal dichalcogenides and find an excellent agreement with recent experiments.

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Cited by in corpus (8)

• Exciton optics, dynamics and transport in atomically thin semiconductors
• Phonon-assisted inter-valley scattering determines ultrafast exciton dynamics in MoSe${}_2$ bilayers
• Microscopic origin of anomalous interlayer exciton transport in van der Waals heterostructures
• Strong coupling regime and hybrid quasinormal modes of a single plasmonic resonator coupled to a TMDC monolayer
• Excitonic theory of doping-dependent optical response in atomically thin semiconductors
• Theory of the Coherent Response of Magneto-Excitons and Magneto-Biexcitons in Monolayer Transition Metal Dichalcogenides
• Doping-induced non-Markovian interference causes excitonic linewidth broadening in monolayer WSe${}_2$
• Influence of local fields on the dynamics of four-wave mixing signals from 2D semiconductor systems