Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides

Abstract

Atomically thin transition metal dichalcogenides (TMDs) are direct-gap semiconductors with strong light-matter and Coulomb interaction. The latter accounts for tightly bound excitons, which dominate the optical properties of these technologically promising materials. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. In a recent study, an experimental evidence for the existence of such dark states has been demonstrated, as well as their strong impact on the quantum efficiency of light emission in TMDs. Here, we reveal the microscopic origin of the excitonic coherence lifetime in two representative TMD materials (WS${}_2$ and MoSe${}_2$) within a joint study combining microscopic theory with optical experiments. We show that the excitonic coherence lifetime is determined by phonon-induced intra- and intervalley scattering into dark excitonic states. Remarkably, and in accordance with the theoretical prediction, we find an efficient exciton relaxation in WS${}_2$ through phonon emission at all temperatures.

References in corpus (7)

• Anomalous Lattice Vibrations of Single and Few-Layer MoS2
• Valley polarization in MoS2 monolayers by optical pumping
• Measurement of the optical dielectric function of transition metal dichalcogenide monolayers: MoS2, MoSe2, WS2 and WSe2
• Tightly bound excitons in monolayer WSe2
• k.p theory for two-dimensional transition metal dichalcogenide semiconductors
• Intrinsic Transport Properties of Electrons and Holes in Monolayer Transition Metal Dichalcogenides
• Exciton band structure of monolayer MoS2

Cited by in corpus (207)

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• Directly visualizing the momentum forbidden dark excitons and their dynamics in atomically thin semiconductors
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• Nanophotonics with 2D Transition Metal Dichalcogenides
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• Exciton-exciton interaction in transition-metal dichalcogenide monolayers
• The ultrafast onset of exciton formation in 2D semiconductors
• Exciton diffusion in monolayer semiconductors with suppressed disorder
• Theory of Exciton-Phonon Coupling
• Exciton Relaxation Cascade in Two-dimensional Transition-metal dichalcogenides
• Accessing high optical quality of MoS2 monolayers grown by chemical vapor deposition
• Momentum-Resolved View of Electron-Phonon Coupling in Multilayer WSe${}_2$
• The role of momentum-dark excitons in the elementary optical response of bilayer WSe${}_2$
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• Direct measurement of key exciton properties: energy, dynamics and spatial distribution of the wave function
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• Strongly coupled coherent phonons in single-layer MoS${}_2$
• Hybridized intervalley moiré excitons and flat bands in twisted WSe${}_2$ bilayers
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• Crossover from exciton polarons to trions in doped two-dimensional semiconductors at finite temperature
• Excitation-Dependent High-Lying Excitonic Exchange via Interlayer Energy Transfer from Lower-to-Higher Bandgap 2D Material
• Phonon-assisted Exciton Dissociation in Transition Metal Dichalcogenides
• Photophysical comparison of liquid and mechanically exfoliated WS${}_2$ monolayers
• Excitonic theory of doping-dependent optical response in atomically thin semiconductors
• Ultrafast charge transfer and vibronic coupling in a laser-excited hybrid inorganic/organic interface
• Coupling of MoS${}_2$ Excitons with Lattice Phonons and Cavity Vibrational Phonons in Hybrid Nanobeam Cavities
• Interacting electrons and bosons in the doubly screened $G\tilde{W}$ approximation: A time-linear scaling method for first-principles simulations
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• Observation of Dynamic Screening in the Excited Exciton States in Multi-layered MoS${}_2$
• A pre-time-zero spatiotemporal microscopy technique for the ultrasensitive determination of the thermal diffusivity of thin films
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• Optical fingerprint of bright and dark localized excitonic states in atomically thin 2D materials
• Rapid multiplex ultrafast nonlinear microscopy for material characterization
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• Theory of the Coherent Response of Magneto-Excitons and Magneto-Biexcitons in Monolayer Transition Metal Dichalcogenides
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• Coherence and de-coherence in the Time-Resolved ARPES of realistic materials: an ab-initio perspective
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• Room-temperature tuning and probing of Fermi polarons in atomically thin semiconductors on a plasmonic metasurface
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