Exciton Relaxation Cascade in Two-dimensional Transition-metal dichalcogenides

Abstract

Monolayers of transition-metal dichalcogenides (TMDs) are characterized by an extraordinarily strong Coulomb interaction giving rise to tightly bound excitons with binding energies of hundreds of meV. Excitons dominate the optical response as well as the ultrafast dynamics in TMDs. As a result, a microscopic understanding of exciton dynamics is the key for technological application of these materials. In spite of this immense importance, elementary processes guiding the formation and relaxation of excitons after optical excitation of an electron-hole plasma has remained unexplored to a large extent. Here, we provide a fully quantum mechanical description of momentum- and energy-resolved exciton dynamics in monolayer molybdenum diselenide (MoSe${}_2$) including optical excitation, formation of excitons, radiative recombination as well as phonon-induced cascade-like relaxation down to the excitonic ground state. Based on the gained insights, we reveal experimentally measurable features in pump-probe spectra providing evidence for the exciton relaxation cascade.

References in corpus (8)

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• 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
• Dark excitons in transition metal dichalcogenides
• Phonon Sidebands in Transition Metal Dichalcogenides
• Dielectric Engineering of Electronic Correlations in a van der Waals Heterostructure

Cited by in corpus (59)

• Exciton physics and device application of two-dimensional transition metal dichalcogenide semiconductors
• Directly visualizing the momentum forbidden dark excitons and their dynamics in atomically thin semiconductors
• Ultrafast transition between exciton phases in van der Waals heterostructures
• Enhanced Light-Matter Interaction in Two-Dimensional Transition Metal Dichalcogenides
• Phonon-assisted Photoluminescence from Dark Excitons in Monolayers of Transition Metal Dichalcogenides
• Control of the Exciton Radiative Lifetime in van der Waals Heterostructures
• The ultrafast onset of exciton formation in 2D semiconductors
• Exciton-Phonon Interaction and Relaxation Times from First Principles
• Theory of Exciton-Phonon Coupling
• Exciton-exciton interaction in transition metal dichalcogenide monolayers and van der Waals heterostructures
• Exciton propagation and halo formation in two-dimensional materials
• Hybridized intervalley moiré excitons and flat bands in twisted WSe${}_2$ bilayers
• Impact of strain on the excitonic linewidth in transition metal dichalcogenides
• Exciton optics, dynamics and transport in atomically thin semiconductors
• Theory of exciton dynamics in time-resolved ARPES: intra- and intervalley scattering in two-dimensional semiconductors
• Intrinsic Lifetime of Higher Excitonic States in Tungsten Diselenide Monolayers
• Mapping of the dark exciton landscape in transition metal dichalcogenides
• Negative excitonic diffusion in transition metal dichalcogenides
• Efficient phonon cascades in hot photoluminescence of WSe${}_2$ monolayers
• Exciton lifetime and optical linewidth profile via exciton-phonon interactions: Theory and first-principles calculations for monolayer MoS${}_2$
• Hot exciton transport in WSe2 monolayers
• First-Principles Calculations of Exciton Radiative Lifetimes in Monolayer Graphitic Carbon Nitride Nanosheets: Implications for Photocatalysis
• Strain-dependent exciton diffusion in transition metal dichalcogenides
• Microscopic picture of electron-phonon interaction in two-dimensional halide perovskites
• Brightening of spin- and momentum-dark excitons in transition metal dichalcogenides
• Phonon-assisted inter-valley scattering determines ultrafast exciton dynamics in MoSe${}_2$ bilayers
• Temporal evolution of low-temperature phonon sidebands in WSe${}_2$ monolayers
• Ultrafast dynamics of bright and dark excitons in monolayer WSe${}_2$ and heterobilayer WSe${}_2$/MoS${}_2$
• Quenching of Intervalley Exchange Coupling in the Presence of Momentum-Dark States in TMDCs
• Dark-exciton based strain sensing in transition metal dichalcogenides
• Exciton-phonon interaction calls for a revision of the "exciton" concept
• Optically induced topological superconductivity via Floquet interaction engineering
• Probing correlations in the exciton landscape of a moiré heterostructure
• Ultrafast phonon-driven charge transfer in van der Waals heterostructures
• Dynamics of incoherent exciton formation in Cu${}_2$O: Time- and angle-resolved photoemission spectroscopy
• Microscopic modelling of exciton-polariton diffusion coefficients in atomically thin semiconductors
• Many-body theory of radiative lifetimes of exciton-trion superposition states in doped two-dimensional materials
• Spectrum of exciton states in monolayer transition metal dichalcogenides: angular momentum and Landau levels
• Phonon-assisted Exciton Dissociation in Transition Metal Dichalcogenides
• Ultrafast charge transfer and vibronic coupling in a laser-excited hybrid inorganic/organic interface
• Ultrafast nano-imaging of dark excitons
• Optical fingerprint of bright and dark localized excitonic states in atomically thin 2D materials
• Distance dependence of the energy transfer mechanism in WS${}_2$-graphene heterostructures
• Spatial control of carrier capture in two-dimensional materials: Beyond energy selection rules
• Signatures of dark excitons in exciton-polariton optics of transition metal dichalcogenides
• Excitonic Bloch equations from first principles
• Excitonic thermalization bottleneck in twisted TMD heterostructures
• Spatially indirect excitons in black and blue phosphorene double layers
• Impact of charge transfer excitons on unidirectional exciton transport in lateral TMD heterostructures
• Valley-exchange coupling probed by angle-resolved photoluminescence
• Two dimensional semiconductors: optical and electronic properties
• Phonon-mediated exciton capture in Mo-based transition metal dichalcogenides
• Spatiotemporal dynamics of Coulomb-correlated carriers in semiconductors
• Hybrid dark excitons in monolayer ${MoS}_2$
• $WS{e}_2$ Monolayers Grown by Molecular Beam Epitaxy on hBN
• Spin dynamics of hot excitons in diluted magnetic semiconductors with spin-orbit interaction
• Role of excited states in the dynamics of excitons and their spins in diluted magnetic semiconductors
• Tracking the photoinduced dynamics of a dark excitonic state in single-layer WS${}_2$ via resonant Autler-Townes splitting
• Excitonic effects in the photocarriers dynamics of two-dimensional materials