Intrinsic Exciton Linewidth in Monolayer Transition Metal Dichalcogenides

Abstract

Monolayer transition metal dichalcogenides feature Coulomb-bound electron-hole pairs (excitons) with exceptionally large binding energy and coupled spin and valley degrees of freedom. These unique attributes have been leveraged for electrical and optical control of excitons for atomically-thin optoelectronics and valleytronics. The development of such technologies relies on understanding and quantifying the fundamental properties of the exciton. A key parameter is the intrinsic exciton homogeneous linewidth, which reflects irreversible quantum dissipation arising from system (exciton) and bath (vacuum and other quasiparticles) interactions. Using optical coherent two-dimensional spectroscopy, we provide the first experimental determination of the exciton homogeneous linewidth in monolayer transition metal dichalcogenides, specifically tungsten diselenide (WSe2). The role of exciton-exciton and exciton-phonon interactions in quantum decoherence is revealed through excitation density and temperature dependent linewidth measurements. The residual homogeneous linewidth extrapolated to zero density and temperature is ~1.5 meV, placing a lower bound of approximately 0.2 ps on the exciton radiative lifetime. The exciton quantum decoherence mechanisms presented in this work are expected to be ubiquitous in atomically-thin semiconductors.

References in corpus (9)

• Exciton Binding Energy and Nonhydrogenic Rydberg Series in Monolayer WS2
• Observation of Long-Lived Interlayer Excitons in Monolayer MoSe2-WSe2 Heterostructures
• Tightly bound excitons in monolayer WSe2
• Strong light-matter coupling in two-dimensional atomic crystals
• Non-linear Optical Spectroscopy of Excited Exciton States for Efficient Valley Coherence Generation in WSe2 Monolayers
• Valley dynamics probed through charged and neutral exciton emission in monolayer WSe2
• Radiative Lifetimes of Excitons and Trions in Monolayers of Metal Dichalcogenide MoS2
• Coherent Electronic Coupling in Atomically Thin MoSe2
• Two-dimensional metal-chalcogenide films in tunable optical microcavities

Cited by in corpus (204)

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• Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides
• Exciton Radiative Lifetime in Transition Metal Dichalcogenide Monolayers
• Two-dimensional semiconductors in the regime of strong light-matter coupling
• Direct Measurement of Exciton Valley Coherence in Monolayer WSe${}_2$
• Observation of tunable charged exciton polaritons in hybrid monolayer WS2 $-$ plasmonic nanoantenna system
• Ultrafast Manipulation of Valley Pseudospin
• Atomically thin mirrors made of monolayer semiconductors
• Trion Formation Dynamics in Monolayer Transition Metal Dichalcogenides
• Valley-Polarized Exciton-Polaritons in a Monolayer Semiconductor
• Dark excitons in transition metal dichalcogenides
• Hybrid tip-enhanced nano-spectroscopy and -imaging of monolayer WSe2 with local strain control
• Van der Waals Heterostructure Polaritons with moiré-Induced Nonlinearity
• Two-dimensional Fröhlich interaction in transition-metal dichalcogenide monolayers: Theoretical modeling and first-principles calculations
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• Exciton Dynamics in Monolayer Transition Metal Dichalcogenides
• Enhanced Light-Matter Interaction in Two-Dimensional Transition Metal Dichalcogenides
• Perspective: Exciton polarons in two-dimensional hybrid metal-halide perovskites
• Phonon Sidebands in Transition Metal Dichalcogenides
• Phonon-assisted Photoluminescence from Dark Excitons in Monolayers of Transition Metal Dichalcogenides
• A- and B-Exciton Photoluminescence Intensity Ratio as a Measure of Sample Quality for Transition Metal Dichalcogenide Monolayers
• Control of the Exciton Radiative Lifetime in van der Waals Heterostructures
• Direct exciton emission from atomically thin transition metal dichalcogenide heterostructures near the lifetime limit
• Enabling valley selective exciton scattering in monolayer WSe${}_2$ through upconversion
• Electrically tunable valley dynamics in twisted WSe${}_2$/WSe${}_2$ bilayers
• Exciton-phonon coupling in MoSe2 monolayers
• Highly nonlinear trion-polaritons in a monolayer semiconductor
• Exciton-plasmon Coupling and Electromagnetically Induced Transparency in Monolayer Semiconductors Hybridized with Ag Nanoparticles
• Theory of Two-Dimensional Spatially Indirect Equilibrium Exciton Condensates
• Directional Interlayer Spin-Valley Transfer in Two-Dimensional Heterostructures
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• Quantum interference in second-harmonic generation from monolayer WSe2
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• Accessing high optical quality of MoS2 monolayers grown by chemical vapor deposition
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• Unusual Exciton-Phonon Interactions at van der Waals Engineered Interfaces
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• Guide to optical spectroscopy of layered semiconductors
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• Exciton Trapping Is Responsible for the Long Apparent Lifetime in Acid-Treated MoS2
• Strongly coupled coherent phonons in single-layer MoS${}_2$
• The valley Zeeman effect in inter- and intra-valley trions in monolayer WSe${}_2$
• Controlling excitons in an atomically thin membrane with a mirror
• 2D Semiconductor Nonlinear Plasmonic Modulators
• Valley Polarization in Size-Tunable Monolayer Semiconductor Quantum Dots
• Condensation signatures of photogenerated interlayer excitons in a van der Waals heterostack
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• Probing Many-Body Interactions in Monolayer Transition-Metal Dichalcogenides
• Roadmap for Photonics with 2D Materials
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• Dynamical screening in monolayer transition-metal dichalcogenides and its manifestations in the exciton spectrum
• Mapping of the dark exciton landscape in transition metal dichalcogenides
• Many-Body Simulation of Two-Dimensional Electronic Spectroscopy of Excitons and Trions in Monolayer Transition-Metal Dichalcogenides
• Valley Trion Dynamics in Monolayer MoSe${}_2$
• Phonon-assisted oscillatory exciton dynamics in monolayer MoSe2
• Exciton-phonon coupling strength in single-layer MoSe2 at room temperature
• Exciton-polaron interactions in monolayer WS${}_2$
• Bright excitons with negative-mass electrons
• Monolayer MoSe2: A candidate for room temperature polaritonics
• Inter-valley dark trion states with spin lifetimes of 150 ns in WSe${}_2$
• Quantum Nonlinear Optics in Atomically Thin Materials
• Trion Valley Coherence in Monolayer Semiconductors
• Resonant photovoltaic effect in doped magnetic semiconductors
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• 2D Magnetic Semiconductors via Substitutional Doping of Transition Metal Dichalcogenides
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• Momentum-Resolved Exciton Coupling and Valley Polarization Dynamics in Monolayer WS${}_2$
• Enhanced screening and spectral diversity in many-body elastic scattering of excitons in two-dimensional hybrid metal-halide perovskites
• Theory of optically induced Förster Coupling in van der Waals coupled Heterostuctures
• Theory of absorption lineshape in monolayers of transition metal dichalcogenides
• Nonequilibrium Carrier Dynamics in Transition Metal Dichalcogenide Semiconductors
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• Engineering Effects of Vacuum Fluctuations on Two-dimensional Semiconductors
• Spin States Protected from Intrinsic Electron-Phonon-Coupling Reaching 100 ns Lifetime at Room Temperature in MoSe${}_2$
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• Chiral light-matter interactions using spin-valley states in transition metal dichalcogenides
• Coherent dynamics and mapping of excitons in single-layer MoSe${}_2$ and WSe${}_2$ at the homogeneous limit
• Coherent exciton-exciton interactions and exciton dynamics in a MoSe\textsubscript{2}/WSe\textsubscript{2} heterostructure
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• Dark-exciton based strain sensing in transition metal dichalcogenides
• Imaging dynamic exciton interactions and coupling in transition metal dichalcogenides
• Optical nonlinearities of excitons in monolayer MoS2
• Nonlinear optics in 2D materials: from classical to quantum
• Fast phase cycling in non-collinear optical two-dimensional coherent spectroscopy
• Separating Pathways in Double-Quantum Optical Spectroscopy Reveals Excitonic Interactions
• Optical fingerprint of dark 2p-states in transition metal dichalcogenides
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• Ultrafast photocurrents in MoSe${}_2$ probed by terahertz spectroscopy
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• A colloquium on the variational method applied to excitons in 2D materials
• Strong light-matter coupling in MoS${}_2$
• Stochastic scattering theory for excitation induced dephasing: Time-dependent nonlinear coherent exciton lineshapes
• Mott-moiré excitons
• Disorder Dependent Valley Properties in Monolayer WSe2
• MoTe2 as a natural hyperbolic material across the visible and the ultraviolet region
• Magneto-optical chirality in a coherently coupled exciton-plasmon system
• Direct Optical-Structure Correlation in Atomically Thin Dichalcogenides and Heterostructures
• Microscopic model of the doping dependence of line widths in monolayer transition metal dichalcogenides
• Phonon signatures in spectra of exciton polaritons in transition metal dichalcogenides
• Negative Compressibility in Graphene-terminated Black Phosphorus Heterostructures
• Radiative and Non-Radiative Exciton Energy Transfer in Monolayers of Two-Dimensional Transition Metal Dichalcogenides
• Theory of coherent phonons coupled to excitons
• Phonon-assisted Exciton Dissociation in Transition Metal Dichalcogenides
• Homogeneous optical linewidths in hybrid Ruddlesden-Popper metal halides can only be measured using nonlinear spectroscopy
• Excitonic magneto-optics in monolayer transition metal dichalcogenides: From nanoribbons to two-dimensional response
• Electroluminescence as a probe of strong exciton-plasmon coupling in few-layer WSe2
• Dark-state impact on the exciton recombination of WS2 monolayers as revealed by multi-time-scale pump-and-probe spectroscopy
• Thermalization of photoexcited carriers in two-dimensional transition metal dichalcogenides and internal quantum efficiency of van der Waals heterostructures
• Valley Coherent Hot Carriers and Thermal Relaxation in Monolayer Transition Metal Dichalcogenides
• Rapid multiplex ultrafast nonlinear microscopy for material characterization
• Enhanced exciton-exciton collisions in an ultra-flat monolayer MoSe2 prepared through deterministic flattening
• Pump-triple sum-frequency-probe spectroscopy of transition metal dichalcogenides
• The Optical Signatures of Stochastic Processes in Many-Body Exciton Scattering
• Multidimensional Spectroscopy of Time-Dependent Impurities in Ultracold Fermions
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• Photonics in Flatland: Challenges and Opportunities for Nanophotonics with 2D Semiconductors
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• Dephasing of Strong-Field-Driven Floquet States Revealed by Time- and Spectrum-Resolved Quantum-Path Interferometry
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• Edge states and spin-valley edge photocurrent in transition metal dichalcogenide monolayers
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• Broadband Optical Two-Dimensional Coherent Spectroscopy of a Rubidium Atomic Vapor
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• The Importance of Pure Dephasing in the Optical Response of Excitons in High-quality van der Waals Heterostructures
• Coherence and de-coherence in the Time-Resolved ARPES of realistic materials: an ab-initio perspective
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• Effect of electron-irradiation on layered quantum materials
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• Spin dependent analysis of homogeneous and inhomogeneous exciton decoherence in magnetic fields
• Mixed quantum-classical modeling of exciton-phonon scattering in solids: Application to optical linewidths of monolayer MoS2
• Phonon-mediated exciton capture in Mo-based transition metal dichalcogenides
• Non-Hermitian theory of valley excitons in two-dimensional semiconductors
• Observing Quantum Coherent Oscillations in a Three-Level Atoms via Electromagnetically Induced Transparency by Two-Dimensional Spectroscopy
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• Exciton-exciton Interactions -- A Quantitative Comparison Between Complimentary Phenomenological Models
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• Approaching the Intrinsic Photoluminescence Linewidth in Transition Metal Dichalcogenide Monolayers
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• Dynamics of resonantly excited excitons in MoSe${}_2$ and WS${}_2$ single-layers monitored with four-wave mixing
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• Interlayer Coupling Effect in van der Waals Heterostructures of Transition Metal Dichalcogenides
• Floquet engineering in the presence of optically excited carriers
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• Valley-controlled many-body exciton interactions in monolayer WSe${}_2$ phototransistors