Fundamental Limits of Exciton-Exciton Annihilation for Light Emission in Transition Metal Dichalcogenide Monolayers

Abstract

We quantitatively illustrate the fundamental limit that exciton-exciton annihilation (EEA) may impose to the light emission of monolayer transition metal dichalcogenide (TMDC) materials. The EEA in TMDC monolayers shows dependence on the interaction with substrates as its rate increases from 0.1 cm2/s (0.05 cm2/s) to 0.3 cm2/s (0.1 cm2/s) with the substrates removed for WS2 (MoS2) monolayers. It turns to be the major pathway of exciton decay and dominates the luminescence efficiency when the exciton density is beyond 1010 cm-2 in suspended monolayers or 1011 cm-2 in supported monolayers. This sets an upper limit on the density of injected charges in light emission devices for the realization of optimal luminescence efficiency. The strong EEA rate also dictates the pumping threshold for population inversion in the monolayers to be 12-18 MW/cm2 (optically) or 2.5-4x105 A/cm2 (electrically).

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Cited by in corpus (52)

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• Enabling valley selective exciton scattering in monolayer WSe${}_2$ through upconversion
• Observation of exciton redshift-blueshift crossover in monolayer WS2
• Exciton diffusion in monolayer semiconductors with suppressed disorder
• Inhibited nonradiative decay at all exciton densities in monolayer semiconductors
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• Collective Excitations in 2D Materials
• Room-Temperature Electron-Hole Liquid in Monolayer MoS2
• Upconverted electroluminescence via Auger scattering of interlayer excitons in van der Waals heterostructures
• Ultra-low power threshold for laser induced changes in optical properties of 2D Molybdenum dichalcogenides
• Direct versus indirect band gap emission and exciton-exciton annihilation in atomically thin molybdenum ditelluride (MoTe${}_2$)
• Exciton states in monolayer MoSe2 and MoTe2 probed by upconversion spectroscopy
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• Nonequilibrium Lattice Dynamics in Monolayer MoS2
• Excitonic emission of monolayer semiconductors near-field coupled to high-Q microresonators
• Boosting quantum yields in 2D semiconductors via proximal metal plates
• Many-body effects in nonlinear optical responses of 2D layered semiconductors
• Enhancing Multifunctionalities of Transition Metal Dichalcogenide Monolayers via Intercalation of Molecules and Ions
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• Auger recombination of dark excitons in $\mathrm{W}{\mathrm{S}}_2$ and $\mathrm{WS}{\mathrm{e}}_2$ monolayers
• Optical control of valley Zeeman effect through many-exciton interactions
• Dark exciton-exciton annihilation in monolayer WSe${}_2$
• Harnessing Exciton-Exciton Annihilation in Two-Dimensional Semiconductors
• Microscopic origin of anomalous interlayer exciton transport in van der Waals heterostructures
• Spin/valley coupled dynamics of electrons and holes at the ${\text{MoS}}_2-{\text{MoSe}}_2$ interface
• Nonlinear optics in 2D materials: from classical to quantum
• Ultrafast photocurrents in MoSe${}_2$ probed by terahertz spectroscopy
• Resonantly excited exciton dynamics in two-dimensional MoSe${}_2$ monolayers
• Ultrafast photocurrent and absorption microscopy of few-layer TMD devices isolate rate-limiting dynamics driving fast and efficient photoresponse
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• Incoherent phonon population and exciton-exciton annihilation in monolayer WS2 revealed by time-resolved spontaneous Raman scattering
• Photophysical comparison of liquid and mechanically exfoliated WS${}_2$ monolayers
• Controlling exciton dynamics in two-dimensional MoS2 on hyperbolic metamaterial-based nanophotonic platform
• Thermalization of photoexcited carriers in two-dimensional transition metal dichalcogenides and internal quantum efficiency of van der Waals heterostructures
• Tuning exciton recombination rates in doped transition metaldichalcogenides
• Dark-state impact on the exciton recombination of WS2 monolayers as revealed by multi-time-scale pump-and-probe spectroscopy
• Fermi Liquid Theory Sheds Light on "Hot" EHL in 1L-MoS${}_2$
• Exciton-Sensitized Second-Harmonic Generation in 2D Heterostructures
• Self-Induced Valley Bosonic Stimulation of Exciton-Polaritons in a Monolayer Semiconductor
• Exciton diffusion and annihilation in nanophotonic Purcell landscapes
• Quantized exciton-exciton annihilation in monolayer WS2 on SrTiO3 substrates with atomically flat terraces
• Dynamic screening of quasiparticles in WS${}_2$ monolayers
• Onset of exciton-exciton annihilation in single layer black phosphorus
• Nonexponential photoluminescence dynamics in an inhomogeneous ensemble of excitons in WSe${}_2$ monolayers
• Exciton Mott Transition in Two-Dimensional Semiconductors
• Microscopic Theory of Exciton-Exciton Annihilation in Two-Dimensional Semiconductors
• Two-dimensional Ga${}_2$O${}_3$ glass: a large scale passivation and protection material for monolayer WS${}_2$
• Excitonic Transport and Intervalley Scattering in Exfoliated MoSe2 Monolayer Revealed by Four-Wave-Mixing Transient Grating Spectroscopy