Intrinsic Lifetime of Higher Excitonic States in Tungsten Diselenide Monolayers

Abstract

The reduced dielectric screening in atomically thin transition metal dichalcogenides allows to study the hydrogen-like series of higher exciton states in optical spectra even at room temperature. The width of excitonic peaks provides information about the radiative decay and phonon-assisted scattering channels limiting the lifetime of these quasi-particles. While linewidth studies so far have been limited to the exciton ground state, encapsulation with hBN has recently enabled quantitative measurements of the broadening of excited exciton resonances. Here, we present a joint experiment-theory study combining microscopic calculations with spectroscopic measurements on the intrinsic linewidth and lifetime of higher exciton states in hBN-encapsulated WSe${}_2$ monolayers. Surprisingly, despite the increased number of scattering channels, we find both in theory and experiment that the linewidth of higher excitonic states is similar or even smaller compared to the ground state. Our microscopic calculations ascribe this behavior to a reduced exciton-phonon scattering efficiency for higher excitons due to spatially extended orbital functions.

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Cited by in corpus (35)

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• Dipolar and magnetic properties of strongly absorbing hybrid interlayer excitons in pristine bilayer MoS${}_2$
• Exciton lifetime and optical linewidth profile via exciton-phonon interactions: Theory and first-principles calculations for monolayer MoS${}_2$
• Exciton landscape in van der Waals heterostructures
• Autoionization and dressing of excited excitons by free carriers in monolayer WSe2
• Strain-dependent exciton diffusion in transition metal dichalcogenides
• Microscopic picture of electron-phonon interaction in two-dimensional halide perovskites
• Dark exciton-exciton annihilation in monolayer WSe${}_2$
• Temporal evolution of low-temperature phonon sidebands in WSe${}_2$ monolayers
• Electron recoil effect in electrically tunable MoSe2 monolayers
• Coherent dynamics and mapping of excitons in single-layer MoSe${}_2$ and WSe${}_2$ at the homogeneous limit
• Theoretical methods for excitonic physics in two-dimensional materials
• Band nesting and exciton spectrum in monolayer MoS${}_2$
• Ultrafast phonon-driven charge transfer in van der Waals heterostructures
• Strong coupling regime and hybrid quasinormal modes of a single plasmonic resonator coupled to a TMDC monolayer
• Trion photoluminescence and trion stability in atomically thin semiconductors
• Direct Observation of Intravalley Phonon Scattering of 2s Excitons in MoSe${}_2$ and WSe${}_2$ Monolayers
• Phonon-assisted Exciton Dissociation in Transition Metal Dichalcogenides
• Excitonic theory of doping-dependent optical response in atomically thin semiconductors
• Circumventing the polariton bottleneck via dark excitons in 2D semiconductors
• Theory of the Coherent Response of Magneto-Excitons and Magneto-Biexcitons in Monolayer Transition Metal Dichalcogenides
• Signatures of dark excitons in exciton-polariton optics of transition metal dichalcogenides
• Electromagnetic field assisted exciton diffusion in moiré superlattices
• Shaping Exciton Polarization Dynamics in 2D Semiconductors by Tailored Ultrafast Pulses
• Thermal effect on magnetoexciton energy spectra in monolayer transition metal dichalcogenides
• Bichromatic four-wave mixing and quadrature-squeezing from biexcitons in atomically thin semiconductor microcavities
• Doping-induced non-Markovian interference causes excitonic linewidth broadening in monolayer WSe${}_2$
• Polariton transport in 2D semiconductors: Phonon-mediated transitions between ballistic, superdiffusive and exciton-limited regimes
• Spectral asymmetry of phonon sideband luminescence in monolayer and bilayer WSe2
• Tracking the photoinduced dynamics of a dark excitonic state in single-layer WS${}_2$ via resonant Autler-Townes splitting
• Efficient quadrature-squeezing from biexcitonic parametric gain in atomically thin semiconductors
• Trion-phonon interaction in atomically thin semiconductors