Fundamental exciton linewidth broadening in monolayer transition metal dichalcogenides

Abstract

Monolayer Transition Metal Dichalcogenides (TMDS) are highly luminescent materials despite being sub-nanometer thick due to the ultra-short ($<1$ ps) radiative lifetime of the strongly bound bright excitons hosted by these materials. The intrinsically short radiative lifetime results in a large broadening in the exciton band with a magnitude that is about two orders greater than the spread of the light cone itself. The situation calls for a need to revisit the conventional light cone picture. We present a modified light cone concept which places the light line $(\hslash cQ)$ as the generalized lower bound for allowed radiative recombination. A self-consistent methodology, which becomes crucial upon inclusion of large radiative broadening in the exciton band, is proposed to segregate the radiative and the non-radiative components of the homogeneous exciton linewidth. We estimate a fundamental radiative linewidth of $1.54\pm 0.17$meV, owing purely to finite radiative lifetime in the absence of non-radiative dephasing processes. As a direct consequence of the large radiative limit, we find a surprisingly large ($\sim 0.27$ meV) linewidth broadening due to zero-point energy of acoustic phonons. This obscures the precise experimental determination of the intrinsic radiative linewidth and sets a fundamental limit on the non-radiative linewidth broadening at $T=0$ K.

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• Layer degree of freedom for excitons in transition metal dichalcogenides
• Imaging dynamic exciton interactions and coupling in transition metal dichalcogenides
• Strong Single- and Two-Photon Luminescence Enhancement by Nonradiative Energy Transfer across Layered Heterostructure
• Anomalous Stark Shift of Excitonic Complexes in Monolayer Semiconductor
• Exciton-exciton interactions in van der Waals heterobilayers
• Observation of ~100% valley-coherent excitons in monolayer MoS2 through giant enhancement of valley coherence time
• Probing biexciton in monolayer WS${}_2$ through controlled many-body interaction
• Coupling of MoS${}_2$ Excitons with Lattice Phonons and Cavity Vibrational Phonons in Hybrid Nanobeam Cavities
• Exciton diffusion in a hBN-encapsulated monolayer MoSe2
• Trion-trion annihilation in monolayer WS${}_2$
• Spectrally tunable, large Raman enhancement from nonradiative energy transfer in van der Waals heterostructure
• Gate-tunable trion switch for excitonic device applications
• Valley-exchange coupling probed by angle-resolved photoluminescence
• Motion of 2D exciton in momentum space leads to pseudospin distribution narrowing on the Bloch Sphere