Intrinsic Exciton Linewidth in Monolayer Transition Metal Dichalcogenides

TL;DR

This paper experimentally determines the intrinsic exciton homogeneous linewidth in monolayer WSe2 using two-dimensional spectroscopy, revealing fundamental decoherence mechanisms and setting bounds on exciton lifetime in atomically-thin semiconductors.

Contribution

First experimental measurement of the intrinsic exciton homogeneous linewidth in monolayer transition metal dichalcogenides using optical coherent spectroscopy.

Findings

Residual linewidth ~1.5 meV at zero density and temperature

Exciton-exciton and exciton-phonon interactions influence decoherence

Lower bound of exciton radiative lifetime ~0.2 ps

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.