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 $(\hbar cQ)$ 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\pm0.17\ $meV, owing purely to finite radiative lifetime in the absence of non-radiative dephasing processes. As a direct consequence of the large radiative limit, we find a surprisingly large ($\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.