Fundamental exciton linewidth broadening in monolayer transition metal dichalcogenides

摘要

Monolayer transition metal dichalcogenides (TMDS) are highly luminescent materials despite being sub-nanometer thick. This is due to the ultrashort (<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 (<(h)over bar>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 nonradiative components of the homogeneous exciton linewidth. We estimate a fundamental radiative linewidth of 1.54 +/- 0.17 meV, owing purely to finite radiative lifetime in the absence of nonradiative dephasing processes. As a direct consequence of the large radiative limit, we find a surprisingly large (similar to 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 nonradiative linewidth broadening at T = 0 K.