Low-temperature photoluminescence (PL) of hBN-encapsulated monolayer tungsten diselenide (WSe2) shows a multitude of sharp emission peaks below the bright exciton. Some of them have been recently identified as phonon sidebands of momentum-dark states. However, the exciton dynamics behind the emergence of these sidebands has not been revealed yet. In this joint theory-experiment study, we theoretically predict and experimentally observe time-resolved PL providing microscopic insights into thermalization of hot excitons formed after optical excitation. In good agreement between theory and experiment, we demonstrate a spectral red-shift of phonon sidebands on a timescale of tens of picoseconds reflecting the phonon-driven thermalization of hot excitons in momentum-dark states. Furthermore, we predict the emergence of a transient phonon sideband that vanishes in the stationary PL. The obtained microscopic insights are applicable to a broad class of 2D materials with multiple exciton valleys.
@article{arxiv.2006.09951,
title = {Temporal evolution of low-temperature phonon sidebands in WSe$_2$ monolayers},
author = {Roberto Rosati and Samuel Brem and Raül Perea-Causín and Koloman Wagner and Edith Wietek and Jonas Zipfel and Malte Selig and Takashi Taniguchi and Kenji Watanabe and Andreas Knorr and Alexey Chernikov and Ermin Malic},
journal= {arXiv preprint arXiv:2006.09951},
year = {2020}
}