arXiv · 2209.08707
Phonon-assisted inter-valley scattering determines ultrafast exciton dynamics in MoSe$_2$ bilayers
Abstract
While valleys (energy extrema) are present in all band structures of solids, their preeminent role in determining exciton resonances and dynamics in atomically thin transition metal dichalcogenides (TMDC) is unique. Using two-dimensional coherent electronic spectroscopy, we find that exciton decoherence occurs on a much faster time scale in MoSe$_2$ bilayers than that in the monolayers. We further identify two population relaxation channels in the bilayer, a coherent and an incoherent one. Our microscopic model reveals that phonon-emission processes facilitate scattering events from the $K$ valley to other lower energy $\Gamma$ and $\Lambda$ valleys in the bilayer. Our combined experimental and theoretical studies unequivocally establish different microscopic mechanisms that determine exciton quantum dynamics in TMDC monolayers and bilayers. Understanding exciton quantum dynamics provides critical guidance to manipulation of spin/valley degrees of freedom in TMDC bilayers.
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Sophia Helmrich, Kevin Sampson, Di Huang, Malte Selig, Kai Hao, Kha Tran, Alexander Achstein, Carter Young, Andreas Knorr, Ermin Malic, Ulrike Woggon, Nina Owschimikow, Xiaoqin Li. 2022-09-19. Phonon-assisted inter-valley scattering determines ultrafast exciton dynamics in MoSe$_2$ bilayers. https://doi.org/10.1103/physrevlett.127.157403
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