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Scientific curiosity to uncover original optical properties and functionalities of atomically thin semiconductors, stemming from unusual Coulomb interactions in the two-dimensional geometry and multi-valley band structure, drives the research on monolayers of transition metal dichalcogenides (TMDs). While recent works ascertained the exotic energetic schemes of exciton complexes in TMDs, we here employ four-wave mixing microscopy to indicate that their subpicosecond dynamics is determined by the surrounding disorder. Focusing on a monolayer WS$_2$, we observe that exciton coherence is lost primarily due to interaction with phonons and relaxation processes towards optically dark excitonic states. Notably, when temperature is low and disorder weak excitons large coherence volume results in huge oscillator strength, allowing to reach the regime of radiatively limited dephasing and we observe long valley coherence. We thus elucidate the crucial role of exciton environment in the TMDs on its dynamics and show that revealed mechanisms are ubiquitous within that family.

Impact of environment on dynamics of exciton complexes in a WS 2 monolayer

Impact of environment on dynamics of exciton complexes in a WS ₂ monolayer