Ultrafast Exciton and Trion Dynamics in High‐Quality Encapsulated MoS2 Monolayers

The extreme confinement and reduced screening in monolayer transition metal dichalcogenides (TMDs) leads to the appearance of tightly bound excitons which can also couple to free charges, forming trions, owing to strong Coulomb interactions. Low temperatures and encapsulation in hexagonal boron nitride (hBN) can narrow the excitonic linewidth, approaching the regime of homogeneous broadening, mostly dominated by the radiative decay. Ultrafast spectroscopy is a perfect tool to study exciton formation and relaxation dynamics in TMD monolayers. However, high-quality hBN-encapsulated structures have usually lateral sizes of the order of a few micrometers, calling for the combination of high spatial and temporal resolution in pump–probe experiments. Herein, a custom broadband pump–probe optical microscope is used to measure the ultrafast dynamics of neutral and charged excitons in high-quality hBN-encapsulated monolayer MoS2 at 8 K. Neutral excitons exhibit a narrow linewidth of 7.5 meV, approaching the homogeneous limit, which is related to the fast recombination time of ≈130 fs measured in pump–probe. Moreover, markedly different dynamics of the trions over the neutral ones are observed. The results provide novel insights on the exciton recombination processes in TMD monolayers, paving the way for exploring the ultrafast behavior of excitons and their many-body complexes in TMD heterostructures