Abstract
Chemical vapor deposition (CVD) allows growing transition metal dichalcogenides (TMDs) over large surface areas on inexpensive substrates. In this work, we correlate the structure of CVD grown MoS2 monolayers (MLs) on SiO2/Si wafers studied by high-resolution transmission electron microscopy (HRTEM) with the optical quality revealed in optical emission and absorption from cryogenic to ambient temperatures. We determine a defect concentration of the order of 1013 cm−2 for our samples with HRTEM. To have access to the intrinsic optical quality of the MLs, we remove the MLs from the SiO2 growth substrate and encapsulate them in hBN flakes with low defect density, to reduce the detrimental impact of dielectric disorder. We show optical transition linewidth of 5 meV at low temperature (T = 4 K) for the free excitons in emission and absorption. This is comparable to the best ML samples obtained by mechanical exfoliation of bulk material. The CVD grown MoS2 ML photoluminescence is dominated by free excitons and not defects even at low temperature. High optical quality of the samples is further confirmed by the observation of excited exciton states of the Rydberg series. We optically generate valley coherence and valley polarization in our CVD grown MoS2 layers, showing the possibility for studying spin and valley physics in CVD samples of large surface area.
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