Here we repair the single-layer MoSe2 field-effect transistors by the EDTA processing, after which the devices room-temperature carrier mobility increases from 0.1 to over 70cm2/Vs. The atomic dynamics is constructed by the combined study of the first-principle calculation, aberration-corrected transmission electron microscopy and Raman spectroscopy. Single/double Se vacancies are revealed originally, which cause some mid-gap impurity states and localize the device carriers. They are found repaired with the result of improved electronic transport. Such a picture is confirmed by a 1.5cm-1 red shift in the Raman spectra.
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