ArXiv · 2026
Transition metal dichalcogenide monolayers are promising materials for electronic and photonic applications, yet the performance of chemical vapour deposition grown films is severely limited by native sulphur vacancies that introduce mid-gap trap states, degrade carrier mobility, and elevate electrical noise. Here we investigate octane thiol passivation of sulphur vacancies in monolayer MoS2 field effect transistors, combining x-ray photoelectron spectroscopy, photoluminescence, and Raman scattering with electrical transport and optically coupled low-frequency noise spectroscopy. Thiol treatment reduces the sulphur vacancy concentration from 7.5% to 5%, which increases the channel resistance 35-fold while restoring gate switching with an on/off ratio of 10^4 and improving field-effect mobility from 1 to 5 cm^2/Vs. Low frequency noise spectroscopy directly quantifies the defect suppression: the Hooge parameter drops by more than two orders of magnitude after passivation. Gate-dependent noise confirms carrier mobility fluctuation as the dominant dark noise mechanism, while optical excitation drives a crossover to carrier number fluctuation dominated noise, reflecting preferential interaction of photogenerated carriers with residual vacancy states via generation-recombination trapping, a mechanistic distinction inaccessible to gate- bias measurements alone. Density functional theory calculations corroborate these findings, showing suppression of vacancy-induced mid-gap states by more than 50% and partial restoration of the intrinsic bandgap. These results establish optically coupled low-frequency noise spectroscopy as a sensitive, low-cost, and non-destructive tool for quantifying defect passivation in TMDC-based devices.
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