Controlled Doping of Vacancy-Containing Few-Layer MoS2 via Highly Stable Thiol-Based Molecular Chemisorption

Abstract

MoS2 is considered a promising two-dimensional active channel material for future nanoelectronics. However, the development of a facile, reliable, and controllable doping methodology is still critical for extending the applicability of MoS2. Here, we report surface charge transfer doping via thiol-based binding chemistry for modulating the electrical properties of vacancy-containing MoS2 (v-MoS2). Although vacancies present in 20 materials are generally regarded as undesirable components, we show that the electrical properties of MoS2 can be systematically engineered by exploiting the tight binding between the thiol group and sulfur vacancies and by choosing different functional groups. For example, we demonstrate that NH2-containing thiol molecules with lone electron pairs can serve as an n-dopant and achieve a substantial increase of electron density (Delta n = 3.7 x 10(12) cm(-2)) On the other hand, fluorine-rich molecules can provide a p-doping effect (Delta n = -7.0 x 10(11) cm(-2)) due to its high electronegativity. Moreover, the n- and p-doping effects were systematically evaluated by photoluminescence (PL), X-ray photoelectron spectroscopy (XPS), and electrical measurement results. The excellent binding stability of thiol molecules and recovery properties by thermal annealing will enable broader applicability of ultrathin MoS2 to various devices.