Hole Transport in Exfoliated Monolayer MoS2

Ideal monolayers of common semiconducting transition metal dichalcogenides (TMDCs) such as MoS2, WS2, MoSe2, and WSe2 possess many similar electronic properties. As it is the case for all semiconductors, however, the physical response of these systems is strongly determined by defects in a way specific to each individual compound. Here we investigate the ability of exfoliated monolayers of these TMDCs to support high-quality, well-balanced ambipolar conduction, which has been demonstrated for WS2, MoSe2, and WSe2, but not for MoS2. Using ionic-liquid gated transistors, we show that, contrary to WS2, MoSe2, and WSe2, hole transport in exfoliated MoS2 monolayers is systematically anomalous, exhibiting a maximum in conductivity at negative gate voltage (V-G) followed by a suppression of up to 100 times upon further increasing V-G. To understand the origin of this difference, we have performed a series of experiments including the comparison of hole transport in MoS2 monolayers and thicker multilayers, in exfoliated and CVD-grown monolayers, as well as gate-dependent optical measurements (Raman and photoluminescence) and scanning tunneling imaging and spectroscopy. In agreement with existing ab initio calculations, the results of all these experiments are consistently explained in terms of defects associated with chalcogen vacancies that only in MoS2 monolayers, but not in thicker MoS2 multilayers nor in monolayers of the other common semiconducting TMDCs, create in-gap states near the top of the valence band that act as strong hole traps. Our results demonstrate the importance of studying systematically how defects determine the properties of 2D semiconducting materials and of developing methods to control them.