Origin of n-type conductivity of monolayer MoS2

Monolayer MoS2 is a promising two-dimensional material for electronic and optoelectronic devices. As-grown MoS2 is an n-type semiconductor, however, the origin of this unintentional doping is still not clear. Here, using hybrid density functional theory (DFT), we carried out an extensive study of often observed native point defects i.e., VS , VMo , VS2 , VMoS3 , VMoS6 , MoS2 , and S2Mo and found that none of them cause n-type doping. Specifically, S vacancy (VS ), which has been widely attributed to n-type conductivity, turns out to be an electron compensating centre. We report that hydrogen, which is almost always present in the growth environments, is most stable in its interstitial (Hi ) and H-S adatom forms in MoS2 and acts as a shallow donor provided the sample is grown under S-rich condition. Furthermore, they have high migration barrier (in excess of 1 eV), which would ensure their stability even at higher temperature and hence, lead to n-type conductivity.