Tuning electrical conductivity of semiconducting materials through substitutional doping is crucial for fabricating functional devices. This, however, has not been fully realized in two-dimensional (2D) materials due to the difficulty of homogeneously controlling the dopant concentrations and the lack of systematic study of the net impact of substitutional dopants separate from that of the unintentional doping from the device fabrication processes. Here, we grow wafer-scale, continuous MoS2 monolayers with tunable concentrations of Nb and Re and fabricate devices using a polymer-free approach to study the direct electrical impact of substitutional dopants in MoS2 monolayers. In particular, the electrical conductivity of Nb doped MoS2 in the absence of electrostatic gating is reproducibly tuned over 7 orders of magnitude by controlling the Nb concentration. Our study further indicates that the dopant carriers do not fully ionize in the 2D limit, unlike in their three-dimensional analogues, which is explained by weaker charge screening and impurity band conduction. Moreover, we show that the dopants are stable, which enables the doped films to be processed as independent building blocks that can be used as electrodes for functional circuitry.
This work was supported by the Air Force Office of Scientific Research (FA9550-16-1-0031 and FA9550-16-1-0347), the Samsung Advanced Institute of Technology, and the National Science Foundation (NSF) through the Cornell Center for Materials Research with funding from the NSF Materials Research Science and Engineering Centers (MRSEC) program (DMR-1719875) and the University of Chicago MRSEC (NSF DMR-1420709). We also acknowledge funding from the Department of Energy through the EFRC for novel pathways to quantum coherence in materials. K.-H.L. acknowledges support by the Ministry of Education of Taiwan through the Government Scholarship to Study Abroad. F.M. acknowledges support by the National Science Foundation Graduate Research Fellowship Program under grant no. DGE-1746045.