Electronic Structure Mosaicity of Monolayer Transition Metal Dichalcogenides by Spontaneous Pattern Formation of Donor Molecules

Modulating the electronic structure of semiconducting materials is critical to developing high-performance electronic and optical devices. Transition metal dichalcogenides (TMDCs) are atomically thin semiconducting materials. However, before they can be used successfully in electronic and optical devices, modulation of their carrier concentration at the nanometer scale must be achieved. Molecular doping has been successful in modulating the carrier concentration; however, the scientific approach for selective and local carrier doping at the nanometer scale is still missing. Here, we demonstrate a proof-of-concept of modulating the carrier concentration of TMDCs laterally on a scale of around 100 nm using spontaneous pattern formation of an ultrathin film consisting of molecular electron dopants. When the water made contact with the molecular film (∼10 nm), a spontaneous pattern formation was observed on both the monolayer and bulk TMDCs. We revealed that the pattern-formation dynamics and nanoscopic flow rate of the molecules were highly dependent on the thickness of the TMDCs, since the band gap varies based on the number of layers. Analyses of topographic images of the molecular patterns and photoluminescence spectra of the TMDCs indicated that the spontaneously patterned molecular films induced a local carrier doping. Our results demonstrate a spontaneous formation of a mosaic electronic structure. This work is useful for making tiny-scale electronic junctions on TMDCs and semiconducting materials to make numerous p/n junctions simultaneously for optoelectronic devices.