Hydrogen-Assisted Growth of Large-Area Continuous Films of MoS2 on Monolayer Graphene.

We show how control over the chemical vapor deposition (CVD) reaction chemistry of molybdenum disulfide (MoS2) by hydrogen addition can enable the direct growth of centimeter-scale continuous films of vertically stacked MoS2 monolayer on graphene under atmospheric pressure conditions. Hydrogen addition enables longer CVD growth times at high temperature by reducing oxidation effects that would otherwise degrade the monolayer graphene. By careful control of nucleation density and growth time, high-quality monolayer MoS2 films could be formed on graphene, realizing all CVD-grown vertically stacked monolayer semimetal/semiconducting interfaces. Photoluminescence spectroscopy shows quenching of MoS2 by the underlying graphene, indicating a good interfacial charge transfer. We utilize the MoS2/graphene vertical stacks as photodetectors, with photoresponsivities reaching 2.4 A/W under 135 μW 532 nm illumination. This approach provides insights into the scalable manufacturing of high-quality two-dimensional electronic and optoelectronic devices.