Spin-valleytronics is a promising new paradigm in electronics. Besides the spins of electrons and holes, valleys in the electronic band structure of some materials may provide another robust identity for information processing. Transition-metal dichalcogenide (TMD) monolayers, exhibiting a layered graphene-like structure, have intrinsically strong spin-valley coupling, essential for harnessing this new physics. However, the quality of the monolayers available at present precludes their use in prototype devices. This proposal aims to alleviate this. As a first objective, methods for high-quality epitaxial TMD monolayer growth using Van der Waals epitaxy will be developed. We aim at (i) simultaneous control over crystallinity, lateral size and thickness, and (ii) all in-situ growth and characterization using state-of-the-art surface science techniques. Next, we will develop non-destructive surface capping, for ex-situ characterization/processing, and molecular charge transfer doping techniques. The latter uses organic donor/acceptor molecules to tune the charge carrier density in TMD monolayers. Last, coupled spin-valley phenomena will be studied in TMD monolayers, for the first time by all-electrical schemes. These tasks require different disciplines, well matched with the applicant’s unique, well-documented profile, combining experience in magnetism, (organic) semiconductors, hybrid interfaces, nanofabrication, and surface science- and magneto-transport techniques. The strong expertise of the outgoing host (National University of Singapore) ensures training in the specialist growth and doping techniques, which have been pioneered mainly in Asia. After transferring these skills to the European host (University of Twente), magnetotransport studies of nanoelectronic devices are enabled by the excellent infrastructure available there. This fellowship will provide the applicant with a new level of professional maturity, enhancing and diversifying his research career.